Perovskite solar cells have drawn much attention in recent years, owing to its world-record setting photovoltaic performances. Despite its promising use in tandem applications and flexible devices, its practicality is still limited by its structural instability often arising from ion migration and defect formation. While it is generally understood that ion instability is a primary cause for degradation, there is still a lack of direct evidence of structural transformation at the atomistic scale. Such an understanding is crucial to evaluate and pin-point how such instabilities are induced relative to external perturbations such as illumination or electrical bias with time, allowing researchers to devise effective strategies to mitigate them. Here, we designed an in-situ TEM setup to enable real-time observation of amorphization in double cation mixed perovskite materials under electrical biasing at 1 V. It is found that amorphization occurs along the (001) and (002) planes, which represents the observation of in-situ facet-dependent amorphization of a perovskite crystal. To reverse the degradation, the samples were heated at 50 oC and was found to recrystallize, effectively regaining its performance losses. This work is vital toward understanding fundamental ion-migration phenomena and address instability challenges of perovskite optoelectronics.

Perovskite solar cells have drawn much attention recently owing to their world-record-setting photovoltaic performances, whereas their practicality is still limited by the structural instability that often arises from ion migration and defect formation. Despite the general understanding that ion instability is a primary cause for degradation, there is no observation of structural transformation at the atomistic scale. Such observation is crucial to understand how instabilities are induced by external perturbations such as illumination or electrical bias, allowing researchers to devise effective strategies to mitigate them. Here, we designed an in situ transmission electron microscopy setup to enable real-time observation of amorphization in perovskite materials under electrical biasing. To reverse the device performance degradation due to such structural changes, the samples were heated at 50 °C and were found to recrystallize, effectively regaining their performance losses. This work presents vital insights on understanding ion-migration phenomena and addressing instability challenges of perovskite optoelectronics.

Li metal anode coupled with solid-state electrolyte is regarded as an important step for next-generation high-energy batteries to boost the performance of electric vehicles. However, commercialization of Li metal anode in all-solid-state batteries have faced challenges, one of which is the interfacial instability originated during battery operation. To overcome the difficulties in characterizing such interfaces due to their sensitivity to beam and ambient air, we applied cryogenic electron microscopy to unravel the stable nature of Li metal/LiPON interface that has exhibited remarkable electrochemical cyclability. An 80-nm-thick interphase with concentration gradients of N and P was observed, with decomposition products embedded in an amorphous matrix and exhibiting a multilayer-mosaic structure. The findings and methodology in this work give rise to a mechanistic understanding of the stability of Li metal/LiPON interface and can then be extended to study other solid-solid interfaces.