Yazdani Nuri, Bodnarchuk Maryna I, Bertolotti Federica, Masciocchi Norberto, Fureraj Ina, Guzelturk Burak, Cotts Benjamin L, Zajac Marc, Rainò Gabriele, Jansen Maximilian, Boehme Simon C, Yarema Maksym, Lin Ming-Fu, Kozina Michael, Reid Alexander, Shen Xiaozhe, Weathersby Stephen, Wang Xijie, Vauthey Eric, Guagliardi Antonietta, Kovalenko Maksym V, Wood Vanessa, Lindenberg Aaron M
Department of Materials Science and Engineering, Stanford University, Stanford, CA USA.
Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, CA USA.
Nat Phys. 2024;20(1):47-53. doi: 10.1038/s41567-023-02253-7. Epub 2023 Nov 9.
Understanding the origin of electron-phonon coupling in lead halide perovskites is key to interpreting and leveraging their optical and electronic properties. Here we show that photoexcitation drives a reduction of the lead-halide-lead bond angles, a result of deformation potential coupling to low-energy optical phonons. We accomplish this by performing femtosecond-resolved, optical-pump-electron-diffraction-probe measurements to quantify the lattice reorganization occurring as a result of photoexcitation in nanocrystals of FAPbBr. Our results indicate a stronger coupling in FAPbBr than CsPbBr. We attribute the enhanced coupling in FAPbBr to its disordered crystal structure, which persists down to cryogenic temperatures. We find the reorganizations induced by each exciton in a multi-excitonic state constructively interfere, giving rise to a coupling strength that scales quadratically with the exciton number. This superlinear scaling induces phonon-mediated attractive interactions between excitations in lead halide perovskites.
理解卤化铅钙钛矿中电子 - 声子耦合的起源是解释和利用其光学和电子特性的关键。在此我们表明,光激发导致卤化铅 - 铅键角减小,这是由于形变势与低能光学声子耦合的结果。我们通过进行飞秒分辨的光泵浦 - 电子衍射探测测量来实现这一点,以量化在FAPbBr纳米晶体中光激发引起的晶格重组。我们的结果表明FAPbBr中的耦合比CsPbBr更强。我们将FAPbBr中增强的耦合归因于其无序的晶体结构,这种结构在低温下依然存在。我们发现多激子态中每个激子诱导的重组产生相长干涉,导致耦合强度与激子数呈二次方比例关系。这种超线性比例关系在卤化铅钙钛矿中诱导了激子间由声子介导的吸引相互作用。