@article{53474, abstract = {{We present a novel approach to characterize and quantify microheterogeneity and microphase separation in computer simulations of complex liquid mixtures. Our post-processing method is based on local density fluctuations of the different constituents in sampling spheres of varying size. It can be easily applied to both molecular dynamics (MD) and Monte Carlo (MC) simulations, including periodic boundary conditions. Multidimensional correlation of the density distributions yields a clear picture of the domain formation due to the subtle balance of different interactions. We apply our approach to the example of force field molecular dynamics simulations of imidazolium-based ionic liquids with different side chain lengths at different temperatures, namely 1-ethyl-3-methylimidazolium chloride, 1-hexyl-3-methylimidazolium chloride, and 1-decyl-3-methylimidazolium chloride, which are known to form distinct liquid domains. We put the results into the context of existing microheterogeneity analyses and demonstrate the advantages and sensitivity of our novel method. Furthermore, we show how to estimate the configuration entropy from our analysis, and we investigate voids in the system. The analysis has been implemented into our program package TRAVIS and is thus available as free software.}}, author = {{Lass, Michael and Kenter, Tobias and Plessl, Christian and Brehm, Martin}}, issn = {{1099-4300}}, journal = {{Entropy}}, number = {{4}}, publisher = {{MDPI AG}}, title = {{{Characterizing Microheterogeneity in Liquid Mixtures via Local Density Fluctuations}}}, doi = {{10.3390/e26040322}}, volume = {{26}}, year = {{2024}}, } @article{45013, author = {{Codescu, M.-A. and Kunze, T. and Weiß, M. and Brehm, Martin and Kornilov, O. and Sebastiani, D. and Nibbering, E. T. J.}}, journal = {{J. Phys. Chem. Lett.}}, pages = {{4775--4785}}, title = {{{Ultrafast Proton Transfer Pathways Mediated by Amphoteric Imidazole}}}, doi = {{10.1021/acs.jpclett.3c00595}}, volume = {{14}}, year = {{2023}}, } @article{45012, author = {{Roos, E. and Sebastiani, D. and Brehm, Martin}}, journal = {{Phys. Chem. Chem. Phys.}}, pages = {{8755--8766}}, title = {{{A Force Field for Bio-Polymers in Ionic Liquids (BILFF) – Part 2: Cellulose in [EMIm][OAc] / Water Mixtures}}}, doi = {{10.1039/D2CP05636D}}, volume = {{25 (12)}}, year = {{2023}}, } @article{45011, author = {{Radicke, J. and Roos, E. and Sebastiani, D. and Brehm, Martin and Kressler, J.}}, journal = {{J. Polym. Sci.}}, pages = {{372--384}}, title = {{{Lactate-Based Ionic Liquids as Chiral Solvents for Cellulose}}}, doi = {{10.1002/pol.20220687}}, volume = {{61 (5)}}, year = {{2023}}, } @article{33679, author = {{Zhang, Ruiming and Ruan, Wei and Yu, Junyao and Gao, Libo and Berger, Helmuth and Forró, László and Watanabe, Kenji and Taniguchi, Takashi and Ranjbar, Ahmad and Belosludov, Rodion V. and Kühne, Thomas and Bahramy, Mohammad Saeed and Xi, Xiaoxiang}}, issn = {{2469-9950}}, journal = {{Physical Review B}}, number = {{8}}, publisher = {{American Physical Society (APS)}}, title = {{{Second-harmonic generation in atomically thin 1T−TiSe2 and its possible origin from charge density wave transitions}}}, doi = {{10.1103/physrevb.105.085409}}, volume = {{105}}, year = {{2022}}, } @article{33682, author = {{Khazaei, Mohammad and Ranjbar, Ahmad and Kang, Yoon‐Gu and Liang, Yunye and Khaledialidusti, Rasoul and Bae, Soungmin and Raebiger, Hannes and Wang, Vei and Han, Myung Joon and Mizoguchi, Hiroshi and Bahramy, Mohammad S. and Kühne, Thomas and Belosludov, Rodion V. and Ohno, Kaoru and Hosono, Hideo}}, issn = {{1616-301X}}, journal = {{Advanced Functional Materials}}, keywords = {{Electrochemistry, Condensed Matter Physics, Biomaterials, Electronic, Optical and Magnetic Materials}}, number = {{20}}, publisher = {{Wiley}}, title = {{{Electronic Structures of Group III–V Element Haeckelite Compounds: A Novel Family of Semiconductors, Dirac Semimetals, and Topological Insulators}}}, doi = {{10.1002/adfm.202110930}}, volume = {{32}}, year = {{2022}}, } @article{33676, author = {{Schulze Lammers, Bertram and López-Salas, Nieves and Stein Siena, Julya and Mirhosseini, Hossein and Yesilpinar, Damla and Heske, Julian Joachim and Kühne, Thomas and Fuchs, Harald and Antonietti, Markus and Mönig, Harry}}, issn = {{1936-0851}}, journal = {{ACS Nano}}, keywords = {{General Physics and Astronomy, General Engineering, General Materials Science}}, number = {{9}}, pages = {{14284--14296}}, publisher = {{American Chemical Society (ACS)}}, title = {{{Real-Space Identification of Non-Noble Single Atomic Catalytic Sites within Metal-Coordinated Supramolecular Networks}}}, doi = {{10.1021/acsnano.2c04439}}, volume = {{16}}, year = {{2022}}, } @unpublished{33678, abstract = {{Accelerated chemistry at the interface with water has received increasing attention. The mechanisms behind the enhanced reactivity On-Water are not yet clear. In this work we use a Langevin scheme in the spirit of second generation Car-Parrinello to accelerate the second-order density functional Tight-Binding (DFTB2) method in order to investigate the free energy of two Diels-Alder reaction On-Water: the cycloaddition between cyclopentadiene and ethyl cinnamate or thionocinnamate. The only difference between the reactants is the substitution of a carbonyl oxygen for a thiocarbonyl sulfur, making possible the distinction between them as strong and weak hydrogen-bond acceptors. We find a different mechanism for the reaction during the transition states and uncover the role of hydrogen bonds along with the reaction path. Our results suggest that acceleration of Diels-Alder reactions do not arise from an increased number of hydrogen bonds at the transition state and charge transfer plays a significant role. However, the presence of water and hydrogen-bonds is determinant for the catalysis of these reactions.}}, author = {{Henao Aristizabal, Andres and Gohar, Yomna and Whilhelm, René and Kühne, Thomas}}, publisher = {{American Chemical Society (ACS)}}, title = {{{On the Role of Hydrogen Bond Strength and Charge Transfer of a Diels-Alder Reaction On-Water: Semiempirical and Free Energy Calculations.}}}, year = {{2022}}, } @article{33680, author = {{Khajehpasha, Ehsan Rahmatizad and Finkler, Jonas A. and Kühne, Thomas and Ghasemi, Alireza}}, issn = {{2469-9950}}, journal = {{Physical Review B}}, number = {{14}}, publisher = {{American Physical Society (APS)}}, title = {{{CENT2: Improved charge equilibration via neural network technique}}}, doi = {{10.1103/physrevb.105.144106}}, volume = {{105}}, year = {{2022}}, } @article{33686, author = {{Elizabeth, Amala and Sahoo, Sudhir K. and Phirke, Himanshu and Kodalle, Tim and Kühne, Thomas and Audinot, Jean-Nicolas and Wirtz, Tom and Redinger, Alex and Kaufmann, Christian A. and Mirhosseini, Hossein and Mönig, Harry}}, issn = {{1944-8244}}, journal = {{ACS Applied Materials & Interfaces}}, keywords = {{General Materials Science}}, number = {{29}}, pages = {{34101--34112}}, publisher = {{American Chemical Society (ACS)}}, title = {{{Surface Passivation and Detrimental Heat-Induced Diffusion Effects in RbF-Treated Cu(In,Ga)Se2 Solar Cell Absorbers}}}, doi = {{10.1021/acsami.2c08257}}, volume = {{14}}, year = {{2022}}, } @article{33689, author = {{Raghuwanshi, Mohit and Chugh, Manjusha and Sozzi, Giovanna and Kanevce, Ana and Kühne, Thomas and Mirhosseini, Hossein and Wuerz, Roland and Cojocaru‐Mirédin, Oana}}, issn = {{0935-9648}}, journal = {{Advanced Materials}}, keywords = {{Mechanical Engineering, Mechanics of Materials, General Materials Science}}, number = {{37}}, publisher = {{Wiley}}, title = {{{Fingerprints Indicating Superior Properties of Internal Interfaces in Cu(In,Ga)Se 2 Thin‐Film Solar Cells}}}, doi = {{10.1002/adma.202203954}}, volume = {{34}}, year = {{2022}}, } @article{33690, author = {{Ibaceta-Jaña, Josefa and Chugh, Manjusha and Novikov, Alexander S. and Mirhosseini, Hossein and Kühne, Thomas and Szyszka, Bernd and Wagner, Markus R. and Muydinov, Ruslan}}, 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 = {{38}}, pages = {{16215--16226}}, publisher = {{American Chemical Society (ACS)}}, title = {{{Do Lead Halide Hybrid Perovskites Have Hydrogen Bonds?}}}, doi = {{10.1021/acs.jpcc.2c02984}}, volume = {{126}}, year = {{2022}}, } @article{33683, author = {{Lepre, Enrico and Heske, Julian Joachim and Nowakowski, Michal and Scoppola, Ernesto and Zizak, Ivo and Heil, Tobias and Kühne, Thomas and Antonietti, Markus and López-Salas, Nieves and Albero, Josep}}, issn = {{2211-2855}}, journal = {{Nano Energy}}, keywords = {{Electrical and Electronic Engineering, General Materials Science, Renewable Energy, Sustainability and the Environment}}, publisher = {{Elsevier BV}}, title = {{{Ni-based electrocatalysts for unconventional CO2 reduction reaction to formic acid}}}, doi = {{10.1016/j.nanoen.2022.107191}}, volume = {{97}}, year = {{2022}}, } @misc{33688, author = {{Balos, Vasileios and Kaliannan, Naveen Kumar and Elgabarty, Hossam and Wolf, Martin and Kühne, Thomas and Sajadi, Mohsen}}, publisher = {{LibreCat University}}, title = {{{Time resolved THz-Raman spectroscopy reveals that cations and anions distinctly modify intermolecular interactions of water}}}, doi = {{10.5281/ZENODO.6514905}}, year = {{2022}}, } @article{33691, abstract = {{Near ambient pressure XPS in nitrogen atmosphere was utilized to investigate gas-solid interactions within porous SiO2 films ranging from 30 to 75 nm thickness. The films were differentiated in terms of porosity and roughness. The XPS N1s core levels of the N2 gas in presence of the SiO2 samples showed variations in width, binding energy and line shape. The width correlated with the surface charge induced in the dielectric films upon X-ray irradiation. The observed different binding energies observed for the N1s peak can only partly be associated with intrinsic work function differences between the samples, opening the possibility that the effect of physisorption at room temperature could be detected by a shift in the measured binding energy. However, the signals also show an increasing asymmetry with rising surface charge. This might be associated with the formation of vertical electrical gradients within the dielectric porous thin films, which complicates the assignment of binding energy positions to specific surface-related effects. With the support of Monte Carlo and first principles density functional theory calculations, the observed shifts were discussed in terms of the possible formation of transitory dipoles upon N2 physisorption within the porous SiO2 films.}}, author = {{de los Arcos, Teresa and Weinberger, Christian and Zysk, Frederik and Raj Damerla, Varun and Kollmann, Sabrina and Vieth, Pascal and Tiemann, Michael and Kühne, Thomas and Grundmeier, Guido}}, issn = {{0169-4332}}, journal = {{Applied Surface Science}}, keywords = {{Surfaces, Coatings and Films, Condensed Matter Physics, Surfaces and Interfaces, General Physics and Astronomy, General Chemistry}}, publisher = {{Elsevier BV}}, title = {{{Challenges in the interpretation of gas core levels for the determination of gas-solid interactions within dielectric porous films by ambient pressure XPS}}}, doi = {{10.1016/j.apsusc.2022.154525}}, volume = {{604}}, year = {{2022}}, } @article{33685, abstract = {{In the spatial confinement of cylindrical mesopores with diameters of a few nanometers, water molecules experience restrictions in hydrogen bonding. This leads to a different behavior regarding the molecular orientational freedom (‘structure of water') compared to the bulk liquid state. In addition to the pore size, the behavior is also strongly affected by the strength of the pore wall-to-water interactions, that is, the pore wall polarity. In this work, this is studied both experimentally and theoretically. The surface polarity of mesoporous silica (SiO2) is modified by functionalization with trimethylsilyl moieties, resulting in a change from a hydrophilic (pristine) to a hydrophobic pore wall. The mesopore surface is characterized by N2 and H2O sorption experiments. Those results are combined with IR spectroscopy to investigate pore wall-to-water interactions leading to different structures of water in the mesopore. Furthermore, the water's structure is studied theoretically to gain deeper insight into the interfacial interactions. For this purpose, the structure of water is analyzed by pairing densities, coordination, and angular distributions with a novel adaptation of surface-specific sum-frequency generation calculation for pore environments.}}, author = {{Weinberger, Christian and Zysk, Frederik and Hartmann, Marc and Kaliannan, Naveen and Keil, Waldemar and Kühne, Thomas and Tiemann, Michael}}, issn = {{2196-7350}}, journal = {{Advanced Materials Interfaces}}, keywords = {{Mechanical Engineering, Mechanics of Materials}}, number = {{20}}, publisher = {{Wiley}}, title = {{{The Structure of Water in Silica Mesopores – Influence of the Pore Wall Polarity}}}, doi = {{10.1002/admi.202200245}}, volume = {{9}}, year = {{2022}}, } @article{45007, author = {{Yang, Y. and Cheramy, J. and Brehm, Martin and Xu, Y.}}, journal = {{ChemPhysChem}}, pages = {{e202200161}}, title = {{{Raman Optical Activity of N-Acetyl-L-Cysteine in Water and in Methanol: The “Clusters-in-a-Liquid” Model and ab initio Molecular Dynamics Simulations}}}, doi = {{10.1002/cphc.202200161}}, volume = {{23 (11)}}, year = {{2022}}, } @article{45010, author = {{Chahal, R. and Roy, S. and Brehm, Martin and Banerjee, S. and Bryantsev, V. and Lam, S.}}, journal = {{JACS Au}}, pages = {{2693--2702}}, title = {{{Transferable Deep Learning Potential Reveals Intermediate-Range Ordering Effects in LiF–NaF–ZrF4 Molten Salt}}}, doi = {{10.1021/jacsau.2c00526}}, volume = {{2 (12)}}, year = {{2022}}, } @article{45008, author = {{Taherivardanjani, S. and Blasius, J. and Brehm, Martin and Dötzer, R. and Kirchner, B.}}, journal = {{J. Phys. Chem. A}}, pages = {{7070--7083}}, title = {{{Conformer Weighting and Differently Sized Cluster Weighting for Nicotine and its Phosphorus Derivatives}}}, doi = {{10.1021/acs.jpca.2c03133}}, volume = {{126 (40)}}, year = {{2022}}, } @article{45009, author = {{Frömbgen, T. and Blasius, J. and Alizadeh, V. and Chaumont, A. and Brehm, Martin and Kirchner, B.}}, journal = {{J. Chem. Inf. Model.}}, pages = {{5634--5644}}, title = {{{Cluster Analysis in Liquids: A Novel Tool in TRAVIS}}}, doi = {{10.1021/acs.jcim.2c01244}}, volume = {{62 (22)}}, year = {{2022}}, }