Related papers: Computing linear optical spectra in the presence o…
While dark transitions made bright by molecular motions determine the optoelectronic properties of many materials, simulating such non-Condon effects in condensed-phase spectroscopy remains a fundamental challenge. We derive a Gaussian…
The interplay of nuclear and electronic dynamics characterizes the multi-dimensional electronic spectra of various molecular and solid-state systems. Theoretically, the observable effect of such interplay can be accounted for by response…
We present a comprehensive theoretical framework for calculating the linear and nonlinear optical responses of time-periodic quantum systems. Using density matrix evolution in the Floquet basis and adopting the length gauge, our approach…
Spectroscopy is an indispensable tool in understanding the structures and dynamics of molecular systems. However computational modelling of spectroscopy is challenging due to the exponential scaling of computational complexity with system…
There is currently much interest in the development of improved trajectory-based methods for the simulation of nonadiabatic processes in complex systems. An important goal for such methods is the accurate calculation of the rate constant…
Nonadiabatic molecular dynamics is an effective method for modeling nonradiative decay in electronically excited molecules. Its accuracy depends strongly on the quality of the potential energy surfaces, and its affordability for long…
Problems in the field of open quantum systems often involve an environment that strongly influences the dynamics of excited states. Here we present a numerical method to model optical spectra of non-Markovian open quantum systems. The…
An antiadiabatic approach is proposed to model how the refractive index of the surrounding medium affects optical spectra of molecular systems in condensed phases. The approach solves some of the issues affecting current implementations of…
Quantum molecular dynamics requires an accurate representation of the molecular potential energy surface from a minimal number of electronic structure calculations, particularly for nonadiabatic dynamics where excited states are required.…
A new methodology of simulating nonadiabatic dynamics using frozen-width Gaussian wavepackets within the moving crude adiabatic representation with the on-the-fly evaluation of electronic structure is presented. The main feature of the new…
Modeling linear absorption spectra of solvated chromophores is highly challenging as contributions are present both from coupling of the electronic states to nuclear vibrations and solute-solvent interactions. In systems where excited…
In this work, we present a linear optical implementation for analog quantum simulation of molecular vibronic spectra, incorporating the non-Condon scattering operation with a quadratically small truncation error. Thus far, analog and…
An approach to non-adiabatic dynamics of atoms in molecular and condensed matter systems under general non-equilibrium conditions is proposed. In this method interaction between nuclei and electrons is considered explicitly up to the second…
We introduce a computational framework for simulating non-adiabatic vibronic dynamics on circuit quantum electrodynamics (cQED) platforms. Our approach leverages hybrid oscillator-qubit quantum hardware with mid-circuit measurements and…
Dielectric spectra are typically obtained in molecular dynamics (MD) simulations by analyzing the fluctuations, in the absence of an applied electric field, of the total dipole moment of the simulation box. We compare this standard method…
Multi-dimensional spectroscopy represents a particularly insightful tool for investigating the interplay of nuclear and electronic dynamics, which plays an important role in a number of photophysical processes and photochemical reactions.…
Quantum computation is an attractive front for many problems that are intractable for computers today. One such problem is nonadiabatic quantum molecular dynamics, where quantized internal states coupling to parameterized modes result in a…
Nonadiabatic effects in chemical reaction at metal surfaces, due to excitation of electron-hole pairs, stand at the frontier of the studies of gas-surface reaction dynamics. However, the first principles description of electronic excitation…
Nonlinear computation is essential for various information processing tasks. Optical implementations are attractive because passive light propagation can manipulate high-dimensional signals with extreme throughput and parallelism; yet…
We introduce a combined molecular dynamics (MD) and quantum trajectories (QT) code to simulate the effects of near-resonant optical fields on state-vector evolution and particle motion in a collisional system. In contrast to collisionless…