@article{33651,
author = {{Sahoo, Sudhir K. and Teixeira, Ivo F. and Naik, Aakash and Heske, Julian Joachim and Cruz, Daniel and Antonietti, Markus and Savateev, Aleksandr and Kühne, Thomas}},
issn = {{1932-7447}},
journal = {{The Journal of Physical Chemistry C}},
keywords = {{Surfaces, Coatings and Films, Physical and Theoretical Chemistry, General Energy, Electronic, Optical and Magnetic Materials}},
number = {{25}},
pages = {{13749--13758}},
publisher = {{American Chemical Society (ACS)}},
title = {{{Photocatalytic Water Splitting Reaction Catalyzed by Ion-Exchanged Salts of Potassium Poly(heptazine imide) 2D Materials}}},
doi = {{10.1021/acs.jpcc.1c03947}},
volume = {{125}},
year = {{2021}},
}
@article{33657,
author = {{Mirhosseini, Hossein and Tahmasbi, Hossein and Kuchana, Sai Ram and Ghasemi, Alireza and Kühne, Thomas}},
issn = {{0927-0256}},
journal = {{Computational Materials Science}},
keywords = {{Computational Mathematics, General Physics and Astronomy, Mechanics of Materials, General Materials Science, General Chemistry, General Computer Science}},
publisher = {{Elsevier BV}},
title = {{{An automated approach for developing neural network interatomic potentials with FLAME}}},
doi = {{10.1016/j.commatsci.2021.110567}},
volume = {{197}},
year = {{2021}},
}
@inproceedings{33654,
author = {{Balos, Vasileios and Elgabarty, Hossam and Wolf, Martin and Kühne, Thomas and Netz, Roland and Bonthuis, Douwe Jan and Kaliannan, Naveen and Loche, Philip and Kampfrath, Tobias and Sajadi, Mohsen}},
booktitle = {{Terahertz Emitters, Receivers, and Applications XII}},
editor = {{Razeghi, Manijeh and Baranov, Alexei N.}},
publisher = {{SPIE}},
title = {{{Ultrafast solvent-to-solvent and solvent-to-solute energy transfer driven by single-cycle THz electric fields}}},
doi = {{10.1117/12.2594143}},
year = {{2021}},
}
@article{33656,
author = {{Wang, Mengying and Ranjbar, Ahmad and Kühne, Thomas and Belosludov, Rodion V. and Kawazoe, Yoshiyuki and Liang, Yunye}},
issn = {{0008-6223}},
journal = {{Carbon}},
keywords = {{General Chemistry, General Materials Science}},
pages = {{370--378}},
publisher = {{Elsevier BV}},
title = {{{A theoretical investigation of topological phase modulation in carbide MXenes: Role of image potential states}}},
doi = {{10.1016/j.carbon.2021.05.026}},
volume = {{181}},
year = {{2021}},
}
@article{33659,
abstract = {{Abstract
We performed a virtual materials screening to identify promising topological materials for photocatalytic water splitting under visible light irradiation. Topological compounds were screened based on band gap, band edge energy, and thermodynamics stability criteria. In addition, topological types for our final candidates were computed based on electronic structures calculated usingthe hybrid density functional theory including exact Hartree–Fock exchange. Our final list contains materials which have band gaps between 1.0 and 2.7 eV in addition to band edge energies suitable for water oxidation and reduction. However, the topological types of these compounds calculated with the hybrid functional differ from those reported previously. To that end, we discuss the importance of computational methods for the calculation of atomic and electronic structures in materials screening processes.}},
author = {{Ranjbar, Ahmad and Mirhosseini, Hossein and Kühne, Thomas}},
issn = {{2515-7639}},
journal = {{Journal of Physics: Materials}},
keywords = {{Condensed Matter Physics, General Materials Science, Atomic and Molecular Physics, and Optics}},
number = {{1}},
publisher = {{IOP Publishing}},
title = {{{On topological materials as photocatalysts for water splitting by visible light}}},
doi = {{10.1088/2515-7639/ac363d}},
volume = {{5}},
year = {{2021}},
}
@article{33681,
author = {{da Silva, Marcos A.R. and Silva, Ingrid F. and Xue, Qi and Lo, Benedict T.W. and Tarakina, Nadezda V. and Nunes, Barbara N. and Adler, Peter and Sahoo, Sudhir K. and Bahnemann, Detlef W. and López-Salas, Nieves and Savateev, Aleksandr and Ribeiro, Caue and Kühne, Thomas and Antonietti, Markus and Teixeira, Ivo F.}},
issn = {{0926-3373}},
journal = {{Applied Catalysis B: Environmental}},
keywords = {{Process Chemistry and Technology, General Environmental Science, Catalysis}},
publisher = {{Elsevier BV}},
title = {{{Sustainable oxidation catalysis supported by light: Fe-poly (heptazine imide) as a heterogeneous single-atom photocatalyst}}},
doi = {{10.1016/j.apcatb.2021.120965}},
volume = {{304}},
year = {{2021}},
}
@article{33675,
abstract = {{The influence of different polymer side chains on the vapor phase infiltration with TMA is investigated and supported by DFT-calculations.}},
author = {{Mai, Lukas and Maniar, Dina and Zysk, Frederik and Schöbel, Judith and Kühne, Thomas and Loos, Katja and Devi, Anjana}},
issn = {{1477-9226}},
journal = {{Dalton Transactions}},
keywords = {{Inorganic Chemistry}},
number = {{4}},
pages = {{1384--1394}},
publisher = {{Royal Society of Chemistry (RSC)}},
title = {{{Influence of different ester side groups in polymers on the vapor phase infiltration with trimethyl aluminum}}},
doi = {{10.1039/d1dt03753f}},
volume = {{51}},
year = {{2021}},
}
@inbook{29936,
author = {{Ramaswami, Arjun and Kenter, Tobias and Kühne, Thomas and Plessl, Christian}},
booktitle = {{Applied Reconfigurable Computing. Architectures, Tools, and Applications}},
isbn = {{9783030790240}},
issn = {{0302-9743}},
publisher = {{Springer International Publishing}},
title = {{{Evaluating the Design Space for Offloading 3D FFT Calculations to an FPGA for High-Performance Computing}}},
doi = {{10.1007/978-3-030-79025-7_21}},
year = {{2021}},
}
@article{19680,
abstract = {{This is the second part of a project on the foundations of first-principle calculations of the electron transport in crystals at finite temperatures, aiming at a predictive first-principles platform that combines ab-initio molecular dynamics (AIMD) and a finite-temperature Kubo-formula with dissipation for thermally disordered crystalline phases. The latter are encoded in an ergodic dynamical system (Ω,G,dP), where Ω is the configuration space of the atomic degrees of freedom, G is the space group acting on Ω and dP is the ergodic Gibbs measure relative to the G-action. We first demonstrate how to pass from the continuum Kohn–Sham theory to a discrete atomic-orbitals based formalism without breaking the covariance of the physical observables w.r.t. (Ω,G,dP). Then we show how to implement the Kubo-formula, investigate its self-averaging property and derive an optimal finite-volume approximation for it. We also describe a numerical innovation that made possible AIMD simulations with longer orbits and elaborate on the details of our simulations. Lastly, we present numerical results on the transport coefficients of crystal silicon at different temperatures.}},
author = {{Kühne, Thomas and Heske, Julian Joachim and Prodan, Emil}},
issn = {{0003-4916}},
journal = {{Annals of Physics}},
pages = {{168290}},
title = {{{Disordered crystals from first principles II: Transport coefficients}}},
doi = {{https://doi.org/10.1016/j.aop.2020.168290}},
volume = {{421}},
year = {{2020}},
}
@article{19823,
abstract = {{Individual grains of chalcopyrite solar cell absorbers can facet in different crystallographic directions at their surfaces. To gain a deeper understanding of the junction formation in these devices, we correlate variations in the surface facet orientation with the defect electronic properties. We use a combined analytical approach based on scanning tunneling spectroscopy (STS), scanning electron microscopy, and electron back scatter diffraction (EBSD), where we perform these experiments on identical surface areas as small as 2 × 2 µm2 with a lateral resolution well below 50 nm. The topography of the absorber surfaces indicates two main morphological features: micro-faceted, long basalt-like columns and their short nano-faceted terminations. Our STS results reveal that the long columns exhibit spectral signatures typical for the presence of pronounced oxidation-induced surface dipoles in conjunction with an increased density of electronic defect levels. In contrast, the nano-faceted terminations of the basalt-like columns are largely passivated in terms of electronic defect levels within the band gap region. Corresponding crystallographic data based on EBSD experiments show that the surface of the basalt-like columns can be assigned to intrinsically polar facet orientations, while the passivated terminations are assigned to non-polar planes. Ab-initio calculations suggest that the polar surfaces are more prone to oxidation and resulting O-induced defects, in comparison to non-polar planes. Our results emphasize the correlation between morphology, surface facet orientations and surface electronic properties. Furthermore, this work aids in gaining a fundamental understanding of oxidation induced lateral inhomogeneities in view of the p-n junction formation in chalcopyrite thin-film solar cells.}},
author = {{Elizabeth, Amala and Conradi, Hauke and K. Sahoo, Sudhir and Kodalle, Tim and A. Kaufmann, Christian and Kühne, Thomas and Mirhosseini, Hossein and Abou-Ras, Daniel and Mönig, Harry}},
issn = {{1359-6454}},
journal = {{Acta Materialia}},
keywords = {{Chalcopyrite absorber, Scanning tunneling spectroscopy, Electron backscatter diffraction, Density functional theory, Surface dipole}},
title = {{{Correlating facet orientation, defect-level density and dipole layer formation at the surface of polycrystalline CuInSe2 thin films}}},
doi = {{https://doi.org/10.1016/j.actamat.2020.09.028}},
volume = {{200}},
year = {{2020}},
}
@article{21239,
abstract = {{The electrochemical nitrogen reduction reaction (NRR) to ammonia (NH3) is a promising alternative route for an NH3 synthesis at ambient conditions to the conventional high temperature and pressure Haber--Bosch process without the need for hydrogen gas. Single metal ions or atoms are attractive candidates for the catalytic activation of non-reactive nitrogen (N2), and for future targeted improvement of NRR catalysts, it is of utmost importance to get detailed insights into structure-performance relationships and mechanisms of N2 activation in such structures. Here, we report density functional theory studies on the NRR catalyzed by single Au and Fe atoms supported in graphitic C2N materials. Our results show that the metal atoms present in the structure of C2N are the reactive sites, which catalyze the aforesaid reaction by strong adsorption and activation of N2. We further demonstrate that a lower onset electrode potential is required for Fe--C2N than for Au--C2N. Thus, Fe--C2N is theoretically predicted to be a potentially better NRR catalyst at ambient conditions than Au--C2N owing to the larger adsorption energy of N2 molecules. Furthermore, we have experimentally shown that single sites of Au and Fe supported on nitrogen-doped porous carbon are indeed active NRR catalysts. However, in contrast to our theoretical results, the Au-based catalyst performed slightly better with a Faradaic efficiency (FE) of 10.1{\%} than the Fe-based catalyst with an FE of 8.4{\%} at −0.2 V vs. RHE. The DFT calculations suggest that this difference is due to the competitive hydrogen evolution reaction and higher desorption energy of ammonia.}},
author = {{Sahoo, Sudhir K. and Heske, Julian Joachim and Antonietti, Markus and Qin, Qing and Oschatz, Martin and Kühne, Thomas}},
journal = {{ACS Applied Energy Materials}},
number = {{10}},
pages = {{10061--10069}},
publisher = {{American Chemical Society}},
title = {{{Electrochemical N2 Reduction to Ammonia Using Single Au/Fe Atoms Supported on Nitrogen-Doped Porous Carbon}}},
doi = {{10.1021/acsaem.0c01740}},
volume = {{3}},
year = {{2020}},
}
@article{21241,
abstract = {{In this work, a high-throughput screening of binary and ternary pnictide- and halide-based compounds is performed to identify promising p-type transparent conductors. Our investigation profits from the emergence of open-access databases based on ab-initio results. The band gap, stability, hole effective mass, and p-type dopability are employed for the materials screening and the validity of these descriptors is discussed. Among the final candidates, BaSiN2 is the most promising compound.}},
author = {{Wiebeler, Hendrik and Kormath Madam Raghupathy, Ramya and Mirhosseini, S. Hossein and Kühne, Thomas}},
journal = {{Journal of Physics: Materials}},
number = {{1}},
pages = {{015004}},
publisher = {{{IOP} Publishing}},
title = {{{Virtual screening of nitrogen-, phosphorous- and halide-containing materials as p-type transparent conductors}}},
doi = {{10.1088/2515-7639/abc762}},
volume = {{4}},
year = {{2020}},
}
@article{17379,
author = {{Kumar Sahoo, Sudhir and Heske, Julian Joachim and Azadi, Sam and Zhang, Zhenzhe and V Tarakina, Nadezda and Oschatz, Martin and Z. Khaliullin, Rustam and Antonietti, Markus and Kühne, Thomas}},
journal = {{Scientific Reports}},
number = {{1}},
title = {{{On the Possibility of Helium Adsorption in Nitrogen Doped Graphitic Materials}}},
doi = {{10.1038/s41598-020-62638-z}},
volume = {{10}},
year = {{2020}},
}
@article{19844,
abstract = {{The defect-electronic properties of {112} microfaceted surfaces of epitaxially grown CuInSe2 thin films are investigated by scanning tunneling spectroscopy and photoelectron spectroscopy techniques after various surface treatments. The intrinsic CuInSe2 surface is found to be largely passivated in terms of electronic defect levels in the band-gap region. However, surface oxidation leads to an overall high density of defect levels in conjunction with a considerable net surface dipole, which persists even after oxide removal. Yet, a subsequent annealing under vacuum restores the initial condition. Such oxidation/reduction cycles are reversible for many times providing robust control of the surface and interface properties in these materials. Based on ab initio simulations, a mechanism where oxygen dissociatively adsorbs and subsequently diffuses to a subsurface site is proposed as the initial step of the observed dipole formation. Our results emphasize the relevance of oxidation-induced dipole effects at the thin film surface and provide a comprehensive understanding toward passivation strategies of these surfaces.}},
author = {{Elizabeth, Amala and Sahoo, Sudhir K. and Lockhorn, David and Timmer, Alexander and Aghdassi, Nabi and Zacharias, Helmut and Kühne, Thomas and Siebentritt, Susanne and Mirhosseini, Hossein and Mönig, Harry}},
journal = {{Phys. Rev. Materials}},
pages = {{063401}},
publisher = {{American Physical Society}},
title = {{{ Oxidation/reduction cycles and their reversible effect on the dipole formation at CuInSe2 surfaces}}},
doi = {{10.1103/PhysRevMaterials.4.063401}},
volume = {{4}},
year = {{2020}},
}
@article{21112,
abstract = {{Photovoltaics is one of the most promising and fastest-growing renewable energy technologies. Although the price-performance ratio of solar cells has improved significantly over recent years{,} further systematic investigations are needed to achieve higher performance and lower cost for future solar cells. In conjunction with experiments{,} computer simulations are powerful tools to investigate the thermodynamics and kinetics of solar cells. Over the last few years{,} we have developed and employed advanced computational techniques to gain a better understanding of solar cells based on copper indium gallium selenide (Cu(In{,}Ga)Se2). Furthermore{,} we have utilized state-of-the-art data-driven science and machine learning for the development of photovoltaic materials. In this Perspective{,} we review our results along with a survey of the field.}},
author = {{Mirhosseini, S. Hossein and Kormath Madam Raghupathy, Ramya and Sahoo, Sudhir K. and Wiebeler, Hendrik and Chugh, Manjusha and Kühne, Thomas}},
journal = {{Phys. Chem. Chem. Phys.}},
pages = {{26682--26701}},
publisher = {{The Royal Society of Chemistry}},
title = {{{In silico investigation of Cu(In,Ga)Se2-based solar cells}}},
doi = {{10.1039/D0CP04712K}},
volume = {{22}},
year = {{2020}},
}
@article{21240,
abstract = {{Rechargeable aqueous Zn-ion energy storage devices are promising candidates for next-generation energy storage technologies. However, the lack of highly reversible Zn2+-storage anode materials with low potential windows remains a primary concern. Here, we report a two-dimensional polyarylimide covalent organic framework (PI-COF) anode with high-kinetics Zn2+-storage capability. The well-organized pore channels of PI-COF allow the high accessibility of the build-in redox-active carbonyl groups and efficient ion diffusion with a low energy barrier. The constructed PI-COF anode exhibits a specific capacity (332 C g–1 or 92 mAh g–1 at 0.7 A g–1), a high rate capability (79.8% at 7 A g–1), and a long cycle life (85% over 4000 cycles). In situ Raman investigation and first-principle calculations clarify the two-step Zn2+-storage mechanism, in which imide carbonyl groups reversibly form negatively charged enolates. Dendrite-free full Zn-ion devices are fabricated by coupling PI-COF anodes with MnO2 cathodes, delivering excellent energy densities (23.9 ∼ 66.5 Wh kg–1) and supercapacitor-level power densities (133 ∼ 4782 W kg–1). This study demonstrates the feasibility of covalent organic framework as Zn2+-storage anodes and shows a promising prospect for constructing reliable aqueous energy storage devices.}},
author = {{Yu, Minghao and Chandrasekhar, Naisa and Kormath Madam Raghupathy, Ramya and Ly, Khoa Hoang and Zhang, Haozhe and Dmitrieva, Evgenia and Liang, Chaolun and Lu, Xihong and Kühne, Thomas and Mirhosseini, S. Hossein and Weidinger, Inez M. and Feng, Xinliang}},
issn = {{0002-7863}},
journal = {{Journal of the American Chemical Society}},
number = {{46}},
pages = {{19570--19578}},
publisher = {{American Chemical Society}},
title = {{{A High-Rate Two-Dimensional Polyarylimide Covalent Organic Framework Anode for Aqueous Zn-Ion Energy Storage Devices}}},
doi = {{10.1021/jacs.0c07992}},
volume = {{142}},
year = {{2020}},
}
@article{17374,
abstract = {{Lead halide perovskite semiconductors providing record efficiencies of solar cells have usually mixed compositions doped in A- and X-sites to enhance the phase stability. The cubic form of formamidinium (FA) lead iodide reveals excellent opto-electronic properties but transforms at room temperature (RT) into a hexagonal structure which does not effectively absorb visible light. This metastable form and the mechanism of its stabilization by Cs+ and Br− incorporation are poorly characterized and insufficiently understood. We report here the vibrational properties of cubic FAPbI3 investigated by DFT calculations on phonon frequencies and intensities, and micro-Raman spectroscopy. The effects of Cs+ and Br− partial substitution are discussed. We support our results with the study of FAPbBr3 which expands the identification of vibrational modes to the previously unpublished low frequency region (<500 cm−1). Our results show that the incorporation of Cs+ and Br− leads to the coupling of the displacement of the A-site components and weakens the bonds between FA+ and the PbX6 octahedra. We suggest that the enhancement of α-FAPbI3 stability can be a product of the release of tensile stresses in the Pb–X bond, which is reflected in a red-shift of the low frequency region of the Raman spectrum (<200 cm−1).}},
author = {{Ibaceta-Jaña, Josefa and Muydinov, Ruslan and Rosado, Pamela and Mirhosseini, Hossein and Chugh, Manjusha and Nazarenko, Olga and Dirin, Dmitry N. and Heinrich, Dirk and Wagner, Markus R. and Kühne, Thomas and Szyszka, Bernd and Kovalenko, Maksym V. and Hoffmann, Axel}},
journal = {{Phys. Chem. Chem. Phys.}},
pages = {{5604--5614}},
publisher = {{The Royal Society of Chemistry}},
title = {{{Vibrational dynamics in lead halide hybrid perovskites investigated by Raman spectroscopy}}},
doi = {{10.1039/C9CP06568G}},
volume = {{22}},
year = {{2020}},
}
@article{17376,
abstract = {{The record conversion efficiency of thin-film solar cells based on Cu(In,Ga)Se2 (CIGS) absorbers has exceeded 23%. Such a high performance is currently only attainable by the incorporation of heavy alkali metals like Cs into the absorber through an alkali fluoride post-deposition treatment (PDT). As the effect of the incorporated heavy alkali metals is under discussion, we investigated the local composition and microstructure of high efficiency CIGS solar cells via various high-resolution techniques in a combinatory approach. An accumulation of Cs is clearly detected at the p-n junction along with variations in the local CIGS composition, showing the formation of a beneficial secondary phase with a laterally inhomogeneous distribution. Additionally, Cs accumulations were detected at grain boundaries with a random misorientation of the adjacent grains where a reduced Cu concentration and increased In and Se concentrations are detected. No accumulation was found at Σ3 twin boundaries as well as the grain interior. These experimental findings are in excellent agreement with complementary ab-initio calculations, demonstrating that the grain boundaries are passivated by the presence of Cs. Further, it is unlikely that Cs with its large ionic radius is incorporated into the CIGS grains where it would cause detrimental defects.}},
author = {{Schöppe, Philipp and Schönherr, Sven and Chugh, Manjusha and Mirhosseini, Hossein and Jackson, Philip and Wuerz, Roland and Ritzer, Maurizio and Johannes, Andreas and Martínez-Criado, Gema and Wisniewski, Wolfgang and Schwarz, Torsten and T. Plass, Christian and Hafermann, Martin and Kühne, Thomas and S. Schnohr, Claudia and Ronning, Carsten}},
issn = {{2211-2855}},
journal = {{Nano Energy}},
pages = {{104622}},
title = {{{Revealing the origin of the beneficial effect of cesium in highly efficient Cu(In,Ga)Se2 solar cells}}},
doi = {{https://doi.org/10.1016/j.nanoen.2020.104622}},
volume = {{71}},
year = {{2020}},
}
@article{34302,
abstract = {{Energy flow in the hydrogen bonding network of water is traced by resonant terahertz excitation and off-resonant optical probing.}},
author = {{Elgabarty, Hossam and Kampfrath, Tobias and Bonthuis, Douwe Jan and Balos, Vasileios and Kaliannan, Naveen Kumar and Loche, Philip and Netz, Roland R. and Wolf, Martin and Kühne, Thomas and Sajadi, Mohsen}},
issn = {{2375-2548}},
journal = {{Science Advances}},
keywords = {{Multidisciplinary}},
number = {{17}},
publisher = {{American Association for the Advancement of Science (AAAS)}},
title = {{{Energy transfer within the hydrogen bonding network of water following resonant terahertz excitation}}},
doi = {{10.1126/sciadv.aay7074}},
volume = {{6}},
year = {{2020}},
}
@article{34301,
abstract = {{
Ab initio molecular dynamics simulations of ambient liquid water and energy decomposition analysis have recently shown that water molecules exhibit significant asymmetry between the strengths of the two donor and/or the two acceptor interactions.
}},
author = {{Elgabarty, Hossam and Kühne, Thomas}},
issn = {{1463-9076}},
journal = {{Physical Chemistry Chemical Physics}},
keywords = {{Physical and Theoretical Chemistry, General Physics and Astronomy}},
number = {{19}},
pages = {{10397--10411}},
publisher = {{Royal Society of Chemistry (RSC)}},
title = {{{Tumbling with a limp: local asymmetry in water's hydrogen bond network and its consequences}}},
doi = {{10.1039/c9cp06960g}},
volume = {{22}},
year = {{2020}},
}