Levine Benjamin G, Esch Michael P, Fales B Scott, Hardwick Dylan T, Peng Wei-Tao, Shu Yinan
Department of Chemistry, Michigan State University, East Lansing, Michigan 48824, USA; email:
Department of Chemistry and the PULSE Institute, Stanford University, Stanford, California 94305, USA.
Annu Rev Phys Chem. 2019 Jun 14;70:21-43. doi: 10.1146/annurev-physchem-042018-052425. Epub 2019 Jan 11.
The ability to predict and describe nonradiative processes in molecules via the identification and characterization of conical intersections is one of the greatest recent successes of theoretical chemistry. Only recently, however, has this concept been extended to materials science, where nonradiative recombination limits the efficiencies of materials for various optoelectronic applications. In this review, we present recent advances in the theoretical study of conical intersections in semiconductor nanomaterials. After briefly introducing conical intersections, we argue that specific defects in materials can induce conical intersections between the ground and first excited electronic states, thus introducing pathways for nonradiative recombination. We present recent developments in theoretical methods, computational tools, and chemical intuition for the prediction of such defect-induced conical intersections. Through examples in various nanomaterials, we illustrate the significance of conical intersections for nanoscience. We also discuss challenges facing research in this area and opportunities for progress.
通过识别和表征锥形交叉点来预测和描述分子中的非辐射过程的能力是理论化学近年来取得的最大成功之一。然而，直到最近，这一概念才被扩展到材料科学领域，在该领域中，非辐射复合限制了各种光电器件材料的效率。在这篇综述中，我们介绍了半导体纳米材料中锥形交叉点理论研究的最新进展。在简要介绍锥形交叉点之后，我们认为材料中的特定缺陷可以诱导基态和第一激发电子态之间的锥形交叉点，从而引入非辐射复合的途径。我们介绍了用于预测此类缺陷诱导的锥形交叉点的理论方法、计算工具和化学直觉方面的最新进展。通过各种纳米材料的实例，我们阐述了锥形交叉点对纳米科学的重要性。我们还讨论了该领域研究面临的挑战和取得进展的机会。
