Triplet-pair spin signatures from macroscopically aligned heteroacenes in an oriented single crystal.
Triplet-pair spin signatures from macroscopically aligned heteroacenes in an oriented single crystal.
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DOI：
10.1073/pnas.2201879119
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发表时间：
2022-07-19
影响因子：
11.1
通讯作者：
中科院分区：
文献类型：
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产生量子信息的有序元素，例如原子系综中的对齐电子自旋，在大尺度和实际温度下具有挑战性。为此，我们已经建模和表征了定制的分子的晶体，该分子与宏观顺序对齐，并且在测量分子对的关键自旋-自旋相互作用的磁共振实验中具有具有特征和良好分辨的自旋签名的光初始化物种。相对于磁场旋转晶体产生特定自旋状态的群体，这些自旋状态在室温下被宏观地和确定性地控制。通过严格的理论模型解释，纯自旋极化及其对取向的依赖性将分子方法推进到量子传感和计算的相关长度和时间尺度。单重态裂变的光驱动过程产生耦合三重态对（TT），其具有基本上有趣且潜在有用的性质。五重态5 TT 0子能级对于量子信息特别有意义，因为它是高度纠缠的，可以用微波脉冲寻址，并且可以用光学技术检测。以前的理论工作的模型哈密顿量和非绝热过渡理论，称为JDE模型，已确定，这个子级可以选择性地填充，如果满足某些条件。其中最具挑战性的是，二聚体内的分子进行单线态裂变必须有其主磁轴平行于彼此和所施加的塞曼场。在这里，我们提出的时间分辨电子顺磁共振（TR-EPR）光谱的一个单一的晶体样品的tetracenethietrin化合物具有阵列的二聚体以这种方式排列，安装，以便可以控制相对于分子轴的方向的字段。在配对的TT和未配对的（T+T）三重态中观察到的自旋子能级粒子数与JDE模型的预测一致，包括在z = B 0处优先形成5 TT 0，但有一个警告-两个5 TT自旋子能级几乎没有粒子数。这可能是由于5 TT和3 TT歧管之间的交叉点在TR-EPR研究的领域范围内，与通过监测光致发光在不同的磁场确定的三重态间交换能一致。
Producing ordered elements of quantum information, such as aligned electron spins in an ensemble of atoms, is challenging at large scales and practical temperatures. Toward this end, we have modelled and characterized crystals of a tailored molecule that aligns with macroscopic order and possesses photo-initialized species with characteristic and well-resolved spin signatures in magnetic resonance experiments that measure key spin–spin interactions for molecular pairs. Rotating the crystal with respect to the magnetic field produces populations of specific spin states that are macroscopically and deterministically controlled at room temperature. Explained through rigorous theoretical modeling, the pure spin polarization and its dependence on orientation advance molecular approaches to relevant length- and timescales for quantum sensing and computation. The photo-driven process of singlet fission generates coupled triplet pairs (TT) with fundamentally intriguing and potentially useful properties. The quintet 5TT0 sublevel is particularly interesting for quantum information because it is highly entangled, is addressable with microwave pulses, and could be detected using optical techniques. Previous theoretical work on a model Hamiltonian and nonadiabatic transition theory, called the JDE model, has determined that this sublevel can be selectively populated if certain conditions are met. Among the most challenging, the molecules within the dimer undergoing singlet fission must have their principal magnetic axes parallel to one another and to an applied Zeeman field. Here, we present time-resolved electron paramagnetic resonance (TR-EPR) spectroscopy of a single crystal sample of a tetracenethiophene compound featuring arrays of dimers aligned in this manner, which were mounted so that the orientation of the field relative to the molecular axes could be controlled. The observed spin sublevel populations in the paired TT and unpaired (T+T) triplets are consistent with predictions from the JDE model, including preferential 5TT0 formation at z ‖ B0, with one caveat—two 5TT spin sublevels have little to no population. This may be due to crossings between the 5TT and 3TT manifolds in the field range investigated by TR-EPR, consistent with the intertriplet exchange energy determined by monitoring photoluminescence at varying magnetic fields.
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影响因子：
6.1
作者：
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