Miyata Kiyoshi, Atallah Timothy L, Zhu X-Y
Department of Chemistry, Columbia University, New York, NY 10027, USA.
Sci Adv. 2017 Oct 13;3(10):e1701469. doi: 10.1126/sciadv.1701469. eCollection 2017 Oct.
Lead halide perovskites have been demonstrated as high performance materials in solar cells and light-emitting devices. These materials are characterized by coherent band transport expected from crystalline semiconductors, but dielectric responses and phonon dynamics typical of liquids. This "crystal-liquid" duality implies that lead halide perovskites belong to phonon glass electron crystals, a class of materials believed to make the most efficient thermoelectrics. We show that the crystal-liquid duality and the resulting dielectric response are responsible for large polaron formation and screening of charge carriers, leading to defect tolerance, moderate charge carrier mobility, and radiative recombination properties. Large polaron formation, along with the phonon glass character, may also explain the marked reduction in hot carrier cooling rates in these materials.
卤化铅钙钛矿已被证明是太阳能电池和发光器件中的高性能材料。这些材料的特征是具有晶体半导体所预期的相干能带输运,但同时具有液体典型的介电响应和声子动力学。这种“晶体-液体”二元性意味着卤化铅钙钛矿属于声子玻璃电子晶体,这是一类被认为能制造出最高效热电材料的材料。我们表明,晶体-液体二元性以及由此产生的介电响应是大极化子形成和电荷载流子屏蔽的原因,导致了缺陷容忍度、适度的电荷载流子迁移率和辐射复合特性。大极化子的形成,连同声子玻璃特性,也可能解释了这些材料中热载流子冷却速率的显著降低。