The last few decades have witnessed the extraordinary advances in theoretical and experimental tools, which enabled manipulation monitoring of ultrafast dynamics with high precisions. For modeling dynamical responses beyond perturbative regime, computational methods based on time-dependent density functional theory (TDDFT) are optimal choices. Here, we introduce TDAP (time-dependent ab initio propagation), a first-principle approach that is aimed at providing robust dynamic simulations...

The temporal characters of laser-driven phase transition from 2H to 1T^{'} has been investigated in the prototype MoTe_{2} monolayer. This process is found be induced by fundamental electron-phonon interactions, with an unexpected phonon excitation and coupling pathway closely related nonequilibrium relaxation photoexcited electrons. order-to-order transformation dissected into three substages, involving energy momentum scattering processes optical (A_{1}^{'} E^{'}) acoustic modes [LA(M)]...

Two-dimensional (2D) heterostructures composed of transition-metal dichalcogenide atomic layers are the new frontier for novel optoelectronic and photovoltaic device applications. Some key properties that make these materials appealing, yet not well understood, ultrafast hole/electron dynamics, interlayer energy transfer formation hot excitons. Here, we study photoexcited electron/hole dynamics in a representative heterostructure, MoS2/WSe2 interface, which exhibits type II band alignment....

To elucidate the nature of light-driven photocatalytic water splitting, a polymeric semiconductor—graphitic carbon nitride (g-C3N4)—has been chosen as prototype substrate for studying atomistic spitting processes in realistic environments. Our nonadiabatic quantum dynamics simulations based on real-time time-dependent density functional theory reveal explicitly transport channel photogenerated charge carriers at g-C3N4/water interface, which shows strong correlation to bond re-forming. A...

Abstract Optical control of structural and electronic properties Weyl semimetals allows development switchable dissipationless topological devices at the ultrafast scale. An unexpected orbital-selective photoexcitation in type-II material WTe 2 is reported under linearly polarized light (LPL), inducing striking transitions among several topologically-distinct phases mediated by effective electron-phonon couplings. The symmetry features atomic orbitals comprising bands result asymmetric near...

With the introduction of single atoms in photocatalysis, a small change electronic and geometric structure substrate can result higher energy conversion efficiency, whereas underlying microscopic dynamics are rarely illustrated. Here, employing real-time time-dependent density functional theory, we explore ultrafast structural single-atom photocatalysts (SAPCs) water splitting at scale. The results demonstrate that Pt loaded on graphitic carbon nitride greatly promotes photogenerated...

Abstract The past decades have witnessed the success of ground‐state density functional theory capturing static electronic properties various materials. However, for time dependent processes especially those involving excited states, real‐time time‐dependent (rt‐TDDFT) and advanced nonadiabatic algorithms are essential, practical simulations molecules materials under occurrence ultrafast laser field. Here we summarize recent progresses in developing rt‐TDDFT approaches within numerical...

Full quantum dynamics of molecules and materials is fundamental importance, which requires a faithful description simultaneous motions the electron nuclei. A new scheme developed for nonadiabatic simulations coupled electron-nuclear with electronic transitions based on Ehrenfest theorem ring polymer molecular dynamics. Built upon isomorphic Hamiltonian, time-dependent multistate Schrödinger equations are solved self-consistently approximate equation Each bead bears distinct configuration...

We report a practical computational scheme for quantum electron-nuclear dynamic simulations, applicable to both finite (e.g. ozone) and periodic systems graphene), using combination of real-time time dependent density functional theory (rt-TDDFT) ring polymer molecular dynamics. This could deal with effects nuclei beyond Ehrenfest dynamics in TDDFT simulations. find that when nuclear (NQEs) are taken into account, the atomic structure ozone splits normal states cyclic upon photoexcitation....

Water is ubiquitous and so its presence in the proximity of surfaces. To determine control properties interfacial water molecules at nanoscale essential for successful applications environmental energy-related fields. It very challenging to explore atomic structure electronic under various conditions, especially Here we review recent progress open challenges describing physicochemical on surfaces solar splitting, corrosion, desalination using first-principles approaches, highlight key role...

First-principles molecular dynamics simulations, which can reveal the microscopic mechanisms and macroscopic properties of molecules condensed systems, have become a significant driving force in development physics. In past decades, ground state electronic various materials be accurately described using first-principles method based on Born-Oppenheimer approximation. However, nonadiabatic processes, such as ultrafast excited-state where laser interacts with matters, approximation evolving...

Polarons play a crucial role in energy conversion, but the microscopic mechanism remains unclear since they are susceptible to local atomic structures. Here, by employing ab initio nonadiabatic dynamic simulations, we investigate electron–hole (e-h) nonradiative recombination at rutile TiO2(110) surface with varied amounts of oxygen vacancies (Vo). The isolated Vo facilitates e-h through forming polarons compared that defect-free surface. However, aggregated clusters induce an...