相关论文: HEOM-Based Numerical Framework for Quantum Simulat…
Molecular vibrations in solutions, especially OH stretching and bending in water, drive ultrafast energy relaxation and dephasing in chemical and biological systems. We present a machine learning approach for constructing system-bath models…
We model, simulate, and analyze the intramolecular modes of liquid H2O and D2O to elucidate how energy excitation, relaxation, and vibrational dephasing interplay through anharmonic mode-mode coupling. Our analysis employs two-dimensional…
Two-dimensional (2D) vibrational spectroscopy is a powerful means of investigating the structure and dynamics of complex molecules in condensed phases. However, even in theory, analysis of 2D spectra resulting from complex inter- and…
An open quantum system refers to a system that is further coupled to a bath system consisting of surrounding radiation fields, atoms, molecules, or proteins. The bath system is typically modeled by an infinite number of harmonic…
The multimode Brownian model with nonlinear system-bath coupling offers a flexible framework for studying both intra- and intermolecular vibrational modes in condensed-phase molecular systems. This approach allows us to calculate linear and…
Studies of quantum thermal effects on molecular excitation dynamics have often relied on oversimplified models, such as energy eigenstates or low-dimensional potentials, which fail to capture the complexity of real chemical systems. In…
Time- and frequency resolved optical signals provide insights into the properties of light harvesting molecular complexes, including excitation energies, dipole strengths and orientations, as well as in the exciton energy flow through the…
A model of a bulk water system describing the vibrational motion of intramolecular and intermolecular modes is constructed, enabling analysis of its linear and nonlinear vibrational spectra, as well as the energy transfer processes between…
Quantum computing offers promising new avenues for tackling the long-standing challenge of simulating the quantum dynamics of complex chemical systems, particularly open quantum systems coupled to external baths. However, simulating such…
Vibrational dynamics of adsorbates near surfaces plays both an important role for applied surface science and as model lab for studying fundamental problems of open quantum systems. We employ a previously developed model for the relaxation…
We introduce sbml4md, a newly developed algorithm implemented as a software package to extract parameters of multimode anharmonic Brownian (MAB) models from molecular dynamics (MD) trajectories for simulating nonlinear vibrational spectra…
Two-dimensional spectroscopy (2DS) is a powerful ultrafast technique for probing electronic and vibrational dynamics in complex microscopic systems. Extracting detailed information on system dynamics and system-bath interactions from 2DS…
The time evolution in open quantum systems, such as a molecular aggregate in contact with a thermal bath, still poses a complex and challenging problem. The influence of the thermal noise can be treated using a plethora of schemes, several…
Open quantum systems that feature non-Markovian dynamics are routinely solved using techniques such as the Hierarchical Equations of Motion (HEOM). However, their usage of the entire system density-matrix renders them intractable for…
Quantum beats in nonlinear spectroscopy of molecular aggregates are often attributed to electronic phenomena of excitonic systems, while nuclear degrees of freedom are commonly included into models as overdamped oscillations of bath…
In this work we develop a model for an undamped vibration in the presence of an overdamped bath. This two-bath model involves a new derivation of the hierarchical equations of motion (HEOM) for an overdamped Lorentz-Drude (LD) environment…
We rigorously investigate the quantum non-Markovian dissipative dynamics of a system coupled to a harmonic oscillator bath by deriving hierarchical Schrodinger equations of motion (HSEOM) and studying their dynamics. The HSEOM are the…
Many-body open quantum systems (OQS) have a profound impact on various subdisciplines of physics, chemistry, and biology. Thus, the development of a computer program capable of accurately, efficiently, and versatilely simulating many-body…
The hierarchical equations of motion (HEOM) approach can describe the reduced dynamics of a system simultaneously coupled to multiple bosonic and fermionic environments. The complexity of exactly describing the system-environment…
The hierarchical equations of motion technique has found widespread success as a tool to generate the numerically exact dynamics of non-Markovian open quantum systems. However, its application to low temperature environments remains a…