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.
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},
issn = {0935-9648},
year = {2021},
date = {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}
}
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}
}
K Jayaramulu, M Esclance Dmello, K Kesavan, A Schneemann, M Otyepka, S Kment, C Narayana, S B Kalidindi, R S Varma, R Zboril, R A Fischer
A multifunctional covalently linked graphene–MOF hybrid as an effective chemiresistive gas sensor Journal Article
In: Journal of Materials Chemistry A, vol. 9, no. 32, pp. 17434-17441, 2021, ISSN: 2050-7488.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{nokey,
title = {A multifunctional covalently linked graphene\textendashMOF hybrid as an effective chemiresistive gas sensor},
author = {K Jayaramulu and M Esclance Dmello and K Kesavan and A Schneemann and M Otyepka and S Kment and C Narayana and S B Kalidindi and R S Varma and R Zboril and R A Fischer},
url = {http://dx.doi.org/10.1039/D1TA03246A},
doi = {10.1039/D1TA03246A},
issn = {2050-7488},
year = {2021},
date = {2021-07-22},
journal = {Journal of Materials Chemistry A},
volume = {9},
number = {32},
pages = {17434-17441},
abstract = {A hybrid of GA@UiO-66-NH2 was synthesized based on the covalent assembly of graphene acid (GA) and the amine functionalized UiO-66 metal\textendashorganic framework through amide bonds. This strategy endows the material with unique properties, such as hierarchical pores, a porous conductive network decorated with functional groups, a high specific surface area, and a good chemical and thermal stability. The resultant hybrid has an electrical resistance of ∼104 Ω, whereas the pristine GA and UiO-66-NH2 possess an electrical resistance of ∼102 Ω and ∼109 Ω, respectively. The hybrid GA@UiO-66-NH2 was demonstrated for CO2 chemiresistive sensing and displayed a very fast response and quick recovery time of ∼18 s for 100% CO2, at 200 °C. While the pristine GA exhibits negligible response under the same conditions, GA@UiO-66-NH2 exhibited a response of 10 ± 0.6%. Further, in situ temperature dependent Raman studies during CO2 exposure confirm the presence of strong hydrogen bonding interaction between CO2 and the amide functionality present on GA@UiO-66-NH2. The resulting gas sensing characteristics of GA@UiO-66-NH2 are majorly attributed to the better interaction of CO2 at the amide/amine functional groups and the readily accessible hierarchical pores. This design strategy opens new horizons in the development of covalently linked hybrids with hierarchical porous conductive networks which can help to improve the gas sensing properties of MOF-based materials.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
A Stefancu, S Lee, L Zhu, M Liu, R C Lucacel, E Cortés, N Leopold
Fermi Level Equilibration at the Metal–Molecule Interface in Plasmonic Systems Journal Article
In: Nano Letters, 2021, ISSN: 1530-6984.
Abstract | Links | Tags: Foundry Inorganic, Molecularly-Functionalized
@article{,
title = {Fermi Level Equilibration at the Metal\textendashMolecule Interface in Plasmonic Systems},
author = {A Stefancu and S Lee and L Zhu and M Liu and R C Lucacel and E Cort\'{e}s and N Leopold},
url = {https://doi.org/10.1021/acs.nanolett.1c02003},
doi = {10.1021/acs.nanolett.1c02003},
issn = {1530-6984},
year = {2021},
date = {2021-07-22},
urldate = {2021-07-22},
journal = {Nano Letters},
abstract = {We highlight a new metal\textendashmolecule charge transfer process by tuning the Fermi energy of plasmonic silver nanoparticles (AgNPs) in situ. The strong adsorption of halide ions upshifts the Fermi level of AgNPs by up to ∼0.3 eV in the order Cl\textendash \< Br\textendash \< I\textendash, favoring the spontaneous charge transfer to aligned molecular acceptor orbitals until charge neutrality across the interface is achieved. By carefully quantifying, experimentally and theoretically, the Fermi level upshift, we show for the first time that this effect is comparable in energy to different plasmonic effects such as the plasmoelectric effect or hot-carriers production. Moreover, by monitoring in situ the adsorption dynamic of halide ions in different AgNP\textendashmolecule systems, we show for the first time that the catalytic role of halide ions in plasmonic nanostructures depends on the surface affinity of halide ions compared to that of the target molecule.},
keywords = {Foundry Inorganic, Molecularly-Functionalized},
pubstate = {published},
tppubtype = {article}
}
D N Purschke, M R P Pielmeier, E Üzer, C Ott, C Jensen, A Degg, A Vogel, N Amer, T Nilges, F A Hegmann
Ultrafast Photoconductivity and Terahertz Vibrational Dynamics in Double-Helix SnIP Nanowires Journal Article
In: Advanced Materials, vol. n/a, no. n/a, pp. 2100978, 2021, ISSN: 0935-9648.
Abstract | Links | Tags: Solid-Solid
@article{,
title = {Ultrafast Photoconductivity and Terahertz Vibrational Dynamics in Double-Helix SnIP Nanowires},
author = {D N Purschke and M R P Pielmeier and E \"{U}zer and C Ott and C Jensen and A Degg and A Vogel and N Amer and T Nilges and F A Hegmann},
url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adma.202100978},
doi = {https://doi.org/10.1002/adma.202100978},
issn = {0935-9648},
year = {2021},
date = {2021-07-19},
journal = {Advanced Materials},
volume = {n/a},
number = {n/a},
pages = {2100978},
abstract = {Abstract Tin iodide phosphide (SnIP), an inorganic double-helix material, is a quasi-1D van der Waals semiconductor that shows promise in photocatalysis and flexible electronics. However, the understanding of the fundamental photophysics and charge transport dynamics of this new material is limited. Here, time-resolved terahertz (THz) spectroscopy is used to probe the transient photoconductivity of SnIP nanowire films and measure the carrier mobility. With insight into the highly anisotropic electronic structure from quantum chemical calculations, an electron mobility as high as 280 cm2 V−1s−1 along the double-helix axis and a hole mobility of 238 cm2 V−1 s−1 perpendicular to the double-helix axis are detected. Additionally, infrared-active (IR-active) THz vibrational modes are measured, which shows excellent agreement with first-principles calculations, and an ultrafast photoexcitation-induced charge redistribution is observed that reduces the amplitude of a twisting mode of the outer SnI helix on picosecond timescales. Finally, it is shown that the carrier lifetime and mobility are limited by a trap density greater than 1018 cm−3. The results provide insight into the optical excitation and relaxation pathways of SnIP and demonstrate a remarkably high carrier mobility for such a soft and flexible material, suggesting that it could be ideally suited for flexible electronics applications.},
keywords = {Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
S Kaiser, F Maleki, K Zhang, W Harbich, U Heiz, S Tosoni, B A J Lechner, G Pacchioni, F Esch
Cluster Catalysis with Lattice Oxygen: Tracing Oxygen Transport from a Magnetite (001) Support onto Small Pt Clusters Journal Article
In: ACS Catalysis, vol. 11, no. 15, pp. 9519–9529, 2021.
Links | Tags: Foundry Inorganic, Molecularly-Functionalized, Solid-Solid
@article{,
title = {Cluster Catalysis with Lattice Oxygen: Tracing Oxygen Transport from a Magnetite (001) Support onto Small Pt Clusters},
author = {S Kaiser and F Maleki and K Zhang and W Harbich and U Heiz and S Tosoni and B A J Lechner and G Pacchioni and F Esch},
url = {https://pubs.acs.org/doi/10.1021/acscatal.1c01451},
year = {2021},
date = {2021-07-16},
urldate = {2021-07-16},
journal = {ACS Catalysis},
volume = {11},
number = {15},
pages = {9519\textendash9529},
keywords = {Foundry Inorganic, Molecularly-Functionalized, Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
T Götsch, H Tuerk, F-P Schmidt, I Vinke, De L B Haart, R Schlögl, K Reuter, R-A Eichel, A Knop-Gericke, C Scheurer
Visualizing the Atomic Structure Between YSZ and LSM: An Interface Stabilized by Complexions? Journal Article
In: ECS Transactions, vol. 103, no. 1, pp. 1331, 2021, ISSN: 1938-5862.
Tags: Solid-Solid
@article{,
title = {Visualizing the Atomic Structure Between YSZ and LSM: An Interface Stabilized by Complexions?},
author = {T G\"{o}tsch and H Tuerk and F-P Schmidt and I Vinke and De L B Haart and R Schl\"{o}gl and K Reuter and R-A Eichel and A Knop-Gericke and C Scheurer},
issn = {1938-5862},
year = {2021},
date = {2021-07-12},
urldate = {2021-07-12},
journal = {ECS Transactions},
volume = {103},
number = {1},
pages = {1331},
keywords = {Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
V W-H Lau, B V Lotsch
In: Advanced Energy Materials, vol. 12, no. 4, pp. 2101078, 2021, ISSN: 1614-6832.
Abstract | Links | Tags: Foundry Inorganic
@article{nokey,
title = {A Tour-Guide through Carbon Nitride-Land: Structure- and Dimensionality-Dependent Properties for Photo(Electro)Chemical Energy Conversion and Storage},
author = {V W-H Lau and B V Lotsch},
url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/aenm.202101078},
doi = {https://doi.org/10.1002/aenm.202101078},
issn = {1614-6832},
year = {2021},
date = {2021-07-11},
journal = {Advanced Energy Materials},
volume = {12},
number = {4},
pages = {2101078},
abstract = {Abstract Despite the explosion in the number of publications on the graphitic carbon nitride family of materials, much still remains unknown about their structure and the underlying properties responsible for their various applications. This critical review covers the state-of-the-art in the understanding of their structure\textendashproperty\textendashphotocatalysis relationship, from their molecular constituents to stacking as a (quasi) two-dimensional structure, highlighting the areas in which there is wide agreement and those still unresolved. This review first recounts how the structural understanding of these materials has evolved since the 19th century, followed by a commentary on the best practice for unambiguously characterizing their molecular structure and two-dimensional stacking arrangements. The recent literature is then examined to elucidate how individual molecular moieties affect their various material properties, particularly their chemical and opto\textendashelectronic properties, carrier dynamics, and catalytic reactivity, and how their use for energy applications can be impacted by the structural features across each dimension. Lastly, the translation of the aforementioned fundamental insights to rational molecular design is demonstrated, highlighting the synthesis of heptazine-based materials for order-of-magnitude improvement in photocatalytic reactivity, as well as the unusual phenomenon of stabilization of light-induced electrons, an effect currently exploited for a new paradigm in solar energy storage.},
keywords = {Foundry Inorganic},
pubstate = {published},
tppubtype = {article}
}
A Buyruk, D Blätte, M Günther, M A Scheel, N F Hartmann, M Döblinger, A Weis, A Hartschuh, P Müller-Buschbaum, T Bein, T Ameri
1,10-Phenanthroline as an Efficient Bifunctional Passivating Agent for MAPbI3 Perovskite Solar Cells Journal Article
In: ACS Applied Materials & Interfaces, 2021, ISSN: 1944-8244.
Abstract | Links | Tags: Foundry Inorganic, Solid-Solid
@article{,
title = {1,10-Phenanthroline as an Efficient Bifunctional Passivating Agent for MAPbI3 Perovskite Solar Cells},
author = {A Buyruk and D Bl\"{a}tte and M G\"{u}nther and M A Scheel and N F Hartmann and M D\"{o}blinger and A Weis and A Hartschuh and P M\"{u}ller-Buschbaum and T Bein and T Ameri},
url = {https://doi.org/10.1021/acsami.1c05055},
doi = {10.1021/acsami.1c05055},
issn = {1944-8244},
year = {2021},
date = {2021-07-09},
urldate = {2021-07-09},
journal = {ACS Applied Materials \& Interfaces},
abstract = {Passivation is one of the most promising concepts to heal defects created at the surface and grain boundaries of polycrystalline perovskite thin films, which significantly deteriorate the photovoltaic performance and stability of corresponding devices. Here, 1,10-phenanthroline, known as a bidentate chelating ligand, is implemented between the methylammonium lead iodide (MAPbI3) film and the hole-transport layer for both passivating the lead-based surface defects (undercoordinated lead ions) and converting the excess/unreacted lead iodide (PbI2) buried at interfaces, which is problematic for the long-term stability, into “neutralized” and beneficial species (PbI2(1,10-phen)x},
keywords = {Foundry Inorganic, Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
S Hou, R M Kluge, R W Haid, E L Gubanova, S A Watzele, A S Bandarenka, B Garlyyev
In: ChemElectroChem, vol. 8, no. 18, pp. 3433-3456, 2021, ISSN: 2196-0216.
Abstract | Links | Tags: Solid-Liquid
@article{nokey,
title = {A Review on Experimental Identification of Active Sites in Model Bifunctional Electrocatalytic Systems for Oxygen Reduction and Evolution Reactions},
author = {S Hou and R M Kluge and R W Haid and E L Gubanova and S A Watzele and A S Bandarenka and B Garlyyev},
url = {https://chemistry-europe.onlinelibrary.wiley.com/doi/abs/10.1002/celc.202100584},
doi = {https://doi.org/10.1002/celc.202100584},
issn = {2196-0216},
year = {2021},
date = {2021-07-08},
urldate = {2021-07-08},
journal = {ChemElectroChem},
volume = {8},
number = {18},
pages = {3433-3456},
abstract = {Abstract Efficient electrocatalysis of the oxygen reduction (ORR) and evolution (OER) reactions is essential in numerous renewable energy conversion systems, such as fuel cells, metal-air batteries, and water electrolyzers. Design and optimization of electrocatalytic materials for such systems primarily rely on understanding the nature of active centers on the catalyst surface. This review focuses on several important aspects of the experimental identification of active sites on various model bifunctional ORR/OER electrocatalytic surfaces. Applications of the state-of-the-art experimental techniques are analyzed. In addition, approaches to investigate and understand the influence of some supporting electrolyte components on the ORR and OER activities are discussed.},
keywords = {Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
W Kaiser, V Janković, N Vukmirović, A Gagliardi
Nonequilibrium Thermodynamics of Charge Separation in Organic Solar Cells Journal Article
In: The Journal of Physical Chemistry Letters, vol. 12, no. 27, pp. 6389-6397, 2021.
Abstract | Links | Tags: Solid-Solid
@article{nokey,
title = {Nonequilibrium Thermodynamics of Charge Separation in Organic Solar Cells},
author = {W Kaiser and V Jankovi\'{c} and N Vukmirovi\'{c} and A Gagliardi},
url = {https://doi.org/10.1021/acs.jpclett.1c01817},
doi = {10.1021/acs.jpclett.1c01817},
year = {2021},
date = {2021-07-07},
journal = {The Journal of Physical Chemistry Letters},
volume = {12},
number = {27},
pages = {6389-6397},
abstract = {This work presents a novel theoretical description of the nonequilibrium thermodynamics of charge separation in organic solar cells (OSCs). Using stochastic thermodynamics, we take realistic state populations derived from the phonon-assisted dynamics of electron\textendashhole pairs within photoexcited organic bilayers to connect the kinetics with the free energy profile of charge separation. Hereby, we quantify for the first time the difference between nonequilibrium and equilibrium free energy profile. We analyze the impact of energetic disorder and delocalization on free energy, average energy, and entropy. For a high disorder, the free energy profile is well-described as equilibrated. We observe significant deviations from equilibrium for delocalized electron\textendashhole pairs at a small disorder, implying that charge separation in efficient OSCs proceeds via a cold but nonequilibrated pathway. Both a large Gibbs entropy and large initial electron\textendashhole distance provide an efficient charge separation, while a decrease in the free energy barrier does not necessarily enhance charge separation.},
keywords = {Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
C Qian, V Villafane, P Soubelet, A Hötger, T Taniguchi, K Watanabe, N P Wilson, A V Stier, A W Holleitner, J J Finley
Strong coupling and non-local interactions in MoS2 monolayers coupled to high-Q nanocavities Journal Article
In: Measurement, vol. 495, no. 445, pp. 105, 2021.
Abstract | Links | Tags: Solid-Solid
@article{nokey,
title = {Strong coupling and non-local interactions in MoS2 monolayers coupled to high-Q nanocavities},
author = {C Qian and V Villafane 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://ui.adsabs.harvard.edu/abs/2021arXiv210704387Q/abstract},
doi = {arXiv:2107.04387},
year = {2021},
date = {2021-07-02},
journal = {Measurement},
volume = {495},
number = {445},
pages = {105},
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/MoS 2 /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 MoS 2 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}
}
H Li, Y Liu, K Chen, J T Margraf, Y Li, K Reuter
Subgroup Discovery Points to the Prominent Role of Charge Transfer in Breaking Nitrogen Scaling Relations at Single-Atom Catalysts on VS2 Journal Article
In: ACS Catalysis, vol. 11, no. 13, pp. 7906-7914, 2021.
Abstract | Links | Tags: Foundry Inorganic, Solid-Solid
@article{,
title = {Subgroup Discovery Points to the Prominent Role of Charge Transfer in Breaking Nitrogen Scaling Relations at Single-Atom Catalysts on VS2},
author = {H Li and Y Liu and K Chen and J T Margraf and Y Li and K Reuter},
url = {https://doi.org/10.1021/acscatal.1c01324},
doi = {10.1021/acscatal.1c01324},
year = {2021},
date = {2021-07-02},
journal = {ACS Catalysis},
volume = {11},
number = {13},
pages = {7906-7914},
abstract = {The electrochemical nitrogen reduction reaction (NRR) is a much sought-after low-energy alternative to Haber\textendashBosch ammonia synthesis. Single-atom catalysts (SACs) promise to break scaling relations between adsorption energies of key NRR reaction intermediates that severely limit the performance of extended catalysts. Here, we perform a computational screening study of transition metal (TM) SACs supported on vanadium disulfide (VS2) and indeed obtain strongly broken scaling relations. A data-driven analysis by means of outlier detection and subgroup discovery reveals that this breaking is restricted to early TMs, while detailed electronic structure analysis rationalizes it in terms of strong charge transfer to the underlying support. This charge transfer selectively weakens *N and *NH adsorption and leads to promising NRR descriptors for SACs formed of earlier TMs like Ta that would conventionally not be associated with nitrogen reduction.},
keywords = {Foundry Inorganic, Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
S Rieger, T Fürmann, J K Stolarczyk, J Feldmann
Optically Induced Coherent Phonons in Bismuth Oxyiodide (BiOI) Nanoplatelets Journal Article
In: Nano Letters, 2021, ISSN: 1530-6984.
Abstract | Links | Tags: Foundry Inorganic, Solid-Solid
@article{,
title = {Optically Induced Coherent Phonons in Bismuth Oxyiodide (BiOI) Nanoplatelets},
author = {S Rieger and T F\"{u}rmann and J K Stolarczyk and J Feldmann},
url = {https://doi.org/10.1021/acs.nanolett.1c00530},
doi = {10.1021/acs.nanolett.1c00530},
issn = {1530-6984},
year = {2021},
date = {2021-06-30},
journal = {Nano Letters},
abstract = {Bismuth oxyiodide (BiOI) is a promising material for photocatalysis combining intriguing optical and structural properties. We show that excitation by a femtosecond laser pulse creates coherent phonons inducing a time-variant oscillating modulation of the optical density. We find that the two underlying frequencies originate from lattice vibrations along the [001] crystallographic axis, the stacking direction of oppositely charged layers in BiOI. This is consistent with a subpicosecond charge separation driven by a built-in dipolar field. This partially screens the field, launching coherent phonons. Further, we determine the two major dephasing mechanisms that lead to the loss of vibronic coherence: (i) the anharmonic decay of an optical phonon into two acoustic phonons and (ii) phonon-carrier scattering. Our results provide a direct demonstration of the presence of an electric field in BiOI along the [001] axis and show its role in efficient charge separation that is crucial for photocatalytic applications of BiOI.},
keywords = {Foundry Inorganic, Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
S Zhao, E Wang, E A Üzer, S Guo, R Qi, J Tan, K Watanabe, T Taniguchi, T Nilges, P Gao, Y Zhang, H-M Cheng, B Liu, X Zou, F Wang
Anisotropic moiré optical transitions in twisted monolayer/bilayer phosphorene heterostructures Journal Article
In: Nature Communications, vol. 12, no. 1, pp. 3947, 2021, ISSN: 2041-1723.
Abstract | Links | Tags: Foundry Inorganic
@article{nokey,
title = {Anisotropic moir\'{e} optical transitions in twisted monolayer/bilayer phosphorene heterostructures},
author = {S Zhao and E Wang and E A \"{U}zer and S Guo and R Qi and J Tan and K Watanabe and T Taniguchi and T Nilges and P Gao and Y Zhang and H-M Cheng and B Liu and X Zou and F Wang},
url = {https://doi.org/10.1038/s41467-021-24272-9},
doi = {10.1038/s41467-021-24272-9},
issn = {2041-1723},
year = {2021},
date = {2021-06-24},
journal = {Nature Communications},
volume = {12},
number = {1},
pages = {3947},
abstract = {Moir\'{e} superlattices of van der Waals heterostructures provide a powerful way to engineer electronic structures of two-dimensional materials. Many novel quantum phenomena have emerged in graphene and transition metal dichalcogenide moir\'{e} systems. Twisted phosphorene offers another attractive system to explore moir\'{e} physics because phosphorene features an anisotropic rectangular lattice, different from isotropic hexagonal lattices previously reported. Here we report emerging anisotropic moir\'{e} optical transitions in twisted monolayer/bilayer phosphorenes. The optical resonances in phosphorene moir\'{e} superlattice depend sensitively on twist angle and are completely different from those in the constitute monolayer and bilayer phosphorene even for a twist angle as large as 19°. Our calculations reveal that the Γ-point direct bandgap and the rectangular lattice of phosphorene give rise to the remarkably strong moir\'{e} physics in large-twist-angle phosphorene heterostructures. This work highlights fresh opportunities to explore moir\'{e} physics in phosphorene and other van der Waals heterostructures with different lattice configurations.},
keywords = {Foundry Inorganic},
pubstate = {published},
tppubtype = {article}
}
X Tian, T A Karl, S Reiter, S Yakubov, R De Vivie-Riedle, B Koenig, J P Barham
Electro-mediated PhotoRedox Catalysis for Selective C(sp3)-O Cleavages of Phosphinated Alcohols to Carbanions Journal Article
In: Angewandte Chemie International Edition, vol. n/a, no. n/a, 2021, ISSN: 1433-7851.
Abstract | Links | Tags: Foundry Organic
@article{,
title = {Electro-mediated PhotoRedox Catalysis for Selective C(sp3)-O Cleavages of Phosphinated Alcohols to Carbanions},
author = {X Tian and T A Karl and S Reiter and S Yakubov and R De Vivie-Riedle and B Koenig and J P Barham},
url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/anie.202105895},
doi = {https://doi.org/10.1002/anie.202105895},
issn = {1433-7851},
year = {2021},
date = {2021-06-24},
urldate = {2021-06-24},
journal = {Angewandte Chemie International Edition},
volume = {n/a},
number = {n/a},
abstract = {We report a novel example of electro-mediated photoredox catalysis (e-PRC) in the reductive cleavage of C(sp 3 )-O bonds of phosphinated alcohols to alkyl carbanions. As well as deoxygenations, olefinations are reported which are E -selective and can be made Z -selective in a tandem reduction/photosensitization process where both steps are photoelectrochemically promoted. Spectroscopy, computation and catalyst structural variations reveal that our new naphthalene monoimide-type catalyst allows for a more intimate dispersive precomplexation of its radical anion form with the phosphinate substrate, facilitating a reactivity-determining C(sp 3 )-O cleavage. Surprisingly and in contrast to previously reported photoexcited radical anion chemistries, our conditions i) tolerate aryl chlorides/bromides and ii) do not give rise to Birch-type reductions.},
keywords = {Foundry Organic},
pubstate = {published},
tppubtype = {article}
}
D M Schwaiger, W Lohstroh, P Müller-Buschbaum
The Influence of the Blend Ratio, Solvent Additive, and Post-production Treatment on the Polymer Dynamics in PTB7:PCBM Blend Films Journal Article
In: Macromolecules, 2021, ISSN: 0024-9297.
Abstract | Links | Tags: Foundry Organic, Solid-Solid
@article{,
title = {The Influence of the Blend Ratio, Solvent Additive, and Post-production Treatment on the Polymer Dynamics in PTB7:PCBM Blend Films},
author = {D M Schwaiger and W Lohstroh and P M\"{u}ller-Buschbaum},
url = {https://doi.org/10.1021/acs.macromol.1c00313},
doi = {10.1021/acs.macromol.1c00313},
issn = {0024-9297},
year = {2021},
date = {2021-06-23},
urldate = {2021-06-23},
journal = {Macromolecules},
abstract = {The polymer dynamics inside a bulk heterojunction (BHJ), as used in organic solar cells, are investigated with quasielastic neutron scattering to study hydrogen motion in the polymer side chains. Different blend ratios of the polymer donor poly(4,8-bis[(2-ethylhexyl)oxy]benzo[1,2-b:4,5-b′]dithiophene-2,6-diyl3-fluoro-2-[(2-ethylhexyl)carbonyl]thieno[3,4-b]thiophenediyl) (PTB7) and the small molecule acceptor [6,6]phenyl-C71-butyric acid methyl ester (PCBM) are investigated. In addition, the influence of performance-enhancing measures, such as the use of the solvent additive 1,8-diiodooctane (DIO) and the post-production treatment of the BHJ films with methanol, on the polymer dynamics is studied. The analysis of mean square displacements as well as relaxation times of diffusional motions of the hydrogen atoms, located mainly in the polymer side chains, shows a gradual stiffening of the PTB7 side chains for higher PCBM loading in the BHJ films. The presence of DIO significantly increases diffusive mobility inside the films, while the methanol treatment does not affect hydrogen motions.},
keywords = {Foundry Organic, Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
J Klein, J Wierzbowski, P Soubelet, T Brumme, L Maschio, A Kuc, K Müller, A V Stier, J J Finley
Electrical control of orbital and vibrational interlayer coupling in bi-and trilayer 2H-MoS $ _2$ Journal Article
In: arXiv preprint arXiv:2106.11839, 2021.
Abstract | Links | Tags: Foundry Inorganic, Solid-Solid
@article{nokey,
title = {Electrical control of orbital and vibrational interlayer coupling in bi-and trilayer 2H-MoS $ _2$},
author = {J Klein and J Wierzbowski and P Soubelet and T Brumme and L Maschio and A Kuc and K M\"{u}ller and A V Stier and J J Finley},
url = {https://arxiv.org/abs/2106.11839},
doi = {arXiv:2106.11839v1},
year = {2021},
date = {2021-06-22},
journal = {arXiv preprint arXiv:2106.11839},
abstract = {Manipulating electronic interlayer coupling in layered van der Waals (vdW) materials is essential for designing opto-electronic devices. Here, we control vibrational and electronic interlayer coupling in bi- and trilayer 2H-MoS2 using large external electric fields in a micro-capacitor device. The electric field lifts Raman selection rules and activates phonon modes in excellent agreement with ab-initio calculations. Through polarization resolved photoluminescence spectroscopy in the same device, we observe a strongly tunable valley dichroism with maximum circular polarization degree of ∼60% in bilayer and ∼35% in trilayer MoS2 that are fully consistent with a rate equation model which includes input from electronic band structure calculations. We identify the highly delocalized electron wave function between the layers close to the high symmetry Q points as the origin of the tunable circular dichroism. Our results demonstrate the possibility of electric field tunable interlayer coupling for controlling emergent spin-valley physics and hybridization driven effects in vdW materials and their heterostructures.},
keywords = {Foundry Inorganic, Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
M T Sirtl, F Ebadi, Van B T Gorkom, P Ganswindt, R J a Janssen, T Bein, W Tress
The Bottlenecks of Cs2AgBiBr6 Solar Cells: How Contacts and Slow Transients Limit the Performance Journal Article
In: Advanced Optical Materials, vol. n/a, no. n/a, pp. 2100202, 2021, ISSN: 2195-1071.
Abstract | Links | Tags: Foundry Inorganic
@article{,
title = {The Bottlenecks of Cs2AgBiBr6 Solar Cells: How Contacts and Slow Transients Limit the Performance},
author = {M T Sirtl and F Ebadi and Van B T Gorkom and P Ganswindt and R J a Janssen and T Bein and W Tress},
url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adom.202100202},
doi = {https://doi.org/10.1002/adom.202100202},
issn = {2195-1071},
year = {2021},
date = {2021-06-21},
journal = {Advanced Optical Materials},
volume = {n/a},
number = {n/a},
pages = {2100202},
abstract = {Abstract Cs2AgBiBr6 has attracted much interest as a potential lead-free alternative for perovskite solar cells. Although this material offers encouraging optoelectronic features, severe bottlenecks limit the performance of the resulting solar cells to a power conversion efficiency of below 3%. Here, the performance-limiting factors of this material are investigated in full solar cells featuring various architectures. It is found that the photovoltaic parameters of Cs2AgBiBr6-based solar cells strongly depend on the scan speed of the J/V measurements, suggesting a strong impact of ionic conductivity in the material. Moreover, a sign change of the photocurrent for bias voltages above 0.9 V during the measurement of the external quantum efficiency (EQE) is revealed, which can be explained by non-selective contacts. The radiative loss of the VOC from sensitive subgap-EQE measurements is calculated and it is revealed that the loss is caused by a low external luminescence yield and therefore a high non-radiative recombination, supported by the first report of a strongly red shifted electroluminescence signal between 800 and 1000 nm. Altogether, these results point to a poor selectivity of the contacts and charge transport layers, caused by poor energy level alignment that can be overcome by optimizing the architecture of the solar cell.},
keywords = {Foundry Inorganic},
pubstate = {published},
tppubtype = {article}
}
S Xue, R W Haid, R M Kluge, X Ding, B Garlyyev, J Fichtner, S Watzele, S J Hou, A S Bandarenka
Enhancing the Hydrogen Evolution Reaction Activity of Platinum Electrodes in Alkaline Media Using Nickel-Iron Clusters Journal Article
In: Angewandte Chemie-International Edition, vol. 59, no. 27, pp. 10934-10938, 2021, ISSN: 1433-7851.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{,
title = {Enhancing the Hydrogen Evolution Reaction Activity of Platinum Electrodes in Alkaline Media Using Nickel-Iron Clusters},
author = {S Xue and R W Haid and R M Kluge and X Ding and B Garlyyev and J Fichtner and S Watzele and S J Hou and A S Bandarenka},
url = {\<Go to ISI\>://WOS:000529657400001},
doi = {10.1002/anie.202000383},
issn = {1433-7851},
year = {2021},
date = {2021-06-18},
urldate = {2020-06-26},
journal = {Angewandte Chemie-International Edition},
volume = {59},
number = {27},
pages = {10934-10938},
abstract = {Herein, we demonstrate an easy way to improve the hydrogen evolution reaction (HER) activity of Pt electrodes in alkaline media by introducing Ni-Fe clusters. As a result, the overpotential needed to achieve a current density of 10 mA cm(-2) in H-2-saturated 0.1 m KOH is reduced for the model single-crystal electrodes down to about 70 mV. To our knowledge, these modified electrodes outperform any other reported electrocatalysts tested under similar conditions. Moreover, the influence of 1) Ni to Fe ratio, 2) cluster coverage, and 3) the nature of the alkali-metal cations present in the electrolyte on the HER activity has been investigated. The observed catalytic performance likely originates from both the improved water dissociation at the Ni-Fe clusters and the subsequent optimal hydrogen adsorption and recombination at Pt atoms present at the Ni-Fe/Pt boundary.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
L Katzenmeier, L Carstensen, S J Schaper, P Müller-Buschbaum, A S Bandarenka
In: Advanced Materials, vol. 33, no. 24, pp. 2100585, 2021, ISSN: 0935-9648.
Abstract | Links | Tags: Foundry Inorganic, Solid-Solid
@article{nokey,
title = {Solid-State Electrolytes: Characterization and Quantification of Depletion and Accumulation Layers in Solid-State Li+-Conducting Electrolytes Using In Situ Spectroscopic Ellipsometry (Adv. Mater. 24/2021)},
author = {L Katzenmeier and L Carstensen and S J Schaper and P M\"{u}ller-Buschbaum and A S Bandarenka},
url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adma.202170190},
doi = {https://doi.org/10.1002/adma.202170190},
issn = {0935-9648},
year = {2021},
date = {2021-06-18},
urldate = {2021-06-18},
journal = {Advanced Materials},
volume = {33},
number = {24},
pages = {2100585},
abstract = {Layers depleted of Li-ions in solid-state electrolytes have a substantial impact on the performance of all-solid-state batteries. In article number 2100585, Aliaksandr S. Bandarenka and co-workers develop a practical strategy to measure the thickness of such space charge layers and the corresponding concentration of Li-ions by applying spectroscopic ellipsometry to emerging battery materials.},
keywords = {Foundry Inorganic, Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
N Li, R Guo, W Chen, V Körstgens, J E Heger, S Liang, C J Brett, M A Hossain, J Zheng, P S Deimel, A Buyruk, F Allegretti, M Schwartzkopf, J G C Veinot, G Schmitz, J V Barth, T Ameri, S V Roth, P Müller-Buschbaum
In: Advanced Functional Materials, vol. n/a, no. n/a, pp. 2102105, 2021, ISSN: 1616-301X.
Abstract | Links | Tags: Foundry Inorganic, Solid-Solid
@article{,
title = {Tailoring Ordered Mesoporous Titania Films via Introducing Germanium Nanocrystals for Enhanced Electron Transfer Photoanodes for Photovoltaic Applications},
author = {N Li and R Guo and W Chen and V K\"{o}rstgens and J E Heger and S Liang and C J Brett and M A Hossain and J Zheng and P S Deimel and A Buyruk and F Allegretti and M Schwartzkopf and J G C Veinot and G Schmitz and J V Barth and T Ameri and S V Roth and P M\"{u}ller-Buschbaum},
url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adfm.202102105},
doi = {https://doi.org/10.1002/adfm.202102105},
issn = {1616-301X},
year = {2021},
date = {2021-06-17},
journal = {Advanced Functional Materials},
volume = {n/a},
number = {n/a},
pages = {2102105},
abstract = {Abstract Based on a diblock-copolymer templated sol\textendashgel synthesis, germanium nanocrystals (GeNCs) are introduced to tailor mesoporous titania (TiO2) films for obtaining more efficient anodes for photovoltaic applications. After thermal annealing in air, the hybrid films with different GeNC content are investigated and compared with films undergoing an argon atmosphere annealing. The surface and inner morphologies of the TiO2/GeOx nanocomposite films are probed via scanning electron microscopy and grazing-incidence small-angle X-ray scattering. The crystal phase, chemical composition, and optical properties of the nanocomposite films are examined with transmission electron microscopy, X-ray photoelectron spectroscopy, and ultraviolet\textendashvisible spectroscopy. Special focus is set on the air-annealed nanocomposite films since they hold greater promise for photovoltaics. Specifically, the charge\textendashcarrier dynamics of these air-annealed nanocomposite films are studied, and it is found that, compared with pristine TiO2 photoanodes, the GeNC addition enhances the electron transfer, yielding an increase in the short-circuit photocurrent density of exemplary perovskite solar cells and thus, an enhanced device efficiency as well as a significantly reduced hysteresis.},
keywords = {Foundry Inorganic, Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
A Dey, J Ye, A De, E Debroye, S K Ha, E Bladt, A S Kshirsagar, Z Wang, J Yin, Y Wang, L N Quan, F Yan, M Gao, X Li, J Shamsi, T Debnath, M Cao, M A Scheel, S Kumar, J A Steele, M Gerhard, L Chouhan, K Xu, X-G Wu, Y Li, Y Zhang, A Dutta, C Han, I Vincon, A L Rogach, A Nag, A Samanta, B A Korgel, C-J Shih, D R Gamelin, D H Son, H Zeng, H Zhong, H Sun, H V Demir, I G Scheblykin, I Mora-Seró, J K Stolarczyk, J Z Zhang, J Feldmann, J Hofkens, J M Luther, J Pérez-Prieto, L Li, L Manna, M I Bodnarchuk, M V Kovalenko, M B J Roeffaers, N Pradhan, O F Mohammed, O M Bakr, P Yang, P Müller-Buschbaum, P V Kamat, Q Bao, Q Zhang, R Krahne, R E Galian, S D Stranks, S Bals, V Biju, W A Tisdale, Y Yan, R L Z Hoye, L Polavarapu
State of the Art and Prospects for Halide Perovskite Nanocrystals Journal Article
In: ACS Nano, 2021, ISSN: 1936-0851.
Abstract | Links | Tags: Foundry Inorganic, Solid-Solid
@article{,
title = {State of the Art and Prospects for Halide Perovskite Nanocrystals},
author = {A Dey and J Ye and A De and E Debroye and S K Ha and E Bladt and A S Kshirsagar and Z Wang and J Yin and Y Wang and L N Quan and F Yan and M Gao and X Li and J Shamsi and T Debnath and M Cao and M A Scheel and S Kumar and J A Steele and M Gerhard and L Chouhan and K Xu and X-G Wu and Y Li and Y Zhang and A Dutta and C Han and I Vincon and A L Rogach and A Nag and A Samanta and B A Korgel and C-J Shih and D R Gamelin and D H Son and H Zeng and H Zhong and H Sun and H V Demir and I G Scheblykin and I Mora-Ser\'{o} and J K Stolarczyk and J Z Zhang and J Feldmann and J Hofkens and J M Luther and J P\'{e}rez-Prieto and L Li and L Manna and M I Bodnarchuk and M V Kovalenko and M B J Roeffaers and N Pradhan and O F Mohammed and O M Bakr and P Yang and P M\"{u}ller-Buschbaum and P V Kamat and Q Bao and Q Zhang and R Krahne and R E Galian and S D Stranks and S Bals and V Biju and W A Tisdale and Y Yan and R L Z Hoye and L Polavarapu},
url = {https://doi.org/10.1021/acsnano.0c08903},
doi = {10.1021/acsnano.0c08903},
issn = {1936-0851},
year = {2021},
date = {2021-06-17},
urldate = {2021-06-17},
journal = {ACS Nano},
abstract = {Metal-halide perovskites have rapidly emerged as one of the most promising materials of the 21st century, with many exciting properties and great potential for a broad range of applications, from photovoltaics to optoelectronics and photocatalysis. The ease with which metal-halide perovskites can be synthesized in the form of brightly luminescent colloidal nanocrystals, as well as their tunable and intriguing optical and electronic properties, has attracted researchers from different disciplines of science and technology. In the last few years, there has been a significant progress in the shape-controlled synthesis of perovskite nanocrystals and understanding of their properties and applications. In this comprehensive review, researchers having expertise in different fields (chemistry, physics, and device engineering) of metal-halide perovskite nanocrystals have joined together to provide a state of the art overview and future prospects of metal-halide perovskite nanocrystal research.},
keywords = {Foundry Inorganic, Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
S Feldmann, T Neumann, R Ciesielski, R H Friend, A Hartschuh, F Deschler
Tailored Local Bandgap Modulation as a Strategy to Maximize Luminescence Yields in Mixed-Halide Perovskites Journal Article
In: Advanced Optical Materials, vol. n/a, no. n/a, pp. 2100635, 2021, ISSN: 2195-1071.
Abstract | Links | Tags: Foundry Inorganic
@article{,
title = {Tailored Local Bandgap Modulation as a Strategy to Maximize Luminescence Yields in Mixed-Halide Perovskites},
author = {S Feldmann and T Neumann and R Ciesielski and R H Friend and A Hartschuh and F Deschler},
url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adom.202100635},
doi = {https://doi.org/10.1002/adom.202100635},
issn = {2195-1071},
year = {2021},
date = {2021-06-12},
journal = {Advanced Optical Materials},
volume = {n/a},
number = {n/a},
pages = {2100635},
abstract = {Abstract Halide perovskites have emerged as high-performance semiconductors for efficient optoelectronic devices, not least because of their bandgap tunability using mixtures of different halide ions. Here, temperature-dependent photoluminescence microscopy with computational modelling is combined to quantify the impact of local bandgap variations from disordered halide distributions on the global photoluminescence yield in mixed-halide perovskite films. It is found that fabrication temperature, surface energy, and charge recombination constants are keys for describing local bandgap variations and charge carrier funneling processes that control the photoluminescence quantum efficiency. It is reported that further luminescence efficiency gains are possible through tailored bandgap modulation, even for materials that have already demonstrated high luminescence yields. The work provides a novel strategy and fabrication guidelines for further improvement of halide perovskite performance in light-emitting and photovoltaic applications.},
keywords = {Foundry Inorganic},
pubstate = {published},
tppubtype = {article}
}
S Yin, W Cao, Q Ji, Y Cheng, L Song, N Li, C L Weindl, M Schwartzkopf, S V Roth, P Müller-Buschbaum
Multidimensional Morphology Control for PS-b-P4VP Templated Mesoporous Iron (III) Oxide Thin Films Journal Article
In: Advanced Materials Interfaces, vol. n/a, no. n/a, pp. 2100141, 2021, ISSN: 2196-7350.
Abstract | Links | Tags: Foundry Inorganic, Solid-Solid
@article{,
title = {Multidimensional Morphology Control for PS-b-P4VP Templated Mesoporous Iron (III) Oxide Thin Films},
author = {S Yin and W Cao and Q Ji and Y Cheng and L Song and N Li and C L Weindl and M Schwartzkopf and S V Roth and P M\"{u}ller-Buschbaum},
url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/admi.202100141},
doi = {https://doi.org/10.1002/admi.202100141},
issn = {2196-7350},
year = {2021},
date = {2021-06-12},
journal = {Advanced Materials Interfaces},
volume = {n/a},
number = {n/a},
pages = {2100141},
abstract = {Abstract Mesoporous α-Fe2O3 thin films with large area homogeneity demonstrate tremendous potential in multiple applications. In the present work, the synthesis of morphology-controlled α-Fe2O3 thin films is realized with polystyrene-block-poly(4-vinyl pyridine) (PS-b-P4VP) diblock copolymer assisted sol-gel chemistry. The solvent category (DMF and 1,4-dioxane) and polymer-to-FeCl3 ratio used for the solution preparation are systematically varied to tune the morphology of the thin films. For both solvents, DMF and 1,4-dioxane, nanocluster structures are obtained with low PS-b-P4VP concentration. When the concentration of PS-b-P4VP reaches the critical micelle concentration, spherical and wormlike porous structures are specifically formed in the DMF and 1,4-dioxane solvent system, respectively. Further increasing the polymer-to-FeCl3 ratios leads to the enlargement of the spherical pore sizes in the DMF system, whereas the center-to-center distances of the wormlike structures in the 1,4-dioxane system decrease. Moreover, DMF/1,4-dioxane solvent mixtures with different volume ratios are applied for the sol\textendashgel solution preparation to gain more insight into how the solvent selectivity affects the thin film morphology. By adjusting the preferential affinity of the solvent mixture to the polymer blocks, a spherical to wormlike pore shape transition is observed with a critical Δχ value of around 0.77.},
keywords = {Foundry Inorganic, Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
X Wang, C Liu, C Gao, K Yao, S S M Masouleh, R Berté, H Ren, L D S Menezes, E Cortés, I C Bicket, H Wang, N Li, Z Zhang, M Li, W Xie, Y Yu, Y Fang, S Zhang, H Xu, A Vomiero, Y Liu, G A Botton, S A Maier, H Liang
Self-Constructed Multiple Plasmonic Hotspots on an Individual Fractal to Amplify Broadband Hot Electron Generation Journal Article
In: ACS Nano, 2021, ISSN: 1936-0851.
Abstract | Links | Tags: Foundry Inorganic
@article{,
title = {Self-Constructed Multiple Plasmonic Hotspots on an Individual Fractal to Amplify Broadband Hot Electron Generation},
author = {X Wang and C Liu and C Gao and K Yao and S S M Masouleh and R Bert\'{e} and H Ren and L D S Menezes and E Cort\'{e}s and I C Bicket and H Wang and N Li and Z Zhang and M Li and W Xie and Y Yu and Y Fang and S Zhang and H Xu and A Vomiero and Y Liu and G A Botton and S A Maier and H Liang},
url = {https://doi.org/10.1021/acsnano.1c03218},
doi = {10.1021/acsnano.1c03218},
issn = {1936-0851},
year = {2021},
date = {2021-06-11},
journal = {ACS Nano},
abstract = {Plasmonic nanoparticles are ideal candidates for hot-electron-assisted applications, but their narrow resonance region and limited hotspot number hindered the energy utilization of broadband solar energy. Inspired by tree branches, we designed and chemically synthesized silver fractals, which enable self-constructed hotspots and multiple plasmonic resonances, extending the broadband generation of hot electrons for better matching with the solar radiation spectrum. We directly revealed the plasmonic origin, the spatial distribution, and the decay dynamics of hot electrons on the single-particle level by using ab initio simulation, dark-field spectroscopy, pump\textendashprobe measurements, and electron energy loss spectroscopy. Our results show that fractals with acute tips and narrow gaps can support broadband resonances (400\textendash1100 nm) and a large number of randomly distributed hotspots, which can provide unpolarized enhanced near field and promote hot electron generation. As a proof-of-concept, hot-electron-triggered dimerization of p-nitropthiophenol and hydrogen production are investigated under various irradiations, and the promoted hot electron generation on fractals was confirmed with significantly improved efficiency.},
keywords = {Foundry Inorganic},
pubstate = {published},
tppubtype = {article}
}
S T Emmerling, L S Germann, P A Julien, I Moudrakovski, M Etter, T Friščić, R E Dinnebier, B V Lotsch
In situ monitoring of mechanochemical covalent organic framework formation reveals templating effect of liquid additive Journal Article
In: Chem, vol. 7, no. 6, pp. 1639-1652, 2021, ISSN: 2451-9294.
Abstract | Links | Tags: Foundry Organic, Molecularly-Functionalized
@article{nokey,
title = {In situ monitoring of mechanochemical covalent organic framework formation reveals templating effect of liquid additive},
author = {S T Emmerling and L S Germann and P A Julien and I Moudrakovski and M Etter and T Fri\v{s}\v{c}i\'{c} and R E Dinnebier and B V Lotsch},
url = {https://www.sciencedirect.com/science/article/pii/S2451929421002138},
doi = {https://doi.org/10.1016/j.chempr.2021.04.012},
issn = {2451-9294},
year = {2021},
date = {2021-06-10},
journal = {Chem},
volume = {7},
number = {6},
pages = {1639-1652},
abstract = {Summary Covalent organic frameworks (COFs) have emerged as a new class of molecularly precise, porous functional materials characterized by broad structural and chemical versatility, with a diverse range of applications. Despite their increasing popularity, fundamental aspects of COF formation are poorly understood, lacking profound experimental insights into their assembly. Here, we use a combination of in situ X-ray powder diffraction and Raman spectroscopy to elucidate the reaction mechanism of mechanochemical synthesis of imine COFs, leading to the observation of key reaction intermediates that offer direct experimental evidence of framework templating through liquid additives. Moreover, the solid-state catalyst scandium triflate is instrumental in directing the reaction kinetics and mechanism, yielding COFs with crystallinity and porosity on par with solvothermal products. This work provides the first experimental evidence of solvent-based COF templating and is a significant advancement in mechanistic understanding of mechanochemistry as a green route for COF synthesis.},
keywords = {Foundry Organic, Molecularly-Functionalized},
pubstate = {published},
tppubtype = {article}
}
K Ortstein, S Hutsch, M Hambsch, K Tvingstedt, B Wegner, J Benduhn, J Kublitski, M Schwarze, S Schellhammer, F Talnack, A Vogt, P Bäuerle, N Koch, S C B Mannsfeld, H Kleemann, F Ortmann, K Leo
Band gap engineering in blended organic semiconductor films based on dielectric interactions Journal Article
In: Nature Materials, 2021, ISSN: 1476-4660.
Abstract | Links | Tags: Foundry Organic, Molecularly-Functionalized
@article{,
title = {Band gap engineering in blended organic semiconductor films based on dielectric interactions},
author = {K Ortstein and S Hutsch and M Hambsch and K Tvingstedt and B Wegner and J Benduhn and J Kublitski and M Schwarze and S Schellhammer and F Talnack and A Vogt and P B\"{a}uerle and N Koch and S C B Mannsfeld and H Kleemann and F Ortmann and K Leo},
url = {https://doi.org/10.1038/s41563-021-01025-z},
doi = {10.1038/s41563-021-01025-z},
issn = {1476-4660},
year = {2021},
date = {2021-06-10},
urldate = {2021-06-10},
journal = {Nature Materials},
abstract = {Blending organic molecules to tune their energy levels is currently being investigated as an approach to engineer the bulk and interfacial optoelectronic properties of organic semiconductors. It has been proven that the ionization energy and electron affinity can be equally shifted in the same direction by electrostatic effects controlled by blending similar halogenated derivatives with different energetics. Here we show that the energy gap of organic semiconductors can also be tuned by blending. We use oligothiophenes with different numbers of thiophene rings as an example and investigate their structure and electronic properties. Photoelectron spectroscopy and inverse photoelectron spectroscopy show tunability of the single-particle gap, with the optical gaps showing similar, but smaller, effects. Theoretical analysis shows that this tuning is mainly caused by a change in the dielectric constant with blend ratio. Further studies will explore the practical impact of this energy-level engineering strategy for optoelectronic devices.},
keywords = {Foundry Organic, Molecularly-Functionalized},
pubstate = {published},
tppubtype = {article}
}
T Neumann, S Feldmann, P Moser, A Delhomme, J Zerhoch, T Van De Goor, S Wang, M Dyksik, T Winkler, J J Finley, P Plochocka, M S Brandt, C Faugeras, A V Stier, F Deschler
In: Nature Communications, vol. 12, no. 1, pp. 3489, 2021, ISSN: 2041-1723.
Abstract | Links | Tags: Foundry Inorganic
@article{nokey,
title = {Manganese doping for enhanced magnetic brightening and circular polarization control of dark excitons in paramagnetic layered hybrid metal-halide perovskites},
author = {T Neumann and S Feldmann and P Moser and A Delhomme and J Zerhoch and T Van De Goor and S Wang and M Dyksik and T Winkler and J J Finley and P Plochocka and M S Brandt and C Faugeras and A V Stier and F Deschler},
url = {https://doi.org/10.1038/s41467-021-23602-1},
doi = {10.1038/s41467-021-23602-1},
issn = {2041-1723},
year = {2021},
date = {2021-06-09},
journal = {Nature Communications},
volume = {12},
number = {1},
pages = {3489},
abstract = {Materials combining semiconductor functionalities with spin control are desired for the advancement of quantum technologies. Here, we study the magneto-optical properties of novel paramagnetic Ruddlesden-Popper hybrid perovskites Mn:(PEA)2PbI4 (PEA = phenethylammonium) and report magnetically brightened excitonic luminescence with strong circular polarization from the interaction with isolated Mn2+ ions. Using a combination of superconducting quantum interference device (SQUID) magnetometry, magneto-absorption and transient optical spectroscopy, we find that a dark exciton population is brightened by state mixing with the bright excitons in the presence of a magnetic field. Unexpectedly, the circular polarization of the dark exciton luminescence follows the Brillouin-shaped magnetization with a saturation polarization of 13% at 4 K and 6 T. From high-field transient magneto-luminescence we attribute our observations to spin-dependent exciton dynamics at early times after excitation, with first indications for a Mn-mediated spin-flip process. Our findings demonstrate manganese doping as a powerful approach to control excitonic spin physics in Ruddlesden-Popper perovskites, which will stimulate research on this highly tuneable material platform with promise for tailored interactions between magnetic moments and excitonic states.},
keywords = {Foundry Inorganic},
pubstate = {published},
tppubtype = {article}
}
C J Brett, W Ohm, B Fricke, A E Alexakis, T Laarmann, V Körstgens, P Müller-Buschbaum, L D Söderberg, S V Roth
Nanocellulose-Assisted Thermally Induced Growth of Silver Nanoparticles for Optical Applications Journal Article
In: ACS Applied Materials & Interfaces, vol. 13, no. 23, pp. 27696-27704, 2021, ISSN: 1944-8244.
Abstract | Links | Tags: Foundry Inorganic, Molecularly-Functionalized
@article{nokey,
title = {Nanocellulose-Assisted Thermally Induced Growth of Silver Nanoparticles for Optical Applications},
author = {C J Brett and W Ohm and B Fricke and A E Alexakis and T Laarmann and V K\"{o}rstgens and P M\"{u}ller-Buschbaum and L D S\"{o}derberg and S V Roth},
url = {https://doi.org/10.1021/acsami.1c07544},
doi = {10.1021/acsami.1c07544},
issn = {1944-8244},
year = {2021},
date = {2021-06-07},
journal = {ACS Applied Materials \& Interfaces},
volume = {13},
number = {23},
pages = {27696-27704},
abstract = {Optically responsive materials are present in everyday life, from screens to sensors. However, fabricating large-area, fossil-free materials for functional biocompatible applications is still a challenge today. Nanocelluloses from various sources, such as wood, can provide biocompatibility and are emerging candidates for templating organic optoelectronics. Silver (Ag) in its nanoscale form shows excellent optical properties. Herein, we combine both materials using thin-film large-area spray-coating to study the fabrication of optical response applications. We characterize the Ag nanoparticle formation by X-ray scattering and UV\textendashvis spectroscopy in situ during growth on the nanocellulose template. The morphology and optical properties of the nanocellulose film are compared to the rigid reference surface SiO2. Our results clearly show the potential to tailor the energy band gap of the resulting hybrid material.},
keywords = {Foundry Inorganic, Molecularly-Functionalized},
pubstate = {published},
tppubtype = {article}
}
X Ding, B Garlyyev, S A Watzele, T Kobina Sarpey, A S Bandarenka
Spotlight on the Effect of Electrolyte Composition on the Potential of Maximum Entropy: Supporting Electrolytes Are Not Always Inert Journal Article
In: Chemistry – A European Journal, vol. 27, no. 39, pp. 10016-10020, 2021, ISSN: 0947-6539.
Abstract | Links | Tags: Solid-Liquid
@article{nokey,
title = {Spotlight on the Effect of Electrolyte Composition on the Potential of Maximum Entropy: Supporting Electrolytes Are Not Always Inert},
author = {X Ding and B Garlyyev and S A Watzele and T Kobina Sarpey and A S Bandarenka},
url = {https://chemistry-europe.onlinelibrary.wiley.com/doi/abs/10.1002/chem.202101537},
doi = {https://doi.org/10.1002/chem.202101537},
issn = {0947-6539},
year = {2021},
date = {2021-05-29},
urldate = {2021-05-29},
journal = {Chemistry \textendash A European Journal},
volume = {27},
number = {39},
pages = {10016-10020},
abstract = {Abstract The influence of electrolyte pH, the presence of alkali metal cations (Na+, K+), and the presence of O2 on the interfacial water structure of polycrystalline gold electrodes has been experimentally studied in detail. The potential of maximum entropy (PME) was determined by the laser-induced current transient (LICT) technique. Our results demonstrate that increasing the electrolyte pH and introducing O2 shift the PME to more positive potentials. Interestingly, the PME exhibits a higher sensitivity to the pH change in the presence of K+ than Na+. Altering the pH of the K2SO4 solution from 4 to 6 can cause a drastic shift in the PME. These findings reveal that, for example, K2SO4 and Na2SO4 cannot be considered as equal supporting electrolytes: it is not a viable assumption. This can likely be extrapolated to other common “inert” supporting electrolytes. Beyond this, knowledge about the near-ideal electrolyte composition can be used to optimize electrochemical devices such as electrolyzers, fuel cells, batteries, and supercapacitors.},
keywords = {Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
E Mohammadi, A Tittl, K L Tsakmakidis, T V Raziman, A G Curto
Dual Nanoresonators for Ultrasensitive Chiral Detection Journal Article
In: ACS Photonics, 2021.
Abstract | Links | Tags: Foundry Organic, Solid-Solid
@article{,
title = {Dual Nanoresonators for Ultrasensitive Chiral Detection},
author = {E Mohammadi and A Tittl and K L Tsakmakidis and T V Raziman and A G Curto},
url = {https://doi.org/10.1021/acsphotonics.1c00311},
doi = {10.1021/acsphotonics.1c00311},
year = {2021},
date = {2021-05-28},
journal = {ACS Photonics},
abstract = {The discrimination of enantiomers is crucial in biochemistry. However, chiral sensing faces significant limitations due to inherently weak chiroptical signals. Nanophotonics is a promising solution to enhance sensitivity thanks to increased optical chirality maximized by strong electric and magnetic fields. Metallic and dielectric nanoparticles can separately provide electric and magnetic resonances. Here we propose their synergistic combination in hybrid metal\textendashdielectric nanostructures to exploit their dual character for superchiral fields beyond the limits of single particles. For optimal optical chirality, in addition to maximization of the resonance strength, the resonances must spectrally coincide. Simultaneously, their electric and magnetic fields must be parallel and π/2 out of phase and spatially overlap. We demonstrate that the interplay between the strength of the resonances and these optimal conditions constrains the attainable optical chirality in resonant systems. Starting from a simple symmetric nanodimer, we derive closed-form expressions elucidating its fundamental limits of optical chirality. Building on the trade-offs of different classes of dimers, we then suggest an asymmetric dual dimer based on realistic materials. These dual nanoresonators provide strong and decoupled electric and magnetic resonances together with optimal conditions for chiral fields. Finally, we introduce more complex dual building blocks for a metasurface with a record 300-fold enhancement of local optical chirality in nanoscale gaps, enabling circular dichroism enhancement by a factor of 20. By combining analytical insight and practical designs, our results put forward hybrid resonators to increase chiral sensitivity, particularly for small molecular quantities.},
keywords = {Foundry Organic, Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
S Stegmaier, R Schierholz, I Povstugar, J Barthel, S P Rittmeyer, S Yu, S Wengert, S Rostami, H Kungl, K Reuter, R-A Eichel, C Scheurer
Nano-Scale Complexions Facilitate Li Dendrite-Free Operation in LATP Solid-State Electrolyte Journal Article
In: Advanced Energy Materials, vol. n/a, no. n/a, pp. 2100707, 2021, ISSN: 1614-6832.
Abstract | Links | Tags: Foundry Inorganic, Solid-Solid
@article{,
title = {Nano-Scale Complexions Facilitate Li Dendrite-Free Operation in LATP Solid-State Electrolyte},
author = {S Stegmaier and R Schierholz and I Povstugar and J Barthel and S P Rittmeyer and S Yu and S Wengert and S Rostami and H Kungl and K Reuter and R-A Eichel and C Scheurer},
url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/aenm.202100707},
doi = {https://doi.org/10.1002/aenm.202100707},
issn = {1614-6832},
year = {2021},
date = {2021-05-28},
journal = {Advanced Energy Materials},
volume = {n/a},
number = {n/a},
pages = {2100707},
abstract = {Abstract Dendrite formation and growth remains a major obstacle toward high-performance all solid-state batteries using Li metal anodes. The ceramic Li(1+x)Al(x)Ti(2−x)(PO4)3 (LATP) solid-state electrolyte shows a higher than expected stability against electrochemical decomposition despite a bulk electronic conductivity that exceeds a recently postulated threshold for dendrite-free operation. Here, transmission electron microscopy, atom probe tomography, and first-principles based simulations are combined to establish atomistic structural models of glass-amorphous LATP grain boundaries. These models reveal a nanometer-thin complexion layer that encapsulates the crystalline grains. The distinct composition of this complexion constitutes a sizable electronic impedance. Rather than fulfilling macroscopic bulk measures of ionic and electronic conduction, LATP might thus gain the capability to suppress dendrite nucleation by sufficient local separation of charge carriers at the nanoscale.},
keywords = {Foundry Inorganic, Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
M H Aufa, S A Watzele, S Hou, R W Haid, R M Kluge, A S Bandarenka, B Garlyyev
Fast and accurate determination of the electroactive surface area of MnOx Journal Article
In: Electrochimica Acta, vol. 389, pp. 138692, 2021, ISSN: 0013-4686.
Abstract | Links | Tags: Foundry Inorganic, Solid-Solid
@article{,
title = {Fast and accurate determination of the electroactive surface area of MnOx},
author = {M H Aufa and S A Watzele and S Hou and R W Haid and R M Kluge and A S Bandarenka and B Garlyyev},
url = {https://www.sciencedirect.com/science/article/pii/S0013468621009828},
doi = {https://doi.org/10.1016/j.electacta.2021.138692},
issn = {0013-4686},
year = {2021},
date = {2021-05-27},
journal = {Electrochimica Acta},
volume = {389},
pages = {138692},
abstract = {Manganese oxide (MnOx)-based materials are widely utilized in the field of electrocatalysis as bifunctional electrocatalysts for the oxygen reduction and evolution reactions. However, for an accurate assessment of their performance, the determination of their electrochemical active surface area (ECSA) is of paramount importance. So far, there is no fast and reproducible methodology. This article presents an easily applicable and affordable technique to determine the ECSA of MnOx accurately. The presented methodology makes use of the specific adsorption capacitance of reaction intermediates close to the onset potential of the oxygen evolution reaction. The electrochemical impedance spectroscopy is utilized to measure the specific adsorption capacitances at different potentials. Using MnOx thin-film electrodes, we determine the specific adsorption capacitances and present calibration values, which can be used for an accurate determination of the ECSA of different, for instance, nanostructured materials.},
keywords = {Foundry Inorganic, Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
C Koschnick, R Stäglich, T Scholz, M W Terban, A Von Mankowski, G Savasci, F Binder, A Schökel, M Etter, J Nuss, R Siegel, L S Germann, C Ochsenfeld, R E Dinnebier, J Senker, B V Lotsch
In: Nature Communications, vol. 12, no. 1, pp. 3099, 2021, ISSN: 2041-1723.
Abstract | Links | Tags: Foundry Inorganic, Molecularly-Functionalized
@article{nokey,
title = {Understanding disorder and linker deficiency in porphyrinic zirconium-based metal\textendashorganic frameworks by resolving the Zr8O6 cluster conundrum in PCN-221},
author = {C Koschnick and R St\"{a}glich and T Scholz and M W Terban and A Von Mankowski and G Savasci and F Binder and A Sch\"{o}kel and M Etter and J Nuss and R Siegel and L S Germann and C Ochsenfeld and R E Dinnebier and J Senker and B V Lotsch},
url = {https://doi.org/10.1038/s41467-021-23348-w},
doi = {10.1038/s41467-021-23348-w},
issn = {2041-1723},
year = {2021},
date = {2021-05-25},
journal = {Nature Communications},
volume = {12},
number = {1},
pages = {3099},
abstract = {Porphyrin-based metal\textendashorganic frameworks (MOFs), exemplified by MOF-525, PCN-221, and PCN-224, are promising systems for catalysis, optoelectronics, and solar energy conversion. However, subtle differences between synthetic protocols for these three MOFs give rise to vast discrepancies in purported product outcomes and description of framework topologies. Here, based on a comprehensive synthetic and structural analysis spanning local and long-range length scales, we show that PCN-221 consists of Zr6O4(OH)4 clusters in four distinct orientations within the unit cell, rather than Zr8O6 clusters as originally published, and linker vacancies at levels of around 50%, which may form in a locally correlated manner. We propose disordered PCN-224 (dPCN-224) as a unified model to understand PCN-221, MOF-525, and PCN-224 by varying the degree of orientational cluster disorder, linker conformation and vacancies, and cluster\textendashlinker binding. Our work thus introduces a new perspective on network topology and disorder in Zr-MOFs and pinpoints the structural variables that direct their functional properties.},
keywords = {Foundry Inorganic, Molecularly-Functionalized},
pubstate = {published},
tppubtype = {article}
}
P M Stanley, J Haimerl, C Thomas, A Urstoeger, M Schuster, N B Shustova, A Casini, B Rieger, J Warnan, R A Fischer
Host–Guest Interactions in a Metal–Organic Framework Isoreticular Series for Molecular Photocatalytic CO2 Reduction Journal Article
In: Angewandte Chemie International Edition, vol. 60, no. 33, pp. 17854-17860, 2021, ISSN: 1433-7851.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{nokey,
title = {Host\textendashGuest Interactions in a Metal\textendashOrganic Framework Isoreticular Series for Molecular Photocatalytic CO2 Reduction},
author = {P M Stanley and J Haimerl and C Thomas and A Urstoeger and M Schuster and N B Shustova and A Casini and B Rieger and J Warnan and R A Fischer},
url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/anie.202102729},
doi = {https://doi.org/10.1002/anie.202102729},
issn = {1433-7851},
year = {2021},
date = {2021-05-20},
journal = {Angewandte Chemie International Edition},
volume = {60},
number = {33},
pages = {17854-17860},
abstract = {Abstract A strategy to improve homogeneous molecular catalyst stability, efficiency, and selectivity is the immobilization on supporting surfaces or within host matrices. Herein, we examine the co-immobilization of a CO2 reduction catalyst [ReBr(CO)3(4,4′-dcbpy)] and a photosensitizer [Ru(bpy)2(5,5′-dcbpy)]Cl2 using the isoreticular series of metal\textendashorganic frameworks (MOFs) UiO-66, -67, and -68. Specific host pore size choice enables distinct catalyst and photosensitizer spatial location\textemdasheither at the outer MOF particle surface or inside the MOF cavities\textemdashaffecting catalyst stability, electronic communication between reaction center and photosensitizer, and consequently the apparent catalytic rates. These results allow for a rational understanding of an optimized supramolecular layout of catalyst, photosensitizer, and host matrix.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}