Reversible spin-optical interface in luminescent organic radicals.
Reversible spin-optical interface in luminescent organic radicals.
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DOI：
10.1038/s41586-023-06222-1
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发表时间：
2023-08
期刊：
影响因子：
64.8
通讯作者：
Evans, Emrys W.
中科院分区：
文献类型：
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作者：
Gorgon, Sebastian;Lv, Kuo;Grune, Jeannine;Drummond, Bluebell H.;Myers, William K.;Londi, Giacomo;Ricci, Gaetano;Valverde, Danillo;Tonnele, Claire;Murto, Petri;Romanov, Alexander S.;Casanova, David;Dyakonov, Vladimir;Sperlich, Andreas;Beljonne, David;Olivier, Yoann;Li, Feng;Friend, Richard H.;Evans, Emrys W.
分子为量子信息科学提供了一个多功能的平台，并且是传感和计算应用的候选者。稳健的自旋光学界面是利用材料量子资源的关键。到目前为止，碳基候选物是不发光的，这阻止了通过发射的光学读出。在这里，我们报告的有机分子显示出有效的发光和激发态的自旋多重数S > 1的近单位产生产率。这是通过设计发射的双重和三重态水平之间的能量共振，在这里共价耦合的三（2，4，6-三氯苯基）甲基-咔唑自由基和蒽。我们观察到，二重光激发离域到链接并苯在几皮秒内，随后演变成一个纯的高自旋状态（四重峰的单价基，五重峰的双自由基）的混合自由基-三重峰字符附近1.8 eV。这些高自旋状态是相干可寻址的微波，即使在295 K，与光学读出使反向系统间交叉发射状态。此外，对于双自由基来说，在返回到基态时，先前不相关的自由基在蒽两侧的自旋表现出很强的自旋相关性。我们的方法同时支持高效率的初始化，自旋操纵和基于光的读出在室温下。发光和高自旋态的整合为新兴的量子技术创造了有机材料平台。我们报告的有机分子显示出高效的发光和激发态的高自旋多重性的近单位生成产率，同时支持高效率的初始化，自旋操纵和基于光的读出在室温下。
Molecules present a versatile platform for quantum information science and are candidates for sensing and computation applications. Robust spin-optical interfaces are key to harnessing the quantum resources of materials. To date, carbon-based candidates have been non-luminescent, which prevents optical readout via emission. Here we report organic molecules showing both efficient luminescence and near-unity generation yield of excited states with spin multiplicity S > 1. This was achieved by designing an energy resonance between emissive doublet and triplet levels, here on covalently coupled tris(2,4,6-trichlorophenyl) methyl-carbazole radicals and anthracene. We observed that the doublet photoexcitation delocalized onto the linked acene within a few picoseconds and subsequently evolved to a pure high-spin state (quartet for monoradical, quintet for biradical) of mixed radical–triplet character near 1.8 eV. These high-spin states are coherently addressable with microwaves even at 295 K, with optical readout enabled by reverse intersystem crossing to emissive states. Furthermore, for the biradical, on return to the ground state the previously uncorrelated radical spins either side of the anthracene shows strong spin correlation. Our approach simultaneously supports a high efficiency of initialization, spin manipulations and light-based readout at room temperature. The integration of luminescence and high-spin states creates an organic materials platform for emerging quantum technologies. We report organic molecules showing both efficient luminescence and near-unity generation yield of excited states with high spin multiplicity, simultaneously supporting a high efficiency of initialization, spin manipulations and light-based readout at room temperature.
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影响因子：
21.8
作者：
Gaita-Arino, A.;Luis, F.;Coronado, E.
通讯作者：
Coronado, E.
影响因子：
64.8
作者：
Leuenberger, MN;Loss, D
通讯作者：
Loss, D
影响因子：
1.7
作者：
Koehler, Silvia Domingo;Hoefel, Sebastian;Drescher, Malte
通讯作者：
Drescher, Malte
影响因子：
1.7
作者：
KOLLMAR, C;SIXL, H
通讯作者：
SIXL, H
DOI：
10.1063/5.0055522
发表时间：
2021-08-28
期刊：
The Journal of chemical physics
影响因子：
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作者：
通讯作者：
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