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Title: Monitoring Long-Range Electron Transfer Pathways in Proteins by Stimulated Attosecond Broadband X-ray Raman Spectroscopy

Abstract

In this study, long-range electron transfer (ET) plays a key role in many biological energy conversion and synthesis processes. We show that nonlinear spectroscopy with attosecond X-ray pulses provides a real time movie of the evolving oxidation states and electron densities around atoms, and can probe these processes with high spatial and temporal resolution. This is demonstrated in a simulation study of the stimulated X-ray Raman (SXRS) signals in Re-modified azurin, which had long served as a benchmark for long-range ET in proteins. Nonlinear SXRS signals are sensitive to the local electronic structure and should offer a novel window for long-range ET.

Authors:
 [1];  [1];  [2];  [1]
  1. Department of Chemistry, University of California, 450 Rowland Hall, Irvine, California 92697, United States
  2. William R. Wiley Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, P.O. Box 999, Richland, Washington 99352, United States
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1163490
Alternate Identifier(s):
OSTI ID: 1167649
Report Number(s):
PNNL-SA-102075
Journal ID: ISSN 1948-7185
Grant/Contract Number:  
ER15571; AC05-76RL01830
Resource Type:
Published Article
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Name: Journal of Physical Chemistry Letters Journal Volume: 5 Journal Issue: 21; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; attosecond; X-ray; Raman; spectroscopy; electron transfer; oxidation; Environmental Molecular Sciences Laboratory

Citation Formats

Zhang, Yu, Biggs, Jason D., Govind, Niranjan, and Mukamel, Shaul. Monitoring Long-Range Electron Transfer Pathways in Proteins by Stimulated Attosecond Broadband X-ray Raman Spectroscopy. United States: N. p., 2014. Web. doi:10.1021/jz501966h.
Zhang, Yu, Biggs, Jason D., Govind, Niranjan, & Mukamel, Shaul. Monitoring Long-Range Electron Transfer Pathways in Proteins by Stimulated Attosecond Broadband X-ray Raman Spectroscopy. United States. https://doi.org/10.1021/jz501966h
Zhang, Yu, Biggs, Jason D., Govind, Niranjan, and Mukamel, Shaul. Tue . "Monitoring Long-Range Electron Transfer Pathways in Proteins by Stimulated Attosecond Broadband X-ray Raman Spectroscopy". United States. https://doi.org/10.1021/jz501966h.
@article{osti_1163490,
title = {Monitoring Long-Range Electron Transfer Pathways in Proteins by Stimulated Attosecond Broadband X-ray Raman Spectroscopy},
author = {Zhang, Yu and Biggs, Jason D. and Govind, Niranjan and Mukamel, Shaul},
abstractNote = {In this study, long-range electron transfer (ET) plays a key role in many biological energy conversion and synthesis processes. We show that nonlinear spectroscopy with attosecond X-ray pulses provides a real time movie of the evolving oxidation states and electron densities around atoms, and can probe these processes with high spatial and temporal resolution. This is demonstrated in a simulation study of the stimulated X-ray Raman (SXRS) signals in Re-modified azurin, which had long served as a benchmark for long-range ET in proteins. Nonlinear SXRS signals are sensitive to the local electronic structure and should offer a novel window for long-range ET.},
doi = {10.1021/jz501966h},
journal = {Journal of Physical Chemistry Letters},
number = 21,
volume = 5,
place = {United States},
year = {Tue Oct 14 00:00:00 EDT 2014},
month = {Tue Oct 14 00:00:00 EDT 2014}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1021/jz501966h

Citation Metrics:
Cited by: 16 works
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