The wavepacket dynamics of CS2 after photoexcitation to the (1)B2((1)Σu(+)) state at 198 nm are studied by time-resolved photoelectron imaging using sub-20 fs 159 nm pulses, which enable single photon ionization from the entire region of the (1)B2 potential energy surface. The time-energy map of the photoelectron intensity reveals vibrational motions along the symmetric stretching and bending coordinates. The time-energy map of the photoelectron anisotropy parameter exhibits time-evolution within single oscillation periods of the ν1 and ν2 modes, which is attributed to variation of the excited state electronic character along these vibrational coordinates. The initially populated (1)B2 state evolves with two time constants of 107 and 394 fs.
Download full-text PDF |
Source |
---|---|
http://dx.doi.org/10.1063/1.4907749 | DOI Listing |
ACS Nano
January 2025
Beijing Academy of Quantum Information Sciences, Beijing 100193, P. R. China.
The quantum-well-like two-dimensional lead-halide perovskites exhibit strongly confined excitons due to the quantum confinement and reduced dielectric screening effect, which feature intriguing excitonic effects. The ionic nature of the perovskite crystal and the "softness" of the lattice induce the complex lattice dynamics. There are still open questions about how the soft lattices decorate the nature of excitons in these hybrid materials.
View Article and Find Full Text PDFPhys Rev E
November 2024
Department of Physics, University of Oxford, Oxford OX1 3PU, United Kingdom.
We present two methods for computing the dynamic structure factor for warm dense hydrogen without invoking either the Born-Oppenheimer approximation or the Chihara decomposition, by employing a wave-packet description that resolves the electron dynamics during ion evolution. First, a semiclassical method is discussed, which is corrected based on known quantum constraints, and second, a direct computation of the density response function within the molecular dynamics. The wave-packet models are compared to PIMC and DFT-MD for the static and low-frequency behavior.
View Article and Find Full Text PDFPhys Chem Chem Phys
December 2024
Department of Physics and Astronomy, University of Nebraska-Lincoln, Lincoln, Nebraska, USA.
Conjugated diene molecules are highly reactive upon photoexcitation and can relax through multiple reaction channels that depend on the position of the double bonds and the degree of molecular rigidity. Understanding the photoinduced dynamics of these molecules is crucial for establishing general rules governing the relaxation and product formation. Here, we investigate the femtosecond time-resolved photoinduced excited-state structural dynamics of ,-1,3-cyclooctadiene, a large-flexible cyclic conjugated diene molecule, upon excitation with 200 nm using mega-electron-volt ultrafast electron diffraction and trajectory surface hopping dynamics simulations.
View Article and Find Full Text PDFJ Chem Theory Comput
December 2024
State Key Laboratory for Mesoscopic Physics and Collaborative Innovation Center of Quantum Matter, School of Physics, Peking University, Beijing 100871, China.
The Jahn-Teller (JT) effect, as a spontaneous symmetry-breaking mechanism arising from the coupling between electronic and nuclear degrees of freedom, is a widespread phenomenon in molecular and condensed matter systems. Here, we investigate the influence of the JT effect on the photodissociation dynamics of CFI molecules. Based on ab initio calculation, we obtain the three-dimensional potential energy surfaces for and states and establish a diabatic Hamiltonian model to study the wavepacket dynamics in the CFI photodissociation process.
View Article and Find Full Text PDFNat Commun
November 2024
Department of Chemistry, Norwegian University of Science and Technology, Trondheim, Norway.
The fate of thymine upon excitation by ultraviolet radiation has been the subject of intense debate. Today, it is widely believed that its ultrafast excited state gas phase decay stems from a radiationless transition from the bright ππ* state to a dark nπ* state. However, conflicting theoretical predictions have made the experimental data difficult to interpret.
View Article and Find Full Text PDFEnter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!