Spin Dynamics of SCRPs in ZnO Quantum Dot–Organic Molecule Conjugates Studied with Pulsed EPR

IF 3.2 3区 化学 Q2 CHEMISTRY, PHYSICAL
Mandefro Y. Teferi, , , Amisha Jain, , , Frida S. Hernandez, , , Autumn Y. Lee, , , Tiffany Tran, , , Ming Lee Tang, , , Jacob H. Olshansky, , , Jens Niklas*, , and , Oleg G. Poluektov*, 
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Abstract

Photogenerated spin-correlated radical pairs (SCRPs) are emerging as promising new candidates for Quantum Information Science applications, where they act as electron spin qubit pairs (SQPs). Historically, these pairs have been mostly investigated in natural photosynthesis and in molecular organic donor–(linker)–acceptor systems. Recently, we have shown that these spin pairs can also be observed by time-resolved electron-paramagnetic resonance (EPR) spectroscopy in hybrid inorganic–organic conjugates. The current study builds on recent work (ACS Nano, 2025, 19, 12194–12207), in which we systematically prepared hybrid inorganic–organic molecule systems with tunable geometries that can host SCRPs/SQPs. Here, we demonstrate using pulsed EPR spectroscopy that we can generate, study, and manipulate the spins in these photogenerated SCRPs hosted on highly tailorable inorganic–organic hybrid systems. Microwave pulse-based spin manipulation is the first step toward developing quantum computing and quantum sensing applications with these promising spin-based qubit materials, which can be reversibly photogenerated in highly spin-polarized states at moderate temperatures. An attractive feature of this new class of hybrid materials is that the g-factor of the unpaired electron spin in the ZnO QD (as part of the SCRP/SQP) can be adjusted using the quantum size effect in these QDs, which allows for the selective addressability of each spin in the SCRP using microwave pulses. Furthermore, we also observed a difference between the g-values of the unpaired electron in the ZnO QD in the transient SCRP state and stable photoreduced state. We hypothesize that the unpaired electron in the SCRP is delocalized as a band-like conduction electron, while in the stable photoreduced state, the electron is delocalized in a shallow electron trap state.

Abstract Image

Abstract Image

用脉冲EPR研究ZnO量子点-有机分子共轭物中SCRPs的自旋动力学
光生自旋相关基对(SCRPs)作为电子自旋量子比特对(SQPs),正在成为量子信息科学应用中有前途的新候选体。从历史上看,这些对主要是在自然光合作用和分子有机供体-(连接体)-受体系统中研究的。最近,我们已经证明这些自旋对也可以通过时间分辨电子顺磁共振(EPR)光谱在无机-有机杂化共轭物中观察到。目前的研究基于最近的工作(ACS Nano, 2025, 19, 12194-12207),我们系统地制备了具有可调几何形状的无机-有机杂化分子体系,可以承载SCRPs/SQPs。在这里,我们证明了使用脉冲EPR光谱,我们可以产生、研究和操纵这些光生成的SCRPs在高度可定制的无机-有机杂化体系上的自旋。基于微波脉冲的自旋操纵是利用这些有前途的基于自旋的量子比特材料开发量子计算和量子传感应用的第一步,这些材料可以在中等温度下以高自旋极化状态可逆地光生成。这种新型杂化材料的一个吸引人的特点是,ZnO QD中未配对电子自旋的g因子(作为SCRP/SQP的一部分)可以使用这些QD中的量子尺寸效应进行调整,这允许使用微波脉冲选择SCRP中的每个自旋的可寻址性。此外,我们还观察到ZnO QD中未配对电子在瞬态SCRP状态和稳定光还原状态下的g值存在差异。我们假设SCRP中的未配对电子离域为带状传导电子,而在稳定的光还原态中,电子离域为浅电子陷阱态。
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来源期刊
The Journal of Physical Chemistry C
The Journal of Physical Chemistry C 化学-材料科学:综合
CiteScore
6.50
自引率
8.10%
发文量
2047
审稿时长
1.8 months
期刊介绍: The Journal of Physical Chemistry A/B/C is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, and chemical physicists.
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