Hybrid quantum/classical simulation of the vibrational relaxation of the bend fundamental in liquid water

Bastida, Adolfo; Zúñiga, José; Requena, A.; Miguel, Beatriz

doi:10.1063/1.3266834

Cited by 15 publications

(23 citation statements)

References 81 publications

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“…Several of such factors exist in literature. 57 As introduced by Bastida and co-workers [48][49][50][51] only the so-called standard correction factor is described below but tests with the harmonic, the Schofield, and Egelstaff variants 57 performed very similarly for the present system. To this end, the couplings between the quantum system and classical system are modified by the so-called standard temperature-dependent quantum correction factor …”

Section: Temperature-corrected Wave Packet Approachmentioning

confidence: 95%

“…(38)- (40). The aforementioned approach by Bastida and coworkers [48][49][50][51] has the drawback that it does not reproduce the high-temperature limit. Therefore, we propose a modification of this scheme by introducing an additional normalization .…”

Section: Temperature-corrected Wave Packet Approachmentioning

confidence: 99%

“…Attempts have been made to overcome this limitation. Here we test and improve the scheme by Bastida et al [48][49][50][51] As discussed above, we have to solve the time-dependent Schrödinger equation with the effective Hamiltonian defined in Eq. (23) and then perform an ensemble average.…”

Section: Temperature-corrected Wave Packet Approachmentioning

confidence: 99%

“…[48][49][50][51] In this method Fermi's golden rule, i.e., the assumption that the rate is proportional to the square of the coupling, is employed. To fulfill detailed balance, a quantum-correction factor is, thus, introduced into the coupling.…”

Section: Temperature-corrected Wave Packet Approachmentioning

confidence: 99%

“…29,40,45,47 In addition to comparing the results of density matrix calculation with those of mean-field Ehrenfest dynamics, the results from a temperature-corrected Ehrenfest dynamics variant are also investigated. This scheme, by Bastida et al, [48][49][50][51] introduced an additional correction factor to fulfill detailed balance and leads to the correct thermal distribution at long times. An improved version of this algorithm will be proposed and tested.…”

Section: Introductionmentioning

confidence: 99%

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Juxtaposing density matrix and classical path-based wave packet dynamics

Aghtar

Liebers

Strümpfer

et al. 2012

The Journal of Chemical Physics

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In many physical, chemical, and biological systems energy and charge transfer processes are of utmost importance. To determine the influence of the environment on these transport processes, equilibrium molecular dynamics simulations become more and more popular. From these simulations, one usually determines the thermal fluctuations of certain energy gaps, which are then either used to perform ensemble-averaged wave packet simulations, also called Ehrenfest dynamics, or to employ a density matrix approach via spectral densities. These two approaches are analyzed through energy gap fluctuations that are generated to correspond to a predetermined spectral density. Subsequently, density matrix and wave packet simulations are compared through population dynamics and absorption spectra for different parameter regimes. Furthermore, a previously proposed approach to enforce the correct long-time behavior in the wave packet simulations is probed and an improvement is proposed.

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Section: Temperature-corrected Wave Packet Approachmentioning

confidence: 95%

Section: Temperature-corrected Wave Packet Approachmentioning

confidence: 99%

Section: Temperature-corrected Wave Packet Approachmentioning

confidence: 99%

Section: Temperature-corrected Wave Packet Approachmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

Juxtaposing density matrix and classical path-based wave packet dynamics

Aghtar

Liebers

Strümpfer

et al. 2012

The Journal of Chemical Physics

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Temperature dependence of vibrational relaxation of the OH bending excitation in liquid H2O

Ashihara

Fujioka

Shibuya

2011

Chemical Physics Letters

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Ultrafast Dynamics of Liquid Water: Energy Relaxation and Transfer Processes of the OH Stretch and the HOH Bend

2015

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The vibrational energy relaxation and transfer processes of the OH stretching and HOH bending vibrations in liquid water are investigated via the theoretical calculation of the pump-probe spectra obtained from nonequilibrium molecular dynamics simulations with the TTM3-F interaction potential. The excitation of the OH stretch induces an instantaneous response of the high frequency librational motions in the 600-1000 cm(-1) range. In addition, the excess energy of the OH stretch of a water molecule quickly transfers to the OH stretches of molecules in its first hydration shell with a time constant of ∼50 fs, followed by relaxation to the HOH bends of the surrounding molecules with a time constant of 230 fs. The excitation of the HOH bend also results in the ultrafast excitation of the high frequency librational motions. The energy of the excited HOH bend of a water molecule decays, with a time constant of 200 fs, mainly to the relaxation of the HOH bends of its surrounding molecules. The energies of the HOH bends were found to transfer quickly to the intermolecular motions via the coupling with the high frequency librational motions. The excess energy of the OH stretch or the HOH bend relaxes to the high frequency intermolecular librational motions and eventually to the hot ground state with a time scale of ∼1 ps via the coupling with the librational and translational motions. The energy relaxation and transfer processes were found to depend on the local hydrogen bonding network; the relaxations of the excess energy of the OH stretch and the HOH bend of four- and five-coordinated molecules are faster than those of a three-coordinated molecule due to the delocalization of the vibrational motions of the former (four- and five-coordinated molecules) compared to those of the later (three-coordinated molecules). The present results highlight the importance of the high frequency intermolecular librational modes in facilitating the ultrafast energy relaxation process in liquid water via their strong nonlinear couplings with the intramolecular OH stretching and HOH bending vibrations.

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Hybrid quantum/classical simulation of the vibrational relaxation of the bend fundamental in liquid water

Cited by 15 publications

References 81 publications

Juxtaposing density matrix and classical path-based wave packet dynamics

Juxtaposing density matrix and classical path-based wave packet dynamics

Temperature dependence of vibrational relaxation of the OH bending excitation in liquid H2O

Ultrafast Dynamics of Liquid Water: Energy Relaxation and Transfer Processes of the OH Stretch and the HOH Bend

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