相关论文: On-the-fly ab initio semiclassical evaluation of t…

To compute and analyze vibrationally resolved electronic spectra at zero temperature, we have recently implemented the on-the-fly ab initio extended thawed Gaussian approximation [A. Patoz et al., J. Phys. Chem. Lett. 9, 2367 (2018)], which…

To alleviate the computational cost associated with on-the-fly ab initio semiclassical calculations of molecular spectra, we propose the single-Hessian thawed Gaussian approximation, in which the Hessian of the potential energy at all…

Evaluation of symmetry-forbidden or weakly-allowed vibronic spectra requires treating the transition dipole moment beyond the Condon approximation. To include vibronic spectral features not captured in the global harmonic models, we have…

To evaluate vibronic spectra beyond the Condon approximation, we extend the on-the-fly ab initio thawed Gaussian approximation by considering the Herzberg-Teller contribution due to the dependence of the electronic transition dipole moment…

Simulating vibrationally resolved electronic spectra of anharmonic systems, especially those involving double-well potential energy surfaces, often requires expensive quantum dynamics methods. Here, we explore the applicability and…

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…

Vibrationally resolved spectra provide a stringent test of the accuracy of theoretical calculations. We combine the thawed Gaussian approximation (TGA) with an on-the-fly ab initio (OTF-AI) scheme to calculate the vibrationally resolved…

Despite its simplicity, the single-trajectory thawed Gaussian approximation has proven useful for calculating vibrationally resolved electronic spectra of molecules with weakly anharmonic potential energy surfaces. Here, we show that the…

A method for performing variable-width (thawed) Gaussian wavepacket (GWP) variational dynamics on machine-learned potentials is presented. Instead of fitting the potential energy surface (PES), the anharmonic correction to the global…

Time-resolved spectroscopy is an important tool for unraveling the minute details of structural changes of molecules of biological and technological significance. The nonlinear femtosecond signals detected for such systems must be…

We describe new developments in the OpenLoops framework based on the recently introduced on-the-fly method. The on-the-fly approach exploits the factorisation of one-loop diagrams into segments in order to perform various operations, such…

Irradiation of a molecular system by an intense laser field can trigger dynamics of both electronic and nuclear subsystems. The lighter electrons usually move on much faster, attosecond time scale but the slow nuclear rearrangement damps…

Hagedorn wavepackets have been used to compute single vibronic level (SVL) spectra efficiently in model harmonic potentials. To make the Hagedorn approach practical for realistic polyatomic molecules with anharmonicity, here we combine…

Harmonic calculations based on density-functional theory are generally the method of choice for the description of phonon spectra of metals and insulators. The inclusion of anharmonic effects is, however, delicate as it relies on…

Quantitative evaluations of the free energy of materials must take into account thermal and zero-point energy fluctuations. While these effects can easily be estimated within a harmonic approximation, corrections arising from the anharmonic…

We develop a new approach for efficient and scalable simulations of measurement and control of quantum systems built upon existing phase-space methods, namely the Truncated Wigner Approximation (TWA). We benchmark against existing…

In this paper we develop and compare different real-time methods to calculate spectral functions. These are classical-statistical simulations, the Gaussian state approximation (GSA), and the functional renormalization group (FRG) formulated…

We report on a new approach to ease the computational overhead of ab initio on-the-fly semiclassical dynamics simulations for vibrational spectroscopy. The well known bottleneck of such computations lies in the necessity to estimate the…

We present an efficient numerical implementation of the quasi-classical doorway-window approximation, specifically designed for on-the-fly simulations of time-resolved nonlinear spectroscopic signals in the Julia package WaveMixings.jl. The…

The theoretical prediction of the rates of nonradiative processes in molecules is fundamental to assess their emissive properties. In this context, global harmonic models have been widely used to simulate vibronic spectra as well as…