Related papers: Which Electronic Structure Method to Choose in Tra…
Experiments indicate that collective coupling of molecular ensembles to confined optical modes can modify excited-state dynamics and photochemical reactivity. To describe such cavity-induced effects at atomic resolution, semi-classical…
An accurate description of nonadiabatic energy relaxation is crucial for modeling atomistic dynamics at metal surfaces. Interfacial energy transfer due to electron-hole pair excitations coupled to motion of molecular adsorbates is often…
We study the dynamics of non-adiabatic transitions in non-Hermitian multi-level parabolic models where the separations of the diabatic energies are quadratic function of time. The model Hamiltonian has been used to describe the…
Damping of structures and systems is often dominated by frictional dissipation in connections, the prediction of which remains a longstanding scientific challenge. Previous studies have shown that the actual topography of contact interfaces…
The primary computational challenge when simulating nonadiabatic ab initio molecular dynamics is the unfavorable compute costs of electronic structure calculations with molecular size. Simple electronic structure theories, like…
We investigate a simple and robust scheme for choosing the phases of adiabatic electronic states smoothly (as a function of geometry) so as to maximize the performance of ab initio non-adiabatic dynamics methods. Our approach is based upon…
Nonequilibrium dynamics governed by electron-phonon (e-ph) interactions plays a key role in electronic devices and spectroscopies and is central to understanding electronic excitations in materials. The real-time Boltzmann transport…
Processes related to electronically excited states are central in many areas of science, however accurately determining excited-state energies remains a major challenge in theoretical chemistry. Recently, higher energy stationary states of…
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 present a highly efficient method to directly simulate the photodissociation followed by Coulomb explosion of methyl iodide. In order to achieve statistical reliability, more than 40,000 trajectories are calculated on accurate potential…
A class of surface hopping algorithms is studied comparing two recent Landau-Zener (LZ) formulas for the probability of nonadiabatic transitions. One of the formulas requires a diabatic representation of the potential matrix while the other…
To expand the QUEST database of highly-accurate vertical transition energies, we consider a series of large organic chromogens ubiquitous in dye chemistry, such as anthraquinone, azobenzene, BODIPY, and naphthalimide. We compute, at the CC3…
We develop a semi-classical method to simulate the motion of atoms in a dissipative optical lattice. Our method treats the internal states of the atom quantum mechanically, including all nonadiabatic couplings, while position and momentum…
We consider an implementation of the adiabatic spin dynamics approach in a tight-binding description of the electronic structure. The adiabatic approximation for spin-degrees of freedom assumes that the faster electronic degrees of freedom…
Stochastic electronic structure theories, e.g., Quantum Monte Carlo methods, enable highly accurate total energy calculations which in principle can be used to construct highly accurate potential energy surfaces. However, their stochastic…
We present a means of studying rare reactive pathways in open quantum systems using Transition Path Theory and ensembles of quantum jump trajectories. This approach allows for elucidation of reactive paths for dissipative, nonadiabatic…
On-the-fly quantum nonadiabatic dynamics for large systems greatly benefits from the adiabatic representation readily available from the electronic structure programs. However, frequently occurring in this representation conical…
First-principles simulations of electronic properties of hybrid inorganic/organic interfaces are challenging, as common density-functional theory (DFT) approximations target specific material classes like bulk semiconductors or gas-phase…
Non-adiabatic molecular dynamics simulations are used to analyze the role of different solvent degrees of freedom in the non-radiative relaxation of the first excited state of the hydrated electron. The relaxation occurs through a…
A general theoretical framework is derived for the recently developed multi-state trajectory (MST) approach from the time dependent Schr\"odinger equation, resulting in equations of motion for coupled nuclear-electronic dynamics equivalent…