TY - JOUR

T1 - Readout of spin quantum beats in a charge-separated radical pair by pump-push spectroscopy

AU - Mims, David

AU - Herpich, Jonathan

AU - Lukzen, Nikita N.

AU - Steiner, Ulrich E.

AU - Lambert, Christoph

N1 - This work was supported by Deutsche Forschungsgemeinschaft grant LA991/20-1 (C.L. and D.M.); the SolTech Initiative of the Bavarian State Ministry of Education, Culture, Science, and the Arts; and Ministry of Science and Higher Education of the Russian Federation grant 075-15-2020-779 (N.N.L.). Publisher Copyright: © 2021 American Association for the Advancement of Science. All rights reserved.

PY - 2021/12/17

Y1 - 2021/12/17

N2 - Spin quantum beats prove the quantum nature of reactions involving radical pairs, the key species of spin chemistry. However, such quantum beats remain hidden to transient absorption-based optical observation because the spin hardly affects the absorption properties of the radical pairs. We succeed in demonstrating such quantum beats in the photoinduced charge-separated state (CSS) of an electron donor-acceptor dyad by using two laser pulses-one for pumping the sample and another one, with variable delay, for further exciting the CSS to a higher electronic state, wherein ultrafast recombination to distinct, optically detectable products of singlet or triplet multiplicity occurs. This represents a spin quantum measurement of the spin state of the CSS at the time instant of the second (push) pulse.

AB - Spin quantum beats prove the quantum nature of reactions involving radical pairs, the key species of spin chemistry. However, such quantum beats remain hidden to transient absorption-based optical observation because the spin hardly affects the absorption properties of the radical pairs. We succeed in demonstrating such quantum beats in the photoinduced charge-separated state (CSS) of an electron donor-acceptor dyad by using two laser pulses-one for pumping the sample and another one, with variable delay, for further exciting the CSS to a higher electronic state, wherein ultrafast recombination to distinct, optically detectable products of singlet or triplet multiplicity occurs. This represents a spin quantum measurement of the spin state of the CSS at the time instant of the second (push) pulse.

UR - http://www.scopus.com/inward/record.url?scp=85122353194&partnerID=8YFLogxK

U2 - 10.1126/science.abl4254

DO - 10.1126/science.abl4254

M3 - Article

C2 - 34914495

AN - SCOPUS:85122353194

VL - 374

SP - 1470

EP - 1474

JO - Science

JF - Science

SN - 0036-8075

IS - 6574

ER -