Metal-halide perovskite semiconductors are of tremendous interest for a variety of applications. Only recently, solar cells based on a representative of this family have been certified with an efficiency in excess of 24%.[1] Aside from their remarkable success in photovoltaics, metal-halide perovskites are also highly promising as light emitters, e.g., in light-emitting diodes (LEDs) or lasers. [2][3][4] LEDs based on the fruit-fly of these compounds, i.e., methylammonium lead iodide (CH 3 NH 3 PbI 3 or MAPbI 3 ), and other related perovskites have been demonstrated with continuously increasing efficiency. [5][6][7] For lasers, there is the vision that perovskites may overcome/avoid the typical limitations and loss mechanisms present in organic gain media, such as triplet-singlet annihilation or absorption due to triplet excitons and
Cesium lead halide perovskites are of interest for light-emitting diodes and lasers. So far, thin-films of CsPbX 3 have typically afforded very low photoluminescence quantum yields (PL-QY < 20%) and amplified spontaneous emission (ASE) only at cryogenic temperatures, as defect related nonradiative recombination dominated at room temperature (RT). There is a current belief that, for efficient light emission from lead halide perovskites at RT, the charge carriers/excitons need to be confined on the nanometer scale, like in CsPbX 3 nanoparticles (NPs).Here, thin films of cesium lead bromide, which show a high PL-QY of 68% and low-threshold ASE at RT, are presented. As-deposited layers are recrystallized by thermal imprint, which results in continuous films (100% coverage of the substrate), composed of large crystals with micrometer lateral extension. Using these layers, the first cesium lead bromide thin-film distributed feedback and vertical cavity surface emitting lasers with ultralow threshold at RT that do not rely on the use of NPs are demonstrated. It is foreseen that these results will have a broader impact beyond perovskite lasers and will advise a revision of the paradigm that efficient light emission from CsPbX 3 perovskites can only be achieved with NPs.
We measure both nonlinear absorption and nonlinear refraction in a
C
H
3
N
H
3
P
b
B
r
3
single crystal using the Z-scan technique with femtosecond laser pulses. At 1000 nm, we obtain values of 5.2 cm/GW and
+
9.5
⋅
10
−
14
c
m
2
/
W
for nonlinear absorption and nonlinear refraction, respectively. The sign and magnitude of the observed refractive nonlinearity are reproduced well by the two-band model. Our results suggest that the large nonlinear refractive index measured in perovskite nanostructures cannot be explained by an intrinsically high bound-electronic nonlinear refractive index in this emerging material class but is possibly caused by free carriers or quantum confinement effects.
Intense phase-locked terahertz (THz) pulses are the bedrock of THz lightwave electronics, where the carrier field creates a transient bias to control electrons on sub-cycle time scales. Key applications such as THz scanning tunnelling microscopy or electronic devices operating at optical clock rates call for ultimately short, almost unipolar waveforms, at megahertz (MHz) repetition rates. Here, we present a flexible and scalable scheme for the generation of strong phase-locked THz pulses based on shift currents in type-II-aligned epitaxial semiconductor heterostructures. The measured THz waveforms exhibit only 0.45 optical cycles at their centre frequency within the full width at half maximum of the intensity envelope, peak fields above 1.1 kV cm−1 and spectral components up to the mid-infrared, at a repetition rate of 4 MHz. The only positive half-cycle of this waveform exceeds all negative half-cycles by almost four times, which is unexpected from shift currents alone. Our detailed analysis reveals that local charging dynamics induces the pronounced positive THz-emission peak as electrons and holes approach charge neutrality after separation by the optical pump pulse, also enabling ultrabroadband operation. Our unipolar emitters mark a milestone for flexibly scalable, next-generation high-repetition-rate sources of intense and strongly asymmetric electric field transients.
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