Excited-State Bond Contraction and Charge Migration in a Platinum Dimer Complex Characterized by X-ray and Optical Transient Absorption Spectroscopy

Author(s):  
Nicholas P. Weingartz ◽  
Michael W. Mara ◽  
Subhangi Roy ◽  
Jiyun Hong ◽  
Arnab Chakraborty ◽  
...  
2021 ◽  
Vol 23 (5) ◽  
pp. 3656-3667
Author(s):  
Lucía Velasco ◽  
Leonel Llanos ◽  
Pedro Levín ◽  
Andrés Vega ◽  
Jin Yu ◽  
...  

Three homoleptic Cu(i) dimeric photosensitizers are studied through ultrafast X-ray and optical absorption spectroscopy. The complexes show distinct excited state lifetimes, due to the solvent type and spacers' flexibilities between the Cu centres.


2010 ◽  
Vol 114 (48) ◽  
pp. 12780-12787 ◽  
Author(s):  
Jenny V. Lockard ◽  
Aaron A. Rachford ◽  
Grigory Smolentsev ◽  
Andrew B. Stickrath ◽  
Xianghuai Wang ◽  
...  

Author(s):  
Lin X. Chen ◽  
Xiaoyi Zhang ◽  
Jenny V. Lockard ◽  
Andrew B. Stickrath ◽  
Klaus Attenkofer ◽  
...  

Transient molecular structures along chemical reaction pathways are important for predicting molecular reactivity, understanding reaction mechanisms, as well as controlling reaction pathways. During the past decade, X-ray transient absorption spectroscopy (XTA, or LITR-XAS, laser-initiated X-ray absorption spectroscopy), analogous to the commonly used optical transient absorption spectroscopy, has been developed. XTA uses a laser pulse to trigger a fundamental chemical process, and an X-ray pulse(s) to probe transient structures as a function of the time delay between the pump and probe pulses. Using X-ray pulses with high photon flux from synchrotron sources, transient electronic and molecular structures of metal complexes have been studied in disordered media from homogeneous solutions to heterogeneous solution–solid interfaces. Several examples from the studies at the Advanced Photon Source in Argonne National Laboratory are summarized, including excited-state metalloporphyrins, metal-to-ligand charge transfer (MLCT) states of transition metal complexes, and charge transfer states of metal complexes at the interface with semiconductor nanoparticles. Recent developments of the method are briefly described followed by a future prospective of XTA. It is envisioned that concurrent developments in X-ray free-electron lasers and synchrotron X-ray facilities as well as other table-top laser-driven femtosecond X-ray sources will make many breakthroughs and realise dreams of visualizing molecular movies and snapshots, which ultimately enable chemical reaction pathways to be controlled.


Author(s):  
Jungkweon Choi ◽  
Mina Ahn ◽  
Jae Hyuk Lee ◽  
Doo-Sik Ahn ◽  
Hosung Ki ◽  
...  

The experimental and calculation results demonstrate that the 3MLppzCT state generated by the spin-forbidden transition rapidly relaxes to 3MLppyCT through internal conversion process with a time constant of ∼450 fs.


2014 ◽  
Vol 136 (24) ◽  
pp. 8804-8809 ◽  
Author(s):  
Xiaoyi Zhang ◽  
Sophie E. Canton ◽  
Grigory Smolentsev ◽  
Carl-Johan Wallentin ◽  
Yizhu Liu ◽  
...  

2018 ◽  
Vol 9 (4) ◽  
pp. 860-875 ◽  
Author(s):  
Dugan Hayes ◽  
Lars Kohler ◽  
Ryan G. Hadt ◽  
Xiaoyi Zhang ◽  
Cunming Liu ◽  
...  

Complementary ultrafast techniques provide clear observation of charge hopping between metals in dinuclear complexes.


ChemSusChem ◽  
2018 ◽  
Vol 11 (14) ◽  
pp. 2421-2428 ◽  
Author(s):  
Jiyun Hong ◽  
Matthew S. Kelley ◽  
Megan L. Shelby ◽  
Dugan K. Hayes ◽  
Ryan G. Hadt ◽  
...  

2014 ◽  
Vol 43 (47) ◽  
pp. 17615-17623 ◽  
Author(s):  
J. Huang ◽  
M. W. Mara ◽  
A. B. Stickrath ◽  
O. Kokhan ◽  
M. R. Harpham ◽  
...  

Steady-state and transient structures of a copper diimine dye sensitizer on TiO2 nanoparticles undergoing photoinduced interfacial electron transfer are determined.


2021 ◽  
Vol 3 (1) ◽  
Author(s):  
Giovanni Cistaro ◽  
Luis Plaja ◽  
Fernando Martín ◽  
Antonio Picón

Author(s):  
Romain Geneaux ◽  
Hugo J. B. Marroux ◽  
Alexander Guggenmos ◽  
Daniel M. Neumark ◽  
Stephen R. Leone

Attosecond science opened the door to observing nuclear and electronic dynamics in real time and has begun to expand beyond its traditional grounds. Among several spectroscopic techniques, X-ray transient absorption spectroscopy has become key in understanding matter on ultrafast time scales. In this review, we illustrate the capabilities of this unique tool through a number of iconic experiments. We outline how coherent broadband X-ray radiation, emitted in high-harmonic generation, can be used to follow dynamics in increasingly complex systems. Experiments performed in both molecules and solids are discussed at length, on time scales ranging from attoseconds to picoseconds, and in perturbative or strong-field excitation regimes. This article is part of the theme issue ‘Measurement of ultrafast electronic and structural dynamics with X-rays’.


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