Using Molecular Design to Enhance the Coherence Time of Quintet Multiexcitons Generated by Singlet Fission in Single Crystals
Using Molecular Design to Enhance the Coherence Time of Quintet Multiexcitons Generated by Singlet Fission in Single Crystals
复制标题
DOI：
10.1021/jacs.1c12414
复制
发表时间：
2022-02-09
影响因子：
15
通讯作者：
Wasielewski, Michael R.
中科院分区：
文献类型：
--
作者：
Jacobberger, Robert M.;Qiu, Yunfan;Wasielewski, Michael R.
多激子五重态，（5）（TT），使用单重态裂变（SF）在有机半导体中光生，由四个量子纠缠自旋组成，有望在量子信息科学中实现新的应用。然而，决定这些状态的自旋相干性的因素仍然没有得到充分的探索。在这里，我们设计并四苯分子在5，12-双（三环己基甲硅烷基乙炔基）并四苯（TCHS-tetracene）单晶中的包装，以证明（5）（TT）状态，该状态表现出有前途的自旋量子比特特性，包括在10 K时的相干时间T-2 = 3 μ s，在5 K时的群体寿命T-pop = 130 μ s，以及即使在室温下的稳定性。单晶平台还实现自旋的全局对准，并且因此实现自旋子能级跃迁的个体可寻址性。退相干机制，包括激子扩散，电子偶极耦合，和核超精细相互作用，阐明，提供设计原则，提高T-2和操作温度（5）（TT）。通过从周围的纺丝浴动态地解耦（5）（TT），实现T-2 = 10 μ s。这些结果证明了利用单重态裂变在下一代基于分子的量子技术中以明确定义的量子态启动多个电子自旋的可行性。
Multiexciton quintet states, (5)(TT), photogenerated in organic semiconductors using singlet fission (SF), consist of four quantum entangled spins, promising to enable new applications in quantum information science. However, the factors that determine the spin coherence of these states remain underexplored. Here, we engineer the packing of tetracene molecules within single crystals of 5,12-bis(tricyclohexylsilylethynyl)tetracene (TCHS-tetracene) to demonstrate a (5)(TT) state that exhibits promising spin qubit properties, including a coherence time, T-2, = 3 mu s at 10 K, a population lifetime, T-pop, = 130 mu s at 5 K, and stability even at room temperature. The single-crystal platform also enables global alignment of the spins and, consequently, individual addressability of the spin- sublevel transitions. Decoherence mechanisms, including exciton diffusion, electronic dipolar coupling, and nuclear hyperfine interactions, are elucidated, providing design principles for increasing T-2 and the operational temperature of (5)(TT). By dynamically decoupling (5)(TT) from the surrounding spin bath, T-2 = 10 mu s is achieved. These results demonstrate the viability of harnessing singlet fission to initiate multiple electron spins in a well-defined quantum state for next-generation molecular-based quantum technologies.