K Gottschling, G Savasci, H Vignolo-Gonzalez, S Schmidt, P Mauker, T Banerjee, P Rovo, C Ochsenfeld, B V Lotsch
Rational Design of Covalent Cobaloxime-Covalent Organic Framework Hybrids for Enhanced Photocatalytic Hydrogen Evolution Journal Article
In: Journal of the American Chemical Society, vol. 142, no. 28, pp. 12146-12156, 2020, ISSN: 0002-7863.
Abstract | Links | Tags: Foundry Organic
@article{,
title = {Rational Design of Covalent Cobaloxime-Covalent Organic Framework Hybrids for Enhanced Photocatalytic Hydrogen Evolution},
author = {K Gottschling and G Savasci and H Vignolo-Gonzalez and S Schmidt and P Mauker and T Banerjee and P Rovo and C Ochsenfeld and B V Lotsch},
url = {\<Go to ISI\>://WOS:000551495700030},
doi = {10.1021/jacs.0c02155},
issn = {0002-7863},
year = {2020},
date = {2020-07-15},
journal = {Journal of the American Chemical Society},
volume = {142},
number = {28},
pages = {12146-12156},
abstract = {Covalent organic frameworks (COFs) display a unique combination of chemical tunability, structural diversity, high porosity, nanoscale regularity, and thermal stability. Recent efforts are directed at using such frameworks as tunable scaffolds for chemical reactions. In particular, COFs have emerged as viable platforms for mimicking natural photosynthesis. However, there is an indisputable need for efficient, stable, and economical alternatives for the traditional platinum-based cocatalysts for light-driven hydrogen evolution. Here, we present azide-functionalized chloro(pyridine)cobaloxime hydrogen-evolution cocatalysts immobilized on a hydrazone-based COF-42 backbone that show improved and prolonged photocatalytic activity with respect to equivalent physisorbed systems. Advanced solid-state NMR and quantum-chemical methods allow us to elucidate details of the improved photoreactivity and the structural composition of the involved active site. We found that a genuine interaction between the COF backbone and the cobaloxime facilitates recoordination of the cocatalyst during the photoreaction, thereby improving the reactivity and hindering degradation of the catalyst. The excellent stability and prolonged reactivity make the herein reported cobaloxime-tethered COF materials promising hydrogen evolution catalysts for future solar fuel technologies.},
keywords = {Foundry Organic},
pubstate = {published},
tppubtype = {article}
}
R M Kluge, N Saxena, W Chen, V Korstgens, M Schwartzkopf, Q Zhong, S V Roth, P Muller-Buschbaum
Doping Dependent In-Plane and Cross-Plane Thermoelectric Performance of Thin n-Type Polymer P(NDI2OD-T2) Films Journal Article
In: Advanced Functional Materials, vol. 30, no. 28, 2020, ISSN: 1616-301X.
Abstract | Links | Tags: Foundry Organic, Solid-Solid
@article{,
title = {Doping Dependent In-Plane and Cross-Plane Thermoelectric Performance of Thin n-Type Polymer P(NDI2OD-T2) Films},
author = {R M Kluge and N Saxena and W Chen and V Korstgens and M Schwartzkopf and Q Zhong and S V Roth and P Muller-Buschbaum},
url = {\<Go to ISI\>://WOS:000535017100001},
doi = {10.1002/adfm.202003092},
issn = {1616-301X},
year = {2020},
date = {2020-07-09},
urldate = {2020-07-09},
journal = {Advanced Functional Materials},
volume = {30},
number = {28},
abstract = {Thermoelectric generators pose a promising approach in renewable energies as they can convert waste heat into electricity. In order to build high efficiency devices, suitable thermoelectric materials, both n- and p-type, are needed. Here, the n-type high-mobility polymer poly[N,N '-bis(2-octyldodecyl)naphthalene-1,4,5,8-bis(dicarboximide)-2,6-diyl]-alt-5,5 '-(2,2 '-bithiophene) (P(NDI2OD-T2)) is focused upon. Via solution doping with 4-(1,3-dimethyl-2,3-dihydro-1H-benzoimidazol-2-yl)-N,N-diphenylaniline (N-DPBI), a maximum power factor of (1.84 +/- 0.13) mu W K-2 m(-1) is achieved in an in-plane geometry for 5 wt% dopant concentration. Additionally, UV-vis spectroscopy and grazing-incidence wide-angle X-ray scattering are applied to elucidate the mechanisms of the doping process and to explain the discrepancy in thermoelectric performance depending on the charge carriers being either transported in-plane or cross-plane. Morphological changes are found such that the crystallites, built-up by extended polymer chains interacting via lamellar and pi-pi stacking, re-arrange from face- to edge-on orientation upon doping. At high doping concentrations, dopant molecules disturb the crystallinity of the polymer, hindering charge transport and leading to a decreased power factor at high dopant concentrations. These observations explain why an intermediate doping concentration of N-DPBI leads to an optimized thermoelectric performance of P(NDI2OD-T2) in an in-plane geometry as compared to the cross-plane case.},
keywords = {Foundry Organic, Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
A M Pütz, M W Terban, S Bette, F Haase, R E Dinnebier, B V Lotsch
Total scattering reveals the hidden stacking disorder in a 2D covalent organic framework Journal Article
In: Chemical Science, 2020, ISSN: 2041-6520.
Abstract | Links | Tags: Foundry Organic
@article{,
title = {Total scattering reveals the hidden stacking disorder in a 2D covalent organic framework},
author = {A M P\"{u}tz and M W Terban and S Bette and F Haase and R E Dinnebier and B V Lotsch},
url = {http://dx.doi.org/10.1039/D0SC03048A},
doi = {10.1039/D0SC03048A},
issn = {2041-6520},
year = {2020},
date = {2020-07-08},
journal = {Chemical Science},
abstract = {Interactions between extended π-systems are often invoked as the main driving force for stacking and crystallization of 2D organic polymers. In covalent organic frameworks (COFs), the stacking strongly influences properties such as the accessibility of functional sites, pore geometry, and surface states, but the exact nature of the interlayer interactions is mostly elusive. The stacking mode is often identified as eclipsed based on observed high symmetry diffraction patterns. However, as pointed out by various studies, the energetics of eclipsed stacking are not favorable and offset stacking is preferred. This work presents lower and higher apparent symmetry modifications of the imine-linked TTI-COF prepared through high- and low-temperature reactions. Through local structure investigation by pair distribution function analysis and simulations of stacking disorder, we observe random local layer offsets in the low temperature modification. We show that while stacking disorder can be easily overlooked due to the apparent crystallographic symmetry of these materials, total scattering methods can help clarify this information and suggest that defective local structures could be much more prevalent in COFs than previously thought. A detailed analysis of the local structure helps to improve the search for and design of highly porous tailor-made materials.},
keywords = {Foundry Organic},
pubstate = {published},
tppubtype = {article}
}
S Wakolbinger, F R Geisenhof, F Winterer, S Palmer, J G Crimmann, K Watanabe, T Taniguchi, F Trixler, R T Weitz
Locally-triggered hydrophobic collapse induces global interface self-cleaning in van-der-Waals heterostructures at room-temperature Journal Article
In: 2d Materials, vol. 7, no. 3, 2020, ISSN: 2053-1583.
Abstract | Links | Tags: Foundry Organic
@article{,
title = {Locally-triggered hydrophobic collapse induces global interface self-cleaning in van-der-Waals heterostructures at room-temperature},
author = {S Wakolbinger and F R Geisenhof and F Winterer and S Palmer and J G Crimmann and K Watanabe and T Taniguchi and F Trixler and R T Weitz},
url = {\<Go to ISI\>://WOS:000528571100001},
doi = {10.1088/2053-1583/ab7bfc},
issn = {2053-1583},
year = {2020},
date = {2020-07-03},
urldate = {2020-07-03},
journal = {2d Materials},
volume = {7},
number = {3},
abstract = {Mutual relative orientation and well defined, uncontaminated interfaces are the key to obtain van-der-Waals heterostacks with defined properties. Even though the van-der-Waals forces are known to promote the 'self-cleaning' of interfaces, residue from the stamping process, which is often found to be trapped between the heterostructure constituents, can interrupt the interlayer interaction and therefore the coupling. Established interfacial cleaning methods usually involve high-temperature steps, which are in turn known to lead to uncontrolled rotations of layers within fragile heterostructures. Here, we present an alternative method feasible at room temperature. Using the tip of an atomic force microscope (AFM), we locally control the activation of interlayer attractive forces, resulting in the global removal of contaminants from the interface (i.e. the contaminants are also removed in regions several mu m away from the line touched by the AFM tip). By testing combinations of various hydrophobic van-der-Waals materials, mild temperature treatments, and by observing the temporal evolution of the contaminant removal process, we identify that the AFM tip triggers a dewetting-induced hydrophobic collapse and the van-der-Waals interaction is driving the cleaning process. We anticipate that this process is at the heart of the known 'self-cleaning' mechanism. Our technique can be utilized to controllably establish interlayer close coupling between a stack of van-der-Waals layers, and additionally allows to pattern and manipulate heterostructures locally for example to confine material into nanoscopic pockets between two van-der-Waals materials.},
keywords = {Foundry Organic},
pubstate = {published},
tppubtype = {article}
}
D Yang, F C Lohrer, V Korstgens, A Schreiber, B Cao, S Bernstorff, P Muller-Buschbaum
In Operando GISAXS and GIWAXS Stability Study of Organic Solar Cells Based on PffBT4T-2OD:PC71BM with and without Solvent Additive Journal Article
In: Advanced Science, 2020.
Abstract | Links | Tags: Foundry Organic, Molecularly-Functionalized
@article{,
title = {In Operando GISAXS and GIWAXS Stability Study of Organic Solar Cells Based on PffBT4T-2OD:PC71BM with and without Solvent Additive},
author = {D Yang and F C Lohrer and V Korstgens and A Schreiber and B Cao and S Bernstorff and P Muller-Buschbaum},
url = {\<Go to ISI\>://WOS:000544597000001},
doi = {10.1002/advs.202001117},
year = {2020},
date = {2020-07-01},
urldate = {2020-07-01},
journal = {Advanced Science},
abstract = {Solvent additives are known to modify the morphology of bulk heterojunction active layers to achieve high efficiency organic solar cells. However, the knowledge about the influence of solvent additives on the morphology degradation is limited. Hence, in operando grazing-incidence small and wide angle X-ray scattering (GISAXS and GIWAXS) measurements are applied on a series of PffBT4T-2OD:PC71BM-based solar cells prepared without and with solvent additives. The solar cells fabricated without a solvent additive, with 1,8-diiodoctane (DIO), and witho-chlorobenzaldehyde (CBA) additive show differences in the device degradation and changes in the morphology and crystallinity of the active layers. The mesoscale morphology changes are correlated with the decay of the short-circuit currentJ(sc)and the evolution of crystalline grain sizes is codependent with the decay of open-circuit voltageV(oc). Without additive, the loss inJ(sc)dominates the degradation, whereas with solvent additive (DIO and CBA) the loss inV(oc)rules the degradation. CBA addition increases the overall device stability as compared to DIO or absence of additive.},
keywords = {Foundry Organic, Molecularly-Functionalized},
pubstate = {published},
tppubtype = {article}
}
K S Wienhold, V Korstgens, S Grott, X Y Jiang, M Schwartzkopf, S V Roth, P Muller-Buschbaum
In: Solar Rrl, vol. 4, no. 7, 2020, ISSN: 2367-198X.
Abstract | Links | Tags: Foundry Organic, Molecularly-Functionalized
@article{,
title = {In Situ Printing: Insights into the Morphology Formation and Optical Property Evolution of Slot-Die-Coated Active Layers Containing Low Bandgap Polymer Donor and Nonfullerene Small Molecule Acceptor},
author = {K S Wienhold and V Korstgens and S Grott and X Y Jiang and M Schwartzkopf and S V Roth and P Muller-Buschbaum},
url = {\<Go to ISI\>://WOS:000527841700001},
doi = {10.1002/solr.202000086},
issn = {2367-198X},
year = {2020},
date = {2020-07-01},
journal = {Solar Rrl},
volume = {4},
number = {7},
abstract = {Printing of active layers for high-efficiency organic solar cells with the slot-die coating technique can overcome the challenge of upscaling, which will be needed for organic photovoltaics on its way to marketability. The morphology of a bulk-heterojunction organic solar cell has a very high impact on its power conversion efficiency. Therefore, it is of particular importance to understand the mechanisms of structure formation during printing of active layers to enable further optimization of the solar cell performance and upscaling of the production process. Meniscus-guided slot-die coating of the blend of a low bandgap conjugated polymer donor with benzodithiophene units PBDB-T-SF and the nonfullerene small molecule acceptor IT-4F is studied in situ with optical microscopy, Ultraviolet-visible spectroscopy, and grazing incidence small angle X-ray scattering. The structure formation is followed from the liquid to the final dry film state. Thereby, five regimes of morphology formation are determined. The morphological evolution in the printed active layer is correlated to changing optical properties of the thin film. In the final dry film, polymer domains of several tens of nanometers are observed, which will be favorable for application in high-efficiency organic solar cells.},
keywords = {Foundry Organic, Molecularly-Functionalized},
pubstate = {published},
tppubtype = {article}
}
L Nguyen, M Dass, M F Ober, L V Besteiro, Z M M Wang, B Nickel, A O Govorov, T Liedl, A Heuer-Jungemann
Chiral Assembly of Gold-Silver Core-Shell Plasmonic Nanorods on DNA Origami with Strong Optical Activity Journal Article
In: Acs Nano, vol. 14, no. 6, pp. 7454-7461, 2020, ISSN: 1936-0851.
Abstract | Links | Tags: Foundry Organic, Molecularly-Functionalized
@article{,
title = {Chiral Assembly of Gold-Silver Core-Shell Plasmonic Nanorods on DNA Origami with Strong Optical Activity},
author = {L Nguyen and M Dass and M F Ober and L V Besteiro and Z M M Wang and B Nickel and A O Govorov and T Liedl and A Heuer-Jungemann},
url = {\<Go to ISI\>://WOS:000543744100103},
doi = {10.1021/acsnano.0c03127},
issn = {1936-0851},
year = {2020},
date = {2020-06-23},
journal = {Acs Nano},
volume = {14},
number = {6},
pages = {7454-7461},
abstract = {The spatial organization of metal nanoparticles has become an important tool for manipulating light in nanophotonic applications. Silver nanoparticles, particularly silver nanorods, have excellent plasmonic properties but are prone to oxidation and are therefore inherently unstable in aqueous solutions and salt-containing buffers. Consequently, gold nanoparticles have often been favored, despite their inferior optical performance. Bimetallic, i.e., gold-silver core-shell nanoparticles, can resolve this issue. We present a method for synthesizing highly stable gold-silver core-shell NRs that are instantaneously functionalized with DNA, enabling chiral self-assembly on DNA origami. The silver shell gives rise to an enhancement of plasmonic properties, reflected here in strongly increased circular dichroism, as compared to pristine gold nanorods. Gold-silver nanorods are ideal candidates for plasmonic sensing with increased sensitivity as needed in pathogen RNA or antibody testing for nonlinear optics and light-funneling applications in surface enhanced Raman spectroscopy. Furthermore, the control of interparticle orientation enables the study of plasmonic phenomena, in particular, synergistic effects arising from plasmonic coupling of such bimetallic systems.},
keywords = {Foundry Organic, Molecularly-Functionalized},
pubstate = {published},
tppubtype = {article}
}
B Lin, X Zhou, H Zhao, J Yuan, K Zhou, K Chen, H Wu, R Guo, M A Scheel, A Chumakov, S V Roth, Y Mao, L Wang, Z Tang, P Müller-Buschbaum, W Ma
In: Energy & Environmental Science, vol. 13, no. 8, pp. 2467-2479, 2020, ISSN: 1754-5692.
Abstract | Links | Tags: Foundry Organic, Solid-Solid
@article{nokey,
title = {Balancing the pre-aggregation and crystallization kinetics enables high efficiency slot-die coated organic solar cells with reduced non-radiative recombination losses},
author = {B Lin and X Zhou and H Zhao and J Yuan and K Zhou and K Chen and H Wu and R Guo and M A Scheel and A Chumakov and S V Roth and Y Mao and L Wang and Z Tang and P M\"{u}ller-Buschbaum and W Ma},
url = {http://dx.doi.org/10.1039/D0EE00774A},
doi = {10.1039/D0EE00774A},
issn = {1754-5692},
year = {2020},
date = {2020-06-12},
journal = {Energy \& Environmental Science},
volume = {13},
number = {8},
pages = {2467-2479},
abstract = {Slot-die coating being compatible with the roll-to-roll technique has been regarded as a promising tool for upscaling the manufacturing of organic solar cells (OSCs). However, there has been a significant gap between the efficiencies of the state-of-the-art spin-coated devices and the scalable processed devices. The active layer morphology is crucial to achieve high efficiency in OSCs, which depends on the conditions of film fabrication. To figure out and optimize the slot-die coating process, a deeper understanding of the film formation kinetics is important. Herein, in situ measurements of the slot-die coating process based on the PM7:IT4F system are demonstrated to illustrate the aggregation and crystallization evolution at various die temperatures and substrate temperatures. OSCs with a high power conversion efficiency of 13.2% are achieved at 60 °C die temperature/60 °C substrate temperature due to the improved exciton dissociation, charge transport and suppressed non-radiative charge recombination. The optimized morphology is attributed to the balanced polymer pre-aggregation and small molecule crystallization kinetics. The unsuitable die temperature leads to overlarge phase separation and consequently inefficient exciton dissociation while the improper substrate temperature results in weak crystallization and the following shrunken carrier lifetime with strong non-radiative combination. This work provides fundamental understanding on the correlations among processing methodology, solution pre-aggregation, morphology formation kinetics, device physics and device performance and affords guidance for device optimization in scalable manufacturing.},
keywords = {Foundry Organic, Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
M Isselstein, L Zhang, V Glembockyte, O Brix, G Cosa, P Tinnefeld, T Cordes
Self-Healing Dyes—Keeping the Promise? Journal Article
In: The Journal of Physical Chemistry Letters, vol. 11, no. 11, pp. 4462-4480, 2020.
Links | Tags: Foundry Organic
@article{,
title = {Self-Healing Dyes\textemdashKeeping the Promise?},
author = {M Isselstein and L Zhang and V Glembockyte and O Brix and G Cosa and P Tinnefeld and T Cordes},
url = {https://doi.org/10.1021/acs.jpclett.9b03833},
doi = {10.1021/acs.jpclett.9b03833},
year = {2020},
date = {2020-06-04},
journal = {The Journal of Physical Chemistry Letters},
volume = {11},
number = {11},
pages = {4462-4480},
keywords = {Foundry Organic},
pubstate = {published},
tppubtype = {article}
}
K S Wienhold, W Chen, S S Yin, R J Guo, M Schwartzkopf, S V Roth, P Muller-Buschbaum
Following in Operando the Structure Evolution-Induced Degradation in Printed Organic Solar Cells with Nonfullerene Small Molecule Acceptor Journal Article
In: Solar Rrl, 2020, ISSN: 2367-198X.
Abstract | Links | Tags: Foundry Organic, Molecularly-Functionalized
@article{,
title = {Following in Operando the Structure Evolution-Induced Degradation in Printed Organic Solar Cells with Nonfullerene Small Molecule Acceptor},
author = {K S Wienhold and W Chen and S S Yin and R J Guo and M Schwartzkopf and S V Roth and P Muller-Buschbaum},
url = {\<Go to ISI\>://WOS:000538529300001},
doi = {10.1002/solr.202000251},
issn = {2367-198X},
year = {2020},
date = {2020-06-01},
urldate = {2020-06-01},
journal = {Solar Rrl},
abstract = {Understanding the degradation mechanisms of printed bulk-heterojunction (BHJ) organic solar cells during operation is essential to achieve long-term stability and realize real-world applications of organic photovoltaics. Herein, the degradation of printed organic solar cells based on the conjugated benzodithiophene polymer PBDB-T-SF and the nonfullerene small molecule acceptor IT-4F with 0.25 vol% 1,8-diiodooctane (DIO) solvent additive is studied in operando for two different donor:acceptor ratios. The inner nano-morphology is analyzed with grazing incidence small angle X-ray scattering (GISAXS), and current-voltage (I-V) characteristics are probed simultaneously. Irrespective of the mixing ratio, degradation occurs by the same degradation mechanism. A decrease in the short-circuit current density (J(SC)) is identified to be the determining factor for the decline of the power conversion efficiency. The decrease in J(SC) is induced by a reduction of the relative interface area between the conjugated polymer and the small molecule acceptor in the BHJ structure, resembling the morphological degradation of the active layer.},
keywords = {Foundry Organic, Molecularly-Functionalized},
pubstate = {published},
tppubtype = {article}
}
J Skotnitzki, A Kremsmair, D Keefer, F Schuppel, B L De Bonneville, R De Vivie-Riedle, P Knochel
Regio- and diastereoselective reactions of chiral secondary alkylcopper reagents with propargylic phosphates: preparation of chiral allenes Journal Article
In: Chemical Science, vol. 11, no. 20, pp. 5328-5332, 2020, ISSN: 2041-6520.
Abstract | Links | Tags: Foundry Organic
@article{,
title = {Regio- and diastereoselective reactions of chiral secondary alkylcopper reagents with propargylic phosphates: preparation of chiral allenes},
author = {J Skotnitzki and A Kremsmair and D Keefer and F Schuppel and B L De Bonneville and R De Vivie-Riedle and P Knochel},
url = {\<Go to ISI\>://WOS:000537133000020},
doi = {10.1039/c9sc05982b},
issn = {2041-6520},
year = {2020},
date = {2020-05-28},
journal = {Chemical Science},
volume = {11},
number = {20},
pages = {5328-5332},
abstract = {The diastereoselective S(N)2 '-substitution of secondary alkylcopper reagents with propargylic phosphates enables the preparation of stereodefined alkylallenes. By using enantiomerically enriched alkylcopper reagents and enantioenriched propargylic phosphates as electrophiles anti-S(N)2 '-substitutions were performend leading to alpha-chiral allenes in good yields with excellent regioselectivity and retention of configuration. DFT-calculations were performed to rationalize the structure of these alkylcopper reagents in various solvents, emphasizing their configurational stability in THF.},
keywords = {Foundry Organic},
pubstate = {published},
tppubtype = {article}
}
J W Borchert, U Zschieschang, F Letzkus, M Giorgio, R T Weitz, M Caironi, J N Burghartz, S Ludwigs, H Klauk
Flexible low-voltage high-frequency organic thin-film transistors Journal Article
In: Science Advances, vol. 6, no. 21, 2020, ISSN: 2375-2548.
Abstract | Links | Tags: Foundry Organic
@article{,
title = {Flexible low-voltage high-frequency organic thin-film transistors},
author = {J W Borchert and U Zschieschang and F Letzkus and M Giorgio and R T Weitz and M Caironi and J N Burghartz and S Ludwigs and H Klauk},
url = {\<Go to ISI\>://WOS:000537235300049},
doi = {10.1126/sciadv.aaz5156},
issn = {2375-2548},
year = {2020},
date = {2020-05-20},
urldate = {2020-05-20},
journal = {Science Advances},
volume = {6},
number = {21},
abstract = {The primary driver for the development of organic thin-film transistors (TFTs) over the past few decades has been the prospect of electronics applications on unconventional substrates requiring low-temperature processing. A key requirement for many such applications is high-frequency switching or amplification at the low operating voltages provided by lithium-ion batteries (similar to 3 V). To date, however, most organic-TFT technologies show limited dynamic performance unless high operating voltages are applied to mitigate high contact resistances and large parasitic capacitances. Here, we present flexible low-voltage organic TFTs with record static and dynamic performance, including contact resistance as small as 10 Omega.cm, on/off current ratios as large as 10(10), subthreshold swing as small as 59 mV/decade, signal delays below 80 ns in inverters and ring oscillators, and transit frequencies as high as 21 MHz, all while using an inverted coplanar TFT structure that can be readily adapted to industry-standard lithographic techniques.},
keywords = {Foundry Organic},
pubstate = {published},
tppubtype = {article}
}
S S Matikonda, G Hammersley, N Kumari, L Grabenhorst, V Glembockyte, P Tinnefeld, J Ivanic, M Levitus, M J Schnermann
Impact of Cyanine Conformational Restraint in the Near-Infrared Range Journal Article
In: The Journal of Organic Chemistry, 2020, ISSN: 0022-3263.
Links | Tags: Foundry Organic
@article{,
title = {Impact of Cyanine Conformational Restraint in the Near-Infrared Range},
author = {S S Matikonda and G Hammersley and N Kumari and L Grabenhorst and V Glembockyte and P Tinnefeld and J Ivanic and M Levitus and M J Schnermann},
url = {https://doi.org/10.1021/acs.joc.0c00236},
doi = {10.1021/acs.joc.0c00236},
issn = {0022-3263},
year = {2020},
date = {2020-04-10},
urldate = {2020-04-10},
journal = {The Journal of Organic Chemistry},
keywords = {Foundry Organic},
pubstate = {published},
tppubtype = {article}
}
K Trofymchuk, V Glembockyte, L Grabenhorst, F Steiner, C Vietz, C Close, M Pfeiffer, L Richter, M L Schütte, F Selbach, R Yaadav, J Zähringer, Q Wei, A Ozcan, B Lalkens, G P Acuna, P Tinnefeld
Addressable Nanoantennas with Cleared Hotspots for Single-Molecule Detection on a Portable Smartphone Microscope Journal Article
In: bioRxiv, pp. 2020.04.09.032037, 2020.
Abstract | Links | Tags: Foundry Inorganic, Foundry Organic, Molecularly-Functionalized
@article{,
title = {Addressable Nanoantennas with Cleared Hotspots for Single-Molecule Detection on a Portable Smartphone Microscope},
author = {K Trofymchuk and V Glembockyte and L Grabenhorst and F Steiner and C Vietz and C Close and M Pfeiffer and L Richter and M L Sch\"{u}tte and F Selbach and R Yaadav and J Z\"{a}hringer and Q Wei and A Ozcan and B Lalkens and G P Acuna and P Tinnefeld},
url = {http://biorxiv.org/content/early/2020/04/09/2020.04.09.032037.abstract},
doi = {10.1101/2020.04.09.032037},
year = {2020},
date = {2020-04-09},
urldate = {2020-04-09},
journal = {bioRxiv},
pages = {2020.04.09.032037},
abstract = {The advent of highly sensitive photodetectors1,2 and the development of photostabilization strategies3 made detecting the fluorescence of a single molecule a routine task in many labs around the world. However, to this day, this process requires cost-intensive optical instruments due to the truly nanoscopic signal of a single emitter. Simplifying single-molecule detection would enable many exciting applications, e.g. in point-of-care diagnostic settings, where costly equipment would be prohibitive.4 Here, we introduce addressable NanoAntennas with Cleared HOtSpots (NACHOS) that are scaffolded by DNA origami nanostructures and can be specifically tailored for the incorporation of bioassays. Single emitters placed in the NACHOS emit up to 461-fold brighter enabling their detection with a customary smartphone camera and an 8-US-dollar objective lens. To prove the applicability of our system, we built a portable, battery-powered smartphone microscope and successfully carried out an exemplary single-molecule detection assay for DNA specific to antibiotic-resistant Klebsiella pneumonia "on the road “.Competing Interest StatementPT and GPA are inventors on a patent of the described Bottom-up method for fluorescence enhancement in molecular assays, EP1260316.1, 2012, US20130252825 A1.},
keywords = {Foundry Inorganic, Foundry Organic, Molecularly-Functionalized},
pubstate = {published},
tppubtype = {article}
}
P Mao, C Liu, F Song, M Han, S A Maier, S Zhang
Manipulating disordered plasmonic systems by external cavity with transition from broadband absorption to reconfigurable reflection Journal Article
In: Nature Communications, vol. 11, no. 1, pp. 1538, 2020, ISSN: 2041-1723.
Abstract | Links | Tags: Foundry Organic
@article{,
title = {Manipulating disordered plasmonic systems by external cavity with transition from broadband absorption to reconfigurable reflection},
author = {P Mao and C Liu and F Song and M Han and S A Maier and S Zhang},
url = {https://doi.org/10.1038/s41467-020-15349-y},
doi = {10.1038/s41467-020-15349-y},
issn = {2041-1723},
year = {2020},
date = {2020-03-24},
journal = {Nature Communications},
volume = {11},
number = {1},
pages = {1538},
abstract = {Disordered biostructures are ubiquitous in nature, usually generating white or black colours due to their broadband optical response and robustness to perturbations. Through judicious design, disordered nanostructures have been realised in artificial systems, with unique properties for light localisation, photon transportation and energy harvesting. On the other hand, the tunability of disordered systems with a broadband response has been scarcely explored. Here, we achieve the controlled manipulation of disordered plasmonic systems, realising the transition from broadband absorption to tunable reflection through deterministic control of the coupling to an external cavity. Starting from a generalised model, we realise disordered systems composed of plasmonic nanoclusters that either operate as a broadband absorber or with a reconfigurable reflection band throughout the visible. Not limited to its significance for the further understanding of the physics of disorder, our disordered plasmonic system provides a novel platform for various practical application such as structural colour patterning.},
keywords = {Foundry Organic},
pubstate = {published},
tppubtype = {article}
}
K S Wienhold, X Y Jiang, P Muller-Buschbaum
Organic solar cells probed with advanced neutron scattering techniques Journal Article
In: Applied Physics Letters, vol. 116, no. 12, 2020, ISSN: 0003-6951.
Abstract | Links | Tags: Foundry Organic, Molecularly-Functionalized
@article{,
title = {Organic solar cells probed with advanced neutron scattering techniques},
author = {K S Wienhold and X Y Jiang and P Muller-Buschbaum},
url = {\<Go to ISI\>://WOS:000522430600001},
doi = {10.1063/5.0003997},
issn = {0003-6951},
year = {2020},
date = {2020-03-23},
journal = {Applied Physics Letters},
volume = {116},
number = {12},
abstract = {Neutron scattering techniques provide unique insights into the active layer morphology of organic solar cells. The nanoscale morphology, the thin film vertical composition, and the intermixing on a molecular level, which all strongly have an impact on the performance of organic solar cells, can be probed with neutrons. In addition to the static structure, also fast dynamics occurring in the active material is accessible with neutrons. This perspective letter highlights the power of grazing incidence small angle neutron scattering and quasi-elastic neutron scattering experiments after shortly introducing into the working principle of organic solar cells.},
keywords = {Foundry Organic, Molecularly-Functionalized},
pubstate = {published},
tppubtype = {article}
}
D Yang, B Cao, V Korstgens, N Saxena, N Li, C Bilko, S Grott, W Chen, X Y Jiang, J E Heger, S Bernstorff, P Muller-Buschbaum
Tailoring Morphology Compatibility and Device Stability by Adding PBDTTPD-COOH as Third Component to Fullerene-Based Polymer Solar Cells Journal Article
In: Acs Applied Energy Materials, vol. 3, no. 3, pp. 2604-2613, 2020, ISSN: 2574-0962.
Abstract | Links | Tags: Foundry Organic, Molecularly-Functionalized
@article{,
title = {Tailoring Morphology Compatibility and Device Stability by Adding PBDTTPD-COOH as Third Component to Fullerene-Based Polymer Solar Cells},
author = {D Yang and B Cao and V Korstgens and N Saxena and N Li and C Bilko and S Grott and W Chen and X Y Jiang and J E Heger and S Bernstorff and P Muller-Buschbaum},
url = {\<Go to ISI\>://WOS:000526598300061},
doi = {10.1021/acsaem.9b02290},
issn = {2574-0962},
year = {2020},
date = {2020-03-23},
journal = {Acs Applied Energy Materials},
volume = {3},
number = {3},
pages = {2604-2613},
abstract = {The crystallinity and morphology of polymer and fullerene have a profound influence on the performance of bulk heterojunction (BHJ) organic photovoltaic devices. The poor compatibility of donor and acceptor molecules in the BHJs hinders the further improvement of the device performance and stability in organic solar cells. In this work, the conjugated polymer PBDTTPD-COOH is introduced as a third component into BHJ films of PTB7-Th:PC71BM and PffBT4T-2OD:PC71BM to improve the crystallinity and morphology. The crystallinity of both donor polymers is enhanced and more face-on orientated crystals are observed in the corresponding films, which is correlated with the improvement of the current density of the related solar cells. Also, the improved BHJ morphology leads to an increased fill factor. Furthermore, the device stability significantly increases by the addition of the third component PBDTTPD-COOH. The T80 lifetime value is enhanced 10 times in the doped devices as compared with the binary solar cells in the case of the PTB7-Th:PC71BM series.},
keywords = {Foundry Organic, Molecularly-Functionalized},
pubstate = {published},
tppubtype = {article}
}
J Skotnitzki, A Kremsmair, B Kicin, R Saeb, V Ruf, P Knochel
In: Synthesis-Stuttgart, vol. 52, no. 6, pp. 873-881, 2020, ISSN: 0039-7881.
Abstract | Links | Tags: Foundry Organic
@article{,
title = {Stereoselective anti-S(N)2 '-Substitutions of Secondary Alkylcopper-Zinc Reagents with Allylic Epoxides: Total Synthesis of (3S,6R,7S)-Zingiberenol},
author = {J Skotnitzki and A Kremsmair and B Kicin and R Saeb and V Ruf and P Knochel},
url = {\<Go to ISI\>://WOS:000519236300009},
doi = {10.1055/s-0039-1690766},
issn = {0039-7881},
year = {2020},
date = {2020-03-17},
journal = {Synthesis-Stuttgart},
volume = {52},
number = {6},
pages = {873-881},
abstract = {Chiral secondary mixed alkylcopper-zinc reagents were prepared from the corresponding alkyl iodides and reacted with allylic epoxides via an anti -S (N) 2 '-substitution and retention of configuration of the chiral alkylorganometallic, leading to chiral allylic alcohols. This method was used in a total synthesis of the natural product (3 S ,6 R ,7 S )-zingiberenol in 8 steps and 9.7% overall yield [dr (3 S ,6 R ) = 99:1; dr (6 R ,7 S ) = 81:19] starting from commercially available 3-methyl-2-cyclohexenone.},
keywords = {Foundry Organic},
pubstate = {published},
tppubtype = {article}
}
L Grabenhorst, K Trofymchuk, F Steiner, V Glembockyte, P Tinnefeld
Fluorophore photostability and saturation in the hotspot of DNA origami nanoantennas Journal Article
In: Methods and Applications in Fluorescence, vol. 8, no. 2, pp. 024003, 2020, ISSN: 2050-6120.
Abstract | Links | Tags: Foundry Inorganic, Foundry Organic, Molecularly-Functionalized
@article{,
title = {Fluorophore photostability and saturation in the hotspot of DNA origami nanoantennas},
author = {L Grabenhorst and K Trofymchuk and F Steiner and V Glembockyte and P Tinnefeld},
url = {http://dx.doi.org/10.1088/2050-6120/ab6ac8},
doi = {10.1088/2050-6120/ab6ac8},
issn = {2050-6120},
year = {2020},
date = {2020-02-05},
urldate = {2020-02-05},
journal = {Methods and Applications in Fluorescence},
volume = {8},
number = {2},
pages = {024003},
abstract = {Fluorescent dyes used for single-molecule spectroscopy can undergo millions of excitation-emission cycles before photobleaching. Due to the upconcentration of light in a plasmonic hotspot, the conditions for fluorescent dyes are even more demanding in DNA origami nanoantennas. Here, we briefly review the current state of fluorophore stabilization for single-molecule imaging and reveal additional factors relevant in the context of plasmonic fluorescence enhancement. We show that despite the improved photostability of single-molecule fluorophores by DNA origami nanoantennas, their performance in the intense electric fields in plasmonic hotspots is still limited by the underlying photophysical processes, such as formation of dim states and photoisomerization. These photophysical processes limit the photon count rates, increase heterogeneity and aggravate quantification of fluorescence enhancement factors. These factors also reduce the time resolution that can be achieved in biophysical single-molecule experiments. Finally, we show how the photophysics of a DNA hairpin assay with a fluorophore-quencher pair can be influenced by plasmonic DNA origami nanoantennas leading to implications for their use in fluorescence-based diagnostic assays. Especially, we show that such assays can produce false positive results by premature photobleaching of the dark quencher.},
keywords = {Foundry Inorganic, Foundry Organic, Molecularly-Functionalized},
pubstate = {published},
tppubtype = {article}
}
M Asher, D Angerer, R Korobko, Y Diskin-Posner, D A Egger, O Yaffe
Anharmonic Lattice Vibrations in Small-Molecule Organic Semiconductors Journal Article
In: Advanced Materials, vol. 32, no. 10, pp. 1908028, 2020, ISSN: 0935-9648.
Abstract | Links | Tags: Foundry Organic
@article{,
title = {Anharmonic Lattice Vibrations in Small-Molecule Organic Semiconductors},
author = {M Asher and D Angerer and R Korobko and Y Diskin-Posner and D A Egger and O Yaffe},
url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adma.201908028},
doi = {10.1002/adma.201908028},
issn = {0935-9648},
year = {2020},
date = {2020-01-31},
journal = {Advanced Materials},
volume = {32},
number = {10},
pages = {1908028},
abstract = {Abstract The intermolecular lattice vibrations in small-molecule organic semiconductors have a strong impact on their functional properties. Existing models treat the lattice vibrations within the harmonic approximation. In this work, polarization-orientation (PO) Raman measurements are used to monitor the temperature-evolution of the symmetry of lattice vibrations in anthracene and pentacene single crystals. Combined with first-principles calculations, it is shown that at 10 K, the lattice dynamics of the crystals are indeed harmonic. However, as the temperature is increased, specific lattice modes gradually lose their PO dependence and become more liquid-like. This finding is indicative of a dynamic symmetry breaking of the crystal structure and shows clear evidence of the strongly anharmonic nature of these vibrations. Pentacene also shows an apparent phase transition between 80 and 150 K, indicated by a change in the vibrational symmetry of one of the lattice modes. These findings lay the groundwork for accurate predictions of the electronic properties of high-mobility organic semiconductors at room temperature.},
keywords = {Foundry Organic},
pubstate = {published},
tppubtype = {article}
}
L Shaw, Y Diao, G C Martin-Noble, H Yan, P Hayoz, R T Weitz, D Kaelblein, M F Toney, Z Bao
Manipulation and statistical analysis of the fluid flow of polymer semiconductor solutions during meniscus-guided coating Journal Article
In: MRS Bulletin, pp. 1-14, 2020, ISSN: 0883-7694.
Abstract | Links | Tags: Foundry Organic, Solid-Liquid
@article{nokey,
title = {Manipulation and statistical analysis of the fluid flow of polymer semiconductor solutions during meniscus-guided coating},
author = {L Shaw and Y Diao and G C Martin-Noble and H Yan and P Hayoz and R T Weitz and D Kaelblein and M F Toney and Z Bao},
url = {https://www.cambridge.org/core/article/manipulation-and-statistical-analysis-of-the-fluid-flow-of-polymer-semiconductor-solutions-during-meniscusguided-coating/B89C6C7985E43178910D8DAA53FF77C3},
doi = {10.1557/mrs.2020.306},
issn = {0883-7694},
year = {2020},
date = {2020-01-01},
journal = {MRS Bulletin},
pages = {1-14},
abstract = {Recent work in structure\textendashprocessing relationships of polymer semiconductors have demonstrated the versatility and control of thin-film microstructure offered by meniscus-guided coating (MGC) techniques. Here, we analyze the qualitative and quantitative aspects of solution shearing, a model MGC method, using coating blades augmented with arrays of pillars. The pillars induce local regions of high strain rates\textemdashboth shear and extensional\textemdashnot otherwise possible with unmodified blades, and we use fluid mechanical simulations to model and study a variety of pillar spacings and densities. We then perform a statistical analysis of 130 simulation variables to find correlations with three dependent variables of interest: thin-film degree of crystallinity and transistor field-effect mobilities for charge-transport parallel (μpara) and perpendicular (μperp) to the coating direction. Our study suggests that simple fluid mechanical models can reproduce substantive correlations between the induced fluid flow and important performance metrics, providing a methodology for optimizing blade design.},
keywords = {Foundry Organic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
J Schedlbauer, P Wilhelm, L Grabenhorst, M E Federl, B Lalkens, F Hinderer, U Scherf, S Höger, P Tinnefeld, S Bange, J Vogelsang, J M Lupton
Ultrafast Single-Molecule Fluorescence Measured by Femtosecond Double-Pulse Excitation Photon Antibunching Journal Article
In: Nano Letters, 2019, ISSN: 1530-6984.
Links | Tags: Foundry Organic, Molecularly-Functionalized
@article{,
title = {Ultrafast Single-Molecule Fluorescence Measured by Femtosecond Double-Pulse Excitation Photon Antibunching},
author = {J Schedlbauer and P Wilhelm and L Grabenhorst and M E Federl and B Lalkens and F Hinderer and U Scherf and S H\"{o}ger and P Tinnefeld and S Bange and J Vogelsang and J M Lupton},
url = {https://doi.org/10.1021/acs.nanolett.9b04354},
doi = {10.1021/acs.nanolett.9b04354},
issn = {1530-6984},
year = {2019},
date = {2019-12-23},
journal = {Nano Letters},
keywords = {Foundry Organic, Molecularly-Functionalized},
pubstate = {published},
tppubtype = {article}
}
A Heuer-Jungemann, T Liedl
From DNA Tiles to Functional DNA Materials Journal Article
In: Trends in Chemistry, vol. 1, no. 9, pp. 799-814, 2019, ISSN: 2589-5974.
Abstract | Links | Tags: Foundry Organic
@article{nokey,
title = {From DNA Tiles to Functional DNA Materials},
author = {A Heuer-Jungemann and T Liedl},
url = {https://www.sciencedirect.com/science/article/pii/S258959741930190X},
doi = {https://doi.org/10.1016/j.trechm.2019.07.006},
issn = {2589-5974},
year = {2019},
date = {2019-12-01},
journal = {Trends in Chemistry},
volume = {1},
number = {9},
pages = {799-814},
abstract = {Over the past few decades, DNA has turned into one of the most widely used molecular linkers and a versatile building block for the self-assembly of DNA nanostructures. Such complexes, composed of only a few oligonucleotides (e.g., DNA tiles) or assembled from hundreds of synthetic and natural scaffolding strands (e.g., DNA origami), are being increasingly assembled into higher-order architectures such as lattices and crystals. A wide variety of assembly methods and techniques (e.g., solution-phase and substrate-assisted sticky-ended cohesion or blunt-end stacking) have emerged and are constantly being refined. This review provides a summary of the methods and building blocks for the assembly of 2D and 3D DNA lattices and crystals, and discusses some of their potential applications in materials science.},
keywords = {Foundry Organic},
pubstate = {published},
tppubtype = {article}
}
L D M Peters, J Kussmann, C Ochsenfeld
Nonadiabatic Molecular Dynamics on Graphics Processing Units: Performance and Application to Rotary Molecular Motors Journal Article
In: Journal of Chemical Theory and Computation, vol. 15, no. 12, pp. 6647-6659, 2019, ISSN: 1549-9618.
Abstract | Links | Tags: Foundry Organic, Molecularly-Functionalized, Solid-Liquid
@article{nokey,
title = {Nonadiabatic Molecular Dynamics on Graphics Processing Units: Performance and Application to Rotary Molecular Motors},
author = {L D M Peters and J Kussmann and C Ochsenfeld},
url = {https://doi.org/10.1021/acs.jctc.9b00859},
doi = {10.1021/acs.jctc.9b00859},
issn = {1549-9618},
year = {2019},
date = {2019-11-25},
journal = {Journal of Chemical Theory and Computation},
volume = {15},
number = {12},
pages = {6647-6659},
abstract = {Nonadiabatic molecular dynamics (NAMD) simulations of molecular systems require the efficient evaluation of excited-state properties, such as energies, gradients, and nonadiabatic coupling vectors. Here, we investigate the use of graphics processing units (GPUs) in addition to central processing units (CPUs) to efficiently calculate these properties at the time-dependent density functional theory (TDDFT) level of theory. Our implementation in the FermiONs++ program package uses the J-engine and a preselective screening procedure for the calculation of Coulomb and exchange kernels, respectively. We observe good speed-ups for small and large molecular systems (comparable to those observed in ground-state calculations) and reduced (down to sublinear) scaling behavior with respect to the system size (depending on the spatial locality of the investigated excitation). As a first illustrative application, we present efficient NAMD simulations of a series of newly designed light-driven rotary molecular motors and compare their S1 lifetimes. Although all four rotors show different S1 excitation energies, their ability to rotate upon excitation is conserved, making the series an interesting starting point for rotary molecular motors with tunable excitation energies.},
keywords = {Foundry Organic, Molecularly-Functionalized, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
K S Wienhold, V Körstgens, S Grott, X Jiang, M Schwartzkopf, S V Roth, P Müller-Buschbaum
Effect of Solvent Additives on the Morphology and Device Performance of Printed Nonfullerene Acceptor Based Organic Solar Cells Journal Article
In: ACS Applied Materials & Interfaces, vol. 11, no. 45, pp. 42313-42321, 2019, ISSN: 1944-8244.
Abstract | Links | Tags: Foundry Organic, Solid-Solid
@article{nokey,
title = {Effect of Solvent Additives on the Morphology and Device Performance of Printed Nonfullerene Acceptor Based Organic Solar Cells},
author = {K S Wienhold and V K\"{o}rstgens and S Grott and X Jiang and M Schwartzkopf and S V Roth and P M\"{u}ller-Buschbaum},
url = {https://doi.org/10.1021/acsami.9b16784},
doi = {10.1021/acsami.9b16784},
issn = {1944-8244},
year = {2019},
date = {2019-11-13},
journal = {ACS Applied Materials \& Interfaces},
volume = {11},
number = {45},
pages = {42313-42321},
abstract = {Printing of active layers of high-efficiency organic solar cells and morphology control by processing with varying solvent additive concentrations are important to realize real-world use of bulk-heterojunction photovoltaics as it enables both up-scaling and optimization of the device performance. In this work, active layers of the conjugated polymer with benzodithiophene units PBDB-T-SF and the nonfullerene small molecule acceptor IT-4F are printed using meniscus guided slot-die coating. 1,8-Diiodooctane (DIO) is added to optimize the power conversion efficiency (PCE). The effect on the inner nanostructure and surface morphology of the material is studied for different solvent additive concentrations with grazing incidence small-angle X-ray scattering (GISAXS), grazing incidence wide-angle X-ray scattering (GIWAXS), scanning electron microscopy (SEM), and atomic force microscopy (AFM). Optical properties are studied with photoluminescence (PL), UV/vis absorption spectroscopy, and external quantum efficiency (EQE) measurements and correlated to the corresponding PCEs. The addition of 0.25 vol % DIO enhances the average PCE from 3.5 to 7.9%, whereas at higher concentrations the positive effect is less pronounced. A solar cell performance of 8.95% is obtained for the best printed device processed with an optimum solvent additive concentration. Thus, with the large-scale preparation method printing similarly well working solar cells can be realized as with the spin-coating method.},
keywords = {Foundry Organic, Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
N Keller, T Sick, N N Bach, A Koszalkowski, J M Rotter, D D Medina, T Bein
Dibenzochrysene enables tightly controlled docking and stabilizes photoexcited states in dual-pore covalent organic frameworks Journal Article
In: Nanoscale, vol. 11, no. 48, pp. 23338-23345, 2019, ISSN: 2040-3364.
Abstract | Links | Tags: Foundry Organic, Molecularly-Functionalized
@article{nokey,
title = {Dibenzochrysene enables tightly controlled docking and stabilizes photoexcited states in dual-pore covalent organic frameworks},
author = {N Keller and T Sick and N N Bach and A Koszalkowski and J M Rotter and D D Medina and T Bein},
url = {http://dx.doi.org/10.1039/C9NR08007D},
doi = {10.1039/C9NR08007D},
issn = {2040-3364},
year = {2019},
date = {2019-11-08},
urldate = {2019-11-08},
journal = {Nanoscale},
volume = {11},
number = {48},
pages = {23338-23345},
abstract = {Covalent organic frameworks (COFs), consisting of covalently connected organic building units, combine attractive features such as crystallinity, open porosity and widely tunable physical properties. For optoelectronic applications, the incorporation of heteroatoms into a 2D COF has the potential to yield desired photophysical properties such as lower band gaps, but can also cause lateral offsets of adjacent layers. Here, we introduce dibenzo[g,p]chrysene (DBC) as a novel building block for the synthesis of highly crystalline and porous 2D dual-pore COFs showing interesting properties for optoelectronic applications. The newly synthesized terephthalaldehyde (TA), biphenyl (Biph), and thienothiophene (TT) DBC-COFs combine conjugation in the a,b-plane with a tight packing of adjacent layers guided through the molecular DBC node serving as specific docking site for successive layers. The resulting DBC-COFs exhibit a hexagonal dual-pore kagome geometry, which is comparable to COFs containing another molecular docking site, namely 4,4′,4′′,4′′′-(ethylene-1,1,2,2-tetrayl)-tetraaniline (ETTA). In this context, the respective interlayer distances decrease from about 4.6 r{A} in ETTA-COFs to about 3.6 r{A} in DBC-COFs, leading to well-defined hexagonally faceted single crystals sized about 50\textendash100 nm. The TT DBC-COF features broad light absorption covering large parts of the visible spectrum, while Biph DBC-COF shows extraordinary excited state lifetimes exceeding 10 ns. In combination with the large number of recently developed linear conjugated building blocks, the new DBC tetra-connected node is expected to enable the synthesis of a large family of highly correlated and ordered 2D COFs with promising optoelectronic properties.},
keywords = {Foundry Organic, Molecularly-Functionalized},
pubstate = {published},
tppubtype = {article}
}
J M Rotter, S Weinberger, J Kampmann, T Sick, M Shalom, T Bein, D D Medina
Covalent Organic Framework Films through Electrophoretic Deposition—Creating Efficient Morphologies for Catalysis Journal Article
In: Chemistry of Materials, vol. 31, no. 24, pp. 10008-10016, 2019, ISSN: 0897-4756.
Abstract | Links | Tags: Foundry Organic, Molecularly-Functionalized
@article{nokey,
title = {Covalent Organic Framework Films through Electrophoretic Deposition\textemdashCreating Efficient Morphologies for Catalysis},
author = {J M Rotter and S Weinberger and J Kampmann and T Sick and M Shalom and T Bein and D D Medina},
url = {https://doi.org/10.1021/acs.chemmater.9b02286},
doi = {10.1021/acs.chemmater.9b02286},
issn = {0897-4756},
year = {2019},
date = {2019-10-03},
urldate = {2019-10-03},
journal = {Chemistry of Materials},
volume = {31},
number = {24},
pages = {10008-10016},
abstract = {The ability to grow covalent organic framework (COF) films allows for studying their properties as solid layers and enables the incorporation of these materials into a variety of functional devices. Here, we report on the fabrication of COF films and coatings by electrophoretic deposition (EPD). We demonstrate that the EPD technique is suitable for depositing COFs featuring two- and three-dimensional structures linked by imine or boronate ester bonds, namely, BDT-ETTA COF, COF-300, and COF-5. For the deposition, COF nanoparticle suspensions are prepared by dispersing the as-synthesized bulk materials in solvents with low dielectric constants. Subsequently, two electrodes are immersed into the COF particle suspensions, and upon inducing electric fields ranging from 100 to 900 V cm\textendash1, COFs are deposited as films on the positively charged electrode. Through EPD, within 2 min, large-area films of up to 25 cm2 are obtained on smooth or corrugated surfaces. COF films prepared by EPD feature an inherent textural porosity and tunable thickness, demonstrated from 400 nm to 24 μm. By controlling the deposition parameters such as duration, particle concentration, and applied potential, deposits of precise thickness can be produced. Furthermore, codepositions of different COFs as well as COF/Pt nanoparticles from mixed suspensions are demonstrated. The film morphologies obtained by EPD are shown to be advantageous for catalysis, as demonstrated for sacrificial agent-free photoelectrochemical water reduction. Here, BDT-ETTA COF photocathodes show a strongly increased photocurrent density compared to the respective dense and oriented films. Typical BDT-ETTA COF/Pt nanoparticle hybrid films exhibit photocurrent densities of over 100 μA cm\textendash2. The rapid and scalable deposition of COF particles as films and coatings through EPD is a versatile addition to the toolbox of COF film fabrication techniques, allowing for tailoring COF film architectures for desired functionalities.},
keywords = {Foundry Organic, Molecularly-Functionalized},
pubstate = {published},
tppubtype = {article}
}
F R Geisenhof, F Winterer, S Wakolbinger, T D Gokus, Y C Durmaz, D Priesack, J Lenz, F Keilmann, K Watanabe, T Taniguchi, R Guerrero-Avilés, M Pelc, A Ayuela, R T Weitz
Anisotropic Strain-Induced Soliton Movement Changes Stacking Order and Band Structure of Graphene Multilayers: Implications for Charge Transport Journal Article
In: ACS Applied Nano Materials, vol. 2, no. 9, pp. 6067-6075, 2019.
Abstract | Links | Tags: Foundry Organic
@article{,
title = {Anisotropic Strain-Induced Soliton Movement Changes Stacking Order and Band Structure of Graphene Multilayers: Implications for Charge Transport},
author = {F R Geisenhof and F Winterer and S Wakolbinger and T D Gokus and Y C Durmaz and D Priesack and J Lenz and F Keilmann and K Watanabe and T Taniguchi and R Guerrero-Avil\'{e}s and M Pelc and A Ayuela and R T Weitz},
url = {https://doi.org/10.1021/acsanm.9b01603},
doi = {10.1021/acsanm.9b01603},
year = {2019},
date = {2019-09-27},
urldate = {2019-09-27},
journal = {ACS Applied Nano Materials},
volume = {2},
number = {9},
pages = {6067-6075},
abstract = {The crystal structure of solid-state matter greatly affects its electronic properties. For example, in multilayer graphene, precise knowledge of the lateral layer arrangement is crucial, since the most stable configurations, Bernal and rhombohedral stacking, exhibit very different electronic properties. Nevertheless, both stacking orders can coexist within one flake, separated by a strain soliton that can host topologically protected states. Clearly, accessing the transport properties of the two stackings and the soliton is of high interest. However, the stacking orders can transform into one another, and therefore, the seemingly trivial question of how reliable electrical contact can be made to either stacking order can a priori not be answered easily. Here, we show that manufacturing metal contacts to multilayer graphene can move solitons by several μm, unidirectionally enlarging Bernal domains due to arising mechanical strain. Furthermore, we also find that during dry transfer of multilayer graphene onto hexagonal boron nitride, such a transformation can happen. Using density functional theory modeling, we corroborate that anisotropic deformations of the multilayer graphene lattice decrease the rhombohedral stacking stability. Finally, we have devised systematics to avoid soliton movement, and how to reliably realize contacts to both stacking configurations, which will aid to reliably access charge transport in both stacking configurations.},
keywords = {Foundry Organic},
pubstate = {published},
tppubtype = {article}
}
K Hübner, M Pilo-Pais, F Selbach, T Liedl, P Tinnefeld, F D Stefani, G P Acuna
Directing Single-Molecule Emission with DNA Origami-Assembled Optical Antennas Journal Article
In: Nano Letters, vol. 19, no. 9, pp. 6629-6634, 2019, ISSN: 1530-6984.
Links | Tags: Foundry Inorganic, Foundry Organic, Molecularly-Functionalized
@article{,
title = {Directing Single-Molecule Emission with DNA Origami-Assembled Optical Antennas},
author = {K H\"{u}bner and M Pilo-Pais and F Selbach and T Liedl and P Tinnefeld and F D Stefani and G P Acuna},
url = {https://doi.org/10.1021/acs.nanolett.9b02886},
doi = {10.1021/acs.nanolett.9b02886},
issn = {1530-6984},
year = {2019},
date = {2019-09-11},
urldate = {2019-09-11},
journal = {Nano Letters},
volume = {19},
number = {9},
pages = {6629-6634},
keywords = {Foundry Inorganic, Foundry Organic, Molecularly-Functionalized},
pubstate = {published},
tppubtype = {article}
}
B S Wei, D C Zhang, Y H Chen, A W Lei, P Knochel
Preparation of Polyfunctional Biaryl Derivatives by Cyclolanthanation of 2-Bromobiaryls and Heterocyclic Analogues Using nBu(2)LaCl.4 LiCl Journal Article
In: Angewandte Chemie-International Edition, vol. 58, no. 44, pp. 15631-15635, 2019, ISSN: 1433-7851.
Links | Tags: Foundry Organic
@article{,
title = {Preparation of Polyfunctional Biaryl Derivatives by Cyclolanthanation of 2-Bromobiaryls and Heterocyclic Analogues Using nBu(2)LaCl.4 LiCl},
author = {B S Wei and D C Zhang and Y H Chen and A W Lei and P Knochel},
url = {\<Go to ISI\>://WOS:000487102700001},
doi = {10.1002/anie.201908046},
issn = {1433-7851},
year = {2019},
date = {2019-08-28},
journal = {Angewandte Chemie-International Edition},
volume = {58},
number = {44},
pages = {15631-15635},
keywords = {Foundry Organic},
pubstate = {published},
tppubtype = {article}
}
H Schlomberg, J Kröger, G Savasci, M Terban, S Bette, I Moudrakovski, V Duppel, F Podjaski, R Siegel, J Senker, R Dinnebier, C Ochsenfeld, B V Lotsch
Structural Insights into Poly(Heptazine Imides): A Light Storing Carbon Nitride Material for Dark Photocatalysis Journal Article
In: Chemistry of Materials, vol. 31, 2019.
Links | Tags: Foundry Organic
@article{,
title = {Structural Insights into Poly(Heptazine Imides): A Light Storing Carbon Nitride Material for Dark Photocatalysis},
author = {H Schlomberg and J Kr\"{o}ger and G Savasci and M Terban and S Bette and I Moudrakovski and V Duppel and F Podjaski and R Siegel and J Senker and R Dinnebier and C Ochsenfeld and B V Lotsch},
doi = {10.1021/acs.chemmater.9b02199},
year = {2019},
date = {2019-08-12},
journal = {Chemistry of Materials},
volume = {31},
keywords = {Foundry Organic},
pubstate = {published},
tppubtype = {article}
}
C Muschielok, H Oberhofer
Aspects of semiconductivity in soft, porous metal-organic framework crystals Journal Article
In: Journal of Chemical Physics, vol. 151, no. 1, 2019, ISSN: 0021-9606.
Links | Tags: Foundry Organic, Molecularly-Functionalized
@article{,
title = {Aspects of semiconductivity in soft, porous metal-organic framework crystals},
author = {C Muschielok and H Oberhofer},
url = {\<Go to ISI\>://WOS:000474214600025},
doi = {10.1063/1.5108995},
issn = {0021-9606},
year = {2019},
date = {2019-07-03},
journal = {Journal of Chemical Physics},
volume = {151},
number = {1},
keywords = {Foundry Organic, Molecularly-Functionalized},
pubstate = {published},
tppubtype = {article}
}
B P Biswal, H A Vignolo-Gonzalez, T Banerjee, L Grunenberg, G Savasci, K Gottschling, J Nuss, C Ochsenfeld, B V Lotsch
Sustained Solar H-2 Evolution from a Thiazolo 5,4-d thiazole-Bridged Covalent Organic Framework and Nickel-Thiolate Cluster in Water Journal Article
In: Journal of the American Chemical Society, vol. 141, no. 28, pp. 11082-11092, 2019, ISSN: 0002-7863.
Links | Tags: Foundry Organic
@article{,
title = {Sustained Solar H-2 Evolution from a Thiazolo 5,4-d thiazole-Bridged Covalent Organic Framework and Nickel-Thiolate Cluster in Water},
author = {B P Biswal and H A Vignolo-Gonzalez and T Banerjee and L Grunenberg and G Savasci and K Gottschling and J Nuss and C Ochsenfeld and B V Lotsch},
url = {\<Go to ISI\>://WOS:000476684700023},
doi = {10.1021/jacs.9b03243},
issn = {0002-7863},
year = {2019},
date = {2019-06-20},
journal = {Journal of the American Chemical Society},
volume = {141},
number = {28},
pages = {11082-11092},
keywords = {Foundry Organic},
pubstate = {published},
tppubtype = {article}
}
T Banerjee, F Haase, S Trenker, B P Biswal, G Savasci, V Duppel, I Moudrakovski, C Ochsenfeld, B V Lotsch
Sub-stoichiometric 2D covalent organic frameworks from tri- and tetratopic linkers Journal Article
In: Nature Communications, vol. 10, 2019, ISSN: 2041-1723.
Links | Tags: Foundry Organic
@article{,
title = {Sub-stoichiometric 2D covalent organic frameworks from tri- and tetratopic linkers},
author = {T Banerjee and F Haase and S Trenker and B P Biswal and G Savasci and V Duppel and I Moudrakovski and C Ochsenfeld and B V Lotsch},
url = {\<Go to ISI\>://WOS:000472032300004},
doi = {10.1038/s41467-019-10574-6},
issn = {2041-1723},
year = {2019},
date = {2019-06-19},
journal = {Nature Communications},
volume = {10},
keywords = {Foundry Organic},
pubstate = {published},
tppubtype = {article}
}
P Alexa, C Oligschleger, P Gröger, C Morchutt, V Vyas, B V Lotsch, J C Schön, R Gutzler, K Kern
Short-Range Structural Correlations in Amorphous 2D Polymers Journal Article
In: ChemPhysChem, vol. 20, no. 18, pp. 2340-2347, 2019, ISSN: 1439-4235.
Abstract | Links | Tags: Foundry Organic
@article{,
title = {Short-Range Structural Correlations in Amorphous 2D Polymers},
author = {P Alexa and C Oligschleger and P Gr\"{o}ger and C Morchutt and V Vyas and B V Lotsch and J C Sch\"{o}n and R Gutzler and K Kern},
url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/cphc.201900326},
doi = {10.1002/cphc.201900326},
issn = {1439-4235},
year = {2019},
date = {2019-05-21},
journal = {ChemPhysChem},
volume = {20},
number = {18},
pages = {2340-2347},
abstract = {Abstract Many 2D covalent polymers synthesized as single layers on surfaces show inherent disorder, expressed for example in their ring-size distribution. Systems which are expected to form the thermodynamically favored hexagonal lattice usually deviate from crystallinity and include high numbers of pentagons, heptagons, and rings of other sizes. The amorphous structure of two different covalent polymers in real space using scanning tunneling microscopy is investigated. Molecular dynamics simulations are employed to extract additional information. We show that short-range correlations exist in the structure of one polymer, i. e. that polygons are not tessellating the surface randomly but that ring neighborhoods have preferential compositions. The correlation is dictated by the energy of formation of the ring neighborhoods.},
keywords = {Foundry Organic},
pubstate = {published},
tppubtype = {article}
}
B Garlyyev, K Kratzl, M Rück, J Michalička, J Fichtner, J M Macak, T Kratky, S Günther, M Cokoja, A S Bandarenka, A Gagliardi, R A Fischer
Optimizing the Size of Platinum Nanoparticles for Enhanced Mass Activity in the Electrochemical Oxygen Reduction Reaction Journal Article
In: Angewandte Chemie International Edition, vol. 58, no. 28, pp. 9596-9600, 2019, ISSN: 1433-7851.
Abstract | Links | Tags: Foundry Organic, Solid-Liquid
@article{,
title = {Optimizing the Size of Platinum Nanoparticles for Enhanced Mass Activity in the Electrochemical Oxygen Reduction Reaction},
author = {B Garlyyev and K Kratzl and M R\"{u}ck and J Michali\v{c}ka and J Fichtner and J M Macak and T Kratky and S G\"{u}nther and M Cokoja and A S Bandarenka and A Gagliardi and R A Fischer},
url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/anie.201904492},
doi = {10.1002/anie.201904492},
issn = {1433-7851},
year = {2019},
date = {2019-05-03},
journal = {Angewandte Chemie International Edition},
volume = {58},
number = {28},
pages = {9596-9600},
abstract = {Abstract High oxygen reduction (ORR) activity has been for many years considered as the key to many energy applications. Herein, by combining theory and experiment we prepare Pt nanoparticles with optimal size for the efficient ORR in proton-exchange-membrane fuel cells. Optimal nanoparticle sizes are predicted near 1, 2, and 3 nm by computational screening. To corroborate our computational results, we have addressed the challenge of approximately 1 nm sized Pt nanoparticle synthesis with a metal\textendashorganic framework (MOF) template approach. The electrocatalyst was characterized by HR-TEM, XPS, and its ORR activity was measured using a rotating disk electrode setup. The observed mass activities (0.87±0.14 A mgPt−1) are close to the computational prediction (0.99 A mgPt−1). We report the highest to date mass activity among pure Pt catalysts for the ORR within similar size range. The specific and mass activities are twice as high as the Tanaka commercial Pt/C catalysis.},
keywords = {Foundry Organic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
T Schröder, M B Scheible, F Steiner, J Vogelsang, P Tinnefeld
Interchromophoric Interactions Determine the Maximum Brightness Density in DNA Origami Structures Journal Article
In: Nano Letters, vol. 19, no. 2, pp. 1275-1281, 2019, ISSN: 1530-6984.
Abstract | Links | Tags: Foundry Organic, Molecularly-Functionalized
@article{,
title = {Interchromophoric Interactions Determine the Maximum Brightness Density in DNA Origami Structures},
author = {T Schr\"{o}der and M B Scheible and F Steiner and J Vogelsang and P Tinnefeld},
url = {https://doi.org/10.1021/acs.nanolett.8b04845},
doi = {10.1021/acs.nanolett.8b04845},
issn = {1530-6984},
year = {2019},
date = {2019-02-13},
urldate = {2019-02-13},
journal = {Nano Letters},
volume = {19},
number = {2},
pages = {1275-1281},
abstract = {An ideal point light source is as small and as bright as possible. For fluorescent point light sources, homogeneity of the light sources is important as well as that the fluorescent units inside the light source maintain their photophysical properties, which is compromised by dye aggregation. Here we propose DNA origami as a rigid scaffold to arrange dye molecules in a dense pixel array with high control of stoichiometry and dye\textendashdye interactions. In order to find the highest labeling density in a DNA origami structure without influencing dye photophysics, we alter the distance of two ATTO647N dyes in single base pair steps and probe the dye\textendashdye interactions on the single-molecule level. For small distances strong quenching in terms of intensity and fluorescence lifetime is observed. With increasing distance, we observe reduced quenching and molecular dynamics. However, energy transfer processes in the weak coupling regime still have a significant impact and can lead to quenching by singlet-dark-state-annihilation. Our study fills a gap of studying the interactions of dyes relevant for superresolution microscopy with dense labeling and for single-molecule biophysics. Incorporating these findings in a 3D DNA origami object will pave the way to bright and homogeneous DNA origami nanobeads.},
keywords = {Foundry Organic, Molecularly-Functionalized},
pubstate = {published},
tppubtype = {article}
}
M Dann, E M Ortiz, M Thomas, A Guljamow, M Lehmann, H Schaefer, D Leister
Enhancing photosynthesis at high light levels by adaptive laboratory evolution Journal Article
In: Nature Plants, vol. 7, no. 5, pp. 681-+, 0000, ISSN: 2055-026X.
Links | Tags: Foundry Organic, Molecularly-Functionalized
@article{nokey,
title = {Enhancing photosynthesis at high light levels by adaptive laboratory evolution},
author = {M Dann and E M Ortiz and M Thomas and A Guljamow and M Lehmann and H Schaefer and D Leister},
url = {\<Go to ISI\>://WOS:000646516500001},
doi = {10.1038/s41477-021-00904-2},
issn = {2055-026X},
journal = {Nature Plants},
volume = {7},
number = {5},
pages = {681-+},
keywords = {Foundry Organic, Molecularly-Functionalized},
pubstate = {published},
tppubtype = {article}
}
M Betker, C Harder, E Erbes, J E Heger, A E Alexakis, B Sochor, Q Chen, M Schwartzkopf, V Körstgens, P Müller-Buschbaum, K Schneider, S A Techert, L D Söderberg, S V Roth
Sprayed Hybrid Cellulose Nanofibril–Silver Nanowire Transparent Electrodes for Organic Electronic Applications Journal Article
In: ACS Applied Nano Materials, vol. 6, no. 14, pp. 13677-13688, 0000.
Abstract | Links | Tags: Foundry Organic
@article{nokey,
title = {Sprayed Hybrid Cellulose Nanofibril\textendashSilver Nanowire Transparent Electrodes for Organic Electronic Applications},
author = {M Betker and C Harder and E Erbes and J E Heger and A E Alexakis and B Sochor and Q Chen and M Schwartzkopf and V K\"{o}rstgens and P M\"{u}ller-Buschbaum and K Schneider and S A Techert and L D S\"{o}derberg and S V Roth},
url = {https://doi.org/10.1021/acsanm.3c02496},
doi = {10.1021/acsanm.3c02496},
journal = {ACS Applied Nano Materials},
volume = {6},
number = {14},
pages = {13677-13688},
abstract = {In times of climate change and resource scarcity, researchers are aiming to find sustainable alternatives to synthetic polymers for the fabrication of biodegradable, eco-friendly, and, at the same time, high-performance materials. Nanocomposites have the ability to combine several favorable properties of different materials in a single device. Here, we evaluate the suitability of two kinds of inks containing silver nanowires for the fast, facile, and industrial-relevant fabrication of two different types of cellulose-based silver nanowire electrodes via layer-by-layer spray deposition only. The Type I electrode has a layered structure, which is composed of a network of silver nanowires sprayed on top of a cellulose nanofibrils layer, while the Type II electrode consists of a homogeneous mixture of silver nanowires and cellulose nanofibrils. A correlation between the surface structure, conductivity, and transparency of both types of electrodes is established. We use the Haacke figure of merit for transparent electrode materials to demonstrate the favorable influence of cellulose nanofibrils in the spray ink by identifying Type II as the electrode with the lowest sheet resistance (minimum 5 ± 0.04 Ω/sq), while at the same time having a lower surface roughness and shorter fabrication time than Type I. Finally, we prove the mechanical stability of the Type II electrode by bending tests and its long-time stability under ambient conditions. The results demonstrate that the mixed spray ink of silver nanowires and cellulose nanofibrils is perfectly suitable for the fast fabrication of highly conductive organic nanoelectronics on an industrial scale.},
keywords = {Foundry Organic},
pubstate = {published},
tppubtype = {article}
}
M L Leidl, C Sachse, K Muller-Caspary
Dynamical scattering in ice-embedded proteins in conventional and scanning transmission electron microscopy Journal Article
In: IUCrJ, vol. 10, no. 4, pp. 475-486, 0000, ISSN: 2052-2525.
Abstract | Links | Tags: Foundry Inorganic, Foundry Organic
@article{nokey,
title = {Dynamical scattering in ice-embedded proteins in conventional and scanning transmission electron microscopy},
author = {M L Leidl and C Sachse and K Muller-Caspary},
url = {https://doi.org/10.1107/S2052252523004505},
doi = {doi:10.1107/S2052252523004505},
issn = {2052-2525},
journal = {IUCrJ},
volume = {10},
number = {4},
pages = {475-486},
abstract = {Structure determination of biological macromolecules using cryogenic electron microscopy is based on applying the phase object (PO) assumption and the weak phase object (WPO) approximation to reconstruct the 3D potential density of the molecule. To enhance the understanding of image formation of protein complexes embedded in glass-like ice in a transmission electron microscope, this study addresses multiple scattering in tobacco mosaic virus (TMV) specimens. This includes the propagation inside the molecule while also accounting for the effect of structural noise. The atoms in biological macromolecules are light but are distributed over several nanometres. Commonly, PO and WPO approximations are used in most simulations and reconstruction models. Therefore, dynamical multislice simulations of TMV specimens embedded in glass-like ice were performed based on fully atomistic molecular-dynamics simulations. In the first part, the impact of multiple scattering is studied using different numbers of slices. In the second part, different sample thicknesses of the ice-embedded TMV are considered in terms of additional ice layers. It is found that single-slice models yield full frequency transfer up to a resolution of 2.5 A, followed by attenuation up to 1.4 A. Three slices are sufficient to reach an information transfer up to 1.0 A. In the third part, ptychographic reconstructions based on scanning transmission electron microscopy (STEM) and single-slice models are compared with conventional TEM simulations. The ptychographic reconstructions do not need the deliberate introduction of aberrations, are capable of post-acquisition aberration correction and promise benefits for information transfer, especially at resolutions beyond 1.8 A.},
keywords = {Foundry Inorganic, Foundry Organic},
pubstate = {published},
tppubtype = {article}
}
S Alam, H Aldosari, C E Petoukhoff, T Váry, W Althobaiti, M Alqurashi, H Tang, J I Khan, V Nádaždy, P Müller-Buschbaum, G C Welch, F Laquai
Thermally-Induced Degradation in PM6:Y6-Based Bulk Heterojunction Organic Solar Cells Journal Article
In: Advanced Functional Materials, vol. n/a, no. n/a, pp. 2308076, 0000, ISSN: 1616-301X.
Abstract | Links | Tags: Foundry Organic, Solid-Solid
@article{nokey,
title = {Thermally-Induced Degradation in PM6:Y6-Based Bulk Heterojunction Organic Solar Cells},
author = {S Alam and H Aldosari and C E Petoukhoff and T V\'{a}ry and W Althobaiti and M Alqurashi and H Tang and J I Khan and V N\'{a}da\v{z}dy and P M\"{u}ller-Buschbaum and G C Welch and F Laquai},
url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adfm.202308076},
doi = {https://doi.org/10.1002/adfm.202308076},
issn = {1616-301X},
journal = {Advanced Functional Materials},
volume = {n/a},
number = {n/a},
pages = {2308076},
abstract = {Abstract Thermally induced degradation of organic photovoltaic devices hinders the commercialization of this emerging PV technology. Thus, a precise understanding of the origin of thermal device instability, as well as identifying strategies to circumvent degradation is of utmost importance. Here, it investigates thermally-induced degradation of state-of-the-art PBDB-T-2F (PM6):BTP (Y6) bulk heterojunction solar cells at different temperatures and reveal changes of their optical properties, photophysics, and morphology. The open-circuit voltage and fill factor of thermally degraded devices are limited by dissociation and charge collection efficiency differences, while the short-circuit current density is only slightly affected. Energy-resolved electrochemical impedance spectroscopy measurements reveal that thermally degraded samples exhibit a higher energy barrier for the charge-transfer state to charge-separated state conversion. Furthermore, the field dependence of charge generation, recombination, and extraction are studied by time-delayed collection field and transient photocurrent and photovoltage experiments, indicating significant bimolecular recombination limits device performance. Finally, coupled optical-electrical device simulations are conducted to fit the devices’ current-voltage characteristics, enabling us to find useful correlations between optical and electrical properties of the active layers and device performance parameters.},
keywords = {Foundry Organic, Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
M Alarcón-Correa, L Kilwing, F Peter, T Liedl, P Fischer
Platinum-DNA Origami Hybrid Structures in Concentrated Hydrogen Peroxide Journal Article
In: ChemPhysChem, vol. 24, no. 22, pp. e202300294, 0000, ISSN: 1439-4235.
Abstract | Links | Tags: Foundry Organic, Molecularly-Functionalized
@article{nokey,
title = {Platinum-DNA Origami Hybrid Structures in Concentrated Hydrogen Peroxide},
author = {M Alarc\'{o}n-Correa and L Kilwing and F Peter and T Liedl and P Fischer},
url = {https://chemistry-europe.onlinelibrary.wiley.com/doi/abs/10.1002/cphc.202300294},
doi = {https://doi.org/10.1002/cphc.202300294},
issn = {1439-4235},
journal = {ChemPhysChem},
volume = {24},
number = {22},
pages = {e202300294},
abstract = {Abstract The DNA origami technique allows fast and large-scale production of DNA nanostructures that stand out with an accurate addressability of their anchor points. This enables the precise organization of guest molecules on the surfaces and results in diverse functionalities. However, the compatibility of DNA origami structures with catalytically active matter, a promising pathway to realize autonomous DNA machines, has so far been tested only in the context of bio-enzymatic activity, but not in chemically harsh reaction conditions. The latter are often required for catalytic processes involving high-energy fuels. Here, we provide proof-of-concept data showing that DNA origami structures are stable in 5 % hydrogen peroxide solutions over the course of at least three days. We report a protocol to couple these to platinum nanoparticles and show catalytic activity of the hybrid structures. We suggest that the presented hybrid structures are suitable to realize catalytic nanomachines combined with precisely engineered DNA nanostructures.},
keywords = {Foundry Organic, Molecularly-Functionalized},
pubstate = {published},
tppubtype = {article}
}
S Caicedo-Dávila, A Cohen, S G Motti, M Isobe, K M Mccall, M V Kovalenko, O Yaffe, L M Herz, D H Fabini, D A Egger
Disentangling the Effects of Structure and Lone-Pair Electrons in the Lattice Dynamics of Halide Perovskites Journal Article
In: arXiv preprint arXiv:2310.03408, 0000.
Abstract | Links | Tags: Foundry Organic
@article{nokey,
title = {Disentangling the Effects of Structure and Lone-Pair Electrons in the Lattice Dynamics of Halide Perovskites},
author = {S Caicedo-D\'{a}vila and A Cohen and S G Motti and M Isobe and K M Mccall and M V Kovalenko and O Yaffe and L M Herz and D H Fabini and D A Egger},
url = {https://arxiv.org/abs/2310.03408},
doi = {https://doi.org/10.48550/arXiv.2310.03408},
journal = {arXiv preprint arXiv:2310.03408},
abstract = {Metal halide perovskites have shown great performance as solar energy materials, but their outstanding optoelectronic properties are paired with unusually strong anharmonic effects. It has been proposed that this intriguing combination of properties derives from the "lone pair" electrons of the octahedral metal cations, but the precise impact of this chemical feature remains unclear. Here we show that in fact a lone pair of electrons is not a prerequisite for the strong anharmonicity and low-energy lattice dynamics encountered in this class of materials. We combine X-ray diffraction, infrared and Raman spectroscopies, and first-principles molecular dynamics calculations to directly contrast the lattice dynamics of CsSrBr3 with those of CsPbBr3, two compounds which bear close structural similarity but with the former lacking lone pairs on the octahedral metal. We exploit low-frequency diffusive Raman scattering, nominally symmetry-forbidden in the cubic phase, as a fingerprint to detect anharmonicity and reveal that low-frequency tilting occurs irrespective of lone pair presence. This work highlights the key role of structure in perovskite lattice dynamics, providing important design rules for the emerging class of soft perovskite semiconductors for optoelectronic and light-harvesting devices.},
keywords = {Foundry Organic},
pubstate = {published},
tppubtype = {article}
}
K Endo, A Raza, L Yao, S Van Gele, A Rodríguez-Camargo, H Vignolo-González, L Grunenberg, B Lotsch
Downsizing Porphyrin Covalent Organic Framework Particles Using Protected Precursors for Electrocatalytic CO2 Reduction Journal Article
In: 0000.
Abstract | Links | Tags: Foundry Organic, Molecularly-Functionalized
@article{nokey,
title = {Downsizing Porphyrin Covalent Organic Framework Particles Using Protected Precursors for Electrocatalytic CO2 Reduction},
author = {K Endo and A Raza and L Yao and S Van Gele and A Rodr\'{i}guez-Camargo and H Vignolo-Gonz\'{a}lez and L Grunenberg and B Lotsch},
url = {https://chemrxiv.org/engage/chemrxiv/article-details/64d12052dfabaf06ffe07a6d},
doi = {10.26434/chemrxiv-2023-skm06},
abstract = {Covalent organic frameworks (COFs) are promising electrocatalyst platforms owing to their designability, porosity, and stability. Recently, COFs with various chemical structures were developed as efficient electrochemical CO2 reduction catalysts. However, controlling the morphology of COF catalysts remains a challenge, which can limit their electrocatalytic performance even if the chemical structure is optimally designed. Especially, while metalated porphyrinoids show great promise as catalytically active COF building blocks, their intermolecular stacking and coordination interactions make it difficult to conduct solution-based COF synthesis which can control the particle size dominated by the aggregation of crystallites. In this work, we report a new synthetic methodology for rationally downsized COF catalyst particles, where a tritylated amine is employed as a novel protected precursor for COF synthesis. Trityl protection provides high solubility to a representative cobalt porphyrin precursor, while its deprotection proceeds in situ under typical solvothermal COF synthesis conditions. This colloidal deprotection\textendashpolycondensation process yields smaller COF particles with less crystallite aggregation than a conventional synthesis, maintaining crystallinity and porosity. The downsized COF particles exhibit superior catalytic performance in electrochemical CO2 reduction, with higher CO production rate and faradaic efficiency with similar stability compared to conventional COF particles. The improved performance of downsized COF particles is attributed to the higher contact area with a conductive agent. This study provides a strategy for the preparation of COF electrocatalysts with controlled morphology and enhanced performance and also reveals an important factor in the evaluation of COF electrocatalysts.},
keywords = {Foundry Organic, Molecularly-Functionalized},
pubstate = {published},
tppubtype = {article}
}
T Guan, W Chen, H Tang, D Li, X Wang, C L Weindl, Y Wang, Z Liang, S Liang, T Xiao, S Tu, S V Roth, L Jiang, P Müller-Buschbaum
Decoding the Self-Assembly Plasmonic Interface Structure in a PbS Colloidal Quantum Dot Solid for a Photodetector Journal Article
In: ACS Nano, vol. 17, no. 22, pp. 23010-23019, 0000, ISSN: 1936-0851.
Abstract | Links | Tags: Foundry Organic, Solid-Solid
@article{nokey,
title = {Decoding the Self-Assembly Plasmonic Interface Structure in a PbS Colloidal Quantum Dot Solid for a Photodetector},
author = {T Guan and W Chen and H Tang and D Li and X Wang and C L Weindl and Y Wang and Z Liang and S Liang and T Xiao and S Tu and S V Roth and L Jiang and P M\"{u}ller-Buschbaum},
url = {https://doi.org/10.1021/acsnano.3c08526},
doi = {10.1021/acsnano.3c08526},
issn = {1936-0851},
journal = {ACS Nano},
volume = {17},
number = {22},
pages = {23010-23019},
abstract = {Hybrid plasmonic nanostructures have gained enormous attention in a variety of optoelectronic devices due to their surface plasmon resonance properties. Self-assembled hybrid metal/quantum dot (QD) architectures offer a means of coupling the properties of plasmonics and QDs to photodetectors, thereby modifying their functionality. The arrangement and localization of hybrid nanostructures have an impact on exciton trapping and light harvesting. Here, we present a hybrid structure consisting of self-assembled gold nanospheres (Au NSs) embedded in a solid matrix of PbS QDs for mapping the interface structures and the motion of charge carriers. Grazing-incidence small-angle X-ray scattering is utilized to analyze the localization and spacing of the Au NSs within the hybrid structure. Furthermore, by correlating the morphology of the Au NSs in the hybrid structure with the corresponding differences observed in the performance of photodetectors, we are able to determine the impact of interface charge carrier dynamics in the coupling structure. From the perspective of architecture, our study provides insights into the performance improvement of optoelectronic devices.},
keywords = {Foundry Organic, Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
P Hosseini, A Rodríguez-Camargo, L Yao, B Lotsch, K Tschulik
Identifying the active species in a cobalt-based covalent organic framework for the electrochemical oxygen evolution reaction Journal Article
In: 0000.
Abstract | Links | Tags: Foundry Organic, Molecularly-Functionalized
@article{nokey,
title = {Identifying the active species in a cobalt-based covalent organic framework for the electrochemical oxygen evolution reaction},
author = {P Hosseini and A Rodr\'{i}guez-Camargo and L Yao and B Lotsch and K Tschulik},
url = {https://chemrxiv.org/engage/chemrxiv/article-details/650cfd18b927619fe79761cb},
doi = {10.26434/chemrxiv-2023-7dl21},
abstract = {While considerable efforts have been devoted to developing functionalized covalent organic frameworks (COFs) as oxygen evolution electrocatalysts in recent years, studies related to the identification of the true catalytically active species for the oxygen evolution reaction (OER) remain lacking in the field. In this work, we investigated the active species of a cobalt-functionalized COF (TpBpy-Co) as electrochemical OER catalyst through a series of electrochemical measurements and post-electrolysis characterizations. Our results demonstrate that Co(II) ions, coordinated to the COF backbone, are transformed to cobalt-based nanoparticles when exposing TpBpy-Co to alkaline media. These nanoparticles act as the true active species for oxygen evolution. It remains unclear whether intact TpBpy-Co acts as a secondary catalytic species, due to its structural instability in alkaline electrolyte and its inferred lower catalytic activity compared to cobalt-based nanoparticles. Our results highlight that caution is warranted when identifying the active species for COF electrocatalysts formed under catalyst working conditions. Specifically, strong coordination between COFs and metal centers under electrochemical operation conditions is crucial to avoid unintended transformation of COF electrocatalysts. Our study thus contributes to the rational development of earth-abundant COF OER catalysts for the production of green hydrogen from renewable resources.},
keywords = {Foundry Organic, Molecularly-Functionalized},
pubstate = {published},
tppubtype = {article}
}
Z Lou, J Tao, B Wei, X Jiang, S Cheng, Z Wang, C Qin, R Liang, H Guo, L Zhu, P Müller-Buschbaum, H-M Cheng, X Xu
Near-Infrared Organic Photodetectors toward Skin-Integrated Photoplethysmography-Electrocardiography Multimodal Sensing System Journal Article
In: Advanced Science, vol. n/a, no. n/a, pp. 2304174, 0000, ISSN: 2198-3844.
Abstract | Links | Tags: Foundry Organic, Solid-Solid
@article{nokey,
title = {Near-Infrared Organic Photodetectors toward Skin-Integrated Photoplethysmography-Electrocardiography Multimodal Sensing System},
author = {Z Lou and J Tao and B Wei and X Jiang and S Cheng and Z Wang and C Qin and R Liang and H Guo and L Zhu and P M\"{u}ller-Buschbaum and H-M Cheng and X Xu},
url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/advs.202304174},
doi = {https://doi.org/10.1002/advs.202304174},
issn = {2198-3844},
journal = {Advanced Science},
volume = {n/a},
number = {n/a},
pages = {2304174},
abstract = {Abstract In the fast-evolving landscape of decentralized and personalized healthcare, the need for multimodal biosensing systems that integrate seamlessly with the human body is growing rapidly. This presents a significant challenge in devising ultraflexible configurations that can accommodate multiple sensors and designing high-performance sensing components that remain stable over long periods. To overcome these challenges, ultraflexible organic photodetectors (OPDs) that exhibit exceptional performance under near-infrared illumination while maintaining long-term stability are developed. These ultraflexible OPDs demonstrate a photoresponsivity of 0.53 A W−1 under 940 nm, shot-noise-limited specific detectivity of 3.4 × 1013 Jones, and cut-off response frequency beyond 1 MHz at −3 dB. As a result, the flexible photoplethysmography sensor boasts a high signal-to-noise ratio and stable peak-to-peak amplitude under hypoxic and hypoperfusion conditions, outperforming commercial finger pulse oximeters. This ensures precise extraction of blood oxygen saturation in dynamic working conditions. Ultraflexible OPDs are further integrated with conductive polymer electrodes on an ultrathin hydrogel substrate, allowing for direct interface with soft and dynamic skin. This skin-integrated sensing platform provides accurate measurement of photoelectric and biopotential signals in a time-synchronized manner, reproducing the functionality of conventional technologies without their inherent limitations.},
keywords = {Foundry Organic, Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
X Ma, D J Zheng, S Hou, S Mukherjee, R Khare, G Gao, Q Ai, B Garlyyev, W Li, M Koch, J Mink, Y Shao-Horn, J Warnan, A S Bandarenka, R A Fischer
Structure–Activity Relationships in Ni- Carboxylate-Type Metal–Organic Frameworks’ Metamorphosis for the Oxygen Evolution Reaction Journal Article
In: ACS Catalysis, vol. 13, no. 11, pp. 7587-7596, 0000.
Abstract | Links | Tags: Foundry Organic, Molecularly-Functionalized
@article{nokey,
title = {Structure\textendashActivity Relationships in Ni- Carboxylate-Type Metal\textendashOrganic Frameworks’ Metamorphosis for the Oxygen Evolution Reaction},
author = {X Ma and D J Zheng and S Hou and S Mukherjee and R Khare and G Gao and Q Ai and B Garlyyev and W Li and M Koch and J Mink and Y Shao-Horn and J Warnan and A S Bandarenka and R A Fischer},
url = {https://doi.org/10.1021/acscatal.3c00625},
doi = {10.1021/acscatal.3c00625},
journal = {ACS Catalysis},
volume = {13},
number = {11},
pages = {7587-7596},
abstract = {Metal\textendashorganic frameworks (MOFs) have been reported to catalyze the oxygen evolution reaction (OER). Despite the established links between the pristine MOFs and their derived metal hydroxide electrocatalysts, several limitations still preclude understanding of the critical factors determining the OER performance. Of prime importance appears the choice of MOF and how its compositions relate to the catalyst stability and in turn to the reconstruction or metamorphosis mechanisms into the active species under OER conditions. An isoreticular series of Ni-carboxylate-type MOFs [Ni2(OH)2L] was chosen to elucidate the effects of the carboxylate linker length expansion and modulation of the linker\textendashlinker π\textendashπ interactions (L = 1,4-benzodicarboxylate, 2,6-napthalenedicarboxylate, biphenyl-4,4′-dicarboxylate, and p-terphenyl-4,4″-dicarboxylate). Degradation and reconstruction of MOFs were systematically investigated. The linker controls the transformation of Ni-MOF into distinct nickel hydroxide phases, and the conversion from α-Ni(OH)2 to β-Ni(OH)2, thus correlating the Ni-MOF composition with the OER activity of the Ni-MOF-derived metastable nickel hydroxide phase mixture.},
keywords = {Foundry Organic, Molecularly-Functionalized},
pubstate = {published},
tppubtype = {article}
}
A L Oechsle, T Schöner, C Geiger, S Tu, P Wang, R Cubitt, P Müller-Buschbaum
In: Macromolecules, vol. 56, no. 22, pp. 9117-9126, 0000, ISSN: 0024-9297.
Abstract | Links | Tags: Foundry Organic, Solid-Solid
@article{nokey,
title = {Unraveling the Humidity Influence on the Electrical Properties of Ionic Liquid Posttreated Poly(3,4-ethylene dioxythiophene):Poly(styrenesulfonate) Films},
author = {A L Oechsle and T Sch\"{o}ner and C Geiger and S Tu and P Wang and R Cubitt and P M\"{u}ller-Buschbaum},
url = {https://doi.org/10.1021/acs.macromol.3c01842},
doi = {10.1021/acs.macromol.3c01842},
issn = {0024-9297},
journal = {Macromolecules},
volume = {56},
number = {22},
pages = {9117-9126},
abstract = {The conductive polymer blend poly(3,4-ethylene dioxythiophene):poly(styrenesulfonate) (PEDOT:PSS), popular for numerous organic applications, is investigated in terms of the influences that ionic liquid (IL) treatment and ambient humidity have on its conductivity properties. PEDOT:PSS thin films posttreated with different concentrations of the IL 1-ethyl-3-methylimidazolium dicyanamide (EMIM DCA) are exposed to different relative humidity (RH) steps from 0% RH up to 90% RH. Simultaneously, the film swelling and increase in the scattering length density (SLD), indicating a water uptake of the films, are monitored in situ with spectral reflectance (SR) and time-of-flight neutron reflectometry (ToF-NR). Additional in situ electrochemical impedance spectroscopy (EIS) shows that the pristine PEDOT:PSS has only an electronic conductivity, while for the IL-treated samples, an additional ionic conductivity contribution is observed. Upon humidity increase, the electronic conductivity of all PEDOT:PSS thin films decreases, while the ionic conductivity for IL posttreated thin films is enhanced by the intake of water molecules.},
keywords = {Foundry Organic, Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
C L M Palenzuela, D Spurling, A Szalai, T Schröder, V Nicolosi, P Tinnefeld
MXene-induced nonradiative energy transfer Journal Article
In: 0000.
Abstract | Links | Tags: Foundry Organic, Molecularly-Functionalized
@article{nokey,
title = {MXene-induced nonradiative energy transfer},
author = {C L M Palenzuela and D Spurling and A Szalai and T Schr\"{o}der and V Nicolosi and P Tinnefeld},
url = {https://chemrxiv.org/engage/chemrxiv/article-details/6544ea8948dad23120fe8d2a},
doi = {10.26434/chemrxiv-2023-r54g8},
abstract = {Since their discovery in 2011, MXenes have risen to prominence for energy storage, electromagnetic shielding, and optoelectronics. Yet, the nonradiative energy transfer properties of this family of 2D materials remain elusive, which may have implications in optoelectronics, photovoltaics and biosensing. Here, we use single-molecule fluorescence confocal microscopy and DNA origami nanopositioners to investigate, for the first time, the distance-dependent energy transfer of an organic emitter (ATTO 542) placed on transparent thin films made of spincast Ti3C2Tx flakes. We propose a specific immobilization chemistry for DNA origami nanostructures based on glycine-MXene interaction, allowing us to precisely control their orientation on the surface. Each DNA origami structure is designed to carry a single dye molecule at predetermined heights. Our findings reveal that when the dye is located at distances of 1 nm \< d \< 8 nm from the surface, the fluorescence is quenched following a distance dependence of d-3. This is in agreement with the F\"{o}rster-type mechanism of energy transfer in transparent conductors at the bulk level. 50% of energy transfer efficiency is reached at 2.7 nm (d0). MXenes could therefore be used as short-distance spectroscopic nanorulers, sensitive at a distance regime that common energy transfer tools cannot access.},
keywords = {Foundry Organic, Molecularly-Functionalized},
pubstate = {published},
tppubtype = {article}
}