Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 113, Issue 36, Pages 10001-10006Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1610729113
Keywords
electron transfer; coherent control; ultrafast X-ray spectroscopy; stimulated Raman
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Funding
- Chemical Sciences, Geosciences and Biosciences Division, Office of Basic Energy Sciences, Office of Science, US Department of Energy (DOE) [DE-FG02-04ER15571]
- DOE
- National Science Foundation [CHE-1361516]
- Science and Engineering Research Council at Singapore Agency for Science, Technology, and Research X-ray Photonics Program [1426500053]
- Direct For Mathematical & Physical Scien [1361516] Funding Source: National Science Foundation
- Division Of Chemistry [1361516] Funding Source: National Science Foundation
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We show that X-ray pulses resonant with selected core transitions can manipulate electron transfer (ET) in molecules with ultrafast and atomic selectivity. We present possible protocols for coherently controlling ET dynamics in donor-bridge-acceptor (DBA) systems by stimulated X-ray resonant Raman processes involving various transitions between the D, B, and A sites. Simulations presented for a Ru(II)-Co(III) model complex demonstrate how the shapes, phases and amplitudes of the X-ray pulses can be optimized to create charge on demand at selected atoms, by opening up otherwise blocked ET pathways.
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