Quantum Thermal Bath for Molecular Dynamics Simulation

Dammak, Hichem; Chalopin, Yann; Laroche, Marine; Hayoun, Marc; Greffet, Jean‐Jacques

doi:10.1103/physrevlett.103.190601

Cited by 156 publications

(248 citation statements)

References 20 publications

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“…simulations (189,190), and have been extended to non-equilibrium thermostat schemes that can be used to mimic nuclear quantum fluctuations in quasi-harmonic systems (191,192).…”

Section: Accelerated Path Integrals With Generalized Langevin Equatiomentioning

confidence: 99%

Nuclear Quantum Effects in Water and Aqueous Systems: Experiment, Theory, and Current Challenges

et al. 2016

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Nuclear quantum effects influence the structure and dynamics of hydrogen bonded systems, such as water, which impacts their observed properties with widely varying magnitudes. This review highlights the recent significant developments in the experiment, theory and simulation of nuclear quantum effects in water. Novel experimental techniques, such as deep inelastic neutron scattering, now provide a detailed view of the role of nuclear quantum effects in water's 2 properties. These have been combined with theoretical developments such as the introduction of the competing quantum effects principle that allows the subtle interplay of water's quantum effects and their manifestation in experimental observables to be explained. We discuss how this principle has recently been used to explain the apparent dichotomy in water's isotope effects, which can range from very large to almost nonexistent depending on the property and conditions. We then review the latest major developments in simulation algorithms and theory that have enabled the efficient inclusion of nuclear quantum effects in molecular simulations, permitting their combination with on-the-fly evaluation of the potential energy surface using electronic structure theory. Finally, we identify current challenges and future opportunities in the area.3

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“…simulations (189,190), and have been extended to non-equilibrium thermostat schemes that can be used to mimic nuclear quantum fluctuations in quasi-harmonic systems (191,192).…”

Section: Accelerated Path Integrals With Generalized Langevin Equatiomentioning

confidence: 99%

Nuclear Quantum Effects in Water and Aqueous Systems: Experiment, Theory, and Current Challenges

et al. 2016

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“…The key idea behind quantum thermal baths (QTB) is to use a Langevin-type approach in which a dissipative force and a Gaussian random force are adjusted to have the power spectral density given by the quantum fluctuation-dissipation theorem (Dammak et al, 2009;Ceriotti, Bussi, and Parrinello, 2009;Barrat and Rodney, 2011). In doing this, the internal energy of the system can be mapped into that of an ensemble of harmonic oscillators whose vibrational modes follow a Bose-Einstein distribution.…”

Section: Quantum Thermal Bathsmentioning

confidence: 99%

Simulation and understanding of atomic and molecular quantum crystals

2017

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Quantum crystals abound in the whole range of solid-state species. Below a certain threshold temperature the physical behavior of rare gases ( 4 He and Ne), molecular solids (H 2 and CH 4 ), and some ionic (LiH), covalent (graphite), and metallic (Li) crystals can be only explained in terms of quantum nuclear effects (QNE). A detailed comprehension of the nature of quantum solids is critical for achieving progress in a number of fundamental and applied scientific fields like, for instance, planetary sciences, hydrogen storage, nuclear energy, quantum computing, and nanoelectronics. This review describes the current physical understanding of quantum crystals formed by atoms and small molecules, as well as the wide palette of simulation techniques that are used to investigate them. Relevant aspects in these materials such as phase transformations, structural properties, elasticity, crystalline defects and the effects of reduced dimensionality, are discussed thoroughly. An introduction to quantum Monte Carlo techniques, which in the present context are the simulation methods of choice, and other quantum simulation approaches (e. g., path-integral molecular dynamics and quantum thermal baths) is provided. The overarching objective of this article is twofold. First, to clarify in which crystals and physical situations the disregard of QNE may incur in important bias and erroneous interpretations. And second, to promote the study and appreciation of QNE, a topic that traditionally has been treated in the context of condensed matter physics, within the broad and interdisciplinary areas of materials science.

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Section: Introductionmentioning

confidence: 99%

“…for temperatures safely above the Debye temperature that signals the onset of quantum effects. The Debye temperature is often of the order of few hundred Kelvins and nuclear quantum effects (NQEs) are thus indeed important over a wide range of temperatures [2,3].Quantum fluctuations stemming from the Heisenberg uncertainty principle make the energy of a particle at 0 K higher than a the potential energy minimum, leading to a concept of zero point energy (ZPE) (see Fig. 1).…”

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confidence: 99%

Hydrogen dynamics in solid formic acid: insights from simulations with quantum colored-noise thermostats

Drużbicki

Krzystyniak

Hollas

et al. 2018

J. Phys.: Conf. Ser.

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Abstract. With an increase of computational capabilities, ab initio molecular dynamics becomes the natural choice for exploring the nuclear dynamics of solids. As based on classical mechanics, the validity of this approach is, in-principle, limited to the high-T regime, whilst low-temperature simulations require inclusion of quantum effects. The methods commonly used to account for nuclear quantum effects are based on the path-integral formalism, which become, however, particularly time consuming when high accuracy methods are used for calculating forces. Recently, new efficient alternative approaches to account for quantum nature of nuclei have been proposed, using so-called quantum thermostats. In this work, we examine the simulations performed with the quantum colored-noise thermostat introduced by Ceriotti [Phys. Rev. Lett., 103:030603, 2009]. We present the tests of portable implementation of the quantum thermostat in the ABIN program, which has been extended to periodic systems through the interface to CASTEP, a leading spectroscopy-oriented plane-wave density functional theory code. The range of applicability of quantum-thermostatted molecular dynamics simulations for the interpretation of neutron scattering data was examined and compared to classical molecular dynamics and lattice-dynamics simulations, using solid formic acid case as a test bed. We find that the approach is particularly useful for the modeling of low-temperature inelastic neutron scattering spectra as well as provides some theoretical estimate for the low-limit of the mean kinetic energy. While finding the quantum-thermostat to seriously affect the dynamic properties of the title system, we illustrate to which extent the unperturbed response can be successfully recovered. IntroductionMolecular dynamics (MD) has evolved into a powerful numerical method to investigate structural and dynamical properties of condensed matter [1]. For an atom, these calculations are, however, only valid in the classical limit, i.e. for temperatures safely above the Debye temperature that signals the onset of quantum effects. The Debye temperature is often of the order of few hundred Kelvins and nuclear quantum effects (NQEs) are thus indeed important over a wide range of temperatures [2,3].Quantum fluctuations stemming from the Heisenberg uncertainty principle make the energy of a particle at 0 K higher than a the potential energy minimum, leading to a concept of zero point energy (ZPE) (see Fig. 1). While ZPE reflects the quantum nature of atomic motion, it can be approximately accounted for by lattice-dynamics calculations, which, by definition, are based on the quantum harmonic oscillator model.

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Quantum Thermal Bath for Molecular Dynamics Simulation

Cited by 156 publications

References 20 publications

Nuclear Quantum Effects in Water and Aqueous Systems: Experiment, Theory, and Current Challenges

Nuclear Quantum Effects in Water and Aqueous Systems: Experiment, Theory, and Current Challenges

Simulation and understanding of atomic and molecular quantum crystals

Hydrogen dynamics in solid formic acid: insights from simulations with quantum colored-noise thermostats

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