相关论文: On-the-fly ab initio three thawed Gaussians approx…

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…

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…

We present a methodology for computing vibrationally and time-resolved pump-probe spectra, which takes into account all vibrational degrees of freedom and is based on the combination of the thawed Gaussian approximation with on-the-fly ab…

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…

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…

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…

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…

We consider a semiclassical approximation for the time evolution of an originally gaussian wave packet in terms of complex trajectories. We also derive additional approximations replacing the complex trajectories by real ones. These yield…

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…

We combine the semiclassical Herman--Kluk approximation with the coherence thermofield dynamics in order to evaluate vibrationally resolved electronic spectra at nonzero temperatures. In coherence thermofield dynamics, the dipole time…

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…

Generalized Plane Waves (GPWs) were introduced to take advantage of Trefftz methods for problems modeled by variable coefficient equations. Despite the fact that GPWs do not satisfy the Trefftz property, i.e. they are not exact solutions to…

We assessed three schemes for propagating a variable-width (thawed) Gaussian wave packet moving under the influence of Morse or double-well potentials with parameters that are chemically representative. The most rigorous scheme is based on…

We numerically compare the semiclassical ``frozen Gaussian'' Herman-Kluk propagator [Chem. Phys. 91, 27 (1984)] and the ``thawed Gaussian'' propagator put forward recently by Baranger et al. [J. Phys. A 34, 7227 (2001)] by studying the…

While dark transitions made bright by molecular motions determine the optoelectronic properties of many materials, simulating such non-Condon effects in condensed-phase spectroscopy remains a fundamental challenge. We derive a Gaussian…

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…

Primordial gravitational waves could be non-Gaussian, just like primordial scalar perturbations. Although the tensor two-point function has thus-far remained elusive, the three-point function could, in principle, be large enough to be…

This paper is devoted to the construction of approximations of the propagator associated with a semi-classical matrix-valued Schr\"odinger operator with symbol presenting smooth eigenvalues crossings. Inspired by the approach of the…

We present a theory of electronic excitation energies and optical absorption spectra which incorporates energy-level renormalization and phonon-assisted optical absorption within a unified framework. Using time-independent perturbation…

Laser photons carrying non-zero orbital angular momentum are known and exploited during the last twenty years. Recently it has been demonstrated experimentally that such (twisted) electrons can be produced and even focused to a subnanometer…