Single-crystal perovskites with excellent photophysical properties are considered to be ideal materials for optoelectronic devices, such as lasers, light-emitting diodes and photodetectors. However, the growth of large-scale perovskite single-crystal films (SCFs) with high optical gain by vapor-phase epitaxy remains challenging. Herein, we demonstrated a facile method to fabricate large-scale thin CsPbBr3 SCFs (∼300 nm) on the c-plane sapphire substrate. High temperature is found to be the key parameter to control low reactant concentration and sufficient surface diffusion length for the growth of continuous CsPbBr3 SCFs. Through the comprehensive study of the carrier dynamics, we clarify that the trapped-related exciton recombination has the main effect under low carrier density, while the recombination of excitons and free carriers coexist until free carriers plays the dominate role with increasing carrier density. Furthermore, an extremely low-threshold (∼8 μJ cm–2) amplified spontaneous emission was achieved at room temperature due to the high optical gain up to 1255 cm–1 at a pump power of 20 times threshold (∼20 P th). A microdisk array was prepared using a focused ion beam etching method, and a single-mode laser was achieved on a 3 μm diameter disk with the threshold of 1.6 μJ cm–2. Our experimental results not only present a versatile method to fabricate large-scale SCFs of CsPbBr3 but also supply an arena to boost the optoelectronic applications of CsPbBr3 with high performance.

Abstract. A new capture vaporizer (CV) has been developed and used recently in the Aerodyne aerosol mass spectrometer (AMS) and aerosol chemical speciation monitor (ACSM) instead of the standard vaporizer (SV) to reduce the particle bounce. It is important to characterize the CV performance in different environments. In this study, we characterized specific organic aerosols (OAs) from vehicle, cooking, biomass burning, and coal burning emissions by a time-of-flight ACSM (TOF-ACSM) with the CV. Their corresponding marker ions that have been defined in the previous SV-based analysis are still valid in the CV mass spectra. Spectra of OAs from cooking and vehicle exhaust show similarities in distinct alkyl fragments but different ratios of m∕z 55 and 57. Ions related to polycyclic aromatic hydrocarbons are present in the OA spectra obtained from burning lignite and bituminous coal but not in the spectra obtained from burning anthracite. Although the relative intensities of m∕z 60 and 73 are much lower in the CV spectra than in the SV spectra for biomass burning OA, they are still relatively greater compared with the spectra for other sources. Our data suggest an atmospheric background of f60 of below 0.03 % for CV. Moreover, we deployed the CV TOF-ACSM along with a SV AMS in urban Beijing during the winter of 2017 to characterize ambient OA with strong anthropogenic influences. The CV TOF-ACSM shows a collection efficiency (CE) of about unity. The CV and SV data show consistent mass concentrations of sulfate, nitrate, ammonium, and OA. Six OA factors are identified by the positive matrix factorization (PMF) analysis for both the CV and the SV data. The SV and CV PMF factors show good correlations in mass concentrations. The SV and CV factors related to coal combustion and cooking differ significantly in loadings, explained by the PMF uncertainty and the lack of understanding of the relative ionization efficiency and CE for primary OA. The CV factors related to secondary sources show greater loadings than the SV factors, which may be associated with the changes in signal-to-noise ratios of various ions in the PMF analysis. Our results support improved mass quantification and useful source identification by the CV for ambient particles in the polluted urban environment. The difference in factor loadings between SV and CV should be considered when interpreting or comparing the PMF results among studies.

Abstract. Oxidation of aromatic volatile organic compounds (VOCs) leads to the formation of tropospheric ozone and secondary organic aerosol, for which gaseous oxygenated products are important intermediates. We show, herein, the experimental results of highly oxygenated organic molecules (HOMs) produced by the oxidation of benzene and toluene in a wide range of OH exposure and NOx conditions. The results suggest that multigeneration OH oxidation plays an important role in the product distribution, which likely proceeds more preferably via H subtraction than OH addition for early generation products from light aromatics. More oxygenated products present in our study than in previous flow tube studies, highlighting the impact of experimental conditions on product distributions. The formation of dimeric products, however, was suppressed and might be unfavorable under conditions of high OH exposure and low NOx in toluene oxidation. Under high-NOx conditions, nitrogen-containing multifunctional products are formed, while the formation of other HOMs is suppressed. Products containing two nitrogen atoms become more important as the NOx level increases, and the concentrations of these compounds depend significantly on NO2. The highly oxygenated nitrogen-containing products might be peroxyacyl nitrates, implying a prolonged effective lifetime of RO2 that facilitates regional pollution. Our results call for further investigation on the roles of high-NO2 conditions in the oxidation of aromatic VOCs.