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Title: Monitoring long-range electron transfer pathways in proteins by stimulated attosecond broadband X-ray Raman spectroscopy

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. Univ. of California, Irvine, CA (United States)
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Publication Date:
Report Number(s):
PNNL-SA-102075
Journal ID: ISSN 1948-7185; 48153; KP1704020
Grant/Contract Number:
AC05-76RL01830; ER15571
Type:
Published Article
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 5; Journal Issue: 21; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Research Org:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; SPECTROSCOPY; ELECTRON TRANSFER; OXIDATION; attosecond; X-ray; Raman; spectroscopy; electron transfer; oxidation; Environmental Molecular Sciences Laboratory
OSTI Identifier:
1163490
Alternate Identifier(s):
OSTI ID: 1167649

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., 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. doi:10.1021/jz501966h.
Zhang, Yu, Biggs, Jason D., Govind, Niranjan, and Mukamel, Shaul. 2014. "Monitoring long-range electron transfer pathways in proteins by stimulated attosecond broadband X-ray Raman spectroscopy". United States. doi: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 = {2014},
month = {10}
}