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Mode selection and high-quality upconversion lasing from perovskite CsPb2Br5 microplates

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Abstract

In recent years, halide perovskite nanostructures have had great advances and have opened up a bright future for micro/nanolasers. However, upconversion lasing by two-photon excitation with mode selection and high quality factor in one device is still rarely reported. Herein, two lasing modes are demonstrated in the all-inorganic perovskite CsPb2Br5 microplates with subwavelength thickness and uniform square shape. The net optical gain is quickly established in less than 1 ps and persists more than 30 ps, revealed by ultrafast transient absorption spectroscopy. The temperature-dependent low-threshold amplified spontaneous emission confirms the net gain for stimulated emission with a high characteristic temperature of 403 K, far surpassing the all-inorganic CsPbBr3 semiconductor gain media. Remarkably, upconversion lasing based on two kinds of microcavity effects, Fabry–Pérot and whispering-gallery modes, from the microplates at room temperature is successfully achieved with a low threshold operating in multi- or single-mode, respectively. Surprisingly, the quality factor (3551) is among the best values obtained from perovskite micro/nanoplate upconversion lasers without an external cavity. Moreover, the highly stable chromaticity with color drift only less than 0.1 nm also outbalances the all-inorganic CsPbBr3 ones. These superior performances of CsPb2Br5 microplate lasing with a facile solution synthesis procedure will offer a feasible structure to fabricate specific functionalities for high-performance frequency upconversion micro/nanoscale photonic integrated devices.

© 2020 Chinese Laser Press

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Figures (12)

Fig. 1.
Fig. 1. Optical characterizations of perovskite CsPb2Br5 microplates. (a) SEM image. The scale bar is 10 μm. (b) Schematic crystal structure. (c) Experimental and standard powder XRD patterns of tetragonal CsPb2Br5. (d) Linear absorption (green) and PL spectrum (red).
Fig. 2.
Fig. 2. TA spectra of perovskite CsPb2Br5. (a) 2D pseudo-color TA spectra. (b) TA spectra at different delay times. (c) The kinetics of prominent PB signal. (d) The kinetics of SE. Inset: a magnified view of the spectroscopic signature of SE before 11 ps.
Fig. 3.
Fig. 3. Temperature-dependent ASE actions from CsPb2Br5 microplates. (a) The PL spectra of two-photon pumped ASE at 300 K. Inset: photograph of the CsPb2Br5 microplate excited above ASE threshold by a cylindrical lens. (b) The integrated intensity and FWHM with respect to pump intensity. (c) Normalized PL intensity as a function of excitation intensity at different temperatures. (d) Pump threshold intensity versus temperature. The solid red line is the fit according to Eq. (1).
Fig. 4.
Fig. 4. F-P mode lasing characterization of a single CsPb2Br5 microplate. (a) Pump-intensity-dependent emission spectra under two-photon excitation. Inset: the bright-field optical image and emission photograph from the single microplate above the lasing threshold, indicating the F-P mode. The scale bar is 5 μm. (b) Output intensity (blue) and FWHM (red) of laser with increasing pump fluence. (c) Fitting of the lasing oscillation mode. The FWHM is 0.15 nm with a quality factor of 3551.
Fig. 5.
Fig. 5. WGM lasing characterization of a single CsPb2Br5 microplate. (a) Pump-intensity-dependent emission spectra under two-photon excitation. Inset: the bright-field optical image and the emission photograph from the single CsPb2Br5 microplate above the lasing threshold, indicating the WGM lasing. The scale bar is 5 μm. (b) Output intensity (red) and FWHM (blue) of laser with increasing pump fluence. (c) Fitting of the lasing oscillation mode. The FWHM is 0.16 nm with a quality factor of 3374.
Fig. 6.
Fig. 6. Log–log plot of the integrated PL intensity as a function of the pump fluence under two-photon excitation.
Fig. 7.
Fig. 7. Pump-intensity-dependent SE dynamics.
Fig. 8.
Fig. 8. Normalized integrated intensity for microplates under pulsed excitation.
Fig. 9.
Fig. 9. Two-photon pumped intensity-dependent emission spectra from a single CsPb2Br5 microplate in the F-P cavity.
Fig. 10.
Fig. 10. Center lasing position of the CsPb2Br5 F-P mode laser.
Fig. 11.
Fig. 11. Two-photon pumped intensity-dependent emission spectra from a single CsPb2Br5 microplate in the WGM cavity.
Fig. 12.
Fig. 12. Center lasing position of the CsPb2Br5 WGM laser.

Equations (1)

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Pth=Pth,0exp(T/T0),
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