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

Research output: Contribution to journalArticle

83 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.

LanguageEnglish
Pages1492-1495
Number of pages4
JournalScience
Volume346
Issue number6216
DOIs
Publication statusPublished - 19 Dec 2014
Externally publishedYes

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Infrared radiation
Molecules
Electrons
Chemical reactivity
Platinum

Cite this

Delor, M., Scattergood, P. A., Sazanovich, I. V., Parker, A. W., Greetham, G. M., Meijer, A. J. H. 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
Delor, Milan ; Scattergood, Paul A. ; Sazanovich, Igor V. ; Parker, Anthony W. ; Greetham, Gregory M. ; Meijer, Anthony J H M ; Towrie, Michael ; Weinstein, Julia A. / Toward control of electron transfer in donor-acceptor molecules by bond-specific infrared excitation. In: Science. 2014 ; Vol. 346, No. 6216. pp. 1492-1495.
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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.",
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Delor, M, Scattergood, PA, Sazanovich, IV, Parker, AW, Greetham, GM, Meijer, AJHM, Towrie, M & Weinstein, JA 2014, 'Toward control of electron transfer in donor-acceptor molecules by bond-specific infrared excitation', Science, vol. 346, no. 6216, pp. 1492-1495. https://doi.org/10.1126/science.1259995

Toward control of electron transfer in donor-acceptor molecules by bond-specific infrared excitation. / Delor, Milan; Scattergood, Paul A.; Sazanovich, Igor V.; Parker, Anthony W.; Greetham, Gregory M.; Meijer, Anthony J H M; Towrie, Michael; Weinstein, Julia A.

In: Science, Vol. 346, No. 6216, 19.12.2014, p. 1492-1495.

Research output: Contribution to journalArticle

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AU - Delor, Milan

AU - Scattergood, Paul A.

AU - Sazanovich, Igor V.

AU - Parker, Anthony W.

AU - Greetham, Gregory M.

AU - Meijer, Anthony J H M

AU - Towrie, Michael

AU - Weinstein, Julia A.

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AB - 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.

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