Nonadiabatic quantum dynamics is important for understanding light-harvesting processes, but its propagation with traditional methods can be rather expensive. Here we present a one-shot trajectory learning approach that allows us to directly make an ultrafast prediction of the entire trajectory of the reduced density matrix for a new set of such simulation parameters as temperature and reorganization

We show that properties of molecules with low-frequency modes calculated with density functional approximations (DFAs) suffer from spurious oscillations along the nuclear displacement coordinate due to numerical integration errors. Occasionally, the problem can be alleviated using extensive integration grids that compromise the favorable cost-accuracy ratio of DFAs. Since spurious oscillations are

In this study, a set of 10 positional indolocarbazole (ICz) isomers substituted with dicyanomethylene groups connected via para or meta positions are computationally investigated with the aim of exploring the efficiency of structural isomerism and substitution position in controlling their optical and electronic properties. Unrestricted density functional theory (DFT), a spin-flip time-dependent DFT

[FeFe] hydrogenases are highly active catalysts for hydrogen conversion. Their active site has two components: a [4Fe−4S] electron relay covalently attached to the H2 binding site and a diiron cluster ligated by CO, CN–, and 2-azapropane-1,3-dithiolate (ADT) ligands. Reduction of the [4Fe−4S] site was proposed to be coupled with protonation of one of its cysteine ligands. Here, we used time-resolved

We employ terahertz-range temperature-dependent Raman spectroscopy and first-principles lattice dynamical calculations to show that the undoped sodium ion conductors Na3PS4 and isostructural Na3PSe4 both exhibit anharmonic lattice dynamics. The anharmonic effects in the compounds involve coupled host lattice–Na+ ion dynamics that drive the tetragonal-to-cubic phase transition in both cases, but with

For the first time, we demonstrated that additional poling at room temperature (cold repoling) of a soda-lime glass thermally poled in open anode configuration causes an increase of the optical second harmonic signal by more than an order of magnitude. Performed experiments allow relating this increase in the optical nonlinearity of the glass to the orientation of hydrogenated dipoles in the vicinity

Terahertz waves have been attracting more attention because of their growing applications in brain science. Most of the studies have demonstrated that terahertz waves have a certain positive impact on neurons. They can promote the growth of ganglion processes and the release of neurotransmitters, but the specific mechanism is still largely unexplored. Our study found that terahertz waves could promote

Conformational transitions of proteins are governed by chemical kinetics, often toggled by passage through an activated state separating two conformational ensembles. The passage time of a protein through the activated state can be too fast to be detected by single-molecule experiments without the aid of viscogenic agents. Here, we use high-bandwidth nanopore measurements to resolve microsecond-duration

By precisely controlling the waveform of ultrashort laser fields, electronic and nuclear motions in molecules can be steered on extremely short time scales, even in the attosecond regime. This new research field, termed “optochemistry”, presents the light field in the time-frequency domain and opens new avenues for tailoring molecular reactions beyond photochemistry. This Perspective summarizes the

Controlling crystal morphology is crucial in analytical chemistry and smart materials synthesis, etc. However, flexible manipulation of 3D crystal morphology still remains challenging. Herein, we present a novel and facile light strategy for droplet evaporative crystallization to manipulate macroscopic crystal morphology on photosensitive hydrophobic substrate possessing photothermal conversion property

By enabling control of valley degrees of freedom in transition-metal dichalcogenides, valley-selective circular dichroism has become a key concept in valleytronics. Herein, we show that valley excitons, bound electron–hole pairs formed at the K or K̅ valleys upon absorption of circularly polarized light, are chiral quasiparticles characterized by a finite orbital angular momentum (OAM). We further

Inorganic perovskites have attracted a great deal of attention because of their stability. Unfortunately, a weak optical response and the toxicity of lead are hampering their development. Motivated by these facts, we focus herein on the perovskite-based doped series CsPb1−αZnαI3−βXβ (X = Cl or Br). The geometric structures and the electronic and optical properties of CsPb1−αZnαI3−βXβ (X = Cl or Br)

The iron hydride molecular cation FeH+ is expected to be present in the interstellar medium. Because of the lack of laboratory data, it is yet to be identified in spectrally resolved astronomic observations. As a benchmark for computational predictions and to guide an experimental search for the ro-vibrational lines of FeH+, we performed infrared multiple photon dissociation (IRMPD) spectroscopy of

Rational control of the luminescent properties of ligand-protected coinage metal clusters has long been pursued but remains challenging. Here we explore the crucial structural and electronic factors governing the fluorescence of a diphosphine-protected [Au13(dppe)5Cl2]3+ cluster by time-dependent density functional theory calculations. By substituting the central Au atom with group 5 to group 11 transition

Bufotenine (5-hydroxy-N,N-dimethyltryptamine) is a natural tryptamine derivative with hallucinogenic activity. In this paper, we present novel chemical and molecular conformational analyses of bufotenine based on an experimental and theoretical approach integrating surface-enhanced Raman scattering (SERS) and density functional theory (DFT). For the first time, low concentrations of bufotenine in acetonitrile

Metal-assisted chemical etching (MACE) is a widely applied process for fabricating Si nanostructures. As an electroless process, it does not require a counter electrode, and it is usually considered that only holes in the Si valence band contribute to the process. In this work, a charge carrier collecting p–n junction structure coated with silver nanoparticles is used to demonstrate that also electrons

The efficient activation of methane and the simultaneous water dissociation are crucial in many catalytic reactions on oxide-supported transition metal catalysts. On very low-loaded Ni/CeO2 surfaces, methane easily fully decomposes, CH4 → C + 4H, and water dissociates, H2O→ OH + H. However, in important reactions such as the direct oxidation of methane to methanol (MTM), where complex interplay exists