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.
The success of oxide electronics depends on the ability to design functional properties such as ferroelectricity with atomic accuracy. However, despite tremendous advances in ferroelectric heterostructures, the development towards multilevel architectures with precise layer-by-layer command over the polarization is impeded by the lack of continuous control over the balance of electrostatics, strain, chemistry and film thickness during growth. Moreover, the polarization in the deeper layers becomes inaccessible when these are buried by the ongoing deposition. Taking ferroelectric BaTiO3 and multiferroic BiFeO3 as model systems, we observe and engineer the emergence, orientation and interaction of ferroelectric polarization in ultrathin heterostructures with monolayer accuracy. We achieve this by optical second harmonic generation which tracks the evolution of spontaneous polarization in real time throughout the deposition process. Such direct and in situ access to the polarization during growth leads us to heterostructures with user-defined polarization sequences—towards a new class of functional ferroic materials.
An optical probe of the ferroelectric domain distribution and manipulation in BiFeO3 thin films is reported using optical second harmonic generation. A unique relation between the domain distribution and its integral symmetry is established. The ferroelectric signature is even resolved when the film is covered by a top electrode. The effect of voltage-induced ferroelectric switching is imaged.
Non-Ising-like 180° ferroelectric domain wall architecture and domain distribution in tetragonal PbZr Ti O thin films are probed using a combination of optical second harmonic generation and scanning transmission electron microscopy. In the remnant state, a specific nonlinear optical signature of tilted 180° domain walls corresponding to a mixed Ising-Néel-type rotation of polarization across the wall is shown.
We identify a transient enhancement of the depolarizing field, leading to an unexpected quench of net polarization, during the growth of a prototypical metal-ferroelectric-metal epitaxial system made of BaTiO 3 and SrRuO 3 . Reduced conductivity and, hence, charge screening efficiency in the early growth stage of the SrRuO 3 top electrode promotes a breakdown of ferroelectric BaTiO 3 into domains. We demonstrate how a thermal annealing procedure can recover the single-domain state. By tracking the polarization state in situ, using optical second harmonic generation, we bring new understanding to interface-related electrostatic effects in ferroelectric capacitors.
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