Toward control of electron transfer in donor-acceptor molecules by bond-specific infrared excitation

Milan Delor, Paul A. Scattergood, Igor V. Sazanovich, Anthony W. Parker, Gregory M. Greetham, Anthony J H M Meijer, Michael Towrie, Julia A. Weinstein

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94 Citations (Scopus)

Abstract

Electron transfer (ET) from donor to acceptor is often mediated by nuclear-electronic (vibronic) interactions in molecular bridges. Using an ultrafast electronic-vibrationalvibrational pulse-sequence, we demonstrate how the outcome of light-induced ET can be radically altered by mode-specific infrared (IR) excitation of vibrations that are coupled to the ET pathway. Picosecond narrow-band IR excitation of high-frequency bridge vibrations in an electronically excited covalent trans-acetylide platinum(II) donor-bridge-acceptor system in solution alters both the dynamics and the yields of competing ET pathways, completely switching a charge separation pathway off. These results offer a step toward quantum control of chemical reactivity by IR excitation. We are grateful to M. Newton (Brookhaven National Laboratory), D. Phillips (Imperial College London), A. Orr-Ewing (Univ. of Bristol), D. Clary (Univ. of Oxford), and G. Worth (Univ. of Birmingham) for comments on the manuscript; to I. Rubtsov and R. Schmehl (Tulane University) for discussions; and to the Engineering and Physical Sciences Research Council, Univ. of Sheffield, and Science and Technology Facilities Council for support.

Original languageEnglish
Pages (from-to)1492-1495
Number of pages4
JournalScience
Volume346
Issue number6216
DOIs
Publication statusPublished - 19 Dec 2014
Externally publishedYes

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    Delor, M., Scattergood, P. A., Sazanovich, I. V., Parker, A. W., Greetham, G. M., Meijer, A. J. H. M., Towrie, M., & Weinstein, J. A. (2014). Toward control of electron transfer in donor-acceptor molecules by bond-specific infrared excitation. Science, 346(6216), 1492-1495. https://doi.org/10.1126/science.1259995