Optical Spin Polarization of a Narrow‐Linewidth Electron‐Spin Qubit in a Chromophore/Stable‐Radical System

Qiu, Yunfan; Equbal, Asif; Lin, Chenjian; Huang, Yuheng; Brown, Paige J.; Young, Ryan M.; Krzyaniak, Matthew D.; Wasielewski, Michael R.

doi:10.1002/anie.202214668

Optical Spin Polarization of a Narrow‐Linewidth Electron‐Spin Qubit in a Chromophore/Stable‐Radical System

Journal Article · Wed Dec 28 00:00:00 EST 2022 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.202214668· OSTI ID:1907028

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Department of Chemistry Center for Molecular Quantum Transduction Institute for Sustainability and Energy at Northwestern Northwestern University Evanston IL 60208-3113 USA

Abstract

Photoexcited organic chromophores appended to stable radicals can serve as qubit and/or qudit candidates for quantum information applications. 1,6,7,12‐Tetra‐(4‐ tert ‐butylphenoxy)‐perylene‐3,4 : 9,10‐bis(dicarboximide) (tpPDI) linked to a partially deuterated α,γ‐bisdiphenylene‐β‐phenylallyl radical (BDPA‐ d ₁₆ ) was synthesized and characterized by time‐resolved optical and electron paramagnetic resonance (EPR) spectroscopies. Photoexcitation of tpPDI‐BDPA‐ d ₁₆ results in ultrafast radical‐enhanced intersystem crossing to produce a quartet state ( Q ) followed by formation of a spin‐polarized doublet ground state ( D ₀ ). Pulse‐EPR experiments confirmed the spin multiplicity of Q and yielded coherence times of T _m =2.1±0.1 μs and 2.8±0.2 μs for Q and D ₀ , respectively. BDPA‐ d ₁₆ eliminates the dominant ¹ H hyperfine couplings, resulting in a single narrow line for both the Q and D ₀ states, which enhances the spectral resolution needed for good qubit addressability.

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Research Organization:: Northwestern Univ., Evanston, IL (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0021314

OSTI ID:: 1907028

Alternate ID(s):: OSTI ID: 2421881
OSTI ID: 1922268

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 6 Vol. 62; ISSN 1433-7851

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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Optical Spin Polarization of a Narrow‐Linewidth Electron‐Spin Qubit in a Chromophore/Stable‐Radical System

Journal Article · Tue Dec 27 19:00:00 EST 2022 · Angewandte Chemie · OSTI ID:1907027

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Optical Spin Polarization of a Narrow‐Linewidth Electron‐Spin Qubit in a Chromophore/Stable‐Radical System

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