Related papers: An accurate and efficient Ehrenfest dynamics appro…
Two-dimensional electronic spectroscopy (2DES) provides a detailed picture of electronically nonadiabatic dynamics that can be interpreted with the aid of simulations. Here, we develop and contrast trajectory-based nonadiabatic dynamics…
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…
Mixed quantum-classical mechanics descriptions are critical to modeling coupled electron-nuclear dynamics, i.e. non-adiabatic molecular dynamics, relevant to photochemical and photophysical processes. We argue that, for polyatomic…
Ehrenfest Dynamics combined with real-time time-dependent density functional theory has proven to be a reliable tool to study non-adiabatic molecular dynamics with a reasonable computational cost. Among other possibilities, it allows for…
Processes involving ultrafast laser driven electron-phonon dynamics play a fundamental role in the response of quantum systems in a growing number of situations of interest, as evidenced by phenomena such as strongly driven phase…
Electronic energy transfer in the condensed phase, such as that occurring in photosynthetic complexes, frequently occurs in regimes where the energy scales of the system and environment are similar. This situation provides a challenge to…
Mixed quantum-classical methods, such as surface hopping and Ehrenfest dynamics, have proven useful for describing molecular processes involving multiple electronic states. These methods require propagating many independent trajectories,…
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 recent development of multidimensional ultrafast spectroscopy techniques calls for the introduction of computational schemes that allow for the simulation of such experiments and the interpretation of the corresponding results from a…
We consider an Ehrenfest approximation for a particle in a double-well potential in the presence of an external environment schematized as a finite resource heat bath. This allows us to explore how the limitations in the applicability of…
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…
Linear and non-linear spectroscopies are powerful tools used to investigate the energetics and dynamics of electronic excited states of both molecules and crystals. While highly accurate \emph{ab initio} calculations of molecular spectra…
Within the well-established optical response function formalism, a new strategy with the central idea of employing the forward-backward stochastic Schr\"{o}dinger equations in a segmented way to accurately obtain the two-dimensional (2D)…
The atomistic resolution recently achieved by ultrafast spectroscopies demands corresponding theoretical advances. Real-time time-dependent density-functional theory (RT-TDDFT) with Ehrenfest dynamics offers an optimal trade-off between…
Simulating electron-ion dynamics using time-dependent density functional theory within an Ehrenfest dynamics scheme can be done in two ways that are in principle exact and identical: propagating time-dependent electronic Kohn-Sham equations…
The Ehrenfest dynamics, representing a quantum-classical mean-field type coupling, is a widely used approximation in quantum molecular dynamics. In this paper, we propose a time-splitting method for an Ehrenfest dynamics, in the form of a…
High-harmonic generation (HHG) is a nonlinear process in which a material sample is irradiated by intense laser pulses, causing the emission of high harmonics of the incident light. HHG has historically been explained by theories employing…
The dynamics of an electronic two-level system coupled to an electromagnetic field are simulated explicitly for one and three dimensional systems through semiclassical propagation of the Maxwell-Liouville equations. We consider three…
Following Ehrenfest's approach, the problem of quantum-classical correspondence can be treated in the class of trajectory-coherent functions that approximate as $\h\to 0$ a quantum-mechanical state. This idea leads to a family of systems of…
Two-dimensional electronic spectroscopy (2DES) provides rich information about how the electronic states of molecules, proteins, and solid-state materials interact with each other and their surrounding environment. Atomistic molecular…