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Proton-coupled electron transfer (PCET) is foundational to catalysis, bioenergetics, and energy conversion, yet capturing and disentangling the coupled motions of electrons, protons, and solvent has remained a major experimental challenge.…

We develop a detailed theoretical model of photo-induced proton-coupled electron transfer (PPCET) processes, which are at the basis of solar energy harvesting in biological systems and photovoltaic materials. Our model enables to analyze…

化学物理 · 物理学 2021-04-13 Jiaji Zhang , Raffaele Borrelli , Yoshitaka Tanimura

Photo-ionization induced ultrafast electron dynamics is considered as a precursor to the slower nuclear dynamics associated with molecular dissociation. Here, using ab initio multielectron wave-packet propagation method, we study the…

化学物理 · 物理学 2022-11-30 K. Chordiya , V. Despré , B. Nagyillés , F. Zeller , Z. Diveki , A. I. Kuleff , M. U. Kahaly

Pump-push-probe spectroscopy was employed for the exploration of charge-separation processes in organic photovoltaic blends as well as for proton-coupled electron-transfer (PCET) reactions in hydrogen-bonded complexes of…

化学物理 · 物理学 2025-05-07 Sebastian V. Pios , Maxim F. Gelin , Wolfgang Domcke , Lipeng Chen

We present a conspectus of recent joint spectroscopic and computational studies which provided novel insight into the photochemistry of hydrogen-bonded complexes of the heptazine (Hz) chromophore with hydroxylic substrate molecules (water…

化学物理 · 物理学 2020-07-01 Wolfgang Domcke , Andrzej L. Sobolewski , Cody W. Schlenker

Hydrogen-release by photoexcitation, excited-state- hydrogen-transfer (ESHT), is one of the important photo- chemical processes that occur in aromatic acids and is responsible for photoprotection of biomolecules. The mecha- nism is…

A deep understanding of molecular photo-transformations is challenging because of the complex interaction between the configurations of electrons and nuclei. An initial optical excitation dissipates energy into electronic and structural…

The interaction of exciton and charge transfer (CT) states plays a central role in photo-induced CT processes in chemistry, biology and physics. In this work, we use a combination of two-dimensional electronic spectroscopy (2D-ES),…

We investigate photoinduced proton-coupled electron transfer (PI-PCET) reaction through a recently devel- oped quasi-diabatic (QD) quantum dynamics propagation scheme. This scheme enables interfacing accurate diabatic-based quantum dynamics…

化学物理 · 物理学 2018-08-01 Arkajit Mandal , Farnaz A. Shakib , Pengfei Huo

The element specificity of soft X-ray spectroscopy makes it an ideal tool for analyzing the microscopic origin of ultrafast dynamics induced by localized optical excitation in metal-insulator heterostructures. Using [Fe/MgO]$_n$ as a model…

Proton-coupled electron transfers (PCET) are elementary steps in electrocatalysis. However, accurate calculations of PCET rates remain challenging, especially considering nuclear quantum effects (NQEs) under a constant potential condition.…

化学物理 · 物理学 2025-06-23 Li Fu , Yifan Li , Menglin Sun , Xiaolong Yang , Bin Jin , Shenzhen Xu

We theoretically investigate an exciton-coupled electron transfer (XCET) process that is conversion of an exciton into a charge transfer state. This conversion happens in an exciton transfer (XT) process, and the electron moves away in an…

量子物理 · 物理学 2017-11-03 Souichi Sakamoto , Yoshitaka Tanimura

Charge transfer is a fundamental phenomenon in biology and chemistry, and involves the movement of charge through a system driven by nuclear dynamics. Because of the involvement of nuclear motion, it is generally assumed that charge…

化学物理 · 物理学 2024-08-27 Simon P. Neville , Martha Yaghoubi Jouybari , Michael S. Schuurman

Excited state hydrogen transfer (ESHT) is responsible to various photochemical processes of aromatics including photoprotection of nuclear basis. Its mechanism is explained by the internal conversion from aromatic $\pi$$\pi$* to…

原子与分子团簇 · 物理学 2017-12-06 Mitsuhiko Miyazaki , Ryuhei Ohara , Claude Dedonder , Christophe Jouvet , Masaaki Fujii

In condensed matter, scattering processes determine the transport of charge carriers. In case of heterostructures, interfaces determine many dynamic properties like charge transfer and transport and spin current dynamics. Here we discuss…

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…

Effective photoinduced charge transfer makes molecular bimetallic assemblies attractive for applications as active light induced proton reduction systems. For a more sustainable future, development of competitive base metal dyads is…

Electronic Energy Transfer (EET) between chromophores is fundamental in many natural light-harvesting complexes, serving as a critical step for solar energy funneling in photosynthetic plants and bacteria. The complicated role of the…

化学物理 · 物理学 2024-02-05 Colin Coane , Marco Romanelli , Giulia Dall'Osto , Rosa Di Felice , Stefano Corni

Ultrafast multistage electron transfer (ET) in molecular systems with multiple redox centers is fundamental to photochemical energy conversion, including processes in natural photosynthesis, molecular optoelectronics, and organic…

化学物理 · 物理学 2025-07-29 Serguei Feskov , Anatoly Ivanov

Photocatalysis induced by sunlight is one of the most promising approach to environmental protection, solar energy conversion and sustainable production of fuels. The computational modeling of photocatalysis is a rapidly expending field…

材料科学 · 物理学 2020-04-14 Yvelin Giret , Pu Guo , Li-Feng Wang , Jun Cheng
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