@unpublished{32404, abstract = {{The CP2K program package, which can be considered as the swiss army knife of atomistic simulations, is presented with a special emphasis on ab-initio molecular dynamics using the second-generation Car-Parrinello method. After outlining current and near-term development efforts with regards to massively parallel low-scaling post-Hartree-Fock and eigenvalue solvers, novel approaches on how we plan to take full advantage of future low-precision hardware architectures are introduced. Our focus here is on combining our submatrix method with the approximate computing paradigm to address the immanent exascale era.}}, author = {{Kühne, Thomas and Plessl, Christian and Schade, Robert and Schütt, Ole}}, booktitle = {{arXiv:2205.14741}}, title = {{{CP2K on the road to exascale}}}, year = {{2022}}, } @article{33684, author = {{Schade, Robert and Kenter, Tobias and Elgabarty, Hossam and Lass, Michael and Schütt, Ole and Lazzaro, Alfio and Pabst, Hans and Mohr, Stephan and Hutter, Jürg and Kühne, Thomas and Plessl, Christian}}, issn = {{0167-8191}}, journal = {{Parallel Computing}}, keywords = {{Artificial Intelligence, Computer Graphics and Computer-Aided Design, Computer Networks and Communications, Hardware and Architecture, Theoretical Computer Science, Software}}, publisher = {{Elsevier BV}}, title = {{{Towards electronic structure-based ab-initio molecular dynamics simulations with hundreds of millions of atoms}}}, doi = {{10.1016/j.parco.2022.102920}}, volume = {{111}}, year = {{2022}}, } @article{33687, author = {{Odziomek, Mateusz and Giusto, Paolo and Kossmann, Janina and Tarakina, Nadezda V. and Heske, Julian Joachim and Rivadeneira, Salvador M. and Keil, Waldemar and Schmidt, Claudia and Mazzanti, Stefano and Savateev, Oleksandr and Perdigón‐Toro, Lorena and Neher, Dieter and Kühne, Thomas and Antonietti, Markus and López‐Salas, Nieves}}, issn = {{0935-9648}}, journal = {{Advanced Materials}}, keywords = {{Mechanical Engineering, Mechanics of Materials, General Materials Science}}, number = {{40}}, publisher = {{Wiley}}, title = {{{“Red Carbon”: A Rediscovered Covalent Crystalline Semiconductor}}}, doi = {{10.1002/adma.202206405}}, volume = {{34}}, year = {{2022}}, } @article{21207, abstract = {{Simple thermal treatment of guanine at temperatures ranging from 600 to 700 °C leads to C1N1 condensates with unprecedented CO2/N2 selectivity when compared to other carbonaceous solid sorbents. Increasing the surface area of the CN condensates in the presence of ZnCl2 salt melts enhances the amount of CO2 adsorbed while preserving the high selectivity values and C1N1 structure. Results indicate that these new materials show a sorption mechanism a step closer to that of natural CO2 caption proteins and based on metal free structural cryptopores.}}, author = {{Kossmann, Janina and Piankova, Diana and V. Tarakina, Nadezda and Heske, Julian Joachim and Kühne, Thomas and Schmidt, Johannes and Antonietti, Markus and López-Salas, Nieves}}, issn = {{0008-6223}}, journal = {{Carbon}}, keywords = {{CN, Cryptopores, Carbon dioxide capture}}, pages = {{497--505}}, title = {{{Guanine condensates as covalent materials and the concept of cryptopores}}}, doi = {{https://doi.org/10.1016/j.carbon.2020.10.047}}, volume = {{172}}, year = {{2021}}, } @article{22220, abstract = {{Abstract Developing resource-abundant and sustainable metal-free bifunctional oxygen electrocatalysts is essential for the practical application of zinc–air batteries (ZABs). 2D black phosphorus (BP) with fully exposed atoms and active lone pair electrons can be promising for oxygen electrocatalysts, which, however, suffers from low catalytic activity and poor electrochemical stability. Herein, guided by density functional theory (DFT) calculations, an efficient metal-free electrocatalyst is demonstrated via covalently bonding BP nanosheets with graphitic carbon nitride (denoted BP-CN-c). The polarized PN covalent bonds in BP-CN-c can efficiently regulate the electron transfer from BP to graphitic carbon nitride and significantly promote the OOH* adsorption on phosphorus atoms. Impressively, the oxygen evolution reaction performance of BP-CN-c (overpotential of 350 mV at 10 mA cm−2, 90\% retention after 10 h operation) represents the state-of-the-art among the reported BP-based metal-free catalysts. Additionally, BP-CN-c exhibits a small half-wave overpotential of 390 mV for oxygen reduction reaction, representing the first bifunctional BP-based metal-free oxygen catalyst. Moreover, ZABs are assembled incorporating BP-CN-c cathodes, delivering a substantially higher peak power density (168.3 mW cm−2) than the Pt/C+RuO2-based ZABs (101.3 mW cm−2). The acquired insights into interfacial covalent bonds pave the way for the rational design of new and affordable metal-free catalysts.}}, author = {{Wang, Xia and Kormath Madam Raghupathy, Ramya and Querebillo, Christine Joy and Liao, Zhongquan and Li, Dongqi and Lin, Kui and Hantusch, Martin and Sofer, Zdeněk and Li, Baohua and Zschech, Ehrenfried and Weidinger, Inez M. and Kühne, Thomas and Mirhosseini, Hossein and Yu, Minghao and Feng, Xinliang}}, journal = {{Advanced Materials}}, keywords = {{2D materials, bifunctional oxygen electrocatalysts, black phosphorus, oxygen evolution reaction, zinc–air batteries}}, number = {{20}}, pages = {{2008752}}, title = {{{Interfacial Covalent Bonds Regulated Electron-Deficient 2D Black Phosphorus for Electrocatalytic Oxygen Reactions}}}, doi = {{https://doi.org/10.1002/adma.202008752}}, volume = {{33}}, year = {{2021}}, } @article{29700, abstract = {{We have carried out an extensive search for stable polymorphs of carbon nitride with C3N5 stoichiometry using the minima hopping method. Contrary to the widely held opinion that stacked{,} planar{,} graphite-like structures are energetically the most stable carbon nitride polymorphs for various nitrogen contents{,} we find that this does not apply for nitrogen-rich materials owing to the high abundance of N–N bonds. In fact{,} our results disclose novel morphologies with moieties not previously considered for C3N5. We demonstrate that nitrogen-rich compounds crystallize in a large variety of different structures due to particular characteristics of their energy landscapes. The newly found low-energy structures of C3N5 have band gaps within good agreement with the values measured in experimental studies.}}, author = {{Ghasemi, Alireza and Mirhosseini, Hossein and Kühne, Thomas}}, journal = {{Phys. Chem. Chem. Phys.}}, pages = {{6422--6432}}, publisher = {{The Royal Society of Chemistry}}, title = {{{Thermodynamically stable polymorphs of nitrogen-rich carbon nitrides: a C3N5 study}}}, doi = {{10.1039/D0CP06185A}}, volume = {{23}}, year = {{2021}}, } @article{33653, author = {{Gurinov, Andrei and Sieland, Benedikt and Kuzhelev, Andrey and Elgabarty, Hossam and Kühne, Thomas and Prisner, Thomas and Paradies, Jan and Baldus, Marc and Ivanov, Konstantin L. and Pylaeva, Svetlana}}, issn = {{1433-7851}}, journal = {{Angewandte Chemie International Edition}}, keywords = {{General Chemistry, Catalysis}}, number = {{28}}, pages = {{15371--15375}}, publisher = {{Wiley}}, title = {{{Mixed‐Valence Compounds as Polarizing Agents for Overhauser Dynamic Nuclear Polarization in Solids}}}, doi = {{10.1002/anie.202103215}}, volume = {{60}}, year = {{2021}}, } @article{29699, author = {{Ghasemi, S. Alireza and Kühne, Thomas D.}}, journal = {{The Journal of Chemical Physics}}, number = {{7}}, pages = {{074107}}, title = {{{Artificial neural networks for the kinetic energy functional of non-interacting fermions}}}, doi = {{10.1063/5.0037319}}, volume = {{154}}, year = {{2021}}, } @article{33587, 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 D}}, 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{33643, abstract = {{The origin of strong interactions between water molecules and porous C2N surfaces is investigated by using a combination of model materials, volumetric physisorption measurements, solid-state NMR spectroscopy, and DFT calculations.}}, author = {{Heske, Julian Joachim and Walczak, Ralf and Epping, Jan D. and Youk, Sol and Sahoo, Sudhir K. and Antonietti, Markus and Kühne, Thomas and Oschatz, Martin}}, issn = {{2050-7488}}, journal = {{Journal of Materials Chemistry A}}, keywords = {{General Materials Science, Renewable Energy, Sustainability and the Environment, General Chemistry}}, number = {{39}}, pages = {{22563--22572}}, publisher = {{Royal Society of Chemistry (RSC)}}, title = {{{When water becomes an integral part of carbon – combining theory and experiment to understand the zeolite-like water adsorption properties of porous C2N materials}}}, doi = {{10.1039/d1ta05122a}}, volume = {{9}}, year = {{2021}}, } @article{33645, abstract = {{AbstractVibrational sum-frequency generation (vSFG) spectroscopy allows the study of the structure and dynamics of interfacial systems. In the present work, we provide a simple recipe, based on a narrowband IR pump and broadband vSFG probe technique, to computationally obtain the two-dimensional vSFG spectrum of water molecules at the air–water interface. Using this technique, to study the time-dependent spectral evolution of hydrogen-bonded and free water molecules, we demonstrate that at the interface, the vibrational spectral dynamics of the free OH bond is faster than that of the bonded OH mode.}}, author = {{Ojha, Deepak and Kühne, Thomas}}, issn = {{2045-2322}}, journal = {{Scientific Reports}}, keywords = {{Multidisciplinary}}, number = {{1}}, publisher = {{Springer Science and Business Media LLC}}, title = {{{Hydrogen bond dynamics of interfacial water molecules revealed from two-dimensional vibrational sum-frequency generation spectroscopy}}}, doi = {{10.1038/s41598-021-81635-4}}, volume = {{11}}, year = {{2021}}, } @article{33644, author = {{Pylaeva, Svetlana and Marx, Patrick and Singh, Gurjot and Kühne, Thomas and Roemelt, Michael and Elgabarty, Hossam}}, issn = {{1089-5639}}, journal = {{The Journal of Physical Chemistry A}}, keywords = {{Physical and Theoretical Chemistry}}, number = {{3}}, pages = {{867--874}}, publisher = {{American Chemical Society (ACS)}}, title = {{{Organic Mixed-Valence Compounds and the Overhauser Effect in Insulating Solids}}}, doi = {{10.1021/acs.jpca.0c11296}}, volume = {{125}}, year = {{2021}}, } @article{33649, author = {{Kessler, Jan and Calcavecchia, Francesco and Kühne, Thomas}}, issn = {{2513-0390}}, journal = {{Advanced Theory and Simulations}}, keywords = {{Multidisciplinary, Modeling and Simulation, Numerical Analysis, Statistics and Probability}}, number = {{4}}, publisher = {{Wiley}}, title = {{{Artificial Neural Networks as Trial Wave Functions for Quantum Monte Carlo}}}, doi = {{10.1002/adts.202000269}}, volume = {{4}}, year = {{2021}}, } @article{33648, author = {{Ghasemi, Alireza and Kühne, Thomas}}, issn = {{0021-9606}}, journal = {{The Journal of Chemical Physics}}, keywords = {{Physical and Theoretical Chemistry, General Physics and Astronomy}}, number = {{7}}, publisher = {{AIP Publishing}}, title = {{{Artificial neural networks for the kinetic energy functional of non-interacting fermions}}}, doi = {{10.1063/5.0037319}}, volume = {{154}}, year = {{2021}}, } @article{33655, abstract = {{Abstract Dual-ion batteries are considered to be an emerging viable energy storage technology owing to their safety, high power capability, low cost, and scalability. Intercalation of anions into a graphite positive electrode provides high operating voltage and improved energy density to such dual-ion batteries. In this work, we have performed a combinatorial study of graphite intercalation compounds considering four anions, namely hexafluorophosphate (PF 6 − ), perchlorate (ClO 4 − ), bis(fluorosulfonyl)imide (FSI−), and bis(trifluoromethanesulfonyl)imide (TFSI−), via first-principles calculations. The structural properties and energetics of the intercalation compounds are compared based on different sizes, geometries, and the physical and chemical properties of the intercalated anions. The staging mechanism of anion intercalation into graphite and the specific capacities, and voltage profiles of the intercalated compounds are investigated. A comparison regarding battery electrochemistry is also done with available experimental observations. Our calculated intercalation energies and voltage profiles show that the initial anion intercalation into graphite is less favorable than subsequent ones for all the anions considered in this study. Although the effect of the size of anions in a graphite cathode on various properties of the intercalated compounds is not as significant as the size of cations in a graphite anode, some distinction between the studied anions can still be made. Among the studied anions, the intercalation compounds based on PF 6 − are the most stable ones. These PF 6 − anions cause relatively small structural deformations of the graphite and have the highest oxidative ability, highest onset voltage, and highest diffusion barrier along the graphene sheets. The overall small diffusion barriers of the anions within graphite explain the high rate capability of dual-ion batteries.}}, author = {{Chugh, Manjusha and Jain, Mitisha and Wang, Gang and Nia, Ali Shaygan and Mirhosseini, Hossein and Kühne, Thomas}}, issn = {{2053-1591}}, journal = {{Materials Research Express}}, keywords = {{Metals and Alloys, Polymers and Plastics, Surfaces, Coatings and Films, Biomaterials, Electronic, Optical and Magnetic Materials}}, number = {{8}}, publisher = {{IOP Publishing}}, title = {{{A combinatorial study of electrochemical anion intercalation into graphite}}}, doi = {{10.1088/2053-1591/ac1965}}, volume = {{8}}, year = {{2021}}, } @article{33658, abstract = {{We demonstrate how to fully ascribe Raman peaks simulated using ab initio molecular dynamics to specific vibrations in the structure at finite temperatures by means of Wannier functions. Here, we adopt our newly introduced method for the simulation of the Raman spectra in which the total polarizability of the system is expressed as a sum over Wannier polarizabilities. The assignment is then based on the calculation of partial Raman activities arising from self- and/or cross-correlations between different types of Wannier functions in the system. Different types of Wannier functions can be distinguished based on their spatial spread. To demonstrate the predictive power of this approach, we applied it to the case of a cyclohexane molecule in the gas phase and were able to fully assign the simulated Raman peaks.}}, author = {{Partovi-Azar, Pouya and Kühne, Thomas}}, issn = {{2072-666X}}, journal = {{Micromachines}}, keywords = {{Electrical and Electronic Engineering, Mechanical Engineering, Control and Systems Engineering}}, number = {{10}}, publisher = {{MDPI AG}}, title = {{{Full Assignment of Ab-Initio Raman Spectra at Finite Temperatures Using Wannier Polarizabilities: Application to Cyclohexane Molecule in Gas Phase}}}, doi = {{10.3390/mi12101212}}, volume = {{12}}, year = {{2021}}, } @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}}, }