Related papers: Inspecting molecular aggregate quadratic vibronic …
The linear absorption spectrum of J and H molecular aggregates is studied using the time-dependent Dirac-Frenkel variational principle (TDVP) with the multi-Davydov D2 (mD2) trial wavefunction (Ansatz). Both the electronic and vibrational…
Effects of non-linear coupling between the system and the bath vibrational modes on the system internal conversion dynamics are investigated using the Dirac-Frenkel variational approach with the defined sD2 ansatz. It explicitly accounts…
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$_1$…
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…
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.…
The computation of the nuclear quantum dynamics of molecules is challenging, requiring both accuracy and efficiency to be applicable to systems of interest. Recently, theories have been developed for employing time-dependent basis functions…
A general theory of electronic excitations in aggregates of molecules coupled to intramolecular vibrations and the harmonic environment is developed for simulation of the third-order nonlinear spectroscopy signals. The model is applied in…
Developed originally for the Holstein polaron, the Davydov D1 ansatz is an efficient, yet extremely accurate trial state for time-dependent variation of the spin-boson model [J. Chem. Phys. 138, 084111 (2013)]. In this work, the…
Representation of molecular vibrational degrees of freedom by independent harmonic oscillators, when describing electronic spectra or electronic excitation energy transport, raises unfavourable effects as vibrational energy relaxation…
The ground state properties and quantum phase transitions of sub-Ohmic spin-boson models are investigated using the multiple Davydov D2 Ansatz in conjunction with the variational principle. Three variants of the model are studied: (i) a…
Multidimensional spectroscopy unveils the interplay of nuclear and electronic dynamics, which characterizes the ultrafast dynamics of various molecular and solid-state systems. In a class of models widely used for the simulation of such…
We introduce a general approach for the simulation of quantum vibrational states of (symmetric and asymmetric) double-well potentials in molecules and materials for thermodynamic and spectroscopic applications. The method involves solving…
Including quantum mechanical effects on the dynamics of nuclei in the condensed phase is challenging, because the complexity of exact methods grows exponentially with the number of quantum degrees of freedom. Efforts to circumvent these…
In the present work, we give an analytical non-perturbative treatment of mode-mode coupling and anharmonicity occurring in molecular vibrational systems analyzed by 2D-infrared spectroscopy. This analytical description allows a detailed…
Vibrational environments are commonly considered to be detrimental to the optical emission properties of solid-state and molecular systems, limiting their performance within quantum information protocols. Given that such environments arise…
We present a comprehensive study of quantum dot (QD) coupling to various phononic modes in a phononic waveguide, combining multiband kp and configuration-interaction (CI) QD state simulations with finite-element waveguide mode modeling. We…
Determining the exponentially scaled ground state wavefunction and the associated molecular properties remains one of the central challenges in quantum chemistry. Hybrid quantum-classical algorithms implemented on quantum computers offer a…
Using second-order perturbation theory in the light-matter interaction, we derive an analytical approximation for the vibronic populations of a diatomic system excited by ultrabroadband frequency entangled photons and evaluate the…
Intensity enhancement in vibrational circular dichroism (VCD) arises in open-shell transition metal complexes from coupling between ground-state vibrational transitions and magnetic dipole-allowed transitions to low-lying excited states…
We propose an excited-state molecular dynamics simulation method based on variational quantum algorithms at a computational cost comparable to that of ground-state simulations. We utilize the feature that excited states can be obtained as…