Excited State Exchange Control of Photoinduced Electron Spin Polarization in Electronic Ground States

Kirk, Martin L.; Shultz, David A.; Hewitt, Patrick; van der Est, Art

doi:10.1021/acs.jpclett.1c03491

Title: Excited State Exchange Control of Photoinduced Electron Spin Polarization in Electronic Ground States

Journal Article · 18 January 2022 · Journal of Physical Chemistry Letters

DOI: https://doi.org/10.1021/acs.jpclett.1c03491 · OSTI ID:1908164

^[1];

^[2]; Hewitt, Patrick ^[2];

^[3]

Univ. of New Mexico, Albuquerque, NM (United States); North Carolina State University
North Carolina State Univ., Raleigh, NC (United States)
Brock University, St. Catharines, ON (Canada)

Ground-state electron spin polarization (ESP) is generated in radical elaborated (bpy)Pt(CAT-NN) and (bpy)Pt(CAT-p-Me₂PhMe₂-NN) (bpy = 5,5'-di-tert-butyl-2,2'-bipyridine, CAT = 3-tert-butylcatecholate, p-Ph = para-phenylene, NN = nitronylnitroxide). Photoexcitation produces an exchange-coupled, three-spin, charge-separated doublet ²S₁ (S = chromophore excited spin singlet configuration) excited state that rapidly decays to a ²T₁ (T = chromophore excited spin triplet configuration) excited state. The SQ-bridge-NN bond torsions affect the magnitude of the excited state exchange interaction (J_SQ-NN), which determines the ²T₁–⁴T₁ energy gap. Ground state ESP is dependent on the magnitude of J_SQ-NN, and we postulate that this results from differences in ²T₁ and ⁴T₁ state mixing. Mechanisms that lead to the rapid transfer of the excited state ESP to the ground state are discussed. Although subnanosecond ²T₁ state lifetimes are measured optically in solution, the ground state ESP decays very slowly at 20 K and is observable for more than a millisecond.

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Research Organization:: North Carolina State Univ., Raleigh, NC (United States)

Sponsoring Organization:: USDOE Office of Science (SC); NSERC

Grant/Contract Number:: SC0020199

OSTI ID:: 1908164

Journal Information:: Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 3 Vol. 13; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
chromophores
exchange coupling
excited states
polarization
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Title: Excited State Exchange Control of Photoinduced Electron Spin Polarization in Electronic Ground States

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