All-inorganic cesium lead halide perovskite nanocrystals are extensively studied because of their outstanding optoelectronic properties. Being of a cubic shape and typically featuring a narrow size distribution, CsPbX3 (X = Cl, Br, and I) nanocrystals are the ideal starting material for the development of homogeneous thin films as required for photovoltaic and optoelectronic applications. Recent experiments reveal spontaneous merging of drop-casted CsPbBr3 nanocrystals, which is promoted by humidity and mild-temperature treatments and arrested by electron beam irradiation. Here, we make use of atom-resolved annular dark-field imaging microscopy and valence electron energy loss spectroscopy in a state-of-the-art low-voltage monochromatic scanning transmission electron microscope to investigate the aggregation between individual nanocrystals at the atomic level. We show that the merging process preserves the elemental composition and electronic structure of CsPbBr3 and takes place between nanocrystals of different sizes and orientations. In particular, we reveal seamless stitching for aligned nanocrystals, similar to that reported in the past for graphene flakes. Because the crystallographic alignment occurs naturally in drop-casted layers of CsPbX3 nanocrystals, our findings constitute the essential first step toward the development of large-area nanosheets with band gap energies predesigned by the nanocrystal choice—the gateway to large-scale photovoltaic applications of inorganic perovskites.

Photon recycling, the iterative process of re-absorption and re-emission of photons in an absorbing medium, can play an important role in the power-conversion efficiency of photovoltaic cells. To date, several studies have proposed that this process may occur in bulk or thin films of inorganic lead-halide perovskites, but conclusive proof of the occurrence and magnitude of this effect is missing. Here, we provide clear evidence and quantitative estimation of photon recycling in CsPbBr 3 nanocrystal suspensions by combining measurements of steady-state and time-resolved photoluminescence (PL) and PL quantum yield with simulations of photon diffusion through the suspension. The steady-state PL shows clear spectral modifications including red shifts and quantum yield decrease, while the time-resolved measurements show prolonged PL decay and rise times. These effects grow as the nanocrystal concentration and distance traveled through the suspension increase. Monte Carlo simulations of photons diffusing through the medium and exhibiting absorption and re-emission account quantitatively for the observed trends and show that up to five re-emission cycles are involved. We thus identify 4 quantifiable measures, PL red shift, PL QY, PL decay time, and PL rise time that together all point toward repeated, energy-directed radiative transfer between nanocrystals. These results highlight the importance of photon recycling for both optical properties and photovoltaic applications of inorganic perovskite nanocrystals.

We present the results of a joint experimental and theoretical study of plasma expansion arising from Nd:YAG laser ablation (laser wavelength λ = 1.064 μm) of tin microdroplets in the context of extreme ultraviolet lithography. Measurements of the ion energy distribution reveal a near-plateau in the distribution for kinetic energies in the range 0.03-1 keV and a peak near 2 keV followed by a sharp fall-off in the distribution for energies above 2 keV. Charge-state resolved measurements attribute this peak to the existence of peaks centered near 2 keV in the Sn 3+ -Sn 8+ ion energy distributions. To better understand the physical processes governing the shape of the ion energy distribution, we have modelled the laser-droplet interaction and subsequent plasma expansion using two-dimensional radiation hydrodynamic simulations. We find excellent agreement between the simulated ion energy distribution and the measurements both in terms of the shape of the distribution and the absolute number of detected ions. We attribute a peak in the distribution near 2 keV to a quasi-spherical expanding shell formed at early times in the expansion.

We present results from a combined experimental and numerical simulation study of the anisotropy of the expansion of a laser-produced plasma into vacuum. Plasma is generated by nanosecond Nd:YAG laser pulse impact (laser wavelength [Formula: see text]) onto tin microdroplets. Simultaneous measurements of ion kinetic energy distributions at seven angles with respect to the direction of the laser beam reveal strong anisotropic emission characteristics, in close agreement with the predictions of two-dimensional radiation-hydrodynamic simulations. Angle-resolved ion spectral measurements are further shown to provide an accurate prediction of the plasma propulsion of the laser-impacted droplet.