Optical readout of singlet fission biexcitons in a heteroacene with photoluminescence detected magnetic resonance

Joshi, Gajadhar; Dill, Ryan D.; Thorley, Karl J.; Anthony, John E.; Reid, Obadiah G.; Johnson, Justin C.

doi:10.1063/5.0103662

Title: Optical readout of singlet fission biexcitons in a heteroacene with photoluminescence detected magnetic resonance

Journal Article · Mon Oct 24 00:00:00 UTC 2022 · Journal of Chemical Physics

DOI: https://doi.org/10.1063/5.0103662 · OSTI ID:1900001

^[1];

^[2]; Thorley, Karl J. ^[3];

^[3]; Reid, Obadiah G. ^[4];

^[4]

National Renewable Energy Lab. (NREL), Golden, CO (United States)
Univ. of Colorado, Boulder, CO (United States)
Univ. of Kentucky, Lexington, KY (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States)

Molecular spin systems based on photoexcited triplet pairs formed via singlet fission (SF) are attractive as carriers of quantum information because of their potentially pure and controllable spin polarization, but developing systems that offer optical routes to readout as well as initialization is challenging. Herein, we characterize the electron spin magnetic resonance change in the photoluminescence intensity for a tailored organic molecular crystal while sweeping a microwave drive up to 10 GHz in a broadband loop structure. We observe resonant transitions for both triplet and quintet spin sublevel populations showing their optical sensitivity and revealing the zero-field parameters for each. We map the evolution of these spectra in both microwave frequency and magnetic field, producing a pattern of optically detected magnetic resonance (ODMR) peaks. Fits to these data using a suitable model suggest significant spin polarization in this system with orientation selectivity. Unusual excitation intensity dependence is also observed, which inverts the sign of the ODMR signal for the triplet features, but not for the quintet. These observations demonstrate optical detection of the spin sublevel population dictated by SF and intermolecular geometry, and highlight anisotropic and multi-scale dynamics of triplet pairs.

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Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 1900001

Report Number(s):: NREL/JA-5900-83446; MainId:84219; UUID:32aa37a1-5b6e-4247-80ea-f9e303946d32; MainAdminID:68056

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 16 Vol. 157; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Optical readout of singlet fission biexcitons in a heteroacene with photoluminescence detected magnetic resonance

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