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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…

化学物理 · 物理学 2024-01-15 Xincheng Miao , Kira Diemer , Roland Mitrić

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…

化学物理 · 物理学 2024-02-15 Jiawei Peng , Hong Liu , Zhenggang Lan

This research examines the nonadiabatic dynamics of cyclobutanone after excitation into the n-3s Rydberg S2 state. It stems from our contribution to the Special Topic of the Journal of Chemical Physics to test the predictive capability of…

化学物理 · 物理学 2024-02-16 Saikat Mukherjee , Rafael S. Mattos , Josene M. Toldo , Hans Lischka , Mario Barbatti

In response to a community prediction challenge, we simulate the nonadiabatic dynamics of cyclobutanone using the mapping approach to surface hopping (MASH). We consider the first 500 fs of relaxation following photo-excitation to the S2…

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…

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…

化学物理 · 物理学 2024-07-23 Ericka Roy Miller , Sean J. Hoehn , Abhijith Kumar , Dehua Jiang , Shane M. Parker

The non-radiative electron-relaxation dynamics in C$_{60}$ molecule is studied after selective initial photoexcitations. The methodology includes nonadibabtic molecular simulation combined with time-dependent density functional theory (DFT)…

原子与分子团簇 · 物理学 2023-06-29 Esam Ali , Mohamed El-Amine Madjet , Ruma De , Thomas Frauenheim , Himadri S. Chakraborty

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…

化学物理 · 物理学 2024-02-16 Olivia Bennett , Antonia Freibert , K. Eryn Spinlove , Graham A. Worth

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 $\pi^{\ast}\leftarrow n$…

化学物理 · 物理学 2024-02-15 Julien Eng , Conor Rankine , Thomas Penfold

The electronic and nuclear dynamics in methanol, following 156~nm photoexcitation, are investigated by combining a detailed analysis of time-resolved photoelectron spectroscopy experiments with electronic structure calculations. The…

Over the last decades, theoretical photochemistry has produced multiple techniques to simulate the nonadiabatic dynamics of molecules. Surprisingly, much less effort has been devoted to adequately describing the first step of a…

化学物理 · 物理学 2024-10-17 Jiří Janoš , Petr Slavíček , Basile F. E. Curchod

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…

We study ultrafast population dynamics in the topological surface state of Sb$_2$Te$_3$ in two-dimensional momentum space with time- and angle-resolved two-photon photoemission. Linear polarized mid-infrared pump pulses are used to permit a…

介观与纳米尺度物理 · 物理学 2023-04-26 J. Reimann , K. Sumida , M. Kakoki , K. A. Kokh , O. E. Tereshchenko , A. Kimura , J. Güdde , U. Höfer

We use the effective Hamiltonian that we recently fitted against the first 306 experimentally observed vibronic transitions of NO2 [J. Chem. Phys. 119, 5923 (2003)] to investigate the time domain nonadiabatic dynamics of this molecule on…

化学物理 · 物理学 2011-11-09 Michaël Sanrey , Marc Joyeux

The ground state carrier dynamics in self-assembled (In,Ga)As/GaAs quantum dots has been studied using time-resolved photoluminescence and transmission. By varying the dot design with respect to confinement and doping, the dynamics is shown…

其他凝聚态物理 · 物理学 2009-11-13 T. Berstermann , T. Auer , H. Kurtze , M. Schwab , D. R. Yakovlev , M. Bayer , J. Wiersig , C. Gies , F. Jahnke , D. Reuter , A. D. Wieck

Through a combined experimental and theoretical approach, we study the nonadiabatic dynamics of the prototypical ethylene (C$_2$H$_4$) molecule upon $\pi \rightarrow \pi^*$ excitation with 161 nm light. Using a novel experimental apparatus,…

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…

化学物理 · 物理学 2024-02-20 Patricia Vindel-Zandbergen , Jesús González-Vázquez

New ab-initio surface hopping simulations of the excited state dynamics of CS$_2$ including spin-orbit coupling are compared to new experimental measurements using a multiphoton ionisation probe in a photoelectron spectroscopy experiment.…

The photodissociation dynamics of N$_3^+$ excited from its $^3 \Sigma_{\rm g}^{-}$ ground to the first excited singlet and triplet states is investigated. Three dimensional potential energy surfaces for the $^1$A$'$, $^1$A$''$, and $^3$A$'$…

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…

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