Connecting the dots for fundamental understanding of structure-photophysics-property relationships of COFs, MOFs, and perovskites using a Multiparticle Holstein Formalism.
Connecting the dots for fundamental understanding of structure-photophysics-property relationships of COFs, MOFs, and perovskites using a Multiparticle Holstein Formalism.
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DOI：
10.1039/d2sc03793a
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发表时间：
2023-02-01
期刊：
影响因子：
8.4
通讯作者：
中科院分区：
文献类型：
--
作者：
光活性有机材料和有机-无机杂化材料，如共轭聚合物、共价有机骨架(COF)、金属有机骨架(MOF)和层状钙钛矿等，在与光相互作用时显示出有趣的光物理特征。阐明广泛的功能材料的结构-光物理-性质关系是不平凡的，需要我们从根本上理解激子(电子-空穴对)、极化子(电荷)、双极化子、声子(振动)、层间堆积相互作用以及不同形式的结构和构象缺陷之间的复杂相互作用。除了积极追求电子结构建模和数据驱动的科学以成功地加速材料发现之外，准确、计算成本低和物理驱动的理论模型也同样重要，它与概念上复杂的实验观测一致地建立了定量联系。在此背景下，这一观点的第一部分强调了一个统一的理论框架，在该框架中，可以有效地描述具有类似结构的Holstein式振动哈密顿量的大范围准粒子的电子耦合以及电子和核自由度之间的局域耦合。这一观点的第二部分讨论了聚合物、COF、MOF和钙钛矿中的激子和极化子光物理特征，并试图使用一个共同的理论构造-多粒子Holstein形式来弥合不同研究领域之间的差距。我们预见，最先进的计算方法与多粒子Holstein形式的协同集成将有助于识别和建立新的、变革性的设计策略，这些策略将指导针对广泛的光电子、自旋和光子应用优化的下一代能源材料的合成和表征。多粒子Holstein形式主义是一个很有前途的理论框架，它有效地弥合了理论和实验之间的鸿沟。
Photoactive organic and hybrid organic–inorganic materials such as conjugated polymers, covalent organic frameworks (COFs), metal–organic frameworks (MOFs), and layered perovskites, display intriguing photophysical signatures upon interaction with light. Elucidating structure–photophysics–property relationships across a broad range of functional materials is nontrivial and requires our fundamental understanding of the intricate interplay among excitons (electron–hole pair), polarons (charges), bipolarons, phonons (vibrations), inter-layer stacking interactions, and different forms of structural and conformational defects. In parallel with electronic structure modeling and data-driven science that are actively pursued to successfully accelerate materials discovery, an accurate, computationally inexpensive, and physically-motivated theoretical model, which consistently makes quantitative connections with conceptually complicated experimental observations, is equally important. Within this context, the first part of this perspective highlights a unified theoretical framework in which the electronic coupling as well as the local coupling between the electronic and nuclear degrees of freedom can be efficiently described for a broad range of quasiparticles with similarly structured Holstein-style vibronic Hamiltonians. The second part of this perspective discusses excitonic and polaronic photophysical signatures in polymers, COFs, MOFs, and perovskites, and attempts to bridge the gap between different research fields using a common theoretical construct – the Multiparticle Holstein Formalism. We envision that the synergistic integration of state-of-the-art computational approaches with the Multiparticle Holstein Formalism will help identify and establish new, transformative design strategies that will guide the synthesis and characterization of next-generation energy materials optimized for a broad range of optoelectronic, spintronic, and photonic applications. The Multiparticle Holstein Formalism is a promising theoretical framework that efficiently bridges the gap between theory and experiments.
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