Abstract
Significant interest exists in lead trihalides that present the perovskite structure owing to their demonstrated potential in photovoltaic, lasing, and display applications. These materials are also notable for their unusual phase behavior often displaying easily accessible phase transitions. In this work, time-resolved X-ray diffraction, performed on perovskite cesium lead bromide nanocrystals, maps the lattice response to controlled excitation fluence. These nanocrystals undergo a reversible, photoinduced orthorhombic-to-cubic phase transition which is discernible at fluences greater than 0.34 mJ cm−2 through the loss of orthorhombic features and shifting of high-symmetry peaks. This transition recovers on the timescale of 510 ± 100 ps. A reversible crystalline-to-amorphous transition, observable through loss of Bragg diffraction intensity, occurs at higher fluences (greater than 2.5 mJ cm−2). These results demonstrate that light-driven phase transitions occur in perovskite materials, which will impact optoelectronic applications and enable the manipulation of non-equilibrium phase characteristics of the broad perovskite material class.
Highlights
Significant interest exists in lead trihalides that present the perovskite structure owing to their demonstrated potential in photovoltaic, lasing, and display applications
The studies reveal multiple regimes of material response ranging from a reversible orthorhombic-to-cubic phase transition, up to reversible, and irreversible melting
In addition to characterizing these photoinduced phase transitions, this work demonstrates that time-resolved X-ray diffraction (TR-XRD) is a promising methodology for understanding phase transitions in perovskite materials
Summary
Significant interest exists in lead trihalides that present the perovskite structure owing to their demonstrated potential in photovoltaic, lasing, and display applications. Time-resolved X-ray diffraction, performed on perovskite cesium lead bromide nanocrystals, maps the lattice response to controlled excitation fluence. These nanocrystals undergo a reversible, photoinduced orthorhombic-to-cubic phase transition which is discernible at fluences greater than 0.34 mJ cm−2 through the loss of orthorhombic features and shifting of high-symmetry peaks. Through exciting above the bandgap, fast electron–phonon coupling and Auger heating impulsively deposit energy into the lattice, which could initiate a phase transition Examining this effect in perovskite NCs will help evaluate their stability under the high carrier injection conditions that they will experience in display and lasing applications. In addition to characterizing these photoinduced phase transitions, this work demonstrates that TR-XRD is a promising methodology for understanding phase transitions in perovskite materials
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