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. 2015 Aug 20:6:8056.
doi: 10.1038/ncomms9056.

Low-threshold amplified spontaneous emission and lasing from colloidal nanocrystals of caesium lead halide perovskites

Sergii Yakunin  1   2 , Loredana Protesescu  1   2 , Franziska Krieg  1   2 , Maryna I Bodnarchuk  1   2 , Georgian Nedelcu  1   2 , Markus Humer  3 , Gabriele De Luca  4 , Manfred Fiebig  4 , Wolfgang Heiss  3   5   6 , Maksym V Kovalenko  1   2
Affiliations

Low-threshold amplified spontaneous emission and lasing from colloidal nanocrystals of caesium lead halide perovskites

Sergii Yakunin et al. Nat Commun. .

Erratum in

Abstract

Metal halide semiconductors with perovskite crystal structures have recently emerged as highly promising optoelectronic materials. Despite the recent surge of reports on microcrystalline, thin-film and bulk single-crystalline metal halides, very little is known about the photophysics of metal halides in the form of uniform, size-tunable nanocrystals. Here we report low-threshold amplified spontaneous emission and lasing from ∼10 nm monodisperse colloidal nanocrystals of caesium lead halide perovskites CsPbX3 (X=Cl, Br or I, or mixed Cl/Br and Br/I systems). We find that room-temperature optical amplification can be obtained in the entire visible spectral range (440-700 nm) with low pump thresholds down to 5±1 μJ cm(-2) and high values of modal net gain of at least 450±30 cm(-1). Two kinds of lasing modes are successfully observed: whispering-gallery-mode lasing using silica microspheres as high-finesse resonators, conformally coated with CsPbX3 nanocrystals and random lasing in films of CsPbX3 nanocrystals.

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Figures

Figure 1
Figure 1. Colloidal caesium lead halide perovskite NCs.
(a) Stable dispersions in toluene under excitation by a ultraviolet lamp (λ=365 nm). (b) Low- and high-resolution transmission electron microscopy images of CsPbBr3 NCs; corresponding scale bars are 100 and 5 nm. (c) PL spectra of the solutions shown in (a). (d) Optical absorption and PL spectra of a ca. 400-nm-CsPbBr3 NC film.
Figure 2
Figure 2. ASE spectra from thin films of CsPbX3 NCs.
(a) Pump-fluence dependence of the emission from a CsPbBr3 NC film (pumping intensity range was 3–25 μJ cm−2). (b) Spectral tunability of ASE via compositional modulation. (c) Threshold behaviour for the intensity of the ASE band of the CsPbBr3 NC film shown in (a). (d) Variable stripe-length experiment for estimation of modal net gain for the CsPbBr3 NC film. All spectra were excited at λ=400 nm with 100 fs laser pulses.
Figure 3
Figure 3. Time-resolved measurements from the CsPbBr3 NC film.
(a) Decay traces at pump fluences varied from subthreshold to well above ASE threshold values with emission recorded at ASE peak wavelengths. (b–e) The corresponding full emission spectra.
Figure 4
Figure 4. ASE from CsPbBr3 NC film under nanosecond excitation.
(a) Evolution of the emission spectra with the increase of pumping fluence and (b) corresponding dependence of the emission at 535 nm on pump fluence. Spectra were excited at λ=355 nm with 10 ns laser pulses.
Figure 5
Figure 5. Lasing in perovskite CsPbX3 NC films.
(a) Evolution from PL to whispering-gallery-mode (WGM) lasing with increasing pump intensity in a microsphere resonator of 15 μm in diameter, covered by a film of CsPbBr3 NCs. (b) Single pump laser shot mode structure of random lasing from CsPb(Br/Cl)3 NC film. The inset shows path-length distribution averaged over 256 pump laser shots. (c) Stochastic mode distribution in a series of 256 pump laser shots (PL background emission is subtracted). (d) Fast Fourier transform (FFT) of (c).
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