论文标题

直接检测通过手性桥的光诱导电荷转移中的自旋极化

Direct detection of spin polarization in photoinduced charge transfer through a chiral bridge

论文作者

Privitera, Alberto, Macaluso, Emilio, Chiesa, Alessandro, Gabbani, Alessio, Faccio, Davide, Giuri, Demetra, Briganti, Matteo, Giaconi, Niccolò, Santanni, Fabio, Jarmouni, Nabila, Poggini, Lorenzo, Mannini, Matteo, Chiesa, Mario, Tomasini, Claudia, Pineider, Francesco, Salvadori, Enrico, Carretta, Stefano, Sessoli, Roberta

论文摘要

可以很好地评估通过手性势垒的电荷传输会导致自旋偏振电荷。通过可见光子驱动这一过程的可能性对于量子信息科学的几个方面(例如,量子的光控制和读数)具有巨大的潜力。在这种情况下,通过自旋敏感光谱镜直接观察这种现象对于建立未来的指南来控制手性结构中的光驱动自旋选择性至关重要。在这里,我们提供了直接证明,表明时间分辨的电子顺磁共振(EPR)可用于检测由光诱导的电荷传递通过手性桥产生的长寿命自旋极化。我们提出了一个包含CDSE QD的系统,作为供体,作为受体,通过饱和寡肽螺旋桥(\ c {hi})共价连接,其刚性结构为〜10Å。时间分辨EPR光谱表明,我们系统中的电荷转移导致C60自由基阴离子,相对于光生的C60三重态的自旋极化最大值在更长的时间内观察到。值得注意的是,EPR光谱的理论建模表明,观察到的特征可能与手性诱导的自旋选择性兼容,并确定哪些参数需要优化以明确检测现象。这项工作为手性诱导的自旋极化的光学产生和直接操纵的基础。

It is well assessed that the charge transport through a chiral potential barrier can result in spin-polarized charges. The possibility of driving this process through visible photons holds tremendous potential for several aspects of quantum information science, e.g., the optical control and readout of qubits. In this context, the direct observation of this phenomenon via spin-sensitive spectroscopies is of utmost importance to establish future guidelines to control photo-driven spin selectivity in chiral structures. Here, we provide direct proof that time-resolved electron paramagnetic resonance (EPR) can be used to detect long-lived spin polarization generated by photoinduced charge transfer through a chiral bridge. We propose a system comprising CdSe QDs, as a donor, and C60, as an acceptor, covalently linked through a saturated oligopeptide helical bridge (\c{hi}) with a rigid structure of ~ 10Å. Time-resolved EPR spectroscopy shows that the charge transfer in our system results in a C60 radical anion, whose spin polarization maximum is observed at longer times with respect to that of the photogenerated C60 triplet state. Notably, the theoretical modeling of the EPR spectra reveals that the observed features may be compatible with chirality-induced spin selectivity and identifies which parameters need optimization for unambiguous detection of the phenomenon. This work lays the basis for the optical generation and direct manipulation of spin polarization induced by chirality.

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