Quantum Dot–Organic Molecule Conjugates as Hosts for Photogenerated Spin Qubit Pairs
Quantum Dot–Organic Molecule Conjugates as Hosts for Photogenerated Spin Qubit Pairs
复制标题
量子点——有机分子共轭物作为光生自旋量子位对的主体
DOI：
10.1021/jacs.2c11952
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发表时间：
2023
影响因子：
15
通讯作者：
Olshansky, Jacob H.
中科院分区：
文献类型：
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作者：
Lee, Autumn Y.;Colleran, Troy A.;Jain, Amisha;Niklas, Jens;Rugg, Brandon K.;Mani, Tomoyasu;Poluektov, Oleg G.;Olshansky, Jacob H.
光生自旋相关自由基对中存在的固有自旋极化使它们成为量子计算和量子传感应用的有希望的候选者。这些系统的自旋状态可以用电子顺磁共振谱仪用微波脉冲探测和操纵。然而，到目前为止，还没有基于磁共振的自旋测量的光生自旋相关的自由基对托管在量子点上的报告。在目前的工作中，我们制备了染料分子-无机量子点共轭物，并表明它们可以产生光生自旋极化态。选择染料分子D131是因为它能够进行有效的电荷分离，而选择纳米颗粒材料ZnO量子点是因为它们有前途的自旋特性。瞬态和稳态光谱进行ZnO量子点-D131共轭物显示，可逆的光生电荷分离发生。瞬态和脉冲电子顺磁共振实验，然后进行了光生自由基对，这表明（1）自由基对在中等温度下极化，并与现有的理论很好地模拟和（2）自旋状态可以访问和操纵与微波脉冲。这项工作为一类新的有前途的量子比特材料打开了大门，这些材料可以在偏振态下光生，并由高度可定制的无机纳米粒子托管。
The inherent spin polarization present in photogenerated spin-correlated radical pairs makes them promising candidates for quantum computing and quantum sensing applications. The spin states of these systems can be probed and manipulated with microwave pulses using electron paramagnetic resonance spectrometers. However, to date, there are no reports on magnetic resonance-based spin measurements of photogenerated spin-correlated radical pairs hosted on quantum dots. In the current work, we prepare dye molecule–inorganic quantum dot conjugates and show that they can produce photogenerated spin-polarized states. The dye molecule, D131, is chosen for its ability to undergo efficient charge separation, and the nanoparticle materials, ZnO quantum dots, are chosen for their promising spin properties. Transient and steady state optical spectroscopy performed on ZnO quantum dot–D131 conjugates shows that reversible photogenerated charge separation is occurring. Transient and pulsed electron paramagnetic resonance experiments are then performed on the photogenerated radical pair, which demonstrate that (1) the radical pair is polarized at moderate temperatures and well modeled by existing theories and (2) the spin states can be accessed and manipulated with microwave pulses. This work opens the door to a new class of promising qubit materials that can be photogenerated in polarized states and hosted by highly tailorable inorganic nanoparticles.