Publications

@article{nokey,

title = {Highly conductive titania supported iridium oxide nanoparticles with low overall iridium density as OER catalyst for large-scale PEM electrolysis},

author = {D B\"{o}hm and M Beetz and C Gebauer and M Bernt and J Schr\"{o}ter and M Kornherr and F Zoller and T Bein and D Fattakhova-Rohlfing},

url = {https://www.sciencedirect.com/science/article/pii/S2352940721001980},

doi = {https://doi.org/10.1016/j.apmt.2021.101134},

issn = {2352-9407},

year  = {2021},

date = {2021-09-01},

journal = {Applied Materials Today},

volume = {24},

pages = {101134},

abstract = {To enable future large-scale generation of hydrogen via proton exchange membrane (PEM) electrolysis, utilization of scarce iridium-based catalysts required for the oxygen evolution reaction (OER) has to be significantly lowered. To address this question, the facile synthesis of a highly active TiO2 supported iridium oxide based OER catalyst with reduced noble metal content and an Ir-density of the catalyst powder as low as 0.05\textendash0.08 gIr cm-3 is described in this work. A high surface area corrosion-resistant titania catalyst support homogeneously coated with a 1-2 nm thin layer of amorphous IrOOHx is oxidized in molten NaNO3 between 350-375°C. This procedure allows for a controllable phase transformation and crystallization to form a layer of interconnected IrO2 nanoparticles of ≈2 nm on the surface of the TiO2 support. The increase in crystallinity is thereby accompanied by a significant increase in conductivity of up to 11 S cm-1 for a 30 wt% Ir loaded catalyst. Oxidized samples further display a significantly increased stability with less detectable Ir dissolution under OER conditions. With a mass-based activity of 59 A g-1 at an overpotential of 300 mV, the electrocatalytic activity is maintained at the level of the highly active amorphous IrOOHx phase used as precursor and outperforms it at higher current densities through the increased conductivity. MEA measurements with catalyst loadings of 0.2-0.3 mg cm-2 further confirm the high catalytic activity and initial stability at industrially relevant current densities. The introduced synthesis approach therefore shows a path for the fabrication of novel highly active and atom-efficient oxide supported catalysts with complex nanostructures and thin homogenous nanoparticle coatings that allows a future large-scale application of PEM electrolysis technology without restrictions by the natural abundance of iridium.},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Single Antibody Detection in a DNA Origami Nanoantenna},

author = {M Pfeiffer and K Trofymchuk and S Ranallo and F Ricci and F Steiner and F Cole and V Glembockyte and P Tinnefeld},

url = {https://www.sciencedirect.com/science/article/pii/S2589004221010403},

doi = {https://doi.org/10.1016/j.isci.2021.103072},

issn = {2589-0042},

year  = {2021},

date = {2021-09-01},

journal = {iScience},

pages = {103072},

abstract = {Summary DNA nanotechnology offers new biosensing approaches by templating different sensor and transducer components. Here, we combine DNA origami nanoantennas with label-free antibody detection by incorporating a nanoswitch in the plasmonic hotspot of the nanoantenna. The nanoswitch contains two antigens that are displaced by antibody binding thereby eliciting a fluorescent signal. Single antibody detection is demonstrated with a DNA origami integrated anti-digoxigenin antibody nanoswitch. In combination with the nanoantenna, the signal generated by the antibody is additionally amplified. This allows the detection of single antibodies on a portable smartphone microscope. Overall, fluorescence enhanced antibody detection in DNA origami nanoantennas shows that fluorescence enhanced biosensing can be expanded beyond the scope of the nucleic acids realm.},

keywords = {Molecularly-Functionalized},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Indirect bandgap, optoelectronic properties, and photoelectrochemical characteristics of high-purity Ta3N5 photoelectrodes},

author = {J Eichhorn and S P Lechner and C-M Jiang and G Folchi Heunecke and F Munnik and I D Sharp},

url = {http://dx.doi.org/10.1039/D1TA05282A},

doi = {10.1039/D1TA05282A},

issn = {2050-7488},

year  = {2021},

date = {2021-08-26},

journal = {Journal of Materials Chemistry A},

abstract = {The (opto)electronic properties of Ta3N5 photoelectrodes are often dominated by defects, such as oxygen impurities, nitrogen vacancies, and low-valent Ta cations, impeding fundamental studies of its electronic structure, chemical stability, and photocarrier transport. Here, we explore the role of ammonia annealing following direct reactive magnetron sputtering of tantalum nitride thin films, achieving near-ideal stoichiometry, with significantly reduced native defect and oxygen impurity concentrations. By analyzing structural, optical, and photoelectrochemical properties as a function of ammonia annealing temperature, we provide new insights into the basic semiconductor properties of Ta3N5, as well as the role of defects on its optoelectronic characteristics. Both the crystallinity and material quality improve up to 940 °C, due to elimination of oxygen impurities. Even higher annealing temperatures cause material decomposition and introduce additional disorder within the Ta3N5 lattice, leading to reduced photoelectrochemical performance. Overall, the high material quality enables us to unambiguously identify the nature of the Ta3N5 bandgap as indirect, thereby resolving a long-standing controversy regarding the most fundamental characteristic of this material as a semiconductor. The compact morphology, low defect content, and high optoelectronic quality of these films provide a basis for further optimization of photoanodes and may open up further application opportunities beyond photoelectrochemical energy conversion.},

keywords = {Solid-Solid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Influence of environmental conditions and surface treatments on the photoluminescence properties of GaN nanowires and nanofins},

author = {M Kraut and F Pantle and S W\"{o}rle and E Sirotti and A Zeidler and F Eckmann and M Stutzmann},

issn = {0957-4484},

year  = {2021},

date = {2021-08-16},

journal = {Nanotechnology},

keywords = {Foundry Inorganic, Solid-Solid},

pubstate = {published},

tppubtype = {article}

}

@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}

}

@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}

}

@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}

}

@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},

issn = {1616-301X},

year  = {2021},

date = {2021-08-12},

journal = {Advanced Functional Materials},

pages = {2011210},

keywords = {Foundry Inorganic, Solid-Solid},

pubstate = {published},

tppubtype = {article}

}

@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}

}

@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}

}

@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}

}

@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}

}

@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},

doi = {10.5185/vpoam.2021.05171},

year  = {2021},

date = {2021-08-03},

journal = {Video Proceedings of Advanced Materials},

volume = {2},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@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},

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},

pubstate = {published},

tppubtype = {article}

}

@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},

journal = {Advanced Materials},

volume = {n/a},

number = {n/a},

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}

}

@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}

}

@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}

}

@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 De R 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},

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}

}

@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},

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},

pubstate = {published},

tppubtype = {article}

}

@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}

}

@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},

journal = {ECS Transactions},

volume = {103},

number = {1},

pages = {1331},

keywords = {Solid-Liquid},

pubstate = {published},

tppubtype = {article}

}

@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},

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},

pubstate = {published},

tppubtype = {article}

}

@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}

}

@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}

}

@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 De R 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},

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}

}

@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},

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 Inorganic, Solid-Solid},

pubstate = {published},

tppubtype = {article}

}

@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}

}

@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}

}

@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},

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},

pubstate = {published},

tppubtype = {article}

}

@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}

}

@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}

}

@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}

}

@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},

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}

}

@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}

}

@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}

}

@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}

}

@article{,

title = {Loading linear arrays of Cu(II) inside aromatic amide helices},

author = {J Wang and B Wicher and A M\'{e}ndez-Ardoy and X Li and G Pecastaings and T Buffeteau and D M Bassani and V Maurizot and I Huc},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/anie.202104734},

doi = {https://doi.org/10.1002/anie.202104734},

issn = {1433-7851},

year  = {2021},

date = {2021-05-20},

journal = {Angewandte Chemie International Edition},

volume = {n/a},

number = {n/a},

abstract = {The very stable helices of 8-amino-2-quinolinecarboxylic acid oligoamides are shown to uptake Cu(II) ions in their cavity through deprotonation of their amide functions with minimal alteration of their shape, unlike most metallo-organic structures which generally much differ from their organic precursors. The outcome is the formation of intramolecular linear arrays of a defined number of Cu(II) centers (up to sixteen in this study) at a 3 r{A} distance, forming a molecular mimic of a metal wire completely surrounded by an organic sheath. The helices pack in the solid state so that the arrays of Cu(II) extend intermolecularly. Conductive-AFM and cyclic voltammetry suggest that electrons are transported throughout the metal-loaded helices in contrast with hole transport observed for analogous foldamers devoid of metal ions.},

keywords = {Foundry Organic},

pubstate = {published},

tppubtype = {article}

}

@article{,

title = {Nanoscale Heterogeneities and Composition\textendashReactivity Relationships in Copper Vanadate Photoanodes},

author = {J Eichhorn and C-M Jiang and J K Cooper and I D Sharp and F M Toma},

url = {https://doi.org/10.1021/acsami.1c01848},

doi = {10.1021/acsami.1c01848},

issn = {1944-8244},

year  = {2021},

date = {2021-05-17},

journal = {ACS Applied Materials & Interfaces},

volume = {13},

number = {20},

pages = {23575-23583},

abstract = {The photoelectrochemical performance of thin film photoelectrodes can be impacted by deviations from the stoichiometric composition, both at the macroscale and at the nanoscale. This issue is especially pronounced for the class of ternary compounds that are currently investigated for simultaneously achieving the optoelectronic characteristics and chemical stability required for solar fuel generation. Here, we combine macroscopic photoelectrochemical testing with atomic force microscopy (AFM) and scanning transmission X-ray microscopy (STXM) to reveal relationships between photoelectrochemical activity, nanoscale morphology, and local chemical composition in copper vanadate (CVO) thin films as a model system. For films with varying Cu/(Cu + V) ratios around the ideal stoichiometry of stoiberite Cu5V2O10, AFM resolves submicrometer morphology variations, which correlate with variations of the Cu content resolved by STXM. Both stoichiometric and Cu-deficient films exhibit a clear photoresponse, which indicates electronic tolerance to reduced Cu content. While both films exhibit homogeneous O and V content, they are also characterized by local regions of Cu enrichment and depletion that extend beyond individual grains. By contrast, Cu-rich photoelectrodes exhibit a tendency toward CuO secondary phase formation and a significantly reduced photoelectrochemical activity, indicating a significantly poor electronic tolerance to Cu-enrichment. These findings highlight that the average film composition at the macroscale is insufficient for defining structure\textendashfunction relationships in complex ternary compounds. Rather, correlating microscopic variations in chemical composition to macroscopic photoelectrochemical performance provides insights into photocatalytic activity and stability that are otherwise not apparent from pure macroscopic characterization.},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@article{,

title = {The Significance of Polarons and Dynamic Disorder in Halide Perovskites},

author = {M J Schilcher and P J Robinson and D J Abramovitch and L Z Tan and A M Rappe and D R Reichman and D A Egger},

url = {https://doi.org/10.1021/acsenergylett.1c00506},

doi = {10.1021/acsenergylett.1c00506},

year  = {2021},

date = {2021-05-17},

journal = {ACS Energy Letters},

pages = {2162-2173},

abstract = {The development of halide perovskite semiconductors led to various technological breakthroughs in optoelectronics, in particular in the areas of photovoltaics and light-emitting diodes. Additionally, the study of their fundamental properties has uncovered intriguing puzzles that demand explanation. Polaronic effects associated with the coupling of electrons and holes to polar lattice vibrations are often invoked as a microscopic mechanism to explain various unusual experimental observations. While some form of polaronic behavior undoubtedly exists in these systems, several assumptions underlying standard models used to describe a polaron mechanism appear to be strongly violated in these materials. In this Perspective, we investigate the role of polaronic effects in halide perovskites and summarize signatures and failures of the polaron picture to explain physical characteristics of the materials. We highlight the importance of the complementary dynamic disorder concept that can rationalize various key properties of halide perovskites for which standard polaron and band-theory pictures of carrier transport fail.},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@article{,

title = {Electronic and Geometric Characterization of TICT Formation in Hemithioindigo Photoswitches by Picosecond Infrared Spectroscopy},

author = {K Stallhofer and M Nuber and F Sch\"{u}ppel and S Thumser and H Iglev and De R Vivie-Riedle and W Zinth and H Dube},

url = {https://doi.org/10.1021/acs.jpca.1c02646},

doi = {10.1021/acs.jpca.1c02646},

issn = {1089-5639},

year  = {2021},

date = {2021-05-14},

journal = {The Journal of Physical Chemistry A},

keywords = {Foundry Organic},

pubstate = {published},

tppubtype = {article}

}

@article{,

title = {Tuning the intermediate reaction barriers by a CuPd catalyst to improve the selectivity of CO2 electroreduction to C2 products},

author = {L Zhu and Y Lin and K Liu and E Cort\'{e}s and H Li and J Hu and A Yamaguchi and X Liu and M Miyauchi and J Fu and M Liu},

url = {https://www.sciencedirect.com/science/article/pii/S1872206720637548},

doi = {https://doi.org/10.1016/S1872-2067(20)63754-8},

issn = {1872-2067},

year  = {2021},

date = {2021-05-12},

journal = {Chinese Journal of Catalysis},

volume = {42},

number = {9},

pages = {1500-1508},

abstract = {Electrochemical CO2 reduction is a promising strategy for the utilization of CO2 and intermittent excess electricity. Cu is the only single metal catalyst that can electrochemically convert CO2 into multicarbon products. However, Cu exhibits an unfavorable activity and selectivity for the generation of C2 products because of the insufficient amount of CO* provided for the C-C coupling. Based on the strong CO2 adsorption and ultrafast reaction kinetics of CO* formation on Pd, an intimate CuPd(100) interface was designed to lower the intermediate reaction barriers and improve the efficiency of C2 product formation. Density functional theory (DFT) calculations showed that the CuPd(100) interface enhanced the CO2 adsorption and decreased the CO2* hydrogenation energy barrier, which was beneficial for the C-C coupling. The potential-determining step (PDS) barrier of CO2 to C2 products on the CuPd(100) interface was 0.61 eV, which was lower than that on Cu(100) (0.72 eV). Encouraged by the DFT calculation results, the CuPd(100) interface catalyst was prepared by a facile chemical solution method and characterized by transmission electron microscopy. CO2 temperature-programmed desorption and gas sensor experiments further confirmed the enhancement of the CO2 adsorption and CO2* hydrogenation ability of the CuPd(100) interface catalyst. Specifically, the obtained CuPd(100) interface catalyst exhibited a C2 Faradaic efficiency of 50.3% ± 1.2% at −1.4 VRHE in 0.1 M KHCO3, which was 2.1 times higher than that of the Cu catalyst (23.6% ± 1.5%). This study provides the basis for the rational design of Cu-based electrocatalysts for the generation of multicarbon products by fine-tuning the intermediate reaction barriers.},

keywords = {Foundry Inorganic, Solid-Solid},

pubstate = {published},

tppubtype = {article}

}

@article{,

title = {Coherent vibrational dynamics reveals lattice anharmonicity in organic\textendashinorganic halide perovskite nanocrystals},

author = {T Debnath and D Sarker and H Huang and Z-K Han and A Dey and L Polavarapu and S V Levchenko and J Feldmann},

url = {https://doi.org/10.1038/s41467-021-22934-2},

doi = {10.1038/s41467-021-22934-2},

issn = {2041-1723},

year  = {2021},

date = {2021-05-11},

journal = {Nature Communications},

volume = {12},

number = {1},

pages = {2629},

abstract = {The halide ions of organic-inorganic hybrid perovskites can strongly influence the interaction between the central organic moiety and the inorganic metal halide octahedral units and thus their lattice vibrations. Here, we report the halide-ion-dependent vibrational coherences in formamidinium lead halide (FAPbX3, X = Br, I) perovskite nanocrystals (PNCs) via the combination of femtosecond pump\textendashprobe spectroscopy and density functional theory calculations. We find that the FAPbX3 PNCs generate halide-dependent coherent vibronic wave packets upon above-bandgap non-resonant excitation. More importantly, we observe several higher harmonics of the fundamental modes for FAPbI3 PNCs as compared to FAPbBr3 PNCs. This is likely due to the weaker interaction between the central FA moiety and the inorganic cage for FAPbI3 PNCs, and thus the PbI64− unit can vibrate more freely. This weakening reveals the intrinsic anharmonicity in the Pb-I framework, and thus facilitating the energy transfer into overtone and combination bands. These findings not only unveil the superior stability of Br\textendashbased PNCs over I\textendashbased PNCs but are also important for a better understanding of their electronic and polaronic properties.},

keywords = {Foundry Inorganic, Foundry Organic},

pubstate = {published},

tppubtype = {article}

}

@article{,

title = {Characterization and Quantification of Depletion and Accumulation Layers in Solid-State Li+-Conducting Electrolytes Using In Situ Spectroscopic Ellipsometry},

author = {L Katzenmeier and L Carstensen and S J Schaper and P M\"{u}ller-Buschbaum and A S Bandarenka},

url = {http://europepmc.org/abstract/MED/33955614 

https://doi.org/10.1002/adma.202100585},

doi = {10.1002/adma.202100585},

issn = {0935-9648},

year  = {2021},

date = {2021-05-06},

journal = {Advanced Materials},

pages = {e2100585},

abstract = {The future of mobility depends on the development of next-generation battery technologies, such as all-solid-state batteries. As the ionic conductivity of solid Li<sup>+</sup> -conductors can, in some cases, approach that of liquid electrolytes, a significant remaining barrier faced by solid-state electrolytes (SSEs) is the interface formed at the anode and cathode materials, with chemical instability and physical resistances arising. The physical properties of space charge layers (SCLs), a widely discussed phenomenon in SSEs, are still unclear. In this work, spectroscopic ellipsometry is used to characterize the accumulation and depletion layers. An optical model is developed to quantify their thicknesses and corresponding concentration changes. It is shown that the Li<sup>+</sup> -depleted layer (≈190 nm at 1 V) is thinner than the accumulation layer (≈320 nm at 1 V) in a glassy lithium-ion-conducting glass ceramic electrolyte (a trademark of Ohara Corporation). The in situ approach combining electrochemistry and optics resolves the ambiguities around SCL formation. It opens up a wide field of optical measurements on SSEs, allowing various experimental studies in the future.},

keywords = {Foundry Inorganic, Solid-Solid},

pubstate = {published},

tppubtype = {article}

}

@article{,

title = {High-Performance Vertical Organic Transistors of Sub-5 nm Channel Length},

author = {J Lenz and A M Seiler and F R Geisenhof and F Winterer and K Watanabe and T Taniguchi and R T Weitz},

url = {https://doi.org/10.1021/acs.nanolett.1c01144},

doi = {10.1021/acs.nanolett.1c01144},

issn = {1530-6984},

year  = {2021},

date = {2021-05-06},

journal = {Nano Letters},

abstract = {Miniaturization of electronic circuits increases their overall performance. So far, electronics based on organic semiconductors has not played an important role in the miniaturization race. Here, we show the fabrication of liquid electrolyte gated vertical organic field effect transistors with channel lengths down to 2.4 nm. These ultrashort channel lengths are enabled by using insulating hexagonal boron nitride with atomically precise thickness and flatness as a spacer separating the vertically aligned source and drain electrodes. The transistors reveal promising electrical characteristics with output current densities of up to 2.95 MA cm\textendash2 at −0.4 V bias, on\textendashoff ratios of up to 106, a steep subthreshold swing of down to 65 mV dec\textendash1 and a transconductance of up to 714 S m\textendash1. Realizing channel lengths in the sub-5 nm regime and operation voltages down to 100 μV proves the potential of organic semiconductors for future highly integrated or low power electronics.},

keywords = {Foundry Organic},

pubstate = {published},

tppubtype = {article}

}

@article{,

title = {Charge Traps in All‐Inorganic CsPbBr3 Perovskite Nanowire Field‐Effect Phototransistors},

author = {F Winterer and L S Walter and J Lenz and S Seebauer and Y Tong and L Polavarapu and R T Weitz},

issn = {2199-160X},

year  = {2021},

date = {2021-05-06},

journal = {Advanced Electronic Materials},

pages = {2100105},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@article{,

title = {Picosecond Charge Localization Dynamics in CH3NH3PbI3 Perovskite Probed by Infrared-Activated Vibrations},

author = {K Stallhofer and M Nuber and D Cortecchia and A Bruno and R Kienberger and F Deschler and C Soci and H Iglev},

url = {https://doi.org/10.1021/acs.jpclett.1c00935},

doi = {10.1021/acs.jpclett.1c00935},

year  = {2021},

date = {2021-05-05},

journal = {The Journal of Physical Chemistry Letters},

pages = {4428-4433},

abstract = {Hybrid metal halide perovskites exhibit well-defined semiconducting properties and efficient optoelectronic performance considering their soft crystal structure and low-energy lattice motions. The response of such a crystal lattice to light-induced charges is a fundamental question, for which experimental insight into ultrafast time scales is still sought. Here, we use infrared-activated vibrations (IRAV) of the organic components within the hybrid perovskite lattice as a sensitive probe for local structural reorganizations after photoexcitation, with femtosecond resolution. We find that the IRAV signal response shows a delayed rise of about 3 ps and subsequent decay of pronounced monomolecular character, distinguishing it from absorption associated with free carriers. We interpret our results as a two-step carrier localization process. Initially, carriers localize transiently in local energy minima formed by lattice fluctuations. A subpopulation of these can then fall into deeper trapped states over picoseconds, likely due to local reorganization of the organic molecules surrounding the carriers.},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@article{,

title = {Carbonaceous Oxygen Evolution Reaction Catalysts: From Defect and Doping-Induced Activity over Hybrid Compounds to Ordered Framework Structures},

author = {F Zoller and S H\"{a}ringer and D B\"{o}hm and J Luxa and Z Sofer and D Fattakhova-Rohlfing},

doi = {10.1002/smll.202007484},

issn = {1613-6810},

year  = {2021},

date = {2021-05-04},

journal = {Small},

pages = {e2007484},

abstract = {Oxygen evolution reaction (OER) is expected to be of great importance for the future energy conversion and storage in form of hydrogen by water electrolysis. Besides the traditional noble-metal or transition metal oxide-based catalysts, carbonaceous electrocatalysts are of great interest due to their huge structural and compositional variety and unrestricted abundance. This review provides a summary of recent advances in the field of carbon-based OER catalysts ranging from "pure" or unintentionally doped carbon allotropes over heteroatom-doped carbonaceous materials and carbon/transition metal compounds to metal oxide composites where the role of carbon is mainly assigned to be a conductive support. Furthermore, the review discusses the recent developments in the field of ordered carbon framework structures (metal organic framework and covalent organic framework structures) that potentially allow a rational design of heteroatom-doped 3D porous structures with defined composition and spatial arrangement of doping atoms to deepen the understanding on the OER mechanism on carbonaceous structures in the future. Besides introducing the structural and compositional origin of electrochemical activity, the review discusses the mechanism of the catalytic activity of carbonaceous materials, their stability under OER conditions, and potential synergistic effects in combination with metal (or metal oxide) co-catalysts.},

keywords = {Foundry Inorganic, Solid-Liquid},

pubstate = {published},

tppubtype = {article}

}

@article{,

title = {Graphene Energy Transfer for Single-Molecule Biophysics, Biosensing, and Super-Resolution Microscopy},

author = {I Kami\'{n}ska and J Bohlen and R Yaadav and P Sch\"{u}ler and M Raab and T Schr\"{o}der and J Z\"{a}hringer and K Zielonka and S Krause and P Tinnefeld},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adma.202101099},

doi = {https://doi.org/10.1002/adma.202101099},

issn = {0935-9648},

year  = {2021},

date = {2021-05-03},

journal = {Advanced Materials},

volume = {n/a},

number = {n/a},

pages = {2101099},

abstract = {Abstract Graphene is considered a game-changing material, especially for its mechanical and electrical properties. This work exploits that graphene is almost transparent but quenches fluorescence in a range up to ≈40 nm. Graphene as a broadband and unbleachable energy-transfer acceptor without labeling, is used to precisely determine the height of molecules with respect to graphene, to visualize the dynamics of DNA nanostructures, and to determine the orientation of F\"{o}rster-type resonance energy transfer (FRET) pairs. Using DNA origami nanopositioners, biosensing, single-molecule tracking, and DNA PAINT super-resolution with <3 nm z-resolution are demonstrated. The range of examples shows the potential of graphene-on-glass coverslips as a versatile platform for single-molecule biophysics, biosensing, and super-resolution microscopy.},

keywords = {Foundry Organic},

pubstate = {published},

tppubtype = {article}

}

@article{,

title = {Anapole-Assisted Absorption Engineering in Arrays of Coupled Amorphous Gallium Phosphide Nanodisks},

author = {L H\"{u}ttenhofer and A Tittl and L K\"{u}hner and E Cort\'{e}s and S A Maier},

url = {https://doi.org/10.1021/acsphotonics.1c00238},

doi = {10.1021/acsphotonics.1c00238},

year  = {2021},

date = {2021-04-26},

journal = {ACS Photonics},

abstract = {Broadband solar light harvesting plays a crucial role for efficient energy conversion. Anapole excitations and associated absorption engineering in dielectric nanoresonators are a focus of nanophotonic research due to the intricate combination of nonradiating modes and strong electromagnetic field confinement in the underlying material. The arising high field strengths are used for enhanced second-harmonic generation and photocatalysis, where devices require large areas with closely spaced nanoresonators for sizable photonic yields. However, most anapole studies have so far been carried out at the single-particle level, neglecting the influence of anapole\textendashanapole interactions. Here, we present a systematic study of coupling mechanisms in rectangular arrays of amorphous GaP nanodisks that support anapole excitations at 600 nm, which is within the lossy spectral regime of the material. Our experimental findings show that maximum visible light extinction by the array and maximum absorption in the GaP are not achieved by the densest packing of resonators. Counterintuitively, increasing the array periodicities such that collective effects spectrally overlap with the anapole excitation of a single particle leads to an absorption enhancement of up to 300% compared to a single disk. An analysis of coupling in one- and two-dimensional arrays with polarization-dependent measurements and numerical simulations allows us to discriminate between coupling interactions parallel and perpendicular to the polarization axis and evaluate their strengths. Utilizing a multipolar decomposition of excitations in single nanodisks embedded in one-dimensional arrays, we can attribute the coupling to enhanced electric and toroidal dipoles under variation of the interparticle spacing. Our results provide a fundamental understanding of tailored light absorption in coupled anapole resonators and reveal important design guidelines for advanced metasurface approaches in a wide range of energy conversion applications.},

keywords = {Foundry Inorganic, Solid-Solid},

pubstate = {published},

tppubtype = {article}

}

@article{,

title = {Photovoltaic Cells Based on Ternary P3HT:PCBM:Ruthenium(II) Complex Bearing 8-(diphenylphosphino)quinoline Active Layer},

author = {S Akel and M A Sharif and R Al-Esseili and M A Al-Wahish and H A Hodali and P M\"{u}ller-Buschbaum and L Schmidt-Mende and M Al-Hussein},

url = {https://www.sciencedirect.com/science/article/pii/S0927775721005549},

doi = {https://doi.org/10.1016/j.colsurfa.2021.126685},

issn = {0927-7757},

year  = {2021},

date = {2021-04-24},

journal = {Colloids and Surfaces A: Physicochemical and Engineering Aspects},

pages = {126685},

abstract = {ABSTRACT Optical, morphological and photovoltaic properties are investigated for ternary solar cells containing a traditional poly(3-hexylthiophene-2,5-diyl):[6,6]-phenyl-C61-butyric-acid-methyl ester (P3HT:PCBM) bulkheterojunction (BHJ) active layer modified with different concentrations of a novel ruthenium complex [Ru(N-P)2(O-O)], where N-P abbreviates 8-(diphenylphosphino)quinolone and O-O = oxalate dianion. At a low concentration of the Ru-complex (2.5wt. %) the device efficiency is improved by 50% compared with the reference binary devices at ambient conditions. This substantial efficiency enhancement is attributed to the role of the Ru-complex in improving light absorption over a wavelength range of (295-800nm) in combination with a better matching of the energy levels of the ternary blend system. Moreover, at low concentration, the Ru-complex has a positive impact on the morphology of the active layer in the device. The inclusion of Ru-complex increases the P3HT crystallinity substantially with virtually no effect on the size and orientation of the crystalline lamellae. The enhancement in device efficiency becomes less pronounced with increasing the concentration of the Ru-complex due to the formation of several micron-size domains of [Ru(N-P)2(O-O)] in the ternary active layers. These large domains negatively affect the optical properties and morphology, thus inhibiting efficient charge generation and transport in the corresponding solar cells.},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}