TY - JOUR
T1 - Optical Spin Polarization of a Narrow-Linewidth Electron-Spin Qubit in a Chromophore/Stable-Radical System
AU - Qiu, Yunfan
AU - Equbal, Asif
AU - Lin, Chenjian
AU - Huang, Yuheng
AU - Brown, Paige J.
AU - Young, Ryan M.
AU - Krzyaniak, Matthew D.
AU - Wasielewski, Michael R.
N1 - Publisher Copyright:
© 2022 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.
PY - 2023/2/1
Y1 - 2023/2/1
N2 - 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-d16) was synthesized and characterized by time-resolved optical and electron paramagnetic resonance (EPR) spectroscopies. Photoexcitation of tpPDI-BDPA-d16 results in ultrafast radical-enhanced intersystem crossing to produce a quartet state (Q) followed by formation of a spin-polarized doublet ground state (D0). Pulse-EPR experiments confirmed the spin multiplicity of Q and yielded coherence times of Tm=2.1±0.1 μs and 2.8±0.2 μs for Q and D0, respectively. BDPA-d16 eliminates the dominant 1H hyperfine couplings, resulting in a single narrow line for both the Q and D0 states, which enhances the spectral resolution needed for good qubit addressability.
AB - 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-d16) was synthesized and characterized by time-resolved optical and electron paramagnetic resonance (EPR) spectroscopies. Photoexcitation of tpPDI-BDPA-d16 results in ultrafast radical-enhanced intersystem crossing to produce a quartet state (Q) followed by formation of a spin-polarized doublet ground state (D0). Pulse-EPR experiments confirmed the spin multiplicity of Q and yielded coherence times of Tm=2.1±0.1 μs and 2.8±0.2 μs for Q and D0, respectively. BDPA-d16 eliminates the dominant 1H hyperfine couplings, resulting in a single narrow line for both the Q and D0 states, which enhances the spectral resolution needed for good qubit addressability.
KW - Chromophores
KW - EPR Spectroscopy
KW - Radicals
KW - Time-Resolved Spectroscopy
UR - http://www.scopus.com/inward/record.url?scp=85144890903&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85144890903&partnerID=8YFLogxK
U2 - 10.1002/anie.202214668
DO - 10.1002/anie.202214668
M3 - Article
C2 - 36469535
AN - SCOPUS:85144890903
SN - 1433-7851
VL - 62
JO - Angewandte Chemie - International Edition
JF - Angewandte Chemie - International Edition
IS - 6
M1 - e202214668
ER -