Related papers: Benchmarking mixed quantum-classical dynamics for …
Exposing a molecule to intense light pulses may bring this molecule to a nonstationary quantum state, thus launching correlated dynamics of electronic and nuclear subsystems. Although much had been achieved in the understanding of…
The recent improvement in experimental capabilities for interrogating and controlling molecular systems with ultrafast coherent light sources calls for the development of theoretical approaches that can accurately and efficiently treat…
The optical response of an electronic two-level system (TLS) coupled to an incident continuous wave (cw) electromagnetic (EM) field is simulated explicitly in one dimension by the following five approaches: (i) the coupled Maxwell-Bloch…
The dynamics of an electronic system interacting with an electromagnetic field is investigated within mixed quantum-classical theory. Beyond the classical path approximation (where we ignore all feedback from the electronic system on the…
A novel mixed quantum-classical approach to simulating nonadiabatic dynamics of molecules at metal surfaces is presented. The method combines the numerically exact hierarchical equations of motion approach for the quantum electronic degrees…
Interest in vibrational polaritonic chemistry, where ground-state chemical kinetics are modified via confined optical modes in a cavity, has surged in recent years. Although models have been developed to understand cavity-modified…
Adequate simulation of non-adiabatic dynamics through conical intersection requires account for a non-trivial geometric phase (GP) emerging in electronic and nuclear wave-functions in the adiabatic representation. Popular mixed…
We describe vacuum fluctuations and photon-field correlations in interacting quantum mechanical light-matter systems, by generalizing the application of mixed quantum-classical dynamics techniques. We employ the multi-trajectory…
While the treatment of chemically relevant systems containing hundreds or even thousands of electrons remains beyond the reach of quantum devices, the development of quantum-classical hybrid algorithms to resolve electronic correlation…
Due to the exponential growth of the state space of coupled quantum systems it is not possible, in general, to numerically store the state of a very large number of quantum systems within a classical computer. We demonstrate a method for…
Semiclassical electrodynamics is an appealing approach for studying light-matter interactions, especially for realistic molecular systems. However, there is no unique semiclassical scheme. On the one hand, intermolecular interactions can be…
We benchmark a set of quantum-chemistry methods, including multitrajectory Ehrenfest, fewest-switches surface-hopping, and multiconfigurational-Ehrenfest dynamics, against exact quantum-many-body techniques by studying real-time dynamics in…
The exact factorization approach has led to the development of new mixed quantum-classical methods for simulating coupled electron-ion dynamics. We compare their performance for dynamics when more than two electronic states are occupied at…
The violation of detailed balance poses a serious problem for the majority of current quasiclassical methods for simulating nonadiabatic dynamics. In order to analyze the severity of the problem, we predict the long-time limits of the…
The mapping approach addresses the mismatch between the continuous nuclear phase space and discrete electronic states by creating an extended, fully continuous phase space using a set of harmonic oscillators to encode the populations and…
When the interaction between a molecular system and confined light modes in an optical or plasmonic cavity is strong enough to overcome the dissipative process, hybrid light-matter states (polaritons) emerge as the fundamental excitations…
We introduce a novel methodology for simulating the excited-state dynamics of extensive molecular aggregates in the framework of the long-range corrected time-dependent density-functional tight-binding fragment molecular orbital method…
We introduce a novel computational framework for excited-states molecular quantum dynamics simulations driven by quantum computing-based electronic-structure calculations. This framework leverages the fewest-switches surface-hopping method…
Understanding the electron dynamics and transport in metallic and semiconductor nanostructures -- such as metallic nanoparticles, thin films, quantum wells and quantum dots -- represents a considerable challenge for today's condensed matter…
We present a nonadiabatic classical-trajectory approach that offers the best of both worlds between fewest-switches surface hopping (FSSH) and quasiclassical mapping dynamics. This mapping approach to surface hopping (MASH) propagates the…