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Tichnell CR, Daley DR, Stein BW, et al. Wave Function Control of Charge-Separated Excited-State Lifetimes. J Am Chem Soc. 2019;141(9):3986-3992doi: 10.1021/jacs.8b13011.
Tichnell, C. R., Daley, D. R., Stein, B. W., Shultz, D. A., Kirk, M. L., & Danilov, E. O. (2019). Wave Function Control of Charge-Separated Excited-State Lifetimes. Journal of the American Chemical Society, 141(9), 3986-3992. https://doi.org/10.1021/jacs.8b13011
Tichnell, Christopher R, et al. "Wave Function Control of Charge-Separated Excited-State Lifetimes." Journal of the American Chemical Society vol. 141,9 (2019): 3986-3992. doi: https://doi.org/10.1021/jacs.8b13011
Tichnell CR, Daley DR, Stein BW, Shultz DA, Kirk ML, Danilov EO. Wave Function Control of Charge-Separated Excited-State Lifetimes. J Am Chem Soc. 2019 Mar 06;141(9):3986-3992. doi: 10.1021/jacs.8b13011. Epub 2019 Feb 22. PMID: 30707581.
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J Am Chem Soc. 2019 Mar 06;141(9):3986-3992. doi: 10.1021/jacs.8b13011. Epub 2019 Feb 22.

Wave Function Control of Charge-Separated Excited-State Lifetimes.

Journal of the American Chemical Society

Christopher R Tichnell, David R Daley, Benjamin W Stein, David A Shultz, Martin L Kirk, Evgeny O Danilov

Affiliations

  1. Department of Chemistry , North Carolina State University , Raleigh , North Carolina 27695-8204 , United States.
  2. Department of Chemistry and Chemical Biology , The University of New Mexico , MSC03 2060, 1 University of New Mexico , Albuquerque , New Mexico 87131-0001 , United States.

PMID: 30707581 DOI: 10.1021/jacs.8b13011

Abstract

Control of excited-state processes is crucial to an increasing number of important device technologies that include displays, photocatalysts, solar energy conversion devices, photovoltaics, and photonics. However, the manipulation and control of electronic excited-state lifetimes and properties continue to be a challenge for molecular scientists. Herein, we present the results of ground-state and transient absorption spectroscopies as they relate to magnetic exchange control of excited-state lifetimes. We describe a novel mechanism for controlling these excited-state lifetimes that involves varying the magnetic exchange interaction between a stable organic radical and the unpaired electrons present in the open-shell configuration of a charge-separated excited state. Specifically, we show that the excited-state lifetime can be controlled in a predictable manner based on an a priori knowledge of the pairwise magnetic exchange interactions between excited-state spins. These magnetic exchange couplings affect the excited-state electronic structure in a manner that introduces variable degrees of spin forbiddenness into the nonradiative decay channel between the excited state and the electronic ground state.

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