Article
Chemistry, Physical
Denis Mashkovtsev, Yuuichi Orimoto, Yuriko Aoki
Summary: The local excitation approximation (LEA) method for localized electronic excitations in a specific region of a molecule has been improved with new approaches to enhance accuracy. The LEA involves isolating the region of interest as a submolecule and calculating electronic excitations within this submolecule. This study examined approaches to improve accuracy in describing the region of interest and accelerated calculations using a new projection technique.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Chemistry, Physical
Sharity Morales-Meza, Maria E. Sanchez-Castro, Marisol Ibarra-Rodriguez, Mario Sanchez
Summary: The study investigated the adsorption energies of Pentalene and alkali elements on hydrogen molecules, demonstrating varying capacities among different complexes. Temperature was found to influence the adsorption process as well.
CHEMICAL PHYSICS LETTERS
(2022)
Article
Chemistry, Physical
Amir Karton, Bun Chan
Summary: We obtained CCSD(T) isomerization energies for 335 polycyclic aromatic hydrocarbons using the G4(MP2) thermochemical protocol. We utilized this extensive and diverse dataset to identify predictive indicators for energetic instability and evaluate the performance of DFT and semiempirical methods. Our findings suggest that dipole moments above 1.0 D, HOMO-LUMO gaps below 2.0 eV, and qneg,avg values below -0.06 e are indicative of energetic instability. Surprisingly, the local density approximation SVWN5 method achieved a mean absolute deviation (MAD) of only 3.8 kJ/mol, outperforming many higher-level functionals from Jacob's Ladder. The best performer was PBE0-D4 with a MAD of 2.8 kJ/mol.
CHEMICAL PHYSICS LETTERS
(2023)
Article
Astronomy & Astrophysics
Kun Xu, Yipeng Jing
Summary: The algorithm proposed is a two-dimensional particle-particle-particle-mesh ((PM)-M-3) algorithm with an optimized Green's function and adaptive softening length for gravitational lensing studies in N-body simulations. The analytical form of the optimized Green's function (G) over cap (k) is also presented.
ASTROPHYSICAL JOURNAL
(2021)
Article
Multidisciplinary Sciences
Simon Batzner, Albert Musaelian, Lixin Sun, Mario Geiger, Jonathan P. Mailoa, Mordechai Kornbluth, Nicola Molinari, Tess E. Smidt, Boris Kozinsky
Summary: This paper introduces an E(3)-equivariant deep learning method for accelerating molecular dynamics simulations. The method shows state-of-the-art accuracy and remarkable sample efficiency in faithfully describing the dynamics of complex systems. The Neural Equivariant Interatomic Potentials (NequIP) approach employs E(3)-equivariant convolutions to interact with geometric tensors, resulting in a more information-rich and faithful representation of atomic environments. NequIP outperforms existing models with significantly fewer training data, challenging the commonly held belief about the necessity of massive training sets for deep neural networks.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Physical
Jiashu Liang, Zhe Wang, Jie Li, Jonathan Wong, Xiao Liu, Brad Ganoe, Teresa Head-Gordon, Martin Head-Gordon
Summary: This paper presents a systematic study on the use of composite method approximations with locally dense basis sets (LDBS) for efficient calculation of NMR shielding constants in small and medium-sized molecules. The pcSseg-n basis sets are found to have similar accuracy to the pcS-n basis sets and can slightly reduce computational costs. Two effective LDBS partition schemes for density functional calculations are identified. A large subset of the NS372 database is selected for assessment, covering a range of conventional electronic structure methods and composite approaches, with and without LDBS.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Chemistry, Physical
Haiyuan Wang, Alexey Tal, Thomas Bischoff, Patrick Gono, Alfredo Pasquarello
Summary: We develop a computationally efficient scheme to accurately determine finite-temperature band gaps for metal halide perovskites. Our scheme improves the accuracy of band gaps by considering spin-orbit coupling and thermal vibrations, and is convenient for large-scale screenings of metal halide perovskite databases.
NPJ COMPUTATIONAL MATERIALS
(2022)
Article
Chemistry, Physical
A. J. C. Varandas
Summary: This paper introduces the concept of partially hydrogenated graphenes as planar infinite benzenes and discusses their growth paths from benzene or coronene to graphene. The difficulty in performing ab initio calculations for large molecules is emphasized, and the use of MINI basis sets in probe calculations is justified. The 'attitudinal-green' approach advocated in this paper contrasts with the brute-force ('attitudinal-red') method.
CHEMICAL PHYSICS LETTERS
(2023)
Article
Chemistry, Physical
Leandro Ramos Marques, Romulo Augusto Ando
Summary: This study provides evidence of weak intermolecular interactions between Lewis acids and Lewis bases by probing fluorine-carbon vibrational modes using infrared spectroscopy, distinguishing the Lewis adduct from FLPs.
Article
Biochemistry & Molecular Biology
Jiri Czernek, Jiri Brus, Vladimira Czernekova
Summary: There is a growing interest in quantitatively predicting the intermolecular binding energy of large complexes. The domain-based local pair natural orbital (DLPNO) scheme is an important quantum chemical technique that can be used for such predictions. In this study, a DLPNO-based focal-point method is developed to obtain values that are close to the canonical CCSD(T)/CBS counterparts, allowing for routine checking of less expensive computational methods.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2022)
Article
Chemistry, Physical
Luke W. Bertels, Joonho Lee, Martin Head-Gordon
Summary: The use of non-HF or kappa-OOMP2 molecular orbitals can improve the performance of CCSD(T) on open-shell systems, especially in calculating harmonic vibrational frequencies. CCSD(T) with B97, kappa-OOMP2, or B97M-rV orbitals as reference orbitals outperform CCSD(T) with UHF, with comparable accuracy and robustness in treating both open-shell and closed-shell systems.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2021)
Review
Chemistry, Applied
Jinghao Zhang, Fangwei Li, Suxia Shen, Zhaotian Yang, Xingyu Ji, Xiao Wang, Xiaojun Liao, Yan Zhang
Summary: The investigation of intermolecular interactions is increasingly important, using analytical approaches such as spectroscopy and molecular simulation techniques to understand the molecular mechanisms involved. These advancements have the potential to revolutionize the future of food research by allowing for the design of new foods with precise nutrition and desired properties.
Article
Chemistry, Multidisciplinary
Rizwan Nabi, Jakob K. Staab, Andrea Mattioni, Jon G. C. Kragskow, Daniel Reta, Jonathan M. Skelton, Nicholas F. Chilton
Summary: Molecular materials are important for the development of optoelectronic and quantum technologies, and the study of spin-phonon coupling is crucial for understanding energy transfer processes and spin dynamics. Ab initio methods can accurately calculate spin-phonon coupling and spin dynamics in molecular solids, as demonstrated in this study.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Oscar N. Ventura, Martina Kieninger, Aline Katz, Mauricio Vega-Teijido, Marc Segovia, Kenneth Irving
Summary: A simplified composite scheme proposed in this study showed promising results when benchmarked against other reaction databases, demonstrating better accuracy and efficiency compared to traditional methods.
INTERNATIONAL JOURNAL OF QUANTUM CHEMISTRY
(2021)
Article
Computer Science, Information Systems
Xinyan Zhang, Peng Gao, Sunxiangyu Liu, Kongya Zhao, Guitao Li, Liuguo Yin, Chang Wen Chen
Summary: The study introduces a global-local adjusting dense super-resolution network (GLADSR) to improve image super-resolution performance while reducing parameters and computational cost, using a global-local adjusting module (GLAM) and a separable pyramid upsampling (SPU) module. Extensive experiments demonstrate the superiority of GLADSR over state-of-the-art methods with less parameters and lower computational cost.
IEEE TRANSACTIONS ON MULTIMEDIA
(2021)
Article
Chemistry, Multidisciplinary
David Kuhness, Hyun Jin Yang, Hagen W. Klemm, Mauricio Prieto, Gina Peschel, Alexander Fuhrich, Dietrich Menzel, Thomas Schmidt, Xin Yu, Shamil Shaikhutdinov, Adrian Lewandowski, Markus Heyde, Anna Kelemen, Radoslaw Wlodarczyk, Denis Usvyat, Martin Schuetz, Joachim Sauer, Hans-Joachim Freund
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2018)
Article
Chemistry, Physical
Daniel Kats, Denis Usvyat, Frederick R. Manby
Article
Chemistry, Multidisciplinary
Giuseppe Sansone, Antti J. Karttunen, Denis Usvyat, Martin Schuetz, Jan Gerit Brandenburg, Lorenzo Maschio
CHEMICAL COMMUNICATIONS
(2018)
Article
Chemistry, Physical
Maristella Alessio, Denis Usvyat, Joachim Sauer
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2019)
Article
Chemistry, Physical
Sophia Heiden, Denis Usvyat, Peter Saalfrank
JOURNAL OF PHYSICAL CHEMISTRY C
(2019)
Article
Chemistry, Multidisciplinary
Mikhail S. Kuklin, Lorenzo Maschio, Denis Usvyat, Florian Kraus, Antti J. Karttunen
CHEMISTRY-A EUROPEAN JOURNAL
(2019)
Article
Chemistry, Physical
J. Fischer, F. Schlaghaufer, E. -M. Lottner, A. Slenczka, L. Christiansen, H. Stapelfeldt, M. Karra, B. Friedrich, Th. Mullan, M. Schuetz, D. Usvyat
JOURNAL OF PHYSICAL CHEMISTRY A
(2019)
Review
Chemistry, Multidisciplinary
Adrian Leandro Lewandowski, Sergio Tosoni, Leonard Gura, Zechao Yang, Alexander Fuhrich, Mauricio J. Prieto, Thomas Schmidt, Denis Usvyat, Wolf-Dieter Schneider, Markus Heyde, Gianfranco Pacchioni, Hans-Joachim Freund
Summary: The review focuses on the preparation and atomic-scale characterization of the thinnest films of silica and germania, using advanced surface science techniques and density functional theory calculations. Comparisons of monolayer, zigzag phase, and bilayer films on different metal supports provide insights into the network structure of glass forming materials, highlighting the crucial role of metal support in the pathway from crystalline to amorphous ultrathin film growth.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Physical
Hung-Hsuan Lin, Lorenzo Maschio, Daniel Kats, Denis Usvyat, Thomas Heine
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2020)
Article
Chemistry, Physical
Ji Chen, Nikolay A. Bogdanov, Denis Usvyat, Wei Fang, Angelos Michaelides, Ali Alavi
JOURNAL OF CHEMICAL PHYSICS
(2020)
Article
Chemistry, Multidisciplinary
N. Frank, I. Pryjomska-Ray, L. Grubert, S. Hecht, D. Usvyat, C. Limberg
Summary: This study investigated the successive reactions of p-tert-butyltetramercaptotetrathiacalix[4]arene with gold(I) phosphine units, leading to the preparation of various complexes with multiple [(PR3)Au](+) moieties. It was found that four gold atoms organized by the coordination platform of the calix[4]arene are able to bind and stabilize other metal entities, such as TlCl, through strong metallophilic interactions, resulting in photoluminescence at low temperatures.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Multidisciplinary
Mauricio J. Prieto, Thomas Mullan, Mark Schlutow, Daniel M. Gottlob, Liviu C. Tanase, Dietrich Menzel, Joachim Sauer, Denis Usvyat, Thomas Schmidt, Hans-Joachim Freund
Summary: The study investigates how physical confinement affects the water formation reaction using a model system, revealing that the rate-determining step remains unchanged in confinement, ruling out the transition state effect. Numerical simulations suggest that the H-2 adsorption process plays a decisive role in reproducing the reaction rate.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Physical
Thomas Mullan, Lorenzo Maschio, Peter Saalfrank, Denis Usvyat
Summary: The quest for chemical accuracy in the field of structure and kinetics of molecules at solid surfaces is examined in this paper, using the example of the barrier for hydrogen diffusion on an alpha-Al2O3 (0001) surface. The barrier is evaluated using density functional theory (DFT) and compared to barriers obtained from other methods. The possible sources of errors are analyzed and corrections to these errors are proposed.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Evelin Martine Christlmaier, Daniel Kats, Ali Alavi, Denis Usvyat
Summary: In this study, an embedded fragment approach for high-level quantum chemical calculations on local features in periodic systems is presented. The approach utilizes localized orbitals from a converged periodic Hartree-Fock solution as the basis for post-Hartree-Fock treatment. The embedding field, including the Coulomb and exchange potential from the crystal, is included in the fragment's Hamiltonian. The approach is applied to investigate the performance of FCIQMC with adaptive shift, providing accurate dissociation and total energies even for large active spaces.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Multidisciplinary Sciences
Thomas Merz, Genaro Bierhance, Ernst-Christian Flach, Daniel Kats, Denis Usvyat, Martin Schutz
Summary: The theoretical treatment of molecules in electronically excited states is more complex than in the ground state, requiring multireference methods or time-dependent response methods. These methods can be used to theoretically investigate photoreactions.
PHYSICAL SCIENCES REVIEWS
(2021)