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We present in detail the recently derived ab-initio molecular dynamics (AIMD) formalism [Phys. Rev. Lett. 101 096403 (2008)], which due to its numerical properties, is ideal for simulating the dynamics of systems containing thousands of…

Ab initio Born-Oppenheimer molecular dynamics (AIMD) is a valuable method for simulating physico-chemical processes of complex systems, including reactive systems, and for training machine learning models and force fields. Speed and…

This work combines for the first time ab initio molecular dynamics (AIMD) within the Born-Oppenheimer approximation, with a global natural orbital functional (GNOF), an approximate functional of the one-particle reduced density matrix. The…

Chemical Physics · Physics 2024-01-10 Alejandro Rivero Santamaría , Mario Piris

We present a new method which combines Car-Parrinello and Born-Oppenheimer molecular dynamics in order to accelerate density functional theory based ab-initio simulations. Depending on the system a gain in efficiency of one to two orders of…

Materials Science · Physics 2007-05-23 Thomas D. Kühne , Matthias Krack , Fawzi R. Mohamed , Michele Parrinello

Ab initio molecular dynamics (AIMD) simulations using hybrid density functionals and plane waves are of great interest owing to the accuracy of this approach in treating condensed matter systems. On the other hand, such AIMD calculations…

Chemical Physics · Physics 2020-01-08 Sagarmoy Mandal , Nisanth N. Nair

Ehrenfest and Car-Parrinello molecular dynamics are computational alternatives to approximate Born-Oppenheimer molecular dynamics without solving the electron eigenvalue problem at each time-step. A non-trivial issue is to choose the…

Chemical Physics · Physics 2014-09-18 Ashraful Kadir , Mattias Sandberg , Anders Szepessy

Ab initio molecular dynamics (AIMD) based on density functional theory (DFT) has become a workhorse for studying the structure, dynamics, and reactions in condensed matter systems. Currently, AIMD simulations are primarily carried out at…

Chemical Physics · Physics 2025-06-10 Ritama Kar , Sagarmoy Mandal , Vaishali Thakkur , Bernd Meyer , Nisanth N. Nair

With the continuous growth of processing power for scientific computing, first principles Born-Oppenheimer molecular dynamics (MD) simulations are becoming increasingly popular for the study of a wide range of problems in materials science,…

Materials Science · Physics 2015-06-04 Anders M. N. Niklasson , Marc J. Cawkwell

We extend the ab initio molecular dynamics (AIMD) method based on density functional theory to the nonequilibrium situation where an electronic current is present in the electronic system. The dynamics is treated using the semi-classical…

Mesoscale and Nanoscale Physics · Physics 2020-05-27 Jing-Tao Lu , Susanne Leitherer , Nick R. Papior , Mads Brandbyge

We present a time-reversible Born-Oppenheimer molecular dynamics scheme, based on self-consistent Hartree-Fock or density functional theory, where both the nuclear and the electronic degrees of freedom are propagated in time. We show how a…

Materials Science · Physics 2009-11-11 Anders M. N. Niklasson , C. J. Tymczak , Matt Challacombe

Simulating electron-ion dynamics using time-dependent density functional theory within an Ehrenfest dynamics scheme can be done in two ways that are in principle exact and identical: propagating time-dependent electronic Kohn-Sham equations…

Chemical Physics · Physics 2021-07-01 Lionel Lacombe , Neepa T. Maitra

An approximate method based on adiabatic time dependent density functional theory (TDDFT) is presented, that allows for the description of the electron dynamics in nanoscale junctions under arbitrary time dependent external potentials. In…

Mesoscale and Nanoscale Physics · Physics 2015-05-27 Y. Wang , C. -Y. Yam , G. H. Chen , Th. Frauenheim , T. A. Niehaus

Density functional theory with linear combination of atomic orbitals (LCAO) basis sets is useful for studying large atomic systems, especially when it comes to computationally highly demanding time-dependent dynamics. We have implemented…

Materials Science · Physics 2025-05-02 Vladimír Zobač , Mikael Kuisma , Ask Hjorth Larsen , Tuomas Rossi , Toma Susi

The route to reliable quantum nanoelectronic devices hinges on precise control of the electrostatic environment. For this reason, accurate methods for electrostatic simulations are essential in the design process. The most widespread…

Mesoscale and Nanoscale Physics · Physics 2023-02-28 Waldemar Svejstrup , Andrea Maiani , Kevin Van Hoogdalem , Karsten Flensberg

Accounting for electrons and nuclei simultaneously is a powerful capability of ab initio molecular dynamics (AIMD). However, AIMD is often unable to accurately reproduce properties of systems such as water due to inaccuracies in the…

Chemical Physics · Physics 2017-01-25 Andrew D. White , Chris Knight , Glen M. Hocky , Gregory A. Voth

We propose a first-principles time-dependent density functional theoretical (TDDFT) approach in momentum (P) space for quantitative study of electron transport in molecular devices under arbitrary biases. In this approach, the basic…

Mesoscale and Nanoscale Physics · Physics 2009-02-10 Zhongyuan Zhou , Shih-I Chu

The relation between ab initio molecular dynamics formalism and the electron-phonon interaction formalism [P.B. Allen and V. Heine, J. Phys. C 9, 2305 (1976)] is explored. The fundamental quantity obtained in the AIMD formalism - total…

Materials Science · Physics 2009-06-13 T. R. S. Prasanna

Ab initio molecular dynamics (AIMD) with hybrid density functionals and plane wave basis is computationally expensive due to the high computational cost of exact exchange energy evaluation. Recently, we proposed a strategy to combine…

Chemical Physics · Physics 2021-01-11 Sagarmoy Mandal , Vaishali Thakkur , Nisanth N. Nair

Ehrenfest, Born-Oppenheimer, Langevin and Smoluchowski dynamics are shown to be accurate approximations of time-independent Schr\"odinger observables for a molecular system avoiding caustics, in the limit of large ratio of nuclei and…

Mathematical Physics · Physics 2010-01-12 Anders Szepessy

Ehrenfest dynamics is a useful approximation for ab initio mixed quantum-classical molecular dynamics that can treat electronically nonadiabatic effects. Although a severe approximation to the exact solution of the molecular time-dependent…

Chemical Physics · Physics 2021-09-24 Seonghoon Choi , Jiří Vaníček
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