Songvilay M, Giles-Donovan N, Bari M, Ye Z-G, Minns J L, Green M A, Xu Guangyong, Gehring P M, Schmalzl K, Ratcliff W D, Brown C M, Chernyshov D, van Beek W, Cochran S, Stock C
School of Physics and Astronomy, University of Edinburgh, Edinburgh EH9 3FD, United Kingdom.
Medical and Industrial Ultrasonics, School of Engineering, University of Glasgow G128QQ, United Kingdom.
Phys Rev Mater. 2019;3(9). doi: https://doi.org/10.1103/physrevmaterials.3.093602.
The acoustic phonons in the organic-inorganic lead halide perovskites have been reported to have anomalously short lifetimes over a large part of the Brillouin zone. The resulting shortened mean free paths of the phonons have been implicated as the origin of the low thermal conductivity. We apply neutron spectroscopy to show that the same acoustic phonon energy linewidth broadening (corresponding to shortened lifetimes) occurs in the fully inorganic CsPbBr by comparing the results on the organic-inorganic CHNHPbCl. We investigate the critical dynamics near the three zone boundaries of the cubic Brillouin zone of CsPbBr and find energy and momentum broadened dynamics at momentum points where the Cs-site (-site) motions contribute to the cross section. Neutron diffraction is used to confirm that both the Cs and Br sites have unusually large thermal displacements with an anisotropy that mirrors the low temperature structural distortions. The presence of an organic molecule is not necessary to disrupt the low-energy acoustic phonons at momentum transfers located away from the zone center in the lead halide perovskites and such damping may be driven by the large displacements or possibly disorder on the site.
据报道,有机-无机卤化铅钙钛矿中的声学声子在布里渊区的很大一部分区域内具有异常短的寿命。由此产生的声子平均自由程缩短被认为是低热导率的起源。我们应用中子光谱学表明,通过比较有机-无机CH₃NH₃PbCl₃的结果,在全无机CsPbBr₃中也会出现相同的声学声子能量线宽展宽(对应于寿命缩短)。我们研究了CsPbBr₃立方布里渊区三个区边界附近的临界动力学,发现在Cs位点(-位点)运动对截面有贡献的动量点处,能量和动量展宽的动力学。中子衍射用于确认Cs和Br位点都具有异常大 的热位移,其各向异性反映了低温结构畸变。在卤化铅钙钛矿中,远离区中心的动量转移处,有机分子的存在并非破坏低能声学声子所必需的,这种阻尼可能是由 位点上的大位移或可能的无序性驱动的。