Journal
SCIENCE
Volume 346, Issue 6216, Pages 1492-1495Publisher
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.1259995
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- Engineering and Physical Sciences Research Council, Univ. of Sheffield
- Science and Technology Facilities Council
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Electron transfer (ET) from donor to acceptor is often mediated by nuclear-electronic (vibronic) interactions in molecular bridges. Using an ultrafast electronic-vibrational-vibrational 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.
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