Related papers: An Improved Ehrenfest Approach to Model Correlated…
The increasing need to simulate the dynamics of photoexcited molecular and nanosystems in the sub-picosecond regime demands new efficient tools able to describe the quantum nature of matter at a low computational cost. By combining the…
Nonadiabatic dynamical processes are one of the most important quantum mechanical phenomena in chemical, materials, biological, and environmental molecular systems, where the coupling between different electronic states is either inherent…
The goal of the present account is to review our efforts to obtain and apply a ``collective'' Hamiltonian for a few, approximately decoupled, adiabatic degrees of freedom, starting from a Hamiltonian system with more or many more degrees of…
Far out-of-equilibrium many-body quantum dynamics in isolated systems necessarily generate interferences beyond an Ehrenfest time scale, where quantum and classical expectation values diverge. Of great recent interest is the role these…
We extend the Mixed Quantum-Classical Initial Value Representation (MQC-IVR), a semiclassical method for computing real-time correlation functions, to electronically nonadiabatic systems using the Meyer-Miller-Stock-Thoss (MMST) Hamiltonian…
In this work, a nonlinear momentum method is introduced to enhance the convergence performance of momentum-based gradient optimization algorithms. Classical momentum methods, such as the Heavy Ball method, can be viewed as a dynamical…
We develop and experimentally demonstrate a methodology for a full molecular frame quantum tomography (MFQT) of dynamical polyatomic systems. We exemplify this approach through the complete characterization of an electronically…
Path integral Monte Carlo approach is used to study the coupled quantum dynamics of the electron and nuclei in hydrogen molecule ion. The coupling effects are demonstrated by comparing differences in adiabatic Born--Oppenheimer and…
We describe quantum and classical Hamiltonian dynamics in a common Hilbert space framework, that allows the treatment of mixed quantum-classical systems. The analysis of some examples illustrates the possibility of entanglement between…
A novel method combining maximum entropy principle, the Bayesian-inference of ensembles approach, and the optimization of empirical forward models is presented. Here we focus on the Karplus parameters for RNA systems, which relate the…
We present a dynamical simulation scheme to model the highly correlated excited state dynamics of linear polyenes. We apply it to investigate the internal conversion processes of carotenoids following their photoexcitation. We use the…
Recently proposed non-adiabatic ring polymer molecular dynamics (NRPMD) approach has shown to provide accurate quantum dynamics by incorporating explicit electronic state descriptions and nuclear quantizations. Here, we present a rigorous…
The simulation of non-Markovian quantum dynamics plays an important role in the understanding of charge and exciton dynamics in the condensed phase environment, and yet it remains computationally expensive on classical computers. We have…
An extension of the CCS-method [Chem. Phys. 2004, 304, p. 103-120] for simulating non-adiabatic dynamics with quantum effects of the nuclei is put forward. The time-dependent Schr\"{o}dinger equation for the motion of the nuclei is solved…
The simulation of non-equilibrium electron distributions is essential for capturing light-metal interactions and therefore the study of photoabsorption, photocatalysis, laser ablation, and many other phenomena. Current methodologies, such…
The transport approach is a useful tool to study dynamics of non-equilibrium systems. For heavy-ion collisions at intermediate energies, where both the smooth nucleon potential and the hard-core nucleon-nucleon collision are important, the…
Non-adiabatic dynamics at molecule-metal interfaces govern diverse and technologically important phenomena, from heterogeneous catalysis to dye-sensitized solar energy conversion and charge transport across molecular junctions. Realistic…
We design a quantum molecular dynamics method for strongly correlated electron metals. The strong electronic correlation effects are treated within a real-space version of the Gutzwiller variational approximation (GA), which is suitable for…
Treated traditionally by the Ehrenfest approximation, dynamics of a one-dimensional molecular crystal model with off-diagonal exciton-phonon coupling is investigated in this work using the Dirac-Frenkel time-dependent variational principle…
We present an efficient \textit{ab initio} algorithm for quantum dynamics simulations of interacting systems that is based on the conditional decomposition of the many-body wavefunction [Phys. Rev. Lett. 113, 083003 (2014)]. Starting with…