The entangled triplet pair state in acene and heteroacene materials.
The entangled triplet pair state in acene and heteroacene materials.
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DOI：
10.1038/ncomms15953
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发表时间：
2017-07-12
影响因子：
16.6
通讯作者：
Sirringhaus H
中科院分区：
文献类型：
--
作者：
Yong CK;Musser AJ;Bayliss SL;Lukman S;Tamura H;Bubnova O;Hallani RK;Meneau A;Resel R;Maruyama M;Hotta S;Herz LM;Beljonne D;Anthony JE;Clark J;Sirringhaus H
状态纠缠是量子力学最令人惊讶和反直觉的结果之一，在密码学和计算中具有潜在的应用。在有机材料中，一种特别重要的表现是自旋纠缠三重态对态，它介导一个自旋0单重态激子自旋守恒裂变为两个自旋1三重态激子。尽管进行了长期的理论和实验探索，三重态对状态和三重态间相互作用的本质仍然难以捉摸。在这里，我们使用一系列经历单线态激子裂变的有机半导体来揭示纠缠三重态对态的光物理性质。我们发现，三重态对相对于自由三重态的束缚具有很大程度上与材料无关的能量（∼30 meV）。在其生命周期内，三重态组分协同表现为单重态，并通过赫茨伯格-特勒型机制发光，从而产生振动结构光致发光。在光伏共混物中，电荷转移可以从结合的三重态对发生，光子-电荷转换效率>100%。有机半导体中的单线态裂变可以产生三线态激子对，这对光伏过程中的电荷产生至关重要，但其性质仍然难以捉摸。在这里，勇等人。表明直接三重态对在一系列并苯和杂并苯材料中被束缚和发射。
Entanglement of states is one of the most surprising and counter-intuitive consequences of quantum mechanics, with potent applications in cryptography and computing. In organic materials, one particularly significant manifestation is the spin-entangled triplet-pair state, which mediates the spin-conserving fission of one spin-0 singlet exciton into two spin-1 triplet excitons. Despite long theoretical and experimental exploration, the nature of the triplet-pair state and inter-triplet interactions have proved elusive. Here we use a range of organic semiconductors that undergo singlet exciton fission to reveal the photophysical properties of entangled triplet-pair states. We find that the triplet pair is bound with respect to free triplets with an energy that is largely material independent (∼30 meV). During its lifetime, the component triplets behave cooperatively as a singlet and emit light through a Herzberg–Teller-type mechanism, resulting in vibronically structured photoluminescence. In photovoltaic blends, charge transfer can occur from the bound triplet pairs with >100% photon-to-charge conversion efficiency. Singlet fission in organic semiconductors can generate triplet exciton pairs that are crucial to the charge generation in a photovoltaic process, whilst their nature remains elusive. Here, Yong et al. show that the immediate triplet pair is bound and emissive in a range of acene and heteroacene materials.
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