Related papers: An Efficient On-the-Fly Nonadiabatic Coupling Fram…
Ultrafast optical techniques allow to study ultrafast molecular dynamics involving both nuclear and electronic motion.To support interpretation, theoretical approaches are needed that can describe both the nuclear and electron…
Direct dynamics methods using Gaussian wavepackets have to rely only on local properties, such as gradients and hessians at the center of the wavepacket, so as to be compatible with the usual quantum chemistry methods. Matrix elements of…
Adiabatic protocols are employed across a variety of quantum technologies, from implementing state preparation and individual operations that are building blocks of larger devices, to higher-level protocols in quantum annealing and…
Nonadiabatic geometric quantum computation (NGQC) has emerged as an excellent proposal for achieving fast and robust quantum control against control errors. However, previous NGQC protocols could not be strongly resilient against the noise…
Chemical relaxation phenomena, including photochemistry and electron transfer processes, form a vigorous area of research in which nonadiabatic dynamics plays a fundamental role. Here, we show that for nonadiabatic dynamics with two…
Flow and diffusion models achieve high-fidelity, high-resolution image synthesis, but often require many function evaluations (NFEs) at sampling time. Existing acceleration methods either require additional training through distillation or…
We examine time-resolved X-ray diffraction from molecules in the gas phase which undergo nonadiabatic avoided-crossing dynamics involving strongly coupled electrons and nuclei. Several contributions to the signal are identified,…
We describe a method that focuses sampling effort on a user-defined selection of a large system, which can lead to substantial decreases in computational effort by speeding up the calculation of nonbonded interactions. A naive approach can…
Complex quantum systems are often multiscale in nature with strong interactions between different scales. We present a novel idea: iteratively suppressing, rather than tracing out, the fast, high-energy degrees of freedom in strongly…
A multiconfigurational adiabatic connection (AC) formalism is an attractive approach to computing dynamic correlation within CASSCF and DMRG models. Practical realizations of AC have been based on two approximations: i) fixing one- and…
Streaking of photoelectrons has long been used for the temporal characterization of attosecond extreme ultraviolet pulses. When the time-resolved photoelectrons originate from a coherent superposition of electronic states, they carry an…
We study effects of nonadiabatic couplings in a model of a diatomic molecule in the context of attosecond transient absorption spectroscopy. By using a model system consisting of four diabatic electronic states and with a variable strength…
Non-radiative decay in photoexcited molecular systems is driven by nuclear motion toward conical intersections (CIs), where electronic states become degenerate and nonadiabatic transitions occur. Identifying the nuclear degrees of freedom…
Understanding molecular structure, dynamics, and reactivity requires bridging processes that occur across widely separated time scales. Conventional molecular dynamics simulations provide atomistic resolution, but their femtosecond time…
A new approach to simulating warm and hot dense matter that combines density functional theory based calculations of the electronic structure to classical molecular dynamics simulations with pair interaction potentials is presented. The new…
Ab initio molecular dynamics (AIMD) simulations using hybrid density functionals and plane waves are of great interest owing to the accuracy of this approach in treating condensed matter systems. On the other hand, such AIMD calculations…
Nonadiabatic molecular dynamics occur in a wide range of chemical reactions and femtochemistry experiments involving electronically excited states. These dynamics are hard to treat numerically as the system's complexity increases and it is…
We introduce a practical calculation scheme for the description of excited electron dynamics in molecular aggregated systems within a locally group diabatic Fock representation. This scheme makes it easy to analyze the interacting…
This paper presents a model-free, data-driven control synthesis method called dynamic mode adaptive control (DMAC) for systems whose mathematical models are unavailable or unsuitable for classical control design. The proposed approach…
An investigation to optimize the application of the third-generation charge optimized many-body (COMB3) interatomic potential and associated input parameters was carried out through the study of solid-liquid interactions in classical…