Article
Chemistry, Physical
Dustin R. Broderick, John M. Herbert
Summary: The many-body expansion is a method used to calculate electronic structure in large systems. This study presents an algorithm to overcome the combinatorial bottleneck in many-body expansion and implements it in a software application called Fragment. The results show that this method allows for unprecedentedly large-scale calculations with high accuracy.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Alexander E. Doran, So Hirata
Summary: A scalable stochastic algorithm for evaluating fourth-order many-body perturbation (MP4) correction to energy has been proposed. The algorithm involves computer-generated diagrams and algebraic formulas expressed in terms of Green's functions, and is evaluated using Monte Carlo integration accelerated by redundant walker and control variate algorithms. The resulting MC-MP4 method is efficiently parallelized with significantly lower cost dependence compared to deterministic MP4 algorithm. It has been shown to accurately evaluate the energy of various molecules with a statistical uncertainty within a certain range after a large number of Monte Carlo steps.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Chemistry, Multidisciplinary
David Abella, Giancarlo Franzese, Javier Hernandez-Rojas
Summary: Many-body interactions in water are important and difficult to treat in atomistic models. Polarizable models explicitly include these interactions but are computationally expensive. We evaluated the relevance of different coordination shells in these interactions and found that including the first coordination shell approximates the global energy minimum within 5%. This result holds for three different polarizable models, suggesting a strategy for developing reliable and computationally efficient many-body potentials for water.
Article
Computer Science, Interdisciplinary Applications
P. Arthuis, A. Tichai, J. Ripoche, T. Duguet
Summary: The second version of the code ADG automates the generation and evaluation of valid off-diagonal Bogoliubov many-body perturbation theory diagrams. It can handle Hamiltonians with both two-body and three-body interactions, and utilizes algebraic Feynman's rules and diagrammatic rules for evaluation. The program has been optimized for efficiency and moved to Python3, while still supporting Python2.
COMPUTER PHYSICS COMMUNICATIONS
(2021)
Article
Materials Science, Multidisciplinary
Kevin Hemery, Frank Pollmann, Adam Smith
Summary: We introduce techniques for analyzing the structure of many-body localized spin chains and validate the method through studying MBL transitions and many-body dynamics. The techniques are computationally inexpensive and easily accessible in experimental settings.
Article
Chemistry, Physical
Pier Paolo Poier, Theo Jaffrelot Inizan, Olivier Adjoua, Louis Lagardere, Jean-Philip Piquemal
Summary: Using a deep neuronal network (DNN) model trained on a large data set, researchers propose a transferable density-free many-body dispersion (DNN-MBD) model. The DNN-MBD model bypasses explicit density partitioning and achieves comparable accuracy to other approaches. It reduces computational cost and can be coupled with other models for large-scale calculations.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Physical
Amiel S. P. Paz, William J. Glover
Summary: The study investigates the convergence of the many-body expansion for a prototypical hole-transfer reaction between Zn(0) and Zn(I) in a condensed-phase environment. By using a charge-localized representation of the electronic Hamiltonian, a diabatic many-body expansion method is introduced for ground- and excited-state potential energy surfaces of a charge-transfer reaction. This approach, combined with a multiconfigurational self-consistent field, provides a fragmentation method that scales quadratically with system size while maintaining chemical accuracy compared to full system calculations.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2021)
Article
Chemistry, Physical
Soumen Ghosh, Frank Neese, Robert Izsak, Giovanni Bistoni
Summary: The paper introduces a fragment-based local coupled cluster embedding approach, combining many-body expansion and local energy decomposition, for accurate quantification and analysis of noncovalent interactions in molecular aggregates. Two different methods are introduced to handle the impact of the environment on the total energy of the system and noncovalent interactions.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2021)
Article
Spectroscopy
Sumalya Kaluva, Venkata Lakshmi Karri, Bhagwat Kharat, Mahadevappa Naganathappa
Summary: The present study investigates the analysis and characterization of linear and cyclic diazene oligomers in gas and water solvent states. Spectroscopic techniques such as geometrical parameters, infrared spectra, electronic absorption spectra, and natural transition orbitals (NTOs) are used to study these oligomers. Many-body analysis techniques are implemented to examine the interactions among the diazene oligomers using B3LYP exchange and correlation functional and 6-311++G (d,p) basis set. Significant changes in vibrational modes are observed when transitioning from gas phase to water solvent phase. The electronic absorption spectra, wavelength of electronic transitions, oscillator strength, and HOMO to LUMO gap are calculated using time-dependent density functional theory (TD-DFT).
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
(2023)
Article
Chemistry, Physical
Kristina M. Herman, Joseph P. Heindel, Sotiris S. Xantheas
Summary: The study conducted a Many Body Energy analysis on the influence of ions at different positions in the Hofmeister series on water molecule interactions, revealing significant differences between kosmotropic and chaotropic ions. Kosmotropic ions dominate with ion-water interactions leading to unfavorable water-water interactions, while chaotropic ions converge more closely to pure water clusters with weaker overall binding energies and ion-water interactions.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2021)
Article
Chemistry, Physical
Janine Hellmers, Carolin Koenig
Summary: A flexible formulation for energy-based molecular fragmentation schemes has been introduced, which can incorporate existing and novel fragmentation expansions. The application of this framework in multi-level approaches and electronic interaction energies has been illustrated, showing its ability to generate well-suited multi-level fragmentation expansions for different cases. The study successfully reproduces electronic protein-protein interaction energies with high accuracy for various structures.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Chemistry, Physical
Viki Kumar Prasad, Alberto Otero-de-la-Roza, Gino A. DiLabio
Summary: In this study, a new low-cost quantum mechanical method using atom-centered potentials (ACPs) was developed to model large molecular systems. Machine learning regression technique was utilized to train and validate the ACP-corrected methods. The proposed ACP-corrected methods showed comparable performance to complete basis set density functional theory at a much lower cost, and could improve the description of covalent and noncovalent bond geometries.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2022)
Article
Physics, Multidisciplinary
Hyunsoo Ha, Alan Morningstar, David A. Huse
Summary: Many-body localized (MBL) systems cannot reach thermal equilibrium under their own dynamics, even though they are interacting, nonintegrable, and in an extensively excited state. One instability toward thermalization of MBL systems is the avalanche, where a locally thermalizing rare region is able to spread thermalization through the full system. We find a detailed connection between many-body resonances and avalanches in MBL systems.
PHYSICAL REVIEW LETTERS
(2023)
Article
Physics, Nuclear
Theodore Depastas, George A. Souliotis, Demeter Tzeli, Sotiris S. Xantheas
Summary: This study extends the many-body expansion (MBE) to the light nuclear systems 3H and 3He, considering the nucleonic degrees of freedom. The total energy of the 2H nucleus is calculated using the Pauli nucleonic dynamics (PND) model and is found to be in good agreement with the experimental value. The application of MBE yields results for the three-body term in the 3H nucleus comparable with previous estimates, and for the first time for the 3He nucleus.
Article
Chemistry, Physical
Shweta Jindal, Po-Jen Hsu, Huu Trong Phan, Pei-Kang Tsou, Jer-Lai Kuo
Summary: This study proposes a new method that utilizes a database of stable conformers and borrows the fragmentation concept of many-body expansion (MBE) methods in ab initio methods to train a deep-learning machine learning (ML) model using SchNet. This method allows for accurate exploration of the structure and properties of molecular clusters with the accuracy of first-principles methods and the computational speed of empirical force-fields.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
DeCarlos E. Taylor, Janos G. Angyan, Giulia Galli, Cui Zhang, Francois Gygi, Kimihiko Hirao, Jong Won Song, Kar Rahul, O. Anatole von Lilienfeld, Rafat Podeszwa, Ireneusz W. Bulik, Thomas M. Henderson, Gustavo E. Scuseria, Julien Toulouse, Roberto Peverati, Donald G. Truhlar, Krzysztof Szalewicz
JOURNAL OF CHEMICAL PHYSICS
(2016)
Article
Chemistry, Multidisciplinary
Anthony M. Reilly, Richard I. Cooper, Claire S. Adjiman, Saswata Bhattacharya, A. Daniel Boese, Jan Gerit Brandenburg, Peter J. Bygrave, Rita Bylsma, Josh E. Campbell, Roberto Car, David H. Case, Renu Chadha, Jason C. Cole, Katherine Cosburn, Herma M. Cuppen, Farren Curtis, Graeme M. Day, Robert A. DiStasio, Alexander Dzyabchenko, Bouke P. van Eijck, Dennis M. Elking, Joost A. van den Ende, Julio C. Facelli, Marta B. Ferraro, Laszlo Fusti-Molnar, Christina-Anna Gatsiou, Thomas S. Gee, Rene de Gelder, Luca M. Ghiringhelli, Hitoshi Goto, Stefan Grimme, Rui Guo, Detlef W. M. Hofmann, Johannes Hoja, Rebecca K. Hylton, Luca Iuzzolino, Wojciech Jankiewicz, Daniel T. de Jong, John Kendrick, Niek J. J. de Klerk, Hsin-Yu Ko, Liudmila N. Kuleshova, Xiayue Li, Sanjaya Lohani, Frank J. J. Leusen, Albert M. Lund, Jian Lv, Yanming Ma, Noa Marom, Artem E. Masunov, Patrick McCabe, David P. McMahon, Hugo Meekes, Michael P. Metz, Alston J. Misquitta, Sharmarke Mohamed, Bartomeu Monserrat, Richard J. Needs, Marcus A. Neumann, Jonas Nyman, Shigeaki Obata, Harald Oberhofer, Artem R. Oganov, Anita M. Orendt, Gabriel I. Pagola, Constantinos C. Pantelides, Chris J. Pickard, Rafal Podeszwa, Louise S. Price, Sarah L. Price, Angeles Pulido, Murray G. Read, Karsten Reuter, Elia Schneider, Christoph Schober, Gregory P. Shields, Pawanpreet Singh, Isaac J. Sugden, Krzysztof Szalewicz, Christopher R. Taylor, Alexandre Tkatchenko, Mark E. Tuckerman, Francesca Vacarro, Manolis Vasileiadis, Alvaro Vazquez-Mayagoitia, Leslie Vogt, Yanchao Wang, Rona E. Watson, Gilles A. de Wijs, Jack Yang, Qiang Zhu, Colin R. Groom
ACTA CRYSTALLOGRAPHICA SECTION B-STRUCTURAL SCIENCE CRYSTAL ENGINEERING AND MATERIALS
(2016)
Editorial Material
Physics, Multidisciplinary
Rafal Podeszwa, Georg Jansen
PHYSICAL REVIEW LETTERS
(2018)
Article
Chemistry, Physical
Rafal Podeszwa, Krzysztof Szalewicz
JOURNAL OF CHEMICAL PHYSICS
(2012)
Article
Chemistry, Physical
Fazle Rob, Alston J. Misquitta, Rafal Podeszwa, Krzysztof Szalewicz
JOURNAL OF CHEMICAL PHYSICS
(2014)
Editorial Material
Chemistry, Physical
Ad van der Avoird, Rafal Podeszwa, Bernd Ensing, Krzysztof Szalewicz
JOURNAL OF CHEMICAL PHYSICS
(2014)
Article
Chemistry, Physical
Matthew R. Kennedy, Ashley Ringer McDonald, A. Eugene DePrince, Michael S. Marshall, Rafal Podeszwa, C. David Sherrill
JOURNAL OF CHEMICAL PHYSICS
(2014)
Article
Chemistry, Physical
Urszula Gora, Wojciech Cencek, Rafal Podeszwa, Ad van der Avoird, Krzysztof Szalewicz
JOURNAL OF CHEMICAL PHYSICS
(2014)
Article
Chemistry, Physical
Rafal Podeszwa, Wojciech Cencek, Krzysztof Szalewicz
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2012)
Article
Chemistry, Physical
Wojciech Jankiewicz, Rafal Podeszwa, Henryk A. Witek
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2018)
Article
Chemistry, Physical
DeCarlos E. Taylor, Fazle Rob, Betsy M. Rice, Rafal Podeszwa, Krzysztof Szalewicz
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2011)
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Chemistry, Physical
Rafal Podeszwa, Wojciech Jankiewicz, Magdalena Krzus, Henryk A. Witek
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(2019)
Article
Chemistry, Physical
Javier Garcia, Rafal Podeszwa, Krzysztof Szalewicz
JOURNAL OF CHEMICAL PHYSICS
(2020)
Proceedings Paper
Computer Science, Interdisciplinary Applications
Ad van der Avoird, Rob van Harrevelt, Claude Leforestier, Rafal Podeszwa, Krzysztof Szalewicz, P. R. Bunker, Gert von Helden, Melanie Schnell, Gerard Meijer
INTERNATIONAL CONFERENCE OF COMPUTATIONAL METHODS IN SCIENCES AND ENGINEERING 2009 (ICCMSE 2009)
(2012)