Related papers: Prediction challenge: First principles simulation …
The comprehension of nonadiabatic dynamics in polyatomic systems relies heavily on the simultaneous advancements in theoretical and experimental domains. The gas-phase electron diffraction (GUED) technique has attracted widespread attention…
We present the result of our calculations of ultrafast electron diffraction (UED) for cyclobutanone excited into $S_2$ electronic state, which are based on the non-adiabatic dynamics simulations with \textit{Ab Initio} Multiple Cloning…
Using the recently developed multistate mapping approach to surface hopping (multistate MASH) method combined with SA(3)-CASSCF(12,12)/aug-cc-pVDZ electronic structure calculations, the gas-phase isotropic ultrafast electron diffraction…
Quantum dynamics simulations are becoming a standard tool for simulating photo-excited molecular systems involving a manifold of coupled states, known as non-adiabatic dynamics. While these simulations have had many successes in explaining…
Gas phase ultrafast electron diffraction (GUED) has become a powerful technique to directly observe the structural dynamics of photoexcited molecules. GUED reveals information about the nuclear motions that is complementary to the…
We study the photoinduced chemical dynamics of cyclobutanone upon excitation at 200 nm to the 3s Rydberg state using MeV ultrafast electron diffraction (UED). We observe both the elastic scattering signal, which contains information about…
We investigated the ultrafast structural dynamics of cyclobutanone following photoexcitation at $\lambda=200$ nm using gas-phase megaelectronvolt ultrafast electron diffraction. Our investigation complements the simulation studies of the…
Simulations of photochemical reaction dynamics have been a challenge to the theoretical chemistry community for some time. In an effort to determine the predictive character of current approaches, we predict the results of an upcoming…
For years, theoretical calculations and scalable computer simulations have complemented ultrafast experiments as they offer the advantage to overcome experimental restrictions and have access to the whole dynamics. This synergy between…
To simulate a 200 nm photoexcitation in cyclobutanone to the n-3s Rydberg state, classical trajectories were excited from a Wigner distribution to the singlet state manifold based on excitation energies and oscillator strenghts. Twelve…
Owing to ring-strain, cyclic ketones exhibit complex excited-state dynamics with multiple competing photochemical channels active on the ultrafast timescale. While the excited-state dynamics of cyclobutanone after $\pi^{\ast}\leftarrow n$…
We present the simulation of the photochemical dynamics of cyclobutanone induced by the excitation of the 3s Rydberg state. For this purpose, we apply the complete active space self-consistent field method together with spin-orbit…
We study the ultrafast time evolution of cyclobutanone excited to singlet n-->Rydberg state through XMS-CASPT2 nonadiabatic surface-hopping simulations. These dynamics predict relaxation to ground-state with a timescale of 822 +/- 45 fs…
This Perspective is part of a Special Topic that explored the maturity of nonadiabatic molecular dynamics for predicting photochemical processes. In 2023, a prediction challenge was issued to the community of computational photochemists to…
Ultrafast electron diffraction (UED) instruments typically operate at kHz or lower repetition rates and rely on indirect detection of electrons. However, these experiments encounter limitations because they are required to use electron…
This work is part of a prediction challenge that invited theoretical/computational chemists to predict the photochemistry of cyclobutanone in the gas phase, excited at 200 nm by a laser pulse, and the expected signal that will be recorded…
Inferring transient molecular structural dynamics from diffraction data is an ambiguous task that often requires different approximation methods. In this paper we present an attempt to tackle this problem using machine learning. While most…
Ultrafast electron diffraction and phonon-diffuse scattering (UED(S)) experiments make use of photo-induced changes to electron scattering intensity across 2D detectors to report on a very wide range of dynamic structural phenomena in…
During the last few years, serial electron crystallography (Serial Electron Diffraction, SerialED) has been gaining attention for the structure determination of crystalline compounds that are sensitive to the irradiation of the electron…
We simulate the photodynamics of gas-phase cyclobutanone excited to the S$_2$ state using fewest switches surface hopping (FSSH) dynamics powered by time-dependent density functional theory (TDDFT). We predict a total C3+C2 photoproduct…