Libra: An open-Source “methodology discovery” library for quantum and classical dynamics simulations

Akimov, Alexey V.

doi:10.1002/jcc.24367

Cited by 91 publications

(123 citation statements)

References 199 publications

(328 reference statements)

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“…The LIBRA platform developed by Akimov enables a "do-it-yourself" strategy through an open-source library including modules to perform quantum and classical dynamics simulations. 432 A large variety of algorithms is available, including modules to perform MFE and TSH (with FSSH, GFSH, and MSSH) based on SCF; routines to deal with trivial crossings and decoherence; algorithms to compute various sorts of matrix elements with Heller Gaussians; and a number of MOLCAS 440 and MOLPRO 95 have implemented FSSH and AIMS respectively. AIMS has also been implemented in development versions of MOPAC and GAMESS, including intersystem crossing.…”

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confidence: 99%

Recent Advances and Perspectives on Nonadiabatic Mixed Quantum–Classical Dynamics

2018

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Nonadiabatic mixed quantum-classical (NA-MQC) dynamics methods form a class of computational theoretical approaches in quantum chemistry tailored to investigate the time evolution of nonadiabatic phenomena in molecules and supramolecular assemblies. NA-MQC is characterized by a partition of the molecular system into two subsystems: one to be treated quantum mechanically (usually but not restricted to electrons) and another to be dealt with classically (nuclei). The two subsystems are connected through nonadiabatic couplings terms to enforce self-consistency. A local approximation underlies the classical subsystem, implying that direct dynamics can be simulated, without needing precomputed potential energy surfaces. The NA-MQC split allows reducing computational costs, enabling the treatment of realistic molecular systems in diverse fields. Starting from the three most well-established methods-mean-field Ehrenfest, trajectory surface hopping, and multiple spawning-this review focuses on the NA-MQC dynamics methods and programs developed in the last 10 years. It stresses the relations between approaches and their domains of application. The electronic structure methods most commonly used together with NA-MQC dynamics are reviewed as well. The accuracy and precision of NA-MQC simulations are critically discussed, and general guidelines to choose an adequate method for each application are delivered.

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confidence: 99%

Recent Advances and Perspectives on Nonadiabatic Mixed Quantum–Classical Dynamics

2018

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“…The charge and energy transfer processes can be investigated by ab initio NAMD only with relatively small systems, involving hundreds of atoms, and on timescales of tens of picoseconds, depending on the approximations used. In order to perform larger‐scale simulations, one needs to develop methods that reduce the computational cost for electronic structure calculations, and in particular, for calculation of reliable NA couplings, which are more sensitive to wave function accuracy than energies. Linear scaling KS‐DFT brings such framework, and enabling description of thousands of atoms at the quantum‐mechanical level.…”

Section: Discussionmentioning

confidence: 99%

Nonadiabatic charge dynamics in novel solar cell materials

Long

Prezhdo

Fang

2017

WIREs Comput Mol Sci

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The review describes recent research into the nonequilibrium phenomena in nanoscale materials, with focus on charge separation and recombination, that form the basis for photovoltaic and photocatalytic devices. Nonadiabatic molecular dynamics combined with ab initio real-time time-dependent density functional theory enable us to model time-resolved laser experiments at the atomistic level, emphasizing realistic aspects of the materials, such as defects, dopants, boundaries, chemical bonding, etc. A variety of systems have been considered, including bulk semiconductors sensitized by semiconducting/metallic nanoparticles and graphene, nanocrystal/molecule junctions, polymer interfaces with carbon nanotubes and nanoclusters, van der Waals heterojunctions, black phosphorus, and hybrid organic-inorganic perovskites. The detailed atomistic knowledge obtained from the explicit time-domain modeling generates comprehensive understanding of electron-vibrational dynamics in complex multicomponent systems, provides critical insights into quantum mechanical transport of energy and charge, and leads to valuable guidelines for improvement of solarto-electric power conversion in photovoltaic and photocatalytic applications and for efficient performance of transport devices. FIGURE 14 | Decay of populations of the first excited state in bilayer black phosphorus (BP) and at the BP/MoS 2 interface. BP/MoS 2 shows slower decay because of electron-hole separation across the interface.

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“…Under this scheme, the knowledge of the ground state, excited states and nonadiabatic couplings (NACs) between them are required. General quantum chemistry method can be used to generate all the information needed and it has been implemented in a few codes . In addition, Tavernelli and coworkers showed that the necessary quantities can also be rigorously derived from LR‐TDDFT.…”

Section: Introductionmentioning

confidence: 99%

Ab initio nonadiabatic molecular dynamics investigations on the excited carriers in condensed matter systems

Zheng

Chu

Zhao

et al. 2019

WIREs Comput Mol Sci

271

258

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The ultrafast dynamics of photoexcited charge carriers in condensed matter systems play an important role in optoelectronics and solar energy conversion. Yet it is challenging to understand such multidimensional dynamics at the atomic scale. Combining the real‐time time‐dependent density functional theory with fewest‐switches surface hopping scheme, we develop time‐dependent ab initio nonadiabatic molecular dynamics (NAMD) code Hefei‐NAMD to simulate the excited carrier dynamics in condensed matter systems. Using this method, we have investigated the interfacial charge transfer dynamics, the electron–hole recombination dynamics, and the excited spin‐polarized hole dynamics in different condensed matter systems. The time‐dependent dynamics of excited carriers are studied in energy, real and momentum spaces. In addition, the coupling of the excited carriers with phonons, defects and molecular adsorptions are investigated. The state‐of‐art NAMD studies provide unique insights to understand the ultrafast dynamics of the excited carriers in different condensed matter systems at the atomic scale. This article is categorized under: Structure and Mechanism > Computational Materials Science Molecular and Statistical Mechanics > Molecular Dynamics and Monte‐Carlo Methods Electronic Structure Theory > Ab Initio Electronic Structure Methods Software > Simulation Methods

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Libra: An open-Source “methodology discovery” library for quantum and classical dynamics simulations

Cited by 91 publications

References 199 publications

Recent Advances and Perspectives on Nonadiabatic Mixed Quantum–Classical Dynamics

Recent Advances and Perspectives on Nonadiabatic Mixed Quantum–Classical Dynamics

Nonadiabatic charge dynamics in novel solar cell materials

Ab initio nonadiabatic molecular dynamics investigations on the excited carriers in condensed matter systems

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