D Han, S Chen, M-H Du
In: The Journal of Physical Chemistry Letters, vol. 12, no. 40, pp. 9754-9760, 2021.
Abstract | Links | Tags: Foundry Inorganic
@article{nokey,
title = {Role of Polycyclic Aromatic Alkylammonium Cations in Tuning the Electronic Properties and Band Alignment of Two-Dimensional Hybrid Perovskite Semiconductors},
author = {D Han and S Chen and M-H Du},
url = {https://doi.org/10.1021/acs.jpclett.1c02603},
doi = {10.1021/acs.jpclett.1c02603},
year = {2021},
date = {2021-09-30},
journal = {The Journal of Physical Chemistry Letters},
volume = {12},
number = {40},
pages = {9754-9760},
abstract = {Two-dimensional hybrid organic\textendashinorganic perovskites (HOIPs) have recently drawn intense attention as potential photovoltaic materials. However},
keywords = {Foundry Inorganic},
pubstate = {published},
tppubtype = {article}
}
O E Dagdeviren, D Glass, R Sapienza, E Cortés, S A Maier, I P Parkin, P Grütter, R Quesada-Cabrera
The Effect of Photoinduced Surface Oxygen Vacancies on the Charge Carrier Dynamics in TiO2 Films Journal Article
In: Nano Letters, vol. 21, no. 19, pp. 8348-8354, 2021, ISSN: 1530-6984.
Abstract | Links | Tags: Solid-Solid
@article{nokey,
title = {The Effect of Photoinduced Surface Oxygen Vacancies on the Charge Carrier Dynamics in TiO2 Films},
author = {O E Dagdeviren and D Glass and R Sapienza and E Cort\'{e}s and S A Maier and I P Parkin and P Gr\"{u}tter and R Quesada-Cabrera},
url = {https://doi.org/10.1021/acs.nanolett.1c02853},
doi = {10.1021/acs.nanolett.1c02853},
issn = {1530-6984},
year = {2021},
date = {2021-09-28},
journal = {Nano Letters},
volume = {21},
number = {19},
pages = {8348-8354},
abstract = {Metal-oxide semiconductors (MOS) are widely utilized for catalytic and photocatalytic applications in which the dynamics of charged carriers (e.g., electrons, holes) play important roles. Under operation conditions, photoinduced surface oxygen vacancies (PI-SOV) can greatly impact the dynamics of charge carriers. However, current knowledge regarding the effect of PI-SOV on the dynamics of hole migration in MOS films, such as titanium dioxide, is solely based upon volume-averaged measurements and/or vacuum conditions. This limits the basic understanding of hole-vacancy interactions, as they are not capable of revealing time-resolved variations during operation. Here, we measured the effect of PI-SOV on the dynamics of hole migration using time-resolved atomic force microscopy. Our findings demonstrate that the time constant associated with hole migration is strongly affected by PI-SOV, in a reversible manner. These results will nucleate an insightful understanding of the physics of hole dynamics and thus enable emerging technologies, facilitated by engineering hole-vacancy interactions.},
keywords = {Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
S Pratap, F Babbe, N S Barchi, Z Yuan, T Luong, Z Haber, T-B Song, J L Slack, C V Stan, N Tamura, C M Sutter-Fella, P Müller-Buschbaum
Out-of-equilibrium processes in crystallization of organic-inorganic perovskites during spin coating Journal Article
In: Nature Communications, vol. 12, no. 1, pp. 5624, 2021, ISSN: 2041-1723.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{nokey,
title = {Out-of-equilibrium processes in crystallization of organic-inorganic perovskites during spin coating},
author = {S Pratap and F Babbe and N S Barchi and Z Yuan and T Luong and Z Haber and T-B Song and J L Slack and C V Stan and N Tamura and C M Sutter-Fella and P M\"{u}ller-Buschbaum},
url = {https://doi.org/10.1038/s41467-021-25898-5},
doi = {10.1038/s41467-021-25898-5},
issn = {2041-1723},
year = {2021},
date = {2021-09-24},
journal = {Nature Communications},
volume = {12},
number = {1},
pages = {5624},
abstract = {Complex phenomena are prevalent during the formation of materials, which affect their processing-structure-function relationships. Thin films of methylammonium lead iodide (CH3NH3PbI3, MAPI) are processed by spin coating, antisolvent drop, and annealing of colloidal precursors. The structure and properties of transient and stable phases formed during the process are reported, and the mechanistic insights of the underlying transitions are revealed by combining in situ data from grazing-incidence wide-angle X-ray scattering and photoluminescence spectroscopy. Here, we report the detailed insights on the embryonic stages of organic-inorganic perovskite formation. The physicochemical evolution during the conversion proceeds in four steps: i) An instant nucleation of polydisperse MAPI nanocrystals on antisolvent drop, ii) the instantaneous partial conversion of metastable nanocrystals into orthorhombic solvent-complex by cluster coalescence, iii) the thermal decomposition (dissolution) of the stable solvent-complex into plumboiodide fragments upon evaporation of solvent from the complex and iv) the formation (recrystallization) of cubic MAPI crystals in thin film.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
N Paul, J Huang, C Liu, T Lin, C Ouyang, Z Liu, C Chen, Z Chen, Z Weng, M Schwartzkopf, S V Roth, P Müller-Buschbaum, A Paul
Real-time observation of nucleation and growth of Au on CdSe quantum dot templates Journal Article
In: Scientific Reports, vol. 11, no. 1, pp. 18777, 2021, ISSN: 2045-2322.
Abstract | Links | Tags: Foundry Inorganic, Solid-Solid
@article{nokey,
title = {Real-time observation of nucleation and growth of Au on CdSe quantum dot templates},
author = {N Paul and J Huang and C Liu and T Lin and C Ouyang and Z Liu and C Chen and Z Chen and Z Weng and M Schwartzkopf and S V Roth and P M\"{u}ller-Buschbaum and A Paul},
url = {https://doi.org/10.1038/s41598-021-97485-z},
doi = {10.1038/s41598-021-97485-z},
issn = {2045-2322},
year = {2021},
date = {2021-09-21},
journal = {Scientific Reports},
volume = {11},
number = {1},
pages = {18777},
abstract = {Semiconductor quantum dot (QD) arrays can be useful for optical devices such as lasers, solar cells and light-emitting diodes. As the size distribution influences the band-gap, it is worthwhile to investigate QDs prepared using different solvents because each of them could influence the overall morphology differently, depending on the ligand network around individual QDs. Here, we follow the nucleation and growth of gold (Au) on CdSe QD arrays to investigate the influence of surface ligands and thereby realized interparticle distance between QDs on Au growth behaviour. We particularly emphasize on the monolayer stage as the Au decoration on individual QDs is expected at this stage. Therefore, we sputter-deposit Au on each QD array to investigate the morphological evolution in real-time using time-resolved grazing-incidence small-angle X-ray scattering (GISAXS). The growth kinetics - independent of the template - signifies that the observed template-mediated nucleation is limited only to the very first few monolayers. Delicate changes in the Au growth morphology are seen in the immediate steps following the initial replicated decoration of the QD arrays. This is followed by a subsequent clustering and finally a complete Au coverage of the QD arrays.},
keywords = {Foundry Inorganic, Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
C Qian, V Villafañe, P Soubelet, A Hötger, T Taniguchi, K Watanabe, N P Wilson, A V Stier, A W Holleitner, J J Finley
Non-Local Exciton-Photon Interactions in Hybrid High-Q Nanocavities with Embedded hBN-Encapsulated MoS2 Monolayers Journal Article
In: arXiv preprint arXiv:2107.04387, 2021.
Abstract | Links | Tags: Solid-Solid
@article{nokey,
title = {Non-Local Exciton-Photon Interactions in Hybrid High-Q Nanocavities with Embedded hBN-Encapsulated MoS2 Monolayers},
author = {C Qian and V Villafa\~{n}e and P Soubelet and A H\"{o}tger and T Taniguchi and K Watanabe and N P Wilson and A V Stier and A W Holleitner and J J Finley},
url = {https://arxiv.org/abs/2107.04387},
doi = {arXiv:2107.04387v2},
year = {2021},
date = {2021-09-20},
journal = {arXiv preprint arXiv:2107.04387},
abstract = {Atomically thin semiconductors can be readily integrated into a wide range of nanophotonic architectures for applications in quantum photonics and novel optoelectronic devices. We report the observation of non-local interactions of textitfree trions in pristine hBN/MoS2/hBN heterostructures coupled to single mode (Q \>104) quasi 0D nanocavities. The high excitonic and photonic quality of the interaction system stem from our integrated nanofabrication approach simultaneously with the hBN encapsulation and the maximized local cavity field amplitude within the MoS2 monolayer. We observe a non-monotonic temperature dependence of the cavity-trion interaction strength, consistent with the non-local light-matter interactions in which the free trion diffuse over lengthscales comparable to the cavity mode volume. Our approach can be generalized to other optically active 2D materials, opening the way towards harnessing novel light-matter interaction regimes for applications in quantum photonics.},
keywords = {Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
J Zhou, F Fang, W Chen, M Mei, P Liu, J Hao, H Tang, S Liang, W Lei, R Pan, J Cheng, P Müller-Buschbaum, X W Sun, W Cao, K Zheng, K Wang
Luminescent perovskite nanocrystal composites via in situ ligand polymerization towards display applications Journal Article
In: Journal of Materials Chemistry C, vol. 9, no. 41, pp. 14740-14748, 2021, ISSN: 2050-7526.
Abstract | Links | Tags: Foundry Inorganic
@article{nokey,
title = {Luminescent perovskite nanocrystal composites via in situ ligand polymerization towards display applications},
author = {J Zhou and F Fang and W Chen and M Mei and P Liu and J Hao and H Tang and S Liang and W Lei and R Pan and J Cheng and P M\"{u}ller-Buschbaum and X W Sun and W Cao and K Zheng and K Wang},
url = {http://dx.doi.org/10.1039/D1TC03775G},
doi = {10.1039/D1TC03775G},
issn = {2050-7526},
year = {2021},
date = {2021-09-17},
journal = {Journal of Materials Chemistry C},
volume = {9},
number = {41},
pages = {14740-14748},
abstract = {Luminescent inorganic perovskite nanocrystals (PeNCs) are promising in various optical applications, particularly in advanced lighting and displays. The instability of PeNCs and PeNC composites from different aspects hinder their practical applications. Many previous methods indicate that an intact and facile wrapping strategy could effectively address this challenge. In this work, we introduce an in situ ligand polymerization (ILP) method for the fabrication of PeNC composites. By introducing (3-aminopropyl)triethoxysilane (APTES) as the initial ligand of the PeNCs directly and polymethylhydrosiloxane (PMHS) as the monomer to form the polymerized matrix, a polymerized and hydrophobic SiO2 matrix structure is formed, which intrinsically protects the PeNCs against moisture-induced deterioration. The stability test indicates that the ILP composite powders demonstrate an improved stability against various solvent conditions and light exposure compared to the conventional PeNCs\textendashSiO2 composite. More importantly, the ILP composite exhibits an excellent compatibility with the acrylate solvent which is widely used for light-solidification in light converting film fabrication. The ILP composite film demonstrates an ultrastable operational performance in our standard test outperforming the conventional PeNCs\textendashSiO2 composite configuration. Thus, the ILP composite demonstrates great potential for use in advanced lighting and displays.},
keywords = {Foundry Inorganic},
pubstate = {published},
tppubtype = {article}
}
M Poblet, R Berté, H D Boggiano, Y Li, E Cortés, G Grinblat, S A Maier, A V Bragas
Acoustic Coupling between Plasmonic Nanoantennas: Detection and Directionality of Surface Acoustic Waves Journal Article
In: ACS Photonics, 2021.
Abstract | Links | Tags: Solid-Solid
@article{nokey,
title = {Acoustic Coupling between Plasmonic Nanoantennas: Detection and Directionality of Surface Acoustic Waves},
author = {M Poblet and R Bert\'{e} and H D Boggiano and Y Li and E Cort\'{e}s and G Grinblat and S A Maier and A V Bragas},
url = {https://doi.org/10.1021/acsphotonics.1c00741},
doi = {10.1021/acsphotonics.1c00741},
year = {2021},
date = {2021-09-17},
urldate = {2021-09-17},
journal = {ACS Photonics},
abstract = {Hypersound waves can be efficient mediators between optical signals at the nanoscale. Having phase velocities several orders of magnitude lower than the speed of light, they propagate with much shorter wavelengths and can be controlled, directed, and even focused in a very small region of space. This work shows how two optical nanoantennas can be coupled through an acoustic wave that propagates with a certain directionality. An “emitter” antenna is first optically excited to generate acoustic coherent phonons that launch surface acoustic waves through the underlying substrate. These waves travel until they are mechanically detected by a “receiver” nanoantenna whose oscillation produces a detectable optical signal. Generation and detection are studied in detail, and new designs are proposed to improve the directionality of the hypersonic surface acoustic wave.},
keywords = {Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
G Q Moretti, E Cortés, S A Maier, A V Bragas, G Grinblat
Engineering gallium phosphide nanostructures for efficient nonlinear photonics and enhanced spectroscopies Journal Article
In: Nanophotonics, no. 000010151520210388, 2021.
Links | Tags: Foundry Inorganic
@article{nokey,
title = {Engineering gallium phosphide nanostructures for efficient nonlinear photonics and enhanced spectroscopies},
author = {G Q Moretti and E Cort\'{e}s and S A Maier and A V Bragas and G Grinblat},
url = {https://doi.org/10.1515/nanoph-2021-0388},
doi = {doi:10.1515/nanoph-2021-0388},
year = {2021},
date = {2021-09-16},
journal = {Nanophotonics},
number = {000010151520210388},
keywords = {Foundry Inorganic},
pubstate = {published},
tppubtype = {article}
}
A Gouder, A Jimenez-Solano, N M Vargas-Barbosa, F Podjaski, B V Lotsch
Photo-memristive sensing with charge storing 2D carbon nitrides Journal Article
In: arXiv preprint arXiv:2109.06964, 2021.
Abstract | Links | Tags: Foundry Inorganic
@article{nokey,
title = {Photo-memristive sensing with charge storing 2D carbon nitrides},
author = {A Gouder and A Jimenez-Solano and N M Vargas-Barbosa and F Podjaski and B V Lotsch},
url = {https://arxiv.org/abs/2109.06964},
doi = {arXiv:2109.06964v1},
year = {2021},
date = {2021-09-14},
journal = {arXiv preprint arXiv:2109.06964},
abstract = {We report the charge storing 2D carbon nitride potassium poly(heptazine imide), K-PHI, as a direct memristive (bio)sensing platform. Memristive devices have the potential to innovate current (bio)electronic systems such as photo-electrochemical sensors by incorporating new sensing capabilities including non-invasive, wireless remote and time-delayed (memory) readout. We demonstrate a direct photomemristive sensing platform that capitalizes on K PHI's visible light bandgap, large oxidation potential and intrinsic optoionic light energy storage properties. Our system simultaneously enables analyte concentration information storage as well as potentiometric, impedimetric and coulo-metric readouts on the same material, with no additional reagents required. Utilizing the light-induced charge storage function of K-PHI, we demonstrate analyte sensing via charge accumulation and present various methods to write/erase this information from the material. Additionally, fully wireless colorimetric and fluorometric detection of the charged state of K-PHI is demonstrated and could facilitate its use as particle-based in-situ sensing probe. The various readout options of the K PHI's response enable us to adapt the sensitivities and dynamic ranges without modifying the sensor. We demonstrate these features using glucose as an example analyte over a wide range of concentrations (50 μM to 50 mM). Moreover, due to the strong oxidative power of K-PHI, this sensing platform is able to detect a large variety of organic or biologically relevant analytes. Since PHI is easily synthesized, based on earth abundant precursors, biocompatible, chemically robust and responsive to visible light, we anticipate that the sensing platform presented herein opens up novel memristive and neuromorphic functions.},
keywords = {Foundry Inorganic},
pubstate = {published},
tppubtype = {article}
}
Y Huang, T Xiao, Z Xie, J Zheng, Y Su, W Chen, K Liu, M Tang, J Zhu, P Müller-Buschbaum, L Li
Multistate Nonvolatile Metamirrors with Tunable Optical Chirality Journal Article
In: ACS Applied Materials & Interfaces, 2021, ISSN: 1944-8244.
Abstract | Links | Tags: Foundry Inorganic, Solid-Solid
@article{nokey,
title = {Multistate Nonvolatile Metamirrors with Tunable Optical Chirality},
author = {Y Huang and T Xiao and Z Xie and J Zheng and Y Su and W Chen and K Liu and M Tang and J Zhu and P M\"{u}ller-Buschbaum and L Li},
url = {https://doi.org/10.1021/acsami.1c14204},
doi = {10.1021/acsami.1c14204},
issn = {1944-8244},
year = {2021},
date = {2021-09-14},
urldate = {2021-09-14},
journal = {ACS Applied Materials \& Interfaces},
abstract = {Compared with conventional mirrors that behave as isotropic electromagnetic (EM) reflectors, metamirrors composed of periodically aligned artificial meta-atoms exhibit increased degrees of freedom for EM manipulations. However, the functionality of most metamirrors is fixed by design, and how to achieve active EM control is still elusive. Here, we propose a multistate metamirror based on the nonvolatile phase change material Ge2Sb2Te5 (GST) with four distinct functionalities that can be realized in the infrared region by exploiting the temperature-activated phase transition. When varying the crystallinity of GST, the metamirror has the capability to perform as a right-handed circular polarization chiral mirror, a narrowband achiral mirror, a left-handed circular polarization chiral mirror, or a broadband achiral mirror, respectively. The inner physics is further explained by the construction or cancellation of extrinsic two-dimensional chirality. As a proof of concept, experimental verification is carried out and the measured results agree well with their simulated counterparts. Such a multifunctional tunable metamirror could address a wide range of applications from sensing and spectroscopy to analytical chemistry and imaging.},
keywords = {Foundry Inorganic, Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
J Klein, M Florian, A Hötger, A Steinhoff, A Delhomme, T Taniguchi, K Watanabe, F Jahnke, A W Holleitner, M Potemski
Trions in MoS2 are quantum superpositions of intra-and intervalley spin states Journal Article
In: arXiv preprint arXiv:2109.06281, 2021.
Abstract | Links | Tags: Solid-Solid
@article{nokey,
title = {Trions in MoS2 are quantum superpositions of intra-and intervalley spin states},
author = {J Klein and M Florian and A H\"{o}tger and A Steinhoff and A Delhomme and T Taniguchi and K Watanabe and F Jahnke and A W Holleitner and M Potemski},
url = {https://arxiv.org/abs/2109.06281},
doi = {arXiv:2109.06281v1},
year = {2021},
date = {2021-09-13},
journal = {arXiv preprint arXiv:2109.06281},
abstract = {We report magneto-photoluminescence spectroscopy of gated MoS2 monolayers in high magnetic fields to 28 T. At B = 0T and electron density ns∼1012cm−2, we observe three trion resonances that cannot be explained within a single-particle picture. Employing ab initio calculations that take into account three-particle correlation effects as well as local and non-local electron-hole exchange interaction, we identify those features as quantum superpositions of inter- and intravalley spin states. We experimentally investigate the mixed character of the trion wave function via the filling factor dependent valley Zeeman shift in positive and negative magnetic fields. Our results highlight the importance of exchange interactions for exciton physics in monolayer MoS2 and provide new insights into the microscopic understanding of trion physics in 2D multi-valley semiconductors for low excess carrier densities.},
keywords = {Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
J Kröger, F Podjaski, G Savaşçı, I Moudrakovski, A Jimenez-Solano, M W Terban, S Bette, V Duppel, M Joos, A Senocrate
Conductivity mechanism in ionic 2D carbon nitrides: from hydrated ion motion to enhanced photocatalysis Journal Article
In: Cambridge University Press, 2021.
Tags: Foundry Inorganic, Molecularly-Functionalized
@article{nokey,
title = {Conductivity mechanism in ionic 2D carbon nitrides: from hydrated ion motion to enhanced photocatalysis},
author = {J Kr\"{o}ger and F Podjaski and G Sava\c{s}\c{c}ı and I Moudrakovski and A Jimenez-Solano and M W Terban and S Bette and V Duppel and M Joos and A Senocrate},
year = {2021},
date = {2021-09-12},
journal = {Cambridge University Press},
keywords = {Foundry Inorganic, Molecularly-Functionalized},
pubstate = {published},
tppubtype = {article}
}
S T Emmerling, R Schuldt, S Bette, L Yao, R E Dinnebier, J Kästner, B V Lotsch
Interlayer Interactions as Design Tool for Large-Pore COFs Journal Article
In: Journal of the American Chemical Society, vol. 143, no. 38, pp. 15711-15722, 2021, ISSN: 0002-7863.
Abstract | Links | Tags: Foundry Organic, Molecularly-Functionalized
@article{nokey,
title = {Interlayer Interactions as Design Tool for Large-Pore COFs},
author = {S T Emmerling and R Schuldt and S Bette and L Yao and R E Dinnebier and J K\"{a}stner and B V Lotsch},
url = {https://doi.org/10.1021/jacs.1c06518},
doi = {10.1021/jacs.1c06518},
issn = {0002-7863},
year = {2021},
date = {2021-09-08},
urldate = {2021-09-08},
journal = {Journal of the American Chemical Society},
volume = {143},
number = {38},
pages = {15711-15722},
abstract = {Covalent organic frameworks (COFs) with a pore size beyond 5 nm are still rarely seen in this emerging field. Besides obvious complications such as the elaborated synthesis of large linkers with sufficient solubility, more subtle challenges regarding large-pore COF synthesis, including pore occlusion and collapse, prevail. Here we present two isoreticular series of large-pore imine COFs with pore sizes up to 5.8 nm and correlate the interlayer interactions with the structure and thermal behavior of the COFs. By adjusting interlayer interactions through the incorporation of methoxy groups acting as pore-directing “anchors”, different stacking modes can be accessed, resulting in modified stacking polytypes and, hence, effective pore sizes. A strong correlation between stacking energy toward highly ordered, nearly eclipsed structures, higher structural integrity during thermal stress, and a novel, thermally induced phase transition of stacking modes in COFs was found, which sheds light on viable design strategies for increased structural control and stability in large-pore COFs.},
keywords = {Foundry Organic, Molecularly-Functionalized},
pubstate = {published},
tppubtype = {article}
}
A L Oechsle, J E Heger, N Li, S Yin, S Bernstorff, P Müller-Buschbaum
Correlation of Thermoelectric Performance, Domain Morphology and Doping Level in PEDOT:PSS Thin Films Post-Treated with Ionic Liquids Journal Article
In: Macromolecular Rapid Communications, vol. 42, no. 20, pp. 2100397, 2021, ISSN: 1022-1336.
Abstract | Links | Tags: Solid-Liquid
@article{nokey,
title = {Correlation of Thermoelectric Performance, Domain Morphology and Doping Level in PEDOT:PSS Thin Films Post-Treated with Ionic Liquids},
author = {A L Oechsle and J E Heger and N Li and S Yin and S Bernstorff and P M\"{u}ller-Buschbaum},
url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/marc.202100397},
doi = {https://doi.org/10.1002/marc.202100397},
issn = {1022-1336},
year = {2021},
date = {2021-09-07},
journal = {Macromolecular Rapid Communications},
volume = {42},
number = {20},
pages = {2100397},
abstract = {Abstract Ionic liquid (IL) post-treatment of poly(3,4-ethylene dioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) thin films with ethyl-3-methylimidazolium dicyanamide (EMIM DCA), allyl-3-methylimidazolium dicyanamide (AMIM DCA), and 1-ethyl-3-methylimidazolium tetracyanoborate (EMIM TCB) is compared. Doping level modifications of PEDOT are characterized using UV\textendashVis spectroscopy and directly correlate with the observed Seebeck coefficient enhancement. With conductive atomic force microscopy (c-AFM) the authors investigate changes in the topographic-current features of the PEDOT:PSS thin film surface due to IL treatment. Grazing incidence small-angle X-ray scattering (GISAXS) demonstrates the morphological rearrangement towards an optimized PEDOT domain distribution upon IL post-treatment, directly facilitating the interconductivity and causing an increased film conductivity. Based on these improvements in Seebeck coefficient and conductivity, the power factor is increased up to 236 µW m−1K−2. Subsequently, a model is developed indicating that ILs, which contain small, sterically unhindered ions with a strong localized charge, appear beneficial to boost the thermoelectric performance of post-treated PEDOT:PSS films.},
keywords = {Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
A Thurn, J Bissinger, S Meinecke, P Schmiedeke, S S Oh, W W Chow, K Lüdge, G Koblmüller, J J Finley
Self-induced ultrafast electron-hole plasma temperature oscillations in nanowire lasers Journal Article
In: arXiv preprint arXiv:2108.11784, 2021.
Abstract | Links | Tags: Solid-Solid
@article{nokey,
title = {Self-induced ultrafast electron-hole plasma temperature oscillations in nanowire lasers},
author = {A Thurn and J Bissinger and S Meinecke and P Schmiedeke and S S Oh and W W Chow and K L\"{u}dge and G Koblm\"{u}ller and J J Finley},
url = {https://arxiv.org/abs/2108.11784},
doi = {arXiv:2108.11784v2},
year = {2021},
date = {2021-09-06},
journal = {arXiv preprint arXiv:2108.11784},
abstract = {Nanowire lasers can be monolithically and site-selectively integrated onto silicon photonic circuits. To assess their full potential for ultrafast opto-electronic devices, a detailed understanding of their lasing dynamics is crucial. However, the roles played by their resonator geometry and the microscopic processes that mediate energy exchange between the photonic, electronic, and phononic systems are largely unexplored. Here, we apply femtosecond pump-probe spectroscopy to show that GaAs-AlGaAs core-shell nanowire lasers exhibit sustained intensity oscillations with frequencies ranging from 160 GHz to 260 GHz. These dynamics are intricately linked to the strong interaction between the lasing mode and the gain material arising from their wavelength-scale dimensions. Combined with dynamic competition between photoinduced carrier heating and cooling via phonon scattering, this enables self-induced electron-hole plasma temperature oscillations, which modulate the laser output. We anticipate that our results will lead to new approaches for ultrafast intensity and phase modulation of chip-integrated nanoscale semiconductor lasers.},
keywords = {Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
J Kühne, J Wang, T Weber, L Kühner, S A Maier, A Tittl
Fabrication robustness in BIC metasurfaces Journal Article
In: Nanophotonics, vol. 10, no. 17, pp. 4305-4312, 2021.
Links | Tags:
@article{nokey,
title = {Fabrication robustness in BIC metasurfaces},
author = {J K\"{u}hne and J Wang and T Weber and L K\"{u}hner and S A Maier and A Tittl},
url = {https://doi.org/10.1515/nanoph-2021-0391},
doi = {doi:10.1515/nanoph-2021-0391},
year = {2021},
date = {2021-09-06},
journal = {Nanophotonics},
volume = {10},
number = {17},
pages = {4305-4312},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
P Mao, C Liu, X Li, M Liu, Q Chen, M Han, S A Maier, E H Sargent, S Zhang
Single-step-fabricated disordered metasurfaces for enhanced light extraction from LEDs Journal Article
In: Light: Science & Applications, vol. 10, no. 1, pp. 180, 2021, ISSN: 2047-7538.
Abstract | Links | Tags: Foundry Inorganic, Solid-Solid
@article{nokey,
title = {Single-step-fabricated disordered metasurfaces for enhanced light extraction from LEDs},
author = {P Mao and C Liu and X Li and M Liu and Q Chen and M Han and S A Maier and E H Sargent and S Zhang},
url = {https://doi.org/10.1038/s41377-021-00621-7},
doi = {10.1038/s41377-021-00621-7},
issn = {2047-7538},
year = {2021},
date = {2021-09-06},
journal = {Light: Science \& Applications},
volume = {10},
number = {1},
pages = {180},
abstract = {While total internal reflection (TIR) lays the foundation for many important applications, foremost fibre optics that revolutionised information technologies, it is undesirable in some other applications such as light-emitting diodes (LEDs), which are a backbone for energy-efficient light sources. In the case of LEDs, TIR prevents photons from escaping the constituent high-index materials. Advances in material science have led to good efficiencies in generating photons from electron\textendashhole pairs, making light extraction the bottleneck of the overall efficiency of LEDs. In recent years, the extraction efficiency has been improved, using nanostructures at the semiconductor/air interface that outcouple trapped photons to the outside continuum. However, the design of geometrical features for light extraction with sizes comparable to or smaller than the optical wavelength always requires sophisticated and time-consuming fabrication, which causes a gap between lab demonstration and industrial-level applications. Inspired by lightning bugs, we propose and realise a disordered metasurface for light extraction throughout the visible spectrum, achieved with single-step fabrication. By applying such a cost-effective light extraction layer, we improve the external quantum efficiency by a factor of 1.65 for commercialised GaN LEDs, demonstrating a substantial potential for global energy-saving and sustainability.},
keywords = {Foundry Inorganic, Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
E Rheinfrank, M Pörtner, M D C Nuñez Beyerle, F Haag, P S Deimel, F Allegretti, K Seufert, J V Barth, M-L Bocquet, P Feulner, W Auwärter
Actinide Coordination Chemistry on Surfaces: Synthesis, Manipulation, and Properties of Thorium Bis(porphyrinato) Complexes Journal Article
In: Journal of the American Chemical Society, vol. 143, no. 36, pp. 14581-14591, 2021, ISSN: 0002-7863.
Abstract | Links | Tags: Foundry Inorganic
@article{nokey,
title = {Actinide Coordination Chemistry on Surfaces: Synthesis, Manipulation, and Properties of Thorium Bis(porphyrinato) Complexes},
author = {E Rheinfrank and M P\"{o}rtner and M D C Nu\~{n}ez Beyerle and F Haag and P S Deimel and F Allegretti and K Seufert and J V Barth and M-L Bocquet and P Feulner and W Auw\"{a}rter},
url = {https://doi.org/10.1021/jacs.1c04982},
doi = {10.1021/jacs.1c04982},
issn = {0002-7863},
year = {2021},
date = {2021-09-03},
journal = {Journal of the American Chemical Society},
volume = {143},
number = {36},
pages = {14581-14591},
abstract = {Actinide-based metal\textendashorganic complexes and coordination architectures encompass intriguing properties and functionalities but are still largely unexplored on surfaces. We introduce the in situ synthesis of actinide tetrapyrrole complexes under ultrahigh-vacuum conditions, on both a metallic support and a 2D material. Specifically, exposure of a tetraphenylporphyrin (TPP) multilayer to an elemental beam of thorium followed by a temperature-programmed reaction and desorption of surplus molecules yields bis(porphyrinato)thorium (Th(TPP)2) assemblies on Ag(111) and hexagonal boron nitride/Cu(111). A multimethod characterization including X-ray photoelectron spectroscopy, scanning tunneling microscopy, temperature-programmed desorption, and complementary density functional theory modeling provides insights into conformational and electronic properties. Supramolecular assemblies of Th(TPP)2 as well as individual double-deckers are addressed with submolecular precision, e.g., demonstrating the reversible rotation of the top porphyrin in Th(TPP)2 by molecular manipulation. Our findings thus demonstrate prospects for actinide-based functional nanoarchitectures.},
keywords = {Foundry Inorganic},
pubstate = {published},
tppubtype = {article}
}
F Bischoff, A Riss, G S Michelitsch, J Ducke, J V Barth, K Reuter, W Auwärter
Surface-Mediated Ring-Opening and Porphyrin Deconstruction via Conformational Distortion Journal Article
In: Journal of the American Chemical Society, vol. 143, no. 37, pp. 15131-15138, 2021, ISSN: 0002-7863.
Abstract | Links | Tags: Molecularly-Functionalized
@article{nokey,
title = {Surface-Mediated Ring-Opening and Porphyrin Deconstruction via Conformational Distortion},
author = {F Bischoff and A Riss and G S Michelitsch and J Ducke and J V Barth and K Reuter and W Auw\"{a}rter},
url = {https://doi.org/10.1021/jacs.1c05348},
doi = {10.1021/jacs.1c05348},
issn = {0002-7863},
year = {2021},
date = {2021-09-02},
urldate = {2021-09-02},
journal = {Journal of the American Chemical Society},
volume = {143},
number = {37},
pages = {15131-15138},
abstract = {The breakdown of macrocyclic compounds is of utmost importance in manifold biological and chemical processes, usually proceeding via oxygenation-induced ring-opening reactions. Here, we introduce a surface chemical route to selectively break a prototypical porphyrin species, cleaving off one pyrrole unit and affording a tripyrrin derivative. This pathway, operational in an ultrahigh vacuum environment at moderate temperature is enabled by a distinct molecular conformation achieved via the specific interaction between the porphyrin and its copper support. We provide an atomic-level characterization of the surface-anchored tripyrrin, its reaction intermediates, and byproducts by bond-resolved atomic force microscopy, unequivocally identifying the molecular skeletons. The ring-opening is rationalized by the distortion reducing the macrocycle’s stability. Our findings open a route to steer ring-opening reactions by conformational design and to study intriguing tetrapyrrole catabolite analogues on surfaces.},
keywords = {Molecularly-Functionalized},
pubstate = {published},
tppubtype = {article}
}
D Böhm, M Beetz, C Gebauer, M Bernt, J Schröter, M Kornherr, F Zoller, T Bein, D Fattakhova-Rohlfing
In: Applied Materials Today, vol. 24, pp. 101134, 2021, ISSN: 2352-9407.
Abstract | Links | Tags: Foundry Inorganic
@article{nokey,
title = {Highly conductive titania supported iridium oxide nanoparticles with low overall iridium density as OER catalyst for large-scale PEM electrolysis},
author = {D B\"{o}hm and M Beetz and C Gebauer and M Bernt and J Schr\"{o}ter and M Kornherr and F Zoller and T Bein and D Fattakhova-Rohlfing},
url = {https://www.sciencedirect.com/science/article/pii/S2352940721001980},
doi = {https://doi.org/10.1016/j.apmt.2021.101134},
issn = {2352-9407},
year = {2021},
date = {2021-09-01},
journal = {Applied Materials Today},
volume = {24},
pages = {101134},
abstract = {To enable future large-scale generation of hydrogen via proton exchange membrane (PEM) electrolysis, utilization of scarce iridium-based catalysts required for the oxygen evolution reaction (OER) has to be significantly lowered. To address this question, the facile synthesis of a highly active TiO2 supported iridium oxide based OER catalyst with reduced noble metal content and an Ir-density of the catalyst powder as low as 0.05\textendash0.08 gIr cm-3 is described in this work. A high surface area corrosion-resistant titania catalyst support homogeneously coated with a 1-2 nm thin layer of amorphous IrOOHx is oxidized in molten NaNO3 between 350-375°C. This procedure allows for a controllable phase transformation and crystallization to form a layer of interconnected IrO2 nanoparticles of ≈2 nm on the surface of the TiO2 support. The increase in crystallinity is thereby accompanied by a significant increase in conductivity of up to 11 S cm-1 for a 30 wt% Ir loaded catalyst. Oxidized samples further display a significantly increased stability with less detectable Ir dissolution under OER conditions. With a mass-based activity of 59 A g-1 at an overpotential of 300 mV, the electrocatalytic activity is maintained at the level of the highly active amorphous IrOOHx phase used as precursor and outperforms it at higher current densities through the increased conductivity. MEA measurements with catalyst loadings of 0.2-0.3 mg cm-2 further confirm the high catalytic activity and initial stability at industrially relevant current densities. The introduced synthesis approach therefore shows a path for the fabrication of novel highly active and atom-efficient oxide supported catalysts with complex nanostructures and thin homogenous nanoparticle coatings that allows a future large-scale application of PEM electrolysis technology without restrictions by the natural abundance of iridium.},
keywords = {Foundry Inorganic},
pubstate = {published},
tppubtype = {article}
}
M Pfeiffer, K Trofymchuk, S Ranallo, F Ricci, F Steiner, F Cole, V Glembockyte, P Tinnefeld
Single Antibody Detection in a DNA Origami Nanoantenna Journal Article
In: iScience, pp. 103072, 2021, ISSN: 2589-0042.
Abstract | Links | Tags: Foundry Inorganic, Foundry Organic
@article{nokey,
title = {Single Antibody Detection in a DNA Origami Nanoantenna},
author = {M Pfeiffer and K Trofymchuk and S Ranallo and F Ricci and F Steiner and F Cole and V Glembockyte and P Tinnefeld},
url = {https://www.sciencedirect.com/science/article/pii/S2589004221010403},
doi = {https://doi.org/10.1016/j.isci.2021.103072},
issn = {2589-0042},
year = {2021},
date = {2021-09-01},
urldate = {2021-09-01},
journal = {iScience},
pages = {103072},
abstract = {Summary DNA nanotechnology offers new biosensing approaches by templating different sensor and transducer components. Here, we combine DNA origami nanoantennas with label-free antibody detection by incorporating a nanoswitch in the plasmonic hotspot of the nanoantenna. The nanoswitch contains two antigens that are displaced by antibody binding thereby eliciting a fluorescent signal. Single antibody detection is demonstrated with a DNA origami integrated anti-digoxigenin antibody nanoswitch. In combination with the nanoantenna, the signal generated by the antibody is additionally amplified. This allows the detection of single antibodies on a portable smartphone microscope. Overall, fluorescence enhanced antibody detection in DNA origami nanoantennas shows that fluorescence enhanced biosensing can be expanded beyond the scope of the nucleic acids realm.},
keywords = {Foundry Inorganic, Foundry Organic},
pubstate = {published},
tppubtype = {article}
}
K Schwärzer, S K Rout, D Bessinger, F Lima, C E Brocklehurst, K Karaghiosoff, T Bein, P Knochel
In: Chemical Science, vol. 12, no. 39, pp. 12993-13000, 2021, ISSN: 2041-6520.
Abstract | Links | Tags: Foundry Organic, Molecularly-Functionalized
@article{nokey,
title = {Selective functionalization of the 1H-imidazo[1,2-b]pyrazole scaffold. A new potential non-classical isostere of indole and a precursor of push\textendashpull dyes},
author = {K Schw\"{a}rzer and S K Rout and D Bessinger and F Lima and C E Brocklehurst and K Karaghiosoff and T Bein and P Knochel},
url = {http://dx.doi.org/10.1039/D1SC04155J},
doi = {10.1039/D1SC04155J},
issn = {2041-6520},
year = {2021},
date = {2021-08-30},
urldate = {2021-08-30},
journal = {Chemical Science},
volume = {12},
number = {39},
pages = {12993-13000},
abstract = {We report the selective functionalization of the 1H-imidazo[1,2-b]pyrazole scaffold using a Br/Mg-exchange, as well as regioselective magnesiations and zincations with TMP-bases (TMP = 2,2,6,6-tetramethylpiperidyl), followed by trapping reactions with various electrophiles. In addition, we report a fragmentation of the pyrazole ring, giving access to push\textendashpull dyes with a proaromatic (1,3-dihydro-2H-imidazol-2-ylidene)malononitrile core. These functionalization methods were used in the synthesis of an isostere of the indolyl drug pruvanserin. Comparative assays between the original drug and the isostere showed that a substitution of the indole ring with a 1H-imidazo[1,2-b]pyrazole results in a significantly improved solubility in aqueous media.},
keywords = {Foundry Organic, Molecularly-Functionalized},
pubstate = {published},
tppubtype = {article}
}
A-K Hatz, R Calaminus, J Feijoo, F Treber, J Blahusch, T Lenz, M Reichel, K Karaghiosoff, N M Vargas-Barbosa, B V Lotsch
Chemical Stability and Ionic Conductivity of LGPS-Type Solid Electrolyte Tetra-Li7SiPS8 after Solvent Treatment Journal Article
In: ACS Applied Energy Materials, vol. 4, no. 9, pp. 9932-9943, 2021.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{nokey,
title = {Chemical Stability and Ionic Conductivity of LGPS-Type Solid Electrolyte Tetra-Li7SiPS8 after Solvent Treatment},
author = {A-K Hatz and R Calaminus and J Feijoo and F Treber and J Blahusch and T Lenz and M Reichel and K Karaghiosoff and N M Vargas-Barbosa and B V Lotsch},
url = {https://doi.org/10.1021/acsaem.1c01917},
doi = {10.1021/acsaem.1c01917},
year = {2021},
date = {2021-08-30},
journal = {ACS Applied Energy Materials},
volume = {4},
number = {9},
pages = {9932-9943},
abstract = {The large-scale production of solid-state batteries necessitates the development of alternative routes for processing air-sensitive thiophosphate-based solid electrolytes. To set a basis for this, we investigate the chemical stability and ionic conductivity of the LGPS-type lithium-ion conductor tetra-Li7SiPS8 (LiSiPS) processed with various organic solvents. We elucidate the nature of colorful polysulfides that arise during solvent treatment and trace back their origin to the dissolution of the Li3PS4-type amorphous side phase typically present in LiSiPS. We find that water and alcohols decompose LiSiPS by the nucleophilic attack into oxygen-substituted thiophosphates and thioethers and propose a reaction mechanism for the latter. Moreover, we confirm that quaternary thiophosphates can be recrystallized from MeOH solutions upon subsequent high-temperature treatment. Aprotic solvents with donor numbers smaller than 15 kcal mol\textendash1 are suitable for wet-processing quaternary thiophosphates because both the crystal structure of the electrolyte and a high ionic conductivity of \>1 mS cm\textendash1 are retained. Using anisole as a case study, we clarify that a residual water content of up to 800 ppm does not lead to a significant deterioration in the ionic conductivity when compared to dry solvents (≤5 ppm). Additionally, we observe a decrease in ionic conductivity with an increasing amount of the solvent residue, which depends not only on the donor number of the solvent but also on the vapor pressure and interactions between the solvent molecules and thiophosphate groups in the solid electrolyte. Thus, optimization of solvent-processing methods of thiophosphate electrolytes is a multifaceted challenge. This work provides transferable insights regarding the stability of LiSiPS against organic solvents that may enable competitive and large-scale thiophosphate-based solid electrolyte processing.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
V Stavila, S Li, C Dun, M T Marple, H E Mason, J L Snider, J E Reynolds Iii, F El Gabaly, J D Sugar, C D Spataru, X Zhou, B Dizdar, E H Majzoub, R Chatterjee, J Yano, H Schlomberg, B V Lotsch, J J Urban, B C Wood, M D Allendorf
Defying Thermodynamics: Stabilization of Alane Within Covalent Triazine Frameworks for Reversible Hydrogen Storage Journal Article
In: Angewandte Chemie International Edition, vol. 60, no. 49, pp. 25815-25824, 2021, ISSN: 1433-7851.
Abstract | Links | Tags: Foundry Organic
@article{nokey,
title = {Defying Thermodynamics: Stabilization of Alane Within Covalent Triazine Frameworks for Reversible Hydrogen Storage},
author = {V Stavila and S Li and C Dun and M T Marple and H E Mason and J L Snider and J E Reynolds Iii and F El Gabaly and J D Sugar and C D Spataru and X Zhou and B Dizdar and E H Majzoub and R Chatterjee and J Yano and H Schlomberg and B V Lotsch and J J Urban and B C Wood and M D Allendorf},
url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/anie.202107507},
doi = {https://doi.org/10.1002/anie.202107507},
issn = {1433-7851},
year = {2021},
date = {2021-08-29},
journal = {Angewandte Chemie International Edition},
volume = {60},
number = {49},
pages = {25815-25824},
abstract = {Abstract The highly unfavorable thermodynamics of direct aluminum hydrogenation can be overcome by stabilizing alane within a nanoporous bipyridine-functionalized covalent triazine framework (AlH3@CTF-bipyridine). This material and the counterpart AlH3@CTF-biphenyl rapidly desorb H2 between 95 and 154 °C, with desorption complete at 250 °C. Sieverts measurements, 27Al MAS NMR and 27Al1H REDOR experiments, and computational spectroscopy reveal that AlH3@CTF-bipyridine dehydrogenation is reversible at 60 °C under 700 bar hydrogen, \>10 times lower pressure than that required to hydrogenate bulk aluminum. DFT calculations and EPR measurements support an unconventional mechanism whereby strong AlH3 binding to bipyridine results in single-electron transfer to form AlH2(AlH3)n clusters. The resulting size-dependent charge redistribution alters the dehydrogenation/rehydrogenation thermochemistry, suggesting a novel strategy to enable reversibility in high-capacity metal hydrides.},
keywords = {Foundry Organic},
pubstate = {published},
tppubtype = {article}
}
F Zoller, S Häringer, D Böhm, H Illner, M Döblinger, Z K Sofer, M Finsterbusch, T Bein, D Fattakhova-Rohlfing
Overcoming the Challenges of Freestanding Tin Oxide-Based Composite Anodes to Achieve High Capacity and Increased Cycling Stability Journal Article
In: Advanced Functional Materials, vol. 31, no. 43, pp. 2106373, 2021, ISSN: 1616-301X.
Abstract | Links | Tags: Foundry Inorganic, Solid-Solid
@article{nokey,
title = {Overcoming the Challenges of Freestanding Tin Oxide-Based Composite Anodes to Achieve High Capacity and Increased Cycling Stability},
author = {F Zoller and S H\"{a}ringer and D B\"{o}hm and H Illner and M D\"{o}blinger and Z K Sofer and M Finsterbusch and T Bein and D Fattakhova-Rohlfing},
url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adfm.202106373},
doi = {https://doi.org/10.1002/adfm.202106373},
issn = {1616-301X},
year = {2021},
date = {2021-08-27},
journal = {Advanced Functional Materials},
volume = {31},
number = {43},
pages = {2106373},
abstract = {Abstract Freestanding electrodes are a promising way to increase the energy density of the batteries by decreasing the overall amount of electrochemically inactive materials. Freestanding antimony doped tin oxide (ATO)-based hybrid materials have not been reported so far, although this material has demonstrated excellent performance in conventionally designed electrodes. Two different strategies, namely electrospinning and freeze-casting, are explored for the fabrication of ATO-based hybrid materials. It is shown that the electrospinning of ATO/carbon based electrodes from polyvinyl pyrrolidone polymer (PVP) solutions was not successful, as the resulting electrode material suffers from rapid degradation. However, freestanding reduced graphene oxide (rGO) containing ATO/C/rGO nanocomposites prepared via a freeze-casting route demonstrates an impressive rate and cycling performance reaching 697 mAh g−1 at a high current density of 4 A g−1, which is 40 times higher as compared to SnO2/rGO and also exceeds the freestanding SnO2-based composites reported so far. Antimony doping of the nanosized tin oxide phase and carbon coating are thereby shown to be essential factors for appealing electrochemical performance. Finally, the freestanding ATO/C/rGO anodes are combined with freestanding LiFe0.2Mn0.8PO4/rGO cathodes to obtain a full freestanding cell operating without metal current collector foils showing nonetheless an excellent cycling stability.},
keywords = {Foundry Inorganic, Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
M Pauly, J Kroger, V Duppel, C Murphey, J Cahoon, B V Lotsch, P Maggard
Unveiling the Complex Configurational Landscape of the Intralayer Cavities in a Crystalline Carbon Nitride Journal Article
In: 2021.
Abstract | Links | Tags: Foundry Inorganic
@article{nokey,
title = {Unveiling the Complex Configurational Landscape of the Intralayer Cavities in a Crystalline Carbon Nitride},
author = {M Pauly and J Kroger and V Duppel and C Murphey and J Cahoon and B V Lotsch and P Maggard},
url = {https://chemrxiv.org/engage/chemrxiv/article-details/6127820165db1ec864a4c3a6},
doi = {10.26434/chemrxiv-2021-90tq7-v2},
year = {2021},
date = {2021-08-26},
urldate = {2021-08-26},
abstract = {The in-depth understanding of the reported photoelectrochemical properties of the layered carbon nitride, poly(triazine imide)/LiCl (PTI/LiCl), has been limited by the apparent disorder of the Li/H atoms within its framework. To understand and resolve the current structural ambiguities, an optimized one-step flux synthesis (470 oC, 36 h, LiCl/KCl flux) was used to prepare PTI/LiCl and deuterated-PTI/LiCl in high purity. Its structure was characterized by a combination of neutron/X-ray diffraction and transmission electron microscopy. The range of possible Li/H atomic configurations were enumerated for the first time and, combined with total energy calculations, reveals a more complex energetic landscape than previously considered. Experimental data were fitted against all possible structural models, exhibiting the most consistency with a new orthorhombic model (Sp. Grp. Ama2) that also has the lowest total energy. In addition, a new Cu(I)-containing PTI (PTI/CuCl) was prepared with the more strongly scattering Cu(I) cations in place of Li, and which also most closely matched with the partially-disorded structure in Cmc21. Thus, a complex configurational landscape of PTI is revealed to consist of a number of ordered crystalline structures that are new potential synthetic targets, such as with the use of metal-exchange reactions.},
keywords = {Foundry Inorganic},
pubstate = {published},
tppubtype = {article}
}
V Glembockyte, L Grabenhorst, K Trofymchuk, P Tinnefeld
DNA Origami Nanoantennas for Fluorescence Enhancement Journal Article
In: Accounts of Chemical Research, vol. 54, no. 17, pp. 3338-3348, 2021, ISSN: 0001-4842.
Abstract | Links | Tags: Foundry Inorganic, Foundry Organic, Molecularly-Functionalized
@article{nokey,
title = {DNA Origami Nanoantennas for Fluorescence Enhancement},
author = {V Glembockyte and L Grabenhorst and K Trofymchuk and P Tinnefeld},
url = {https://doi.org/10.1021/acs.accounts.1c00307},
doi = {10.1021/acs.accounts.1c00307},
issn = {0001-4842},
year = {2021},
date = {2021-08-26},
urldate = {2021-08-26},
journal = {Accounts of Chemical Research},
volume = {54},
number = {17},
pages = {3338-3348},
abstract = {ConspectusThe possibility to increase fluorescence by plasmonic effects in the near-field of metal nanostructures was recognized more than half a century ago. A major challenge, however, was to use this effect because placing single quantum emitters in the nanoscale plasmonic hotspot remained unsolved for a long time. This not only presents a chemical problem but also requires the nanostructure itself to be coaligned with the polarization of the excitation light. Additional difficulties arise from the complex distance dependence of fluorescence emission: in contrast to other surface-enhanced spectroscopies (such as Raman spectroscopy), the emitter should not be placed as close as possible to the metallic nanostructure but rather needs to be at an optimal distance on the order of a few nanometers to avoid undesired quenching effects.Our group addressed these challenges almost a decade ago by exploiting the unique positioning ability of DNA nanotechnology and reported the first self-assembled DNA origami nanoantennas. This Account summarizes our work spanning from this first proof-of-principle study to recent advances in utilizing DNA origami nanoantennas for single DNA molecule detection on a portable smartphone microscope.We summarize different aspects of DNA origami nanoantennas that are essential for achieving strong fluorescence enhancement and discuss how single-molecule fluorescence studies helped us to gain a better understanding of the interplay between fluorophores and plasmonic hotspots. Practical aspects of preparing the DNA origami nanoantennas and extending their utility are also discussed.Fluorescence enhancement in DNA origami nanoantennas is especially exciting for signal amplification in molecular diagnostic assays or in single-molecule biophysics, which could strongly benefit from higher time resolution. Additionally, biophysics can greatly profit from the ultrasmall effective detection volumes provided by DNA nanoantennas that allow single-molecule detection at drastically elevated concentrations as is required, e.g., in single-molecule DNA sequencing approaches.Finally, we describe our most recent progress in developing DNA NanoAntennas with Cleared HOtSpots (NACHOS) that are fully compatible with biomolecular assays. The developed DNA origami nanoantennas have proven robustness and remain functional after months of storage. As an example, we demonstrated for the first time the single-molecule detection of DNA specific to antibiotic-resistant bacteria on a portable and battery-driven smartphone microscope enabled by DNA origami nanoantennas. These recent developments mark a perfect moment to summarize the principles and the synthesis of DNA origami nanoantennas and give an outlook of new exciting directions toward using different nanomaterials for the construction of nanoantennas as well as for their emerging applications.},
keywords = {Foundry Inorganic, Foundry Organic, Molecularly-Functionalized},
pubstate = {published},
tppubtype = {article}
}
J Eichhorn, S P Lechner, C-M Jiang, G Folchi Heunecke, F Munnik, I D Sharp
Indirect bandgap, optoelectronic properties, and photoelectrochemical characteristics of high-purity Ta3N5 photoelectrodes Journal Article
In: Journal of Materials Chemistry A, vol. 9, pp. 20653, 2021, ISSN: 2050-7488.
Abstract | Links | Tags: Foundry Inorganic
@article{nokey,
title = {Indirect bandgap, optoelectronic properties, and photoelectrochemical characteristics of high-purity Ta3N5 photoelectrodes},
author = {J Eichhorn and S P Lechner and C-M Jiang and G Folchi Heunecke and F Munnik and I D Sharp},
url = {http://dx.doi.org/10.1039/D1TA05282A},
doi = {10.1039/D1TA05282A},
issn = {2050-7488},
year = {2021},
date = {2021-08-26},
urldate = {2021-08-26},
journal = {Journal of Materials Chemistry A},
volume = {9},
pages = {20653},
abstract = {The (opto)electronic properties of Ta3N5 photoelectrodes are often dominated by defects, such as oxygen impurities, nitrogen vacancies, and low-valent Ta cations, impeding fundamental studies of its electronic structure, chemical stability, and photocarrier transport. Here, we explore the role of ammonia annealing following direct reactive magnetron sputtering of tantalum nitride thin films, achieving near-ideal stoichiometry, with significantly reduced native defect and oxygen impurity concentrations. By analyzing structural, optical, and photoelectrochemical properties as a function of ammonia annealing temperature, we provide new insights into the basic semiconductor properties of Ta3N5, as well as the role of defects on its optoelectronic characteristics. Both the crystallinity and material quality improve up to 940 °C, due to elimination of oxygen impurities. Even higher annealing temperatures cause material decomposition and introduce additional disorder within the Ta3N5 lattice, leading to reduced photoelectrochemical performance. Overall, the high material quality enables us to unambiguously identify the nature of the Ta3N5 bandgap as indirect, thereby resolving a long-standing controversy regarding the most fundamental characteristic of this material as a semiconductor. The compact morphology, low defect content, and high optoelectronic quality of these films provide a basis for further optimization of photoanodes and may open up further application opportunities beyond photoelectrochemical energy conversion.},
keywords = {Foundry Inorganic},
pubstate = {published},
tppubtype = {article}
}
S Hutsch, M Panhans, F Ortmann
Time-consistent hopping transport with vibration-mode-resolved electron-phonon couplings Journal Article
In: Physical Review B, vol. 104, no. 5, pp. 054306, 2021.
Abstract | Links | Tags: Foundry Inorganic
@article{nokey,
title = {Time-consistent hopping transport with vibration-mode-resolved electron-phonon couplings},
author = {S Hutsch and M Panhans and F Ortmann},
url = {https://link.aps.org/doi/10.1103/PhysRevB.104.054306},
doi = {10.1103/PhysRevB.104.054306},
year = {2021},
date = {2021-08-25},
journal = {Physical Review B},
volume = {104},
number = {5},
pages = {054306},
abstract = {Charge transport in organic semiconductors is affected by the complex interaction between charge carriers and molecular vibrations. A common way to treat the molecular vibrations in hopping approaches is by condensing them into a single analytical parameter, the reorganization energy. In contrast, here we present a nonadiabatic hopping transport approach that avoids this approximation by dividing the vibrational spectrum of organic molecules into three distinct analytical classes, namely the quasistatic, low-frequency dynamic, and high-frequency dynamic modes. The quasistatic and dynamic regimes are separated time consistently with respect to the timescale of the hopping events, which results in charge transfer events driven by a set of strongly coupling driving modes. Using these time-consistent hopping rates, we compute the charge carrier mobilities for a set of hopping transport materials and a control set of band-transport materials and compare them to experimental values. The resulting mobilities are consistent for both sets by showing similar values for the hopping transport materials and lower values for the control set of band-transport materials due to the absence of coherent transport contributions. We further study other popular hopping approaches such as the Marcus theory and the Levich-Jortner theory and observe substantial inconsistencies for them.},
keywords = {Foundry Inorganic},
pubstate = {published},
tppubtype = {article}
}
A-K Hatz, I Moudrakovski, S Bette, M W Terban, M Etter, M Joos, N M Vargas-Barbosa, R E Dinnebier, B V Lotsch
Fast Water-Assisted Lithium Ion Conduction in Restacked Lithium Tin Sulfide Nanosheets Journal Article
In: Chemistry of Materials, vol. 33, no. 18, pp. 7337-7349, 2021, ISSN: 0897-4756.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{nokey,
title = {Fast Water-Assisted Lithium Ion Conduction in Restacked Lithium Tin Sulfide Nanosheets},
author = {A-K Hatz and I Moudrakovski and S Bette and M W Terban and M Etter and M Joos and N M Vargas-Barbosa and R E Dinnebier and B V Lotsch},
url = {https://doi.org/10.1021/acs.chemmater.1c01755},
doi = {10.1021/acs.chemmater.1c01755},
issn = {0897-4756},
year = {2021},
date = {2021-08-25},
journal = {Chemistry of Materials},
volume = {33},
number = {18},
pages = {7337-7349},
abstract = {While two-dimensional (2D) materials may preserve some intrinsic properties of the corresponding layered bulk material, new characteristics arise from their pronounced anisotropy or confinement effects. Recently, exceptionally high ionic conductivities were discovered in 2D materials such as graphene oxide and vermiculite. Here, we report on the water-assisted fast conduction of lithium ions in restacked lithium tin sulfide nanosheets. Li0.8Sn0.8S2 exfoliates spontaneously in water and can be restacked into homogeneous films in which the lithium content is decreased, and a partial substitution of sulfur with hydroxyl groups takes place. Using a recursive supercell refinement approach in reciprocal space along with real-space pair distribution function analysis, we describe restacked lithium tin sulfide as a partially turbostratically disordered material composed of lithium-containing and lithium-depleted layers. In humid air, the material takes up multiple layers of water that coordinate lithium ions in the space between the layers, increasing the stacking distance and screening the interaction between lithium ions and the anionic layers. This results in a 1000-fold increase in ionic conductivity up to 47 mS cm\textendash1 at high humidities. Orientation-dependent impedance spectroscopy suggests a facile in-plane conduction and a hindered out-of-plane conduction. Pulsed field gradient nuclear magnetic resonance spectroscopy reveals a fast, simultaneous diffusion of a majority and a minority species for both 7Li and 1H, suggesting water-assisted lithium diffusion to be at play. This study enlarges the family of nanosheet-based ionic conductors and helps to rationalize the transport mechanism of lithium ions enabled by hydration in a nanoconfined 2D space.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
H Türk, F-P Schmidt, T Götsch, F Girgsdies, A Hammud, D Ivanov, I C Vinke, L G J De Haart, R-A Eichel, K Reuter, R Schlögl, A Knop-Gericke, C Scheurer, T Lunkenbein
Complexions at the Electrolyte/Electrode Interface in Solid Oxide Cells Journal Article
In: Advanced Materials Interfaces, vol. 8, no. 18, pp. 2100967, 2021, ISSN: 2196-7350.
Abstract | Links | Tags: Foundry Inorganic, Solid-Solid
@article{nokey,
title = {Complexions at the Electrolyte/Electrode Interface in Solid Oxide Cells},
author = {H T\"{u}rk and F-P Schmidt and T G\"{o}tsch and F Girgsdies and A Hammud and D Ivanov and I C Vinke and L G J De Haart and R-A Eichel and K Reuter and R Schl\"{o}gl and A Knop-Gericke and C Scheurer and T Lunkenbein},
url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/admi.202100967},
doi = {https://doi.org/10.1002/admi.202100967},
issn = {2196-7350},
year = {2021},
date = {2021-08-21},
journal = {Advanced Materials Interfaces},
volume = {8},
number = {18},
pages = {2100967},
abstract = {Abstract Rapid deactivation presently limits a wide spread use of high-temperature solid oxide cells (SOCs) as otherwise highly efficient chemical energy converters. With deactivation triggered by the ongoing conversion reactions, an atomic-scale understanding of the active triple-phase boundary between electrolyte, electrode, and gas phase is essential to increase cell performance. Here, a multi-method approach is used comprising transmission electron microscopy and first-principles calculations and molecular simulations to untangle the atomic arrangement of the prototypical SOC interface between a lanthanum strontium manganite (LSM) anode and a yttria-stabilized zirconia (YSZ) electrolyte in the as-prepared state after sintering. An interlayer of self-limited width with partial amorphization and strong compositional gradient is identified, thus exhibiting the characteristics of a complexion that is stabilized by the confinement between two bulk phases. This offers a new perspective to understand the function of SOCs at the atomic scale. Moreover, it opens up a hitherto unrealized design space to tune the conversion efficiency.},
keywords = {Foundry Inorganic, Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
B Wei, P Knochel
Recent Advances in Cross-Couplings of Functionalized Organozinc Reagents Journal Article
In: Synthesis, vol. 54, no. 02, pp. 246-254, 2021, ISSN: 0039-7881 DOI - 10.1055/a-1589-0150.
Abstract | Links | Tags: Foundry Organic
@article{nokey,
title = {Recent Advances in Cross-Couplings of Functionalized Organozinc Reagents},
author = {B Wei and P Knochel},
url = {https://www.thieme-connect.com/products/ejournals/abstract/10.1055/a-1589-0150},
doi = {10.1055/a-1589-0150},
issn = {0039-7881 DOI - 10.1055/a-1589-0150},
year = {2021},
date = {2021-08-16},
journal = {Synthesis},
volume = {54},
number = {02},
pages = {246-254},
abstract = {Cross-couplings involving organozinc reagents usually require a Pd-catalyst (Negishi cross-coupling), however, uncatalyzed cross-couplings of zinc organometallics proceed well in the absence of transition-metal catalysts with reactive electrophiles such as benzal 1,1-diacetates, benzhydryl acetates, and iminium trifluoroacetates. Organozinc compounds also undergo C\textendashN bond formation with O-benzoylhydroxylamines or organic azides in the presence of cobalt- or iron-catalysts. Highly diastereoselective and enantioselective cross-couplings can be readily performed with room-temperature configurationally stable alkylzinc species, producing diastereoselectively and enantiomerically enriched products. Finally, highly regioselective magnesiations of functionalized arenes and heteroarenes undergo Negishi (after transmetalation with ZnCl2) or Cu-catalyzed cross-couplings.},
keywords = {Foundry Organic},
pubstate = {published},
tppubtype = {article}
}
M Kraut, F Pantle, S Wörle, E Sirotti, A Zeidler, F Eckmann, M Stutzmann
Influence of environmental conditions and surface treatments on the photoluminescence properties of GaN nanowires and nanofins Journal Article
In: Nanotechnology, 2021, ISSN: 0957-4484.
Tags: Foundry Inorganic, Solid-Solid
@article{nokey,
title = {Influence of environmental conditions and surface treatments on the photoluminescence properties of GaN nanowires and nanofins},
author = {M Kraut and F Pantle and S W\"{o}rle and E Sirotti and A Zeidler and F Eckmann and M Stutzmann},
issn = {0957-4484},
year = {2021},
date = {2021-08-16},
journal = {Nanotechnology},
keywords = {Foundry Inorganic, Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
D Potamianos, M Nuber, A Schletter, M Schnitzenbaumer, M Haimerl, P Scigalla, M Wörle, L I Wagner, R Kienberger, H Iglev
Full Dynamics Description of Mg Phthalocyanine Crystalline and Amorphous Semiconductor Systems Journal Article
In: The Journal of Physical Chemistry C, 2021, ISSN: 1932-7447.
Abstract | Links | Tags: Foundry Inorganic, Foundry Organic
@article{nokey,
title = {Full Dynamics Description of Mg Phthalocyanine Crystalline and Amorphous Semiconductor Systems},
author = {D Potamianos and M Nuber and A Schletter and M Schnitzenbaumer and M Haimerl and P Scigalla and M W\"{o}rle and L I Wagner and R Kienberger and H Iglev},
url = {https://doi.org/10.1021/acs.jpcc.1c04698},
doi = {10.1021/acs.jpcc.1c04698},
issn = {1932-7447},
year = {2021},
date = {2021-08-16},
journal = {The Journal of Physical Chemistry C},
abstract = {Based on visible and mid-infrared transient absorption studies, probing the inter- and intraband dynamics, respectively, of magnesium phthalocyanine (MgPc) organic semiconductors, we were able to develop a model to describe the dynamics and the resulting optical response. We demonstrate how the model could offer insights into the dynamics of more complicated systems such as amorphous MgPc samples obtained by established preparation methods. In particular, we show a clear dimensionality difference of the exciton dissipation mechanism between crystalline and amorphous MgPc, which we resolve in the intraband dynamics, and how this result can also be deduced from the interband dynamics through the implementation of the developed model.},
keywords = {Foundry Inorganic, Foundry Organic},
pubstate = {published},
tppubtype = {article}
}
R Shivhare, G J Moore, A Hofacker, S Hutsch, Y Zhong, M Hambsch, T Erdmann, A Kiriy, S C Mannsfeld, F Ortmann
Short Excited‐State Lifetimes Mediate Charge‐Recombination Losses in Organic Solar Cell Blends with Low Charge‐Transfer Driving Force Journal Article
In: Advanced Materials, pp. 2101784, 2021, ISSN: 0935-9648.
Links | Tags: Foundry Organic
@article{nokey,
title = {Short Excited‐State Lifetimes Mediate Charge‐Recombination Losses in Organic Solar Cell Blends with Low Charge‐Transfer Driving Force},
author = {R Shivhare and G J Moore and A Hofacker and S Hutsch and Y Zhong and M Hambsch and T Erdmann and A Kiriy and S C Mannsfeld and F Ortmann},
doi = {https://doi.org/10.1002/adma.202101784},
issn = {0935-9648},
year = {2021},
date = {2021-08-15},
urldate = {2021-08-15},
journal = {Advanced Materials},
pages = {2101784},
keywords = {Foundry Organic},
pubstate = {published},
tppubtype = {article}
}
J Wang, J Kühne, T Karamanos, C Rockstuhl, S A Maier, A Tittl
All‐Dielectric Crescent Metasurface Sensor Driven by Bound States in the Continuum Journal Article
In: Advanced Functional Materials, pp. 2104652, 2021, ISSN: 1616-301X.
Tags: Foundry Inorganic
@article{nokey,
title = {All‐Dielectric Crescent Metasurface Sensor Driven by Bound States in the Continuum},
author = {J Wang and J K\"{u}hne and T Karamanos and C Rockstuhl and S A Maier and A Tittl},
issn = {1616-301X},
year = {2021},
date = {2021-08-13},
journal = {Advanced Functional Materials},
pages = {2104652},
keywords = {Foundry Inorganic},
pubstate = {published},
tppubtype = {article}
}
M Beetz, S Häringer, P Elsässer, J Kampmann, L Sauerland, F Wolf, M Günther, A Fischer, T Bein
Ultra‐Thin Protective Coatings for Sustained Photoelectrochemical Water Oxidation with Mo: BiVO4 Journal Article
In: Advanced Functional Materials, pp. 2011210, 2021, ISSN: 1616-301X.
Links | Tags: Foundry Inorganic, Solid-Solid
@article{nokey,
title = {Ultra‐Thin Protective Coatings for Sustained Photoelectrochemical Water Oxidation with Mo: BiVO4},
author = {M Beetz and S H\"{a}ringer and P Els\"{a}sser and J Kampmann and L Sauerland and F Wolf and M G\"{u}nther and A Fischer and T Bein},
url = {https://doi.org/10.1002/adfm.202011210},
issn = {1616-301X},
year = {2021},
date = {2021-08-12},
urldate = {2021-08-12},
journal = {Advanced Functional Materials},
pages = {2011210},
keywords = {Foundry Inorganic, Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
T Tian, S Yin, S Tu, C L Weindl, K S Wienhold, S Liang, M Schwartzkopf, S V Roth, P Müller-Buschbaum
In: Advanced Functional Materials, vol. n/a, no. n/a, pp. 2105644, 2021, ISSN: 1616-301X.
Abstract | Links | Tags: Foundry Inorganic, Molecularly-Functionalized
@article{nokey,
title = {Morphology Transformation Pathway of Block Copolymer-Directed Cooperative Self-Assembly of ZnO Hybrid Films Monitored In Situ during Slot-Die Coating},
author = {T Tian and S Yin and S Tu and C L Weindl and K S Wienhold and S Liang and M Schwartzkopf and S V Roth and P M\"{u}ller-Buschbaum},
url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adfm.202105644},
doi = {https://doi.org/10.1002/adfm.202105644},
issn = {1616-301X},
year = {2021},
date = {2021-08-12},
journal = {Advanced Functional Materials},
volume = {n/a},
number = {n/a},
pages = {2105644},
abstract = {Abstract Cooperative self-assembly (co-assembly) of diblock copolymers (DBCs) and inorganic precursors that takes inspiration from the rich phase separation behavior of DBCs can enable the realization of a broad spectrum of functional nanostructures with the desired sizes. In a DBC assisted sol\textendashgel chemistry approach with polystyrene-block-poly(ethylene oxide) and ZnO, hybrid films are formed with slot-die coating. Pure DBC films are printed as control. In situ grazing-incidence small-angle X-ray scattering measurements are performed to investigate the self-assembly and co-assembly process during the film formation. Combining complementary ex situ characterizations, several distinct regimes are differentiated to describe the morphological transformations from the initially solvent-dispersed to the ultimately solidified films. The comparison of the assembly pathway evidences that the key step in the establishment of the pure DBC film is the coalescence of spherical micelles toward cylindrical domains. Due to the presence of the phase-selective precursor, the formation of cylindrical aggregates in the solution is crucial for the structural development of the hybrid film. The pre-existing cylinders in the ink impede the domain growth of the hybrid film during the subsequent drying process. The precursor reduces the degree of order, prevents crystallization of the PEO block, and introduces additional length scales in the hybrid films.},
keywords = {Foundry Inorganic, Molecularly-Functionalized},
pubstate = {published},
tppubtype = {article}
}
F Li, Y Liu, G Shi, W Chen, R Guo, D Liu, Y Zhang, Y Wang, X Meng, X Zhang, Y Lv, W Deng, Q Zhang, Y Shi, Y Chen, K Wang, Q Shen, Z Liu, P Müller-Buschbaum, W Ma
Matrix Manipulation of Directly-Synthesized PbS Quantum Dot Inks Enabled by Coordination Engineering Journal Article
In: Advanced Functional Materials, vol. n/a, no. n/a, pp. 2104457, 2021, ISSN: 1616-301X.
Abstract | Links | Tags: Foundry Inorganic
@article{,
title = {Matrix Manipulation of Directly-Synthesized PbS Quantum Dot Inks Enabled by Coordination Engineering},
author = {F Li and Y Liu and G Shi and W Chen and R Guo and D Liu and Y Zhang and Y Wang and X Meng and X Zhang and Y Lv and W Deng and Q Zhang and Y Shi and Y Chen and K Wang and Q Shen and Z Liu and P M\"{u}ller-Buschbaum and W Ma},
url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adfm.202104457},
doi = {https://doi.org/10.1002/adfm.202104457},
issn = {1616-301X},
year = {2021},
date = {2021-08-06},
journal = {Advanced Functional Materials},
volume = {n/a},
number = {n/a},
pages = {2104457},
abstract = {Abstract The direct-synthesis of conductive PbS quantum dot (QD) ink is facile, scalable, and low-cost, boosting the future commercialization of optoelectronics based on colloidal QDs. However, manipulating the QD matrix structures still is a challenge, which limits the corresponding QD solar cell performance. Here, for the first time a coordination-engineering strategy to finely adjust the matrix thickness around the QDs is presented, in which halogen salts are introduced into the reaction to convert the excessive insulating lead iodide into soluble iodoplumbate species. As a result, the obtained QD film exhibits shrunk insulating shells, leading to higher charge carrier transport and superior surface passivation compared to the control devices. A significantly improved power-conversion efficiency from 10.52% to 12.12% can be achieved after the matrix engineering. Therefore, the work shows high significance in promoting the practical application of directly synthesized PbS QD inks in large-area low-cost optoelectronic devices.},
keywords = {Foundry Inorganic},
pubstate = {published},
tppubtype = {article}
}
M Kick, C Scheurer, H Oberhofer
Polaron-Assisted Charge Transport in Li-Ion Battery Anode Materials Journal Article
In: ACS Applied Energy Materials, 2021.
Abstract | Links | Tags: Foundry Inorganic, Solid-Solid
@article{,
title = {Polaron-Assisted Charge Transport in Li-Ion Battery Anode Materials},
author = {M Kick and C Scheurer and H Oberhofer},
url = {https://doi.org/10.1021/acsaem.1c01767},
doi = {10.1021/acsaem.1c01767},
year = {2021},
date = {2021-08-04},
journal = {ACS Applied Energy Materials},
abstract = {Lithium-ion batteries are without a doubt a key technology in the coming energy revolution. It is thus all the more surprising that one of the more prevalent Li battery anode materials, reduced lithium titanium oxide (LTO, Li4Ti5O12), is still poorly understood on a microscopic level. While recent theoretical and experimental evidence suggests that a polaron hopping mechanism is responsible for the increased electronic conductivity of reduced LTO, no such explanation exists for the concurrent improvements to the ionic mobility. In this computational study, we show that the presence of polaronic Ti3+ centers can indeed lead to a significant lowering of Li hopping barriers in both bulk and surface reduced LTO. For the latter, we find a reduced barrier height of roughly 40 meV compared to that of our pristine reference. This is in accordance with experimental findings showing that lithium-ion diffusion in reduced LTO is twice as high as that for pristine LTO. Finally, we show that\textemdashin accordance with experimental observations\textemdashpolaron formation upon lithiation of LTO leads to a similar behavior. Altogether, our analysis hints at a correlated movement of Li ions and polarons, highlighting LTO’s potential for rational defect engineering.},
keywords = {Foundry Inorganic, Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
Z Wang, L S Walter, M Wang, P S Petkov, B Liang, H Qi, N N Nguyen, M Hambsch, H Zhong, M Wang, S Park, L Renn, K Watanabe, T Taniguchi, S C B Mannsfeld, T Heine, U Kaiser, S Zhou, R T Weitz, X Feng, R Dong
Interfacial Synthesis of Layer-Oriented 2D Conjugated Metal–Organic Framework Films toward Directional Charge Transport Journal Article
In: Journal of the American Chemical Society, 2021, ISSN: 0002-7863.
Abstract | Links | Tags: Molecularly-Functionalized
@article{,
title = {Interfacial Synthesis of Layer-Oriented 2D Conjugated Metal\textendashOrganic Framework Films toward Directional Charge Transport},
author = {Z Wang and L S Walter and M Wang and P S Petkov and B Liang and H Qi and N N Nguyen and M Hambsch and H Zhong and M Wang and S Park and L Renn and K Watanabe and T Taniguchi and S C B Mannsfeld and T Heine and U Kaiser and S Zhou and R T Weitz and X Feng and R Dong},
url = {https://doi.org/10.1021/jacs.1c05051},
doi = {10.1021/jacs.1c05051},
issn = {0002-7863},
year = {2021},
date = {2021-08-03},
journal = {Journal of the American Chemical Society},
abstract = {The development of layer-oriented two-dimensional conjugated metal\textendashorganic frameworks (2D c-MOFs) enables access to direct charge transport, dial-in lateral/vertical electronic devices, and the unveiling of transport mechanisms but remains a significant synthetic challenge. Here we report the novel synthesis of metal-phthalocyanine-based p-type semiconducting 2D c-MOF films (Cu2[PcM\textendashO8]},
keywords = {Molecularly-Functionalized},
pubstate = {published},
tppubtype = {article}
}
T Ameri, L Ke, N Gasparini, R Soltani, M Günther, A Buyruk, A A Amin
Advanced Printed Semiconductors for Energy and Electronic Applications Journal Article
In: Video Proceedings of Advanced Materials, vol. 2, 2021.
Links | Tags: Foundry Organic, Molecularly-Functionalized
@article{nokey,
title = {Advanced Printed Semiconductors for Energy and Electronic Applications},
author = {T Ameri and L Ke and N Gasparini and R Soltani and M G\"{u}nther and A Buyruk and A A Amin},
url = {https://www.proceedings.iaamonline.org/image/article/1628028399Tayebeh-Ameri---Abstract.pdf},
doi = {https://www.proceedings.iaamonline.org/image/article/1628028399Tayebeh-Ameri---Abstract.pdf},
year = {2021},
date = {2021-08-03},
urldate = {2021-08-03},
journal = {Video Proceedings of Advanced Materials},
volume = {2},
keywords = {Foundry Organic, Molecularly-Functionalized},
pubstate = {published},
tppubtype = {article}
}
C Zhu, C Fan, E Cortés, W Xie
In situ surface-enhanced Raman spectroelectrochemistry reveals the molecular conformation of electrolyte additives in Li-ion batteries Journal Article
In: Journal of Materials Chemistry A, vol. 9, no. 35, pp. 20024-20031, 2021, ISSN: 2050-7488.
@article{nokey,
title = {In situ surface-enhanced Raman spectroelectrochemistry reveals the molecular conformation of electrolyte additives in Li-ion batteries},
author = {C Zhu and C Fan and E Cort\'{e}s and W Xie},
url = {http://dx.doi.org/10.1039/D1TA04218A},
doi = {10.1039/D1TA04218A},
issn = {2050-7488},
year = {2021},
date = {2021-08-02},
journal = {Journal of Materials Chemistry A},
volume = {9},
number = {35},
pages = {20024-20031},
abstract = {We report the mechanism of rhodamine B (RhB) acting as an electrolyte additive in Li/graphite cells. We show that the cycle performance and rate capability of graphite are enhanced in carbonate-based electrolytes containing 0.2 wt% RhB. By using silica-encapsulated Au nanoparticles, in situ surface-enhanced Raman spectroscopy (SERS) is applied to study the graphite/electrolyte interface. We find that the adsorption orientation of RhB molecules on the surface of graphite can be modulated by the applied potential: vertical adsorption at higher potentials while horizontal adsorption takes place at lower potentials. This behavior effectively suppresses the electrolyte solvent decomposition, as well as electrode corrosion while improving the Li+ diffusion. This work shows that SERS is a powerful tool for interfacial analysis of battery systems and provides new ideas for rational design of electrolyte additives.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
D Han, C Feng, M-H Du, T Zhang, S Wang, G Tang, T Bein, H Ebert
Design of High-Performance Lead-Free Quaternary Antiperovskites for Photovoltaics via Ion Type Inversion and Anion Ordering Journal Article
In: Journal of the American Chemical Society, vol. 143, no. 31, pp. 12369-12379, 2021, ISSN: 0002-7863.
Abstract | Links | Tags: Foundry Inorganic, Solid-Solid
@article{,
title = {Design of High-Performance Lead-Free Quaternary Antiperovskites for Photovoltaics via Ion Type Inversion and Anion Ordering},
author = {D Han and C Feng and M-H Du and T Zhang and S Wang and G Tang and T Bein and H Ebert},
url = {https://doi.org/10.1021/jacs.1c06403},
doi = {10.1021/jacs.1c06403},
issn = {0002-7863},
year = {2021},
date = {2021-08-02},
urldate = {2021-08-02},
journal = {Journal of the American Chemical Society},
volume = {143},
number = {31},
pages = {12369-12379},
abstract = {The emergence of halide double perovskites significantly increases the compositional space for lead-free and air-stable photovoltaic absorbers compared to halide perovskites. Nevertheless, most halide double perovskites exhibit oversized band gaps (\>1.9 eV) or dipole-forbidden optical transition, which are unfavorable for efficient single-junction solar cell applications. The current device performance of halide double perovskite is still inferior to that of lead-based halide perovskites, such as CH3NH3PbI3 (MAPbI3). Here, by ion type inversion and anion ordering on perovskite lattice sites, two new classes of pnictogen-based quaternary antiperovskites with the formula of X6B2AA′ and X6BB′A2 are designed. Phase stability and tunable band gaps in these quaternary antiperovskites are demonstrated based on first-principles calculations. Further photovoltaic-functionality-directed screening of these materials leads to the discovery of 5 stable compounds (Ca6N2AsSb, Ca6N2PSb, Sr6N2AsSb, Sr6N2PSb, and Ca6NPSb2) with suitable direct band gaps, small carrier effective masses and low exciton binding energies, and dipole-allowed strong optical absorption, which are favorable properties for a photovoltaic absorber material. The calculated theoretical maximum solar cell efficiencies based on these five compounds are all larger than 29%, comparable to or even higher than that of the MAPbI3 based solar cell. Our work reveals the huge potential of quaternary antiperovskites in the optoelectronic field and provides a new strategy to design lead-free and air-stable perovskite-based photovoltaic absorber materials.},
keywords = {Foundry Inorganic, Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
S Hou, W Li, S Watzele, R M Kluge, S Xue, S Yin, X Jiang, M Döblinger, A Welle, B Garlyyev, M Koch, P Müller-Buschbaum, C Wöll, A S Bandarenka, R A Fischer
Metamorphosis of Heterostructured Surface-Mounted Metal–Organic Frameworks Yielding Record Oxygen Evolution Mass Activities Journal Article
In: Advanced Materials, vol. 33, pp. 2103218, 2021, ISSN: 0935-9648.
Abstract | Links | Tags: Foundry Inorganic, Molecularly-Functionalized
@article{,
title = {Metamorphosis of Heterostructured Surface-Mounted Metal\textendashOrganic Frameworks Yielding Record Oxygen Evolution Mass Activities},
author = {S Hou and W Li and S Watzele and R M Kluge and S Xue and S Yin and X Jiang and M D\"{o}blinger and A Welle and B Garlyyev and M Koch and P M\"{u}ller-Buschbaum and C W\"{o}ll and A S Bandarenka and R A Fischer},
url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adma.202103218},
doi = {https://doi.org/10.1002/adma.202103218},
issn = {0935-9648},
year = {2021},
date = {2021-08-01},
urldate = {2021-08-01},
journal = {Advanced Materials},
volume = {33},
pages = {2103218},
abstract = {Abstract Materials derived from surface-mounted metal\textendashorganic frameworks (SURMOFs) are promising electrocatalysts for the oxygen evolution reaction (OER). A series of mixed-metal, heterostructured SURMOFs is fabricated by the facile layer-by-layer deposition method. The obtained materials reveal record-high electrocatalyst mass activities of ≈2.90 kA g−1 at an overpotential of 300 mV in 0.1 m KOH, superior to the benchmarking precious and nonprecious metal electrocatalysts. This property is assigned to the particular in situ self-reconstruction and self-activation of the SURMOFs during the immersion and the electrochemical treatment in alkaline aqueous electrolytes, which allows for the generation of NiFe (oxy)hydroxide electrocatalyst materials of specific morphology and microstructure.},
keywords = {Foundry Inorganic, Molecularly-Functionalized},
pubstate = {published},
tppubtype = {article}
}
S A Watzele, L Katzenmeier, J P Sabawa, B Garlyyev, A S Bandarenka
Temperature dependences of the double layer capacitance of some solid/liquid and solid/solid electrified interfaces. An experimental study Journal Article
In: Electrochimica Acta, vol. 391, pp. 138969, 2021, ISSN: 0013-4686.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid, Solid-Solid
@article{,
title = {Temperature dependences of the double layer capacitance of some solid/liquid and solid/solid electrified interfaces. An experimental study},
author = {S A Watzele and L Katzenmeier and J P Sabawa and B Garlyyev and A S Bandarenka},
url = {https://www.sciencedirect.com/science/article/pii/S0013468621012597},
doi = {https://doi.org/10.1016/j.electacta.2021.138969},
issn = {0013-4686},
year = {2021},
date = {2021-07-30},
journal = {Electrochimica Acta},
volume = {391},
pages = {138969},
abstract = {This study investigates the influence of the temperature on the electrical double layer capacitance (CDL) of various materials, which are essential for fuel cells and solid-state Li-ion batteries. Electrochemical impedance spectroscopy is utilized to measure the CDL of polycrystalline Pt/aqueous electrolytes interfaces, cathode catalyst layers of polymer electrolyte membrane fuel cells (PEMFC), and Au or Li electrodes in contact with a solid-state electrolyte (SSE), a prime example for solid-state ionics. Our results show that within the investigated temperature ranges, the CDL decreases with an increase in the temperature for Pt electrodes in an aqueous acidic electrolyte. However, for SSE and PEMFC cathode catalyst layers, the CDL increases with temperature. The CDL behavior with the temperature of herein presented systems is important for understanding and modeling of the interface processes for renewable energy conversion systems such as fuel cells, water electrolyzers, and batteries.},
keywords = {Foundry Inorganic, Solid-Liquid, Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
P I Scheurle, A Mähringer, A Biewald, A Hartschuh, T Bein, D D Medina
MOF-74(M) Films Obtained through Vapor-Assisted Conversion—Impact on Crystal Orientation and Optical Properties Journal Article
In: Chemistry of Materials, vol. 33, no. 15, pp. 5896-5904, 2021, ISSN: 0897-4756.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{nokey,
title = {MOF-74(M) Films Obtained through Vapor-Assisted Conversion\textemdashImpact on Crystal Orientation and Optical Properties},
author = {P I Scheurle and A M\"{a}hringer and A Biewald and A Hartschuh and T Bein and D D Medina},
url = {https://doi.org/10.1021/acs.chemmater.1c00743},
doi = {10.1021/acs.chemmater.1c00743},
issn = {0897-4756},
year = {2021},
date = {2021-07-28},
journal = {Chemistry of Materials},
volume = {33},
number = {15},
pages = {5896-5904},
abstract = {In recent years, metal\textendashorganic frameworks (MOFs) with the structure MOF-74 have attracted much interest owing to their tunable pore aperture, high surface area, and electrical conductivity. The synthesis of well-defined, highly crystalline thin films of MOF-74 is of paramount importance for their implementation into device-based applications such as in chemical sensing, optoelectronics, gas storage, and separations. Here, we present the synthesis of highly crystalline MOF-74 (M = Zn2+, Mg2+, Ni2+, and Co2+) films by vapor-assisted conversion. MOF-74(M) thin films were grown on bare glass, quartz, gold, and silicon surfaces, showing high crystallinity, crystal orientation, and average thicknesses of 500 nm. By including a benzoic acid modulator, oriented MOF-74(Zn) films, with the crystallographic c-axis of the MOF crystallites oriented horizontally to the surface, were obtained on all substrates. In addition, highly crystalline MOF-74(Mg) was grown on glass and gold substrates with the crystallographic c-axis aligned orthogonally to the surface. Moreover, randomly oriented highly crystalline MOF-74(Co) and MOF-74(Ni) films were synthesized on glass, quartz, gold, and silicon. The pore accessibility of the obtained films was examined by means of krypton sorption measurements, revealing permanent and accessible porosity, reaching a BET surface area of 975 cm2/cm2 for MOF-74(Mg). Steady-state and time-resolved photoluminescence studies show emission in the blue spectral region of MOF-74(Zn and Mg) on quartz with a biexponential decay. In addition, confocal photoluminescence mapping confirmed a homogeneous MOF film surface with a similar emission profile over the whole examined area of 70 μm × 70 μm.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
L K Reb, M Böhmer, B Predeschly, S Grott, C Dreißigacker, J Drescher, A Meyer, P Müller-Buschbaum
An experiment for novel material thin-film solar cell characterization on sounding rocket flights Journal Article
In: Review of Scientific Instruments, vol. 92, no. 7, pp. 074501, 2021.
Links | Tags: Foundry Inorganic
@article{,
title = {An experiment for novel material thin-film solar cell characterization on sounding rocket flights},
author = {L K Reb and M B\"{o}hmer and B Predeschly and S Grott and C Drei\ssigacker and J Drescher and A Meyer and P M\"{u}ller-Buschbaum},
url = {https://aip.scitation.org/doi/abs/10.1063/5.0047346},
doi = {10.1063/5.0047346},
year = {2021},
date = {2021-07-26},
journal = {Review of Scientific Instruments},
volume = {92},
number = {7},
pages = {074501},
keywords = {Foundry Inorganic},
pubstate = {published},
tppubtype = {article}
}
M Joos, C Schneider, A Münchinger, I Moudrakovski, R Usiskin, J Maier, B V Lotsch
Impact of hydration on ion transport in Li2Sn2S5·xH2O Journal Article
In: Journal of Materials Chemistry A, vol. 9, no. 30, pp. 16532-16544, 2021, ISSN: 2050-7488.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{nokey,
title = {Impact of hydration on ion transport in Li2Sn2S5·xH2O},
author = {M Joos and C Schneider and A M\"{u}nchinger and I Moudrakovski and R Usiskin and J Maier and B V Lotsch},
url = {http://dx.doi.org/10.1039/D1TA04736A},
doi = {10.1039/D1TA04736A},
issn = {2050-7488},
year = {2021},
date = {2021-07-23},
journal = {Journal of Materials Chemistry A},
volume = {9},
number = {30},
pages = {16532-16544},
abstract = {This work investigates the structure and transport properties of the layered material Li2Sn2S5·xH2O. The anhydrous phase shows a room-temperature Li+ diffusivity below 10−9 cm2 s−1 and conductivity below 10−5 S cm−1. Upon exposure to humidity, water intercalates between the layers and increases the interlayer distance, inducing first-order transitions to a hydrated phase (x ≈ 2\textendash4) and then to a second hydrated phase (x ≈ 8\textendash10). The latter is soft and sticky but remains solid. Diffusion of both Li+ ions and H2O remains predominantly two-dimensional under all conditions. The Li+ diffusivity and conductivity both increase by three orders of magnitude upon hydration, reaching values of 5 × 10−7 cm2 s−1 and 10−2 S cm−1 in the second hydrate. These transport rates are extraordinary for a solid electrolyte and approach what is typically seen in aqueous solutions. The material Li2Sn2S5·xH2O thus bridges the gap between a hydrated solid electrolyte and a confined liquid electrolyte, which is scientifically interesting and potentially useful in battery applications. In the light of these findings, a previous work on Li2Sn2S5 from our groups is revisited.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
G C Tok, S Reiter, A T S Freiberg, L Reinschlüssel, H A Gasteiger, R De Vivie-Riedle, C R Hess
H2 Evolution from Electrocatalysts with Redox-Active Ligands: Mechanistic Insights from Theory and Experiment vis-à-vis Co-Mabiq Journal Article
In: Inorganic Chemistry, 2021, ISSN: 0020-1669.
Abstract | Links | Tags: Foundry Inorganic, Molecularly-Functionalized
@article{,
title = {H2 Evolution from Electrocatalysts with Redox-Active Ligands: Mechanistic Insights from Theory and Experiment vis-\`{a}-vis Co-Mabiq},
author = {G C Tok and S Reiter and A T S Freiberg and L Reinschl\"{u}ssel and H A Gasteiger and R De Vivie-Riedle and C R Hess},
url = {https://doi.org/10.1021/acs.inorgchem.1c01157},
doi = {10.1021/acs.inorgchem.1c01157},
issn = {0020-1669},
year = {2021},
date = {2021-07-23},
urldate = {2021-07-23},
journal = {Inorganic Chemistry},
abstract = {Electrocatalytic hydrogen production via transition metal complexes offers a promising approach for chemical energy storage. Optimal platforms to effectively control the proton and electron transfer steps en route to H2 evolution still need to be established, and redox-active ligands could play an important role in this context. In this study, we explore the role of the redox-active Mabiq (Mabiq = 2\textendash4:6\textendash8-bis(3,3,4,4-tetramethlyldihydropyrrolo)-10\textendash15-(2,2-biquinazolino)-[15]-1,3,5,8,10,14-hexaene1,3,7,9,11,14-N6) ligand in the hydrogen evolution reaction (HER). Using spectro-electrochemical studies in conjunction with quantum chemical calculations, we identified two precatalytic intermediates formed upon the addition of two electrons and one proton to [CoII(Mabiq)(THF)](PF6) (CoMbq). We further examined the acid strength effect on the generation of the intermediates. The generation of the first intermediate, CoMbq-H1, involves proton addition to the bridging imine-nitrogen atom of the ligand and requires strong proton activity. The second intermediate, CoMbq-H2, acquires a proton at the diketiminate carbon for which a weaker proton activity is sufficient. We propose two decoupled H2 evolution pathways based on these two intermediates, which operate at different overpotentials. Our results show how the various protonation sites of the redox-active Mabiq ligand affect the energies and activities of HER intermediates.},
keywords = {Foundry Inorganic, Molecularly-Functionalized},
pubstate = {published},
tppubtype = {article}
}