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.
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.
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 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.
We present the results of the calibration of a channeltron-based electrostatic analyzer operating in time-of-flight mode (ESA-ToF) using tin ions resulting from laser-produced plasma, over a wide range of charge states and energies. Specifically, the channeltron electron multiplier detection efficiency and the spectrometer resolution are calibrated, and count rate effects are characterized. With the obtained overall response function, the ESA-ToF is shown to accurately reproduce charge-integrated measurements separately and simultaneously obtained from a Faraday cup (FC), up to a constant factor the finding of which enables absolute cross-calibration of the ESA-ToF using the FC as an absolute benchmark. Absolute charge-state-resolved ion energy distributions are obtained from ns-pulse Nd:YAG-laser-produced microdroplet tin plasmas in a setting relevant for state-of-the-art extreme ultraviolet nanolithography.
Charge-state-resolved kinetic energy spectra of Sn ions ejected from a laser-produced plasma (LPP) of Sn have been measured at different densities of the H2 buffer gas surrounding a micro-droplet LPP. In the absence of H2, energetic keV Sn ions with charge states ranging from 4+ to 8+ are measured. For the H2 densities used in the experiments no appreciable stopping or energy loss of the ions is observed. However, electron capture by Sn ions from H2 results in a rapid shift towards lower charge states. At the highest H2 pressure of 6×10−4 mbar, only Sn2+ and Sn+ ions are measured. The occurrence of Sn+ ions is remarkable due to the endothermic nature of electron capture by Sn2+ ions from H2. To explain the production of keV Sn+ ions, it is proposed that their generation is due to electron capture by metastable Sn2+∗ ions. The gateway role of metastable Sn2+∗ is underpinned by model simulations using atomic collision cross sections to track the charge states of Sn ions while traversing the H2 buffer gas.
The emission properties of tin plasmas, produced by the irradiation of preformed liquid tin targets by several-ns-long 2 µm-wavelength laser pulses, are studied in the extreme ultraviolet (EUV) regime. In a two-pulse scheme, a pre-pulse laser is first used to deform tin microdroplets into thin, extended disks before the main (2 µm) pulse creates the EUV-emitting plasma. Irradiating 30-to 300 µm-diameter targets with 2 µm laser pulses, we find that the efficiency in creating EUV light around 13.5 nm follows the fraction of laser light that overlaps with the target. Next, the effects of a change in 2 µm drive laser intensity (0.6-1.8 × 10 11 W cm −2 ) and pulse duration (3.7-7.4 ns) are studied. It is found that the angular dependence of the emission of light within a 2% bandwidth around 13.5 nm and within the backward 2π hemisphere around the incoming laser beam is almost independent of intensity and duration of the 2 µm drive laser. With increasing target diameter, the emission in this 2% bandwidth becomes increasingly anisotropic, with a greater fraction of light being emitted into the hemisphere of the incoming laser beam. For direct comparison, a similar set of experiments is performed with a 1 µm-wavelength drive laser. Emission spectra, recorded in a 5.5-25.5 nm wavelength range, show significant self-absorption of light around 13.5 nm in the 1 µm case, while in the 2 µm case only an opacity-related broadening of the spectral feature at 13.5 nm is observed. This work demonstrates the enhanced capabilities and performance of 2 µm-driven plasmas produced from disk targets when compared to 1 µm-driven plasmas, providing strong motivation for the use of 2 µm lasers as drive lasers in future high-power sources of EUV light.
We present a method to obtain the individual charge-state-dependent kinetic-energy distributions of tin ions emanating from a laser-produced plasma from their joint overlapping energy distributions measured by means of a retarding field energy analyzer (RFA). The method of extracting charge state specific parameters from the ion signals is described mathematically, and reinforced with experimental results. The absolute charge-state-resolved ion energy distributions is obtained from ns-pulse Nd:YAG-laser-produced microdroplet tin plasmas in a setting relevant for state-of-the-art extreme ultraviolet nanolithography.
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