Light-induced relaxation dynamics of the ferricyanide ion revisited by ultrafast XUV photoelectron spectroscopy
文献信息
Nicholas Engel, Sergey I. Bokarev, Alexandre Moguilevski, Azhr A. Raheem, Ruba Al-Obaidi, Tobias Möhle, Gilbert Grell, Katrin R. Siefermann, Bernd Abel, Saadullah G. Aziz, Oliver Kühn, Mario Borgwardt, Igor Yu. Kiyan
Photoinduced charge transfer in transition-metal coordination complexes plays a prominent role in photosynthesis and is fundamental for light-harvesting processes in catalytic materials. However, revealing the relaxation pathways of charge separation remains a very challenging task because of the complexity of relaxation channels and ultrashort time scales. Here, we employ ultrafast XUV photoemission spectroscopy to monitor fine mechanistic details of the electron dynamics following optical ligand-to-metal charge-transfer excitation of ferricyanide in aqueous solution. XUV probe light with a time resolution of 100 fs, in combination with density functional theory employing the Dyson orbital formalism, enabled us to decipher the primary and subsequently populated electronic states involved in the relaxation, as well as their energetics on sub-picosecond timescales. We find strong evidence for the spin crossover followed by geometrical distortions due to vibronic interactions (Jahn–Teller effect) in the excited electronic states, rather than localization/delocalization dynamics, as suggested previously.
期刊推荐

European Journal of Wood and Wood Products

Nature

Molecular Pharmacology

Organic Preparations and Procedures International

Science Progress

Journal of Catalysis

Russian Chemical Reviews

Journal of Medicinal Chemistry

Proceedings of the National Academy of Sciences of the United States of America

Pure and Applied Chemistry
相关文献
A chemoenzymatic route to N-acetylglucosamine-1-phosphate analogues: substrate specificity investigations of N-acetylhexosamine 1-kinase
Li Cai, Motomitsu Kitaoka, Jie Shen, Chengfeng Xia, Wenlan Chen, Peng George Wang
DOI: 10.1039/B904853G
High performance, acene-based organic thin film transistors
Gonzalo Rincon Llorente, Marie-Beatrice Dufourg-Madec, David J. Crouch, Robin G. Pritchard, Simon Ogier, Stephen G. Yeates
DOI: 10.1039/B901448A
Sonochemical synthesis of MOF-5
Won-Jin Son, Jun Kim, Jaheon Kim, Wha-Seung Ahn
DOI: 10.1039/B814740J
7-Mercapto-4-methylcoumarin as a reporter of thiol binding to the CdSe quantum dot surface
María González-Béjar, Mathieu Frenette, Larissa Jorge, J. C. Scaiano
DOI: 10.1039/B900606K
meso-Octamethylcalix[4]pyrrole: an old yet new transmembrane ion-pair transporter‡
Christine C. Tong, Roberto Quesada, Jonathan L. Sessler, Philip A. Gale
DOI: 10.1039/B814988G
Controlled catch and release of small molecules with cucurbit[6]urilvia a kinetic trap
Li Liu, Nicolas Nouvel, Oren A. Scherman
DOI: 10.1039/B903033F
Fabrication of living cellosomes of rod-like and rhombohedral morphologies based on magnetically responsive templates
Vesselin N. Paunov
DOI: 10.1039/B902260K
Site-isolated, intermolecularly photocrosslinkable and patternable dendritic quinacridones
Gemma D. D’Ambruoso, Eric E. Ross, Neal R. Armstrong, Dominic V. McGrath
DOI: 10.1039/B901897B
An efficient didehydroxylation method for the biomass-derived polyols glycerol and erythritol. Mechanistic studies of a formic acid-mediated deoxygenation
Elena Arceo, Peter Marsden, Robert G. Bergman, Jonathan A. Ellman
DOI: 10.1039/B907746D
您可能还喜欢
N-2,2-丙烯基-2-丙烯酰胺(CAS号:2555-13-7)通常如何合成?
N-2,2-丙烯基-2-丙烯酰胺通常通过丙烯酰胺与丙烯基卤化物的缩合反应合成。该反应通常在温和的条件下进行,使用适量的碱如吡啶作为催化剂。反应的选择性良好,产率...
什么是1,2-二碘四氟代乙烷(CAS号:354-65-4)?
1,2-二碘四氟代乙烷是一种有机化合物,化学式为C2F4I2,CAS号为354-65-4。它是一种无色透明液体,具有特殊的化学性质和物理性质,包括高沸点、低挥发...
3-溴-1H-吡咯[3,2-c]吡啶-4-碳腈(CAS号:1000341-71-8)适用哪些法规指南?
根据GHS(全球化学品统一分类和标签制度),3-溴-1H-吡咯[3,2-c]吡啶-4-碳腈被归类为第2类易燃液体。在欧盟,该化合物需要符合REACH法规的要求,...
1-氯甲基萘磺酸(CAS号:87491-79-0)安全吗?
1-氯甲基萘磺酸在使用时需要谨慎,因为它具有一定的刺激性和腐蚀性。操作时应佩戴适当的防护装备,如防化服、手套、护目镜等,避免直接接触皮肤和吸入其蒸汽。
二氯(二环戊二烯)铂(CAS号:12083-92-0)的主要用途是什么?
该化合物主要用于催化剂领域,特别是在有机合成中的催化氧化反应以及作为某些药物合成的中间体。此外,它还被研究用于纳米材料的制备。
3-溴-7-氯噻吩并[3,2-b]吡啶-6-甲腈(CAS号:798574-82-0)安全吗?
3-溴-7-氯噻吩并[3,2-b]吡啶-6-甲腈在处理时需要谨慎,因其含有溴和氯等强卤素,可能具有一定的刺激性和腐蚀性。使用时应佩戴适当的个人防护装备,避免皮肤...
(R)-1-((R)-2-(2’-二环己基膦苯基)三戊铁基]乙基(双-3,5-三氟甲基苯基)膦(CAS号:494227-32-6)的主要用途是什么?
该化合物主要用于有机合成领域,特别是作为催化剂或配体,在有机合成反应中发挥重要作用。此外,它还可能应用于催化加氢反应、偶联反应等。
3-[6-(Diphenylphosphoryl)-2-naphthyl]-1,10-phenanthroline(CAS号:1480371-38-7)安全吗?
3-[6-(Diphenylphosphoryl)-2-naphthyl]-1,10-phenanthroline在正常使用条件下相对安全,但在操作时应穿戴适当...
在合成中是否有ETHYL 2-(4-(4,4,5,5-TETRAMETHYL-1,3,2-DIOXABOROLAN-2-YL)CYCLOHEX-3-ENYL)ACETATE(CAS号:1166829-70-4)的替代品?
可以考虑使用类似结构的化合物作为替代品,如2-(4-环戊基环己烯基)乙酸酯,这种化合物在结构上相似,可能在某些合成路径中作为替代品。
如何处理含有3-(3-氨基丙基)丙酮缩甘油(CAS号:131606-42-3)的废料?
处理含有3-(3-氨基丙基)丙酮缩甘油的废料时,首先应确保遵守当地的环保法规。对于危险废物,应进行分类收集,然后送至专业的废物处理设施进行焚烧或安全填埋。在处理...
来源期刊
Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.



![1-Benzyl-1,7-diazaspiro[4.4]nonane dihydrochloride structure 1-Benzyl-1,7-diazaspiro[4.4]nonane dihydrochloride structure](https://cnstatic.chemtradehub.com/structs/115/1159822-71-5-0320.webp)
![1H-Imidazo[4,5-c]pyridine-7-carboxylic acid structure 1H-Imidazo[4,5-c]pyridine-7-carboxylic acid structure](https://cnstatic.chemtradehub.com/structs/123/1234616-39-7-1344.webp)