Visualizing Interfacial Charge Transfer in Ru-Dye-Sensitized TiO2 Nanoparticles Using X-ray Transient Absorption Spectroscopy

2011 ◽  
Vol 2 (6) ◽  
pp. 628-632 ◽  
Author(s):  
Xiaoyi Zhang ◽  
Grigory Smolentsev ◽  
Jianchang Guo ◽  
Klaus Attenkofer ◽  
Chuck Kurtz ◽  
...  
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.


2021 ◽  
Author(s):  
Ying Liu ◽  
Jianmin Lu ◽  
Qianxiao Zhang ◽  
Yajie Bai ◽  
Xuliang Pang ◽  
...  

Decoration of Ag-ultrathin Ni-MOF onside Cu2O was firstly fabricated. The charge-transfer dynamics at heterostructure was in-depth revealed by ultrafast transient absorption spectroscopy. NH3 yield rate (4.63 μg h-1 cm-2) with...


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’.


2013 ◽  
Vol 117 (39) ◽  
pp. 9807-9813 ◽  
Author(s):  
Michael R. Harpham ◽  
Andrew, B. Stickrath ◽  
Xiaoyi, Zhang ◽  
Jier Huang ◽  
Michael W. Mara ◽  
...  

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