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Toward time-resolved laser T-jump/X-ray probe spectroscopy in aqueous solutions
Most chemical and biochemical reactions in nature and in industrial processes are driven by thermal effects that bring the reactants above the energy barrier for reaction. In aqueous solutions, this process can also be triggered by the laser driven temperature jump (T-jump) method, in which the wate...
Autores principales: | , , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
American Crystallographic Association
2019
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6906120/ https://www.ncbi.nlm.nih.gov/pubmed/31832487 http://dx.doi.org/10.1063/1.5129626 |
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author | Cannelli, O. Bacellar, C. Ingle, R. A. Bohinc, R. Kinschel, D. Bauer, B. Ferreira, D. S. Grolimund, D. Mancini, G. F. Chergui, M. |
author_facet | Cannelli, O. Bacellar, C. Ingle, R. A. Bohinc, R. Kinschel, D. Bauer, B. Ferreira, D. S. Grolimund, D. Mancini, G. F. Chergui, M. |
author_sort | Cannelli, O. |
collection | PubMed |
description | Most chemical and biochemical reactions in nature and in industrial processes are driven by thermal effects that bring the reactants above the energy barrier for reaction. In aqueous solutions, this process can also be triggered by the laser driven temperature jump (T-jump) method, in which the water vibrational (stretch, bend, or combination) modes are excited by a short laser pulse, leading to a temperature increase in the irradiated volume within a few picoseconds. The combination of the laser T-jump with X-ray spectroscopic probes would add element-specificity as well as sensitivity to the structure, the oxidation state, and the spin state of the intermediates of reactions. Here, we present preliminary results of a near infrared pump/X-ray absorption spectroscopy probe to study the ligand exchange of an octahedral aqueous Cobalt complex, which is known to pass through intermediate steps yielding tetrahedral chlorinated as final species. The structural changes of the chemical reaction are monitored with great sensitivity, even in the presence of a mild local increase in temperature. This work opens perspectives for the study of non-light-driven reactions using time-resolved X-ray spectroscopic methods. |
format | Online Article Text |
id | pubmed-6906120 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2019 |
publisher | American Crystallographic Association |
record_format | MEDLINE/PubMed |
spelling | pubmed-69061202019-12-12 Toward time-resolved laser T-jump/X-ray probe spectroscopy in aqueous solutions Cannelli, O. Bacellar, C. Ingle, R. A. Bohinc, R. Kinschel, D. Bauer, B. Ferreira, D. S. Grolimund, D. Mancini, G. F. Chergui, M. Struct Dyn ARTICLES Most chemical and biochemical reactions in nature and in industrial processes are driven by thermal effects that bring the reactants above the energy barrier for reaction. In aqueous solutions, this process can also be triggered by the laser driven temperature jump (T-jump) method, in which the water vibrational (stretch, bend, or combination) modes are excited by a short laser pulse, leading to a temperature increase in the irradiated volume within a few picoseconds. The combination of the laser T-jump with X-ray spectroscopic probes would add element-specificity as well as sensitivity to the structure, the oxidation state, and the spin state of the intermediates of reactions. Here, we present preliminary results of a near infrared pump/X-ray absorption spectroscopy probe to study the ligand exchange of an octahedral aqueous Cobalt complex, which is known to pass through intermediate steps yielding tetrahedral chlorinated as final species. The structural changes of the chemical reaction are monitored with great sensitivity, even in the presence of a mild local increase in temperature. This work opens perspectives for the study of non-light-driven reactions using time-resolved X-ray spectroscopic methods. American Crystallographic Association 2019-12-11 /pmc/articles/PMC6906120/ /pubmed/31832487 http://dx.doi.org/10.1063/1.5129626 Text en © 2019 Author(s). 2329-7778/2019/6(6)/064303/8 All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/). |
spellingShingle | ARTICLES Cannelli, O. Bacellar, C. Ingle, R. A. Bohinc, R. Kinschel, D. Bauer, B. Ferreira, D. S. Grolimund, D. Mancini, G. F. Chergui, M. Toward time-resolved laser T-jump/X-ray probe spectroscopy in aqueous solutions |
title | Toward time-resolved laser T-jump/X-ray probe spectroscopy in aqueous solutions |
title_full | Toward time-resolved laser T-jump/X-ray probe spectroscopy in aqueous solutions |
title_fullStr | Toward time-resolved laser T-jump/X-ray probe spectroscopy in aqueous solutions |
title_full_unstemmed | Toward time-resolved laser T-jump/X-ray probe spectroscopy in aqueous solutions |
title_short | Toward time-resolved laser T-jump/X-ray probe spectroscopy in aqueous solutions |
title_sort | toward time-resolved laser t-jump/x-ray probe spectroscopy in aqueous solutions |
topic | ARTICLES |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6906120/ https://www.ncbi.nlm.nih.gov/pubmed/31832487 http://dx.doi.org/10.1063/1.5129626 |
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