Department of Chemistry, Center for Molecular Quantum Transduction, Institute for Sustainability and Energy at Northwestern, Northwestern University, Evanston, IL 60208-3113, USA.
Angew Chem Int Ed Engl. 2023 Feb 1;62(6):e202214668. doi: 10.1002/anie.202214668. Epub 2022 Dec 28.
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 ) was synthesized and characterized by time-resolved optical and electron paramagnetic resonance (EPR) spectroscopies. Photoexcitation of tpPDI-BDPA-d results in ultrafast radical-enhanced intersystem crossing to produce a quartet state (Q) followed by formation of a spin-polarized doublet ground state (D ). Pulse-EPR experiments confirmed the spin multiplicity of Q and yielded coherence times of T =2.1±0.1 μs and 2.8±0.2 μs for Q and D , respectively. BDPA-d eliminates the dominant H hyperfine couplings, resulting in a single narrow line for both the Q and D states, which enhances the spectral resolution needed for good qubit addressability.
通过将稳定自由基与光激发有机发色团偶联，可以得到用于量子信息应用的量子位（qubit）和/或量子数元（qudit）候选物。本文合成了一种部分氘代的α,γ-双二苯并[ p ，q]吩嗪-3,4-：9,10-双（二羧酸酰亚胺）（tpPDI）与部分去氘的α,γ-双二苯并[ p ，q]吩嗪-3,4-：9,10-双（二羧酸酰亚胺）自由基（BDPA-d）相连，并通过时间分辨光和电子顺磁共振（EPR）光谱对其进行了表征。tpPDI-BDPA-d 的光激发导致超快自由基增强的系间穿越，产生四重态（Q），随后形成自旋极化的基态 doublet（D）。脉冲 EPR 实验证实了 Q 的自旋多重性，并分别得出了 Q 和 D 的相干时间 T =2.1±0.1 μs 和 2.8±0.2 μs。BDPA-d 消除了主要的 H 超精细耦合，导致 Q 和 D 态均呈现单一的窄线，从而提高了良好的量子位可寻址性所需的光谱分辨率。
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