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We present systematic comparison of three quantum mechanical approaches describing excitation dynamics in molecular complexes using the Time-Dependent variational principle (TDVP) with three increasing sophistication trial wavefunctions…

Chemical Physics · Physics 2023-06-02 Mantas Jakučionis , Agnius Žukas , Darius Abramavičius

By employing the Dirac-Frenkel time-dependent variational principle, we study the dynamical properties of the Holstein molecular crystal model with diagonal and off-diagonal exciton-phonon coupling. A linear combination of the Davydov D$_1$…

Statistical Mechanics · Physics 2019-08-27 Nengji Zhou , Lipeng Chen , Zhongkai Huang , Kewei Sun , Yoshitaka Tanimura , Yang Zhao

Numerical implementation of an explicit phonon bath requires a large number of oscillator modes in order to maintain oscillators at the initial temperature when modeling energy relaxation processes. An additional thermalization algorithm…

Chemical Physics · Physics 2023-06-12 Mantas Jakucionis , Darius Abramavicius

Following the Dirac-Frenkel time-dependent variational principle, dynamics of a one-dimensional Holstein polaron is probed by employing the Davydov D2 Ansatz with two sets of variational parameters, one for each constituting particle in the…

Materials Science · Physics 2015-05-18 Jin Sun , Bin Luo , Yang Zhao

Molecular hydrogen normally has only weak, quadrupole transitions between its rovibrational states, but in a static electric field it acquires a dipole moment and a set of allowed transitions. Here we use published ab initio calculations of…

Astrophysics of Galaxies · Physics 2022-06-09 Mark A. Walker

Adsorption geometry and stability of organic molecules on surfaces are key parameters that determine the observable properties and functions of hybrid inorganic/organic systems (HIOSs). Despite many recent advances in precise experimental…

Absorption spectra of small molecular aggregates (oligomers) are considered. The dipole-dipole interaction between the monomers leads to shifts of the oligomer spectra with respect to the monomer absorption. The line-shapes of monomer as…

Chemical Physics · Physics 2011-02-03 Jan Roden , Walter T. Strunz , Alexander Eisfeld

In this paper, we present a new method for calculating linear absorption spectra for large molecular aggregates, called dyadic adaptive HOPS (DadHOPS). This method combines the adaptive HOPS (adHOPS) framework, which uses locality to…

A new synchrotron study for CH$_2$F$_2$ from has been combined with earlier data. The onset of absorption, band I and also band IV, is resolved into broad vibrational peaks, which contrast with the continuous absorption previously claimed.…

Hydrogen adsorption by the metal organic framework (MOF) structure Zn2(BDC)2(TED) is investigated using a combination of experimental and theoretical methods. By use of the nonempirical van der Waals density-functional (vdW-DF) approach, it…

Materials Science · Physics 2009-11-13 Lingzhu Kong , Valentino R. Cooper , Nour Nijem , Kunhao Li , Jing Li , Yves J. Chabal , David C. Langreth

In this work, using theoretical calculations within the framework of the density functional theory, taking into account the dispersive VDW interaction, the processes of adsorption and interaction of a water molecule with a TiO2 surface in…

We describe a fast parallel iterative method for computing molecular absorption spectra within TDDFT linear response and using the LCAO method. We use a local basis of "dominant products" to parametrize the space of orbital products that…

Other Condensed Matter · Physics 2011-04-19 Peter Koval , Dietrich Foerster , Olivier Coulaud

The absorption sites and the low-lying rotational and vibrational (RV) energy states for H$_2$ adsorbed within a metal-organic framework are calculated via van der Waals density functional theory. The induced dipole due to bond stretching…

Other Condensed Matter · Physics 2015-05-20 Lingzhu Kong , Yves J. Chabal , David C. Langreth

The time-development of photoexcitations in molecular aggregates exhibits specific dynamics of electronic states and vibrational wavefunction. We discuss the dynamical formation of entanglement between electronic and vibrational degrees of…

Quantum Physics · Physics 2007-05-23 Dmitri S. Kilin , Jeffrey A. Cina , Oleg V. Prezhdo

A relativistic transient absorption theory is derived, implemented and validated within the dipole approximation based on the time-dependent Dirac equation. Time-dependent simulations have been performed using the Dirac equation and the…

Atomic Physics · Physics 2020-10-14 Felipe Zapata , Jimmy Vinbladh , Eva Lindroth , Jan Marcus Dahlström

Linear-response time-dependent (TD) density-functional theory (DFT) has been implemented in the pseudopotential wavelet-based electronic structure program BigDFT and results are compared against those obtained with the all-electron…

We implement and apply time-dependent density matrix renormalization group (TD-DMRG) algorithms at zero and finite temperature to compute the linear absorption and fluorescence spectra of molecular aggregates. Our implementation is within a…

Chemical Physics · Physics 2019-07-30 Jiajun Ren , Zhigang Shuai , Garnet Kin-Lic Chan

The coherent two-dimensional (2D) electronic spectra with respect to the singlet fission (SF) process in organic molecular aggregates are simulated by the Davydov ansatz combined with the Frenkel-Dirac time-dependent variational algorithm.…

Mesoscale and Nanoscale Physics · Physics 2018-01-17 Ke-Wei Sun , Yao Yao

The influence of molecular vibrations on dissociative adsorption is studied by six-dimensional quantum dynamical calculations. For the system H_2 at Pd(100), which possesses non-activated pathways, it is shown that large vibrational effects…

mtrl-th · Physics 2009-10-30 Axel Gross , Matthias Scheffler

Using the Dirac-Frenkel variational principle, a time-dependent description of the dynamics of a two-level system coupled to a bosonic bath is formulated. The method is applied to the case of a gas of cold atoms adsorbing to an elastic…

Mesoscale and Nanoscale Physics · Physics 2024-12-04 Dennis P. Clougherty
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