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Xiaoming Wen

Publications and source records attributed to Xiaoming Wen.

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Lattice Energy Reservoir in Metal Halide Perovskites

Metal halide perovskite-based technologies have been rapidly developed during the last decade. However, to date, the fundamental question, why are halide perovskites superior to conventional semiconductors? has remained elusive. Here, we propose a new theory of lattice energy reservoir (LER) in halide perovskites and elucidate that LER can comprehensively impact charge carrier dynamics and thus enhance device performance, from hot carrier cooling, carrier recombination, anomalous upconversion fluorescence, illumination induced fluorescence enhancement (photobrightening), to high efficiency solar cells and light-emitting diodes. An LER is a dynamic nanodomain in halide perovskites with suppressed thermal transport that can accumulate energy from phonon coupling and then feedback to subgap carriers and result in subgap carrier upconversion. The LER directly results in slowed cooling of hot carriers and significantly prolonged carrier recombination, anomalous upconversion fluorescence, as usually termed as defect tolerance, as well as the anomalous ultraslow phenomena including persistent polarization, memory effect, and photobrightening. The LER theory rationalizes the superior optoelectronic properties and device performance and provides a novel physical understanding for anomalous phenomena observed uniquely in halide perovskites.

cond-mat.mtrl-sci

Fundamental cause for superior optoelectronic properties in halide perovskites

Halide perovskites have emerged as revolutionary materials for high performance photovoltaics and optoelectronics due to their superior optoelectronic properties. The physical origin for the superior optoelectronic properties of halide perovskites so far is still poorly understood. Here we propose and demonstrate a hypothesis that electron upconversion (detrapping) driven by ionic energy reservoir is the fundamental cause for the superior optoelectronic properties of halide perovskites. We fully consider ionic influence on the electronic dynamics in mixed ionic-electronic conduction system by introducing new concepts of ionic energy reservoir, ion-electron coupling and ion-phonon scattering. We clarified that the ionic beneficial effect originates from the different mechanisms from that of the detrimental effect of mobile ion. Our hypothesis consistently interprets that the electron detrapping directly leads to significantly enhanced fluorescence efficiency, prolonged carrier lifetime, and increased diffusion length, as well as the anomalous phenomena of defect healing and defect tolerance, which are responsible for the excellent device performance of halide perovskites. By adding the ion-electron coupling into the rate equations, we establish the physical correlation between electronic dynamics in the timescale of nanosecond-microsecond and ionic dynamics in the timescales of second to hour. This finding adds the missing puzzle into the holistic physics picture and provides a deep understanding of halide perovskites and ion-electron interaction in mixed ionic-electronic semiconductors. Our results suggest the possibility of maximizing the potential of halide perovskite devices through enhancing ion-electron coupling.

physics.app-ph