Investigation of Singlet Fission-Halide Perovskite Interfaces.
Investigation of Singlet Fission-Halide Perovskite Interfaces.
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调查单线裂变 - 半甲基钙钛矿界面。
DOI：
10.1021/acs.chemmater.1c04310
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发表时间：
2022-06-14
影响因子：
8.6
通讯作者：
Monserrat, Bartomeu
中科院分区：
文献类型：
--
作者：
Bowman, Alan R.;Stranks, Samuel D.;Monserrat, Bartomeu
一种提高太阳能电池效率的方法是将低带隙半导体与单线态裂变材料（其在光激发后将一个高能单线态转化为两个低能三线态）结合。在这里，我们提出了一个单重态裂变分子和低带隙卤化物钙钛矿之间的界面的研究。我们简要介绍了150个实验筛选三重态转移到卤化物钙钛矿。然而，在所有情况下，三重态转移没有观察到。这促使我们通过使用并四苯和碘化铯铅进行第一性原理计算来更好地理解卤化物钙钛矿-单线态裂变界面。我们发现，并四苯分子/薄膜优先取向平行/垂直于卤化物钙钛矿的表面。这一结果与并四苯（和其他棒状分子）在广泛的无机半导体上的模拟一致。我们提出的所有接口的形成能，这是显着不如散装并四苯，弱相互作用的界面指示。由于计算限制，不可能在整个界面处计算激子态，因此我们提出了并四苯和卤化物钙钛矿结构之间的高度推测性界面。在这些模型中，我们专注于正确复制并四苯的电子状态。我们发现，并四苯的单重态和三重态的能量是可比的散装并四苯，和三重态是强烈本地化的一个单一的并四苯分子，即使在一个接口。我们的工作提供了新的理解并四苯和卤化物钙钛矿之间的界面，探讨了在界面处建模激子的潜力，并开始解释直接将三重态提取到无机半导体中的困难。
A method for improving the efficiency of solar cells is combining a low-band-gap semiconductor with a singlet fission material (which converts one high-energy singlet into two low-energy triplets following photoexcitation). Here, we present a study of the interface between singlet fission molecules and low-band-gap halide pervoskites. We briefly present 150 experiments screening for triplet transfer into a halide perovskite. However, in all cases, triplet transfer was not observed. This motivated us to understand the halide perovskite–singlet fission interface better by carrying out first-principles calculations using tetracene and cesium lead iodide. We found that tetracene molecules/thin films preferentially orient themselves parallel to/perpendicular to the halide perovskite’s surface. This result is in agreement with simulations of tetracene (and other rodlike molecules) on a wide range of inorganic semiconductors. We present formation energies of all interfaces, which are significantly less favorable than for bulk tetracene, indicative of weak interaction at the interface. It was not possible to calculate excitonic states at the full interface due to computational limitations, so we instead present highly speculative toy interfaces between tetracene and a halide-perovskite-like structure. In these models, we focus on replicating tetracene’s electronic states correctly. We find that tetracene’s singlet and triplet energies are comparable to that of bulk tetracene, and the triplet is strongly localized on a single tetracene molecule, even at an interface. Our work provides new understanding of the interface between tetracene and halide perovskites, explores the potential for modeling excitons at interfaces, and begins to explain the difficulties in extracting triplets directly into inorganic semiconductors.
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影响因子：
2.8
作者：
Piland, Geoffrey B.;Burdett, Jonathan J.;Bardeen, Christopher J.
通讯作者：
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影响因子：
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作者：
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作者：
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Castelli, Ivano E.
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通讯作者：
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作者：
DEXTER, DL
通讯作者：
DEXTER, DL