Related papers: Two-dimensional electronic spectra from trajectory…
Mixed-quantum-classical molecular dynamics simulation implies an effective measurement on the electronic states owing to continuously tracking the atomic forces.Based on this insight, we propose a quantum trajectory mean-field approach for…
Vibrational coherences in ultrafast pump-probe (PP) and 2D electronic spectroscopy (2DES) provide insight into the excited state dynamics of molecules. Femtosecond coherence spectra (FCS) and 2D beat maps yield information about…
We theoretically investigate an electron transfer (ET) process in a dissipative environment by means of two-dimensional (2D) correlation spectroscopy. We extend the reduced hierarchy equations of motion approach to include both overdamped…
We present a widefield two-dimensional electronic spectroscopy microscope (2DESM) that integrates multidimensional coherent spectroscopy with optical imaging, enabling femtosecond temporal and micrometer spatial resolution. The broadband…
Ab initio computation of two-dimensional electronic spectra is an expanding field, whose goal is improving upon simple, few-dimensional models often employed to explain experiments. Here, we propose an accurate and computationally…
Spectroscopic methods involving the sudden injection or ejection of electrons in materials are a powerful probe of electronic structure and interactions. These techniques, such as photoemission and tunneling, yield measurements of the…
We present a partially linearized method based on spin mapping for computing both linear and nonlinear optical spectra. As observables are obtained from ensembles of classical trajectories, the approach can be applied to the large…
Electronic energy transfer in photosynthesis occurs over a range of time scales and under a variety of intermolecular coupling conditions. Recent work has shown that electronic coupling between chromophores can lead to coherent oscillations…
Non-adiabatic dynamics simulations have become a standard approach to explore photochemical reactions. Such simulations require underlying potential energy surfaces and couplings between them, calculated at a chosen level of theory, yet…
We show that adiabatic evolution of a low-dimensional lattice of quantum spins with a spectral gap can be simulated efficiently. In particular, we show that as long as the spectral gap \Delta E between the ground state and the first excited…
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…
The single-particle spectral function measures the density of electronic states (DOS) in a material as a function of both momentum and energy, providing central insights into phenomena such as superconductivity and Mott insulators. While…
A long-standing challenge in mixed quantum-classical trajectory simulations is the treatment of entanglement between the classical and quantal degrees of freedom. We present a novel approach which describes the emergence of entangled states…
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…
In this work we provide an exact and efficient numerical approach to simulate multi-time correlation functions in the Mahan-Nozi\`{e}res-De Dominicis model, which crudely mimics the spectral properties of doped two-dimensional…
Accurate simulation of the non-adiabatic dynamics of molecules in excited electronic states is key to understanding molecular photo-physical processes. Here we present a novel method, based on a semiclassical approximation, that is as…
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…
We present a new partially linearized mapping-based approach for approximating real-time quantum correlation functions in condensed-phase nonadiabatic systems, called spin-PLDM. Within a classical trajectory picture, partially linearized…
Two-dimensional spectroscopy is discussed for open quantum systems with multiple simultaneously measurable fluxes. In particular, we discuss a junction where optical measurements of photon flux are complemented with simultaneous transport…
We present a new formulation of the correlated electron-ion dynamics (CEID) scheme, which systematically improves Ehrenfest dynamics by including quantum fluctuations around the mean-field atomic trajectories. We show that the method can…