A5074366619- Spectroscopy and Quantum Chemical Studies
- Advanced Chemical Physics Studies
- Mass Spectrometry Techniques and Applications
- Spectroscopy and Laser Applications
- Radical Photochemical Reactions
- Porphyrin and Phthalocyanine Chemistry
- Quantum optics and atomic interactions
- Atomic and Molecular Physics
- CO2 Reduction Techniques and Catalysts
- Electron and X-Ray Spectroscopy Techniques
- nanoparticles nucleation surface interactions
- X-ray Spectroscopy and Fluorescence Analysis
- Neonatal Health and Biochemistry
- Laser-Matter Interactions and Applications
- Cold Atom Physics and Bose-Einstein Condensates
- Organic Chemistry Cycloaddition Reactions
- Quantum, superfluid, helium dynamics
- Heme Oxygenase-1 and Carbon Monoxide
- Photochemistry and Electron Transfer Studies
Stony Brook University
2024
University of Chemistry and Technology, Prague
2017-2022
The vast majority of<italic>ab initio</italic>excited-state simulations are performed within semiclassical, trajectory-based approaches. Apart from the underlying electronic-structure theory, reliability of is controlled by a selection initial conditions for classical trajectories. We discuss appropriate choices different experimental arrangements: dynamics initiated continuum-wave (CW) laser fields or triggered ultrashort pulses.
Ab initio excited state photodynamical simulations have entered the mainstream in past two decades, bringing techniques of various sophistication and computational requirements for description nonadiabatic transitions. We explore this work performance recently reformulated Landau–Zener surface hopping (LZSH) approach extend it simultaneous treatment internal conversion intersystem crossing events. studied photochemical reactions four model molecules (cyclopropanone, methaniminium cation,...
Computer simulation has long been an essential partner of ultrafast experiments, allowing the assignment microscopic mechanistic detail to low-dimensional spectroscopic data. However, ability theory make a priori predictions experimental results is relatively untested. Herein, as part community challenge, we attempt predict signal upcoming photochemical experiment using state-of-the-art in context preexisting Specifically, employ ab initio Ehrenfest with collapse block mixed...
Electronic coherences can be leveraged to control molecular dynamics, but such is limited by ultrafast decoherence driven coupling between electronic excitations and vibrations. With the goal of understanding controlling coherence in molecules, we introduce a first-principles approach that enables direct simulation creation decay molecules. Simulations long-lived experimentally-observed created upon multiphoton excitation thiophene reveal coherent motions within dense manifold Rydberg...
2D Resonant Auger maps showing the site-specific excitations in butadiene.
The combination of supersonic expansions with IR action spectroscopy techniques is the basis many successful approaches to study cluster structure and dynamics. In this paper we elucidate temperature effect excitation evaporative cooling on sodium solvation in water clusters.
Abstract Triplet state mechanism of [2 + 2] photocycloaddition forming a cyclobutane ring from two ethylenes is investigated in the context photocatalysis. High‐level ab initio calculations are combined with adiabatic molecular dynamics and metadynamics for rare events modeling. In photocatalytic scheme, reactant reaches triplet either via intersystem crossing (ISC) or sensitization. The model system adopts biradical structure, which represents energy intersection ground state. completes...
The transport of free electrons in a water environment is still poorly understood. We show that additional insight can be brought about by investigating fragmentation patterns finite-size particles upon electron impact ionization. have developed composite protocol aiming to simulate clusters with kinetic energies the range up 100 eV. ionization events for atomistically described molecular are identified Monte Carlo procedure. subsequently model classical dynamics simulations, calibrated...
Long-range intermolecular forces are able to steer polar molecules submerged in superfluid helium nanodroplets into highly metastable configurations. We demonstrate that the presence of such special structures can be identified, a direct and determinative way, by electrostatic deflection doped nanodroplet beam. The measurement also establishes structures' electric dipole moments. In consequence, introduced approach is complementary spectroscopic studies low-temperature molecular assembly...
The photochemistry of bilirubin has been extensively studied due to its importance in the phototherapy hyperbilirubinemia. In present work, we investigated ultrafast photodynamics a dipyrrinone subunit, vinylneoxanthobilirubic acid methyl ester. photoisomerization and photocyclization reactions (E) (Z) isomers were using femtosecond transient absorption spectroscopy by multireference electronic structure theory, where nonadiabatic dynamics was modeled with Landau–Zener surface hopping...
Computer simulation has long been an essential partner of ultrafast experiments, allowing the assignment microscopic mechanistic detail to low-dimensional spectroscopic data. However, ability theory make a priori predictions experimental results is relatively untested. Herein, as part community challenge, we attempt predict signal upcoming photochemical experiment using state-of-the-art in context preexisting Specifically, employ ab initio Ehrenfest with collapse block (TAB) mixed...
Photodissociation of the C–Cl bond in chloroalkanes probed by <italic>ab initio</italic> simulations and velocity map imaging identify alkyl chain as a soft energy absorbing unit an increasing role spin–orbit coupling with prolongation.