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We used time-of-flight photocurrent measurements to determine the role of grain boundaries in charge carrier transport in thin layers of methyl ammonium lead iodide (CH₃NH₃PbI₃). The measurement results were compared to Kinetic Monte Carlo simulations, based on a transport model, which disentangles the transport within crystallites and hopping across grain boundaries. The observed mobilities of electrons are in the order ∼2.5 × 10⁻¹ cm²V⁻¹s⁻¹. The hopping across grains is modeled with an Arrhenius-type probability rate, characterized by activation energy (E_a). It was found that the E_a estimated from the slope of a mobility-temperature dependence is in the range of ∼56–70 meV. The factors contributing to E_a are shunting pathways and the grain-size variations including energy level misalignments at the grain boundaries. These results represent a step toward a design of novel windowless organic-inorganic perovskite solar cells.

We optimized the parameters of a laser-produced plasma source based on a solid-state Nd: YAG laser (λ = 1.06 nm, pulse duration 4 ns, energy per pulse up to 500 mJ, repetition rate 10 Hz, lens focus distance 45 mm, maximum power density of laser radiation in focus 9 × 10¹¹ W/cm²) and a double-stream Xe/He gas jet to obtain a maximum of radiation intensity around 11 nm wavelength. It was shown that the key factor determining the ionization composition of the plasma is the jet density. With the decreased density, the ionization composition shifts toward a smaller degree of ionization, which leads to an increase in emission peak intensity around 11 nm. We attribute the dominant spectral feature centred near 11 nm originating from an unidentified 4d-4f transition array in Xe^+10…+13 ions. The exact position of the peak and the bandwidth of the emission line were determined. We measured the dependence of the conversion efficiency of laser energy into an EUV in-band energy with a peak at 10.82 nm from the xenon pressure and the distance between the nozzle and the laser focus. The maximum conversion efficiency (CE) into the spectral band of 10–12 nm measured at a distance between the nozzle and the laser beam focus of 0.5 mm was CE = 4.25 ± 0.30%. The conversion efficiencies of the source in-bands of 5 and 12 mirror systems at two wavelengths of 10.8 and 11.2 nm have been evaluated; these efficiencies may be interesting for beyond extreme ultraviolet lithography.

Degradation of organic materials is responsible for the short operation lifetimes of organic light-emitting devices, but the mechanism by which such degradation is initiated has yet to be fully established. Here we report a new mechanism for degradation of emitting layers in blue-phosphorescent devices. We investigate binary mixtures of a wide bandgap host and a series of novel Ir(III) complex dopants having N-heterocyclocarbenic ligands. Our mechanistic study reveals the charge-neutral generation of polaron pairs (radical ion pairs) by electron transfer from the dopant to host excitons. Annihilation of the radical ion pair occurs by charge recombination, with such annihilation competing with bond scission. Device lifetime correlates linearly with the rate constant for the annihilation of the radical ion pair. Our findings demonstrate the importance of controlling exciton-induced electron transfer, and provide novel strategies to design materials for long-lifetime blue electrophosphorescence devices.

Photoacoustic microscopy (PAM) is an emerging imaging technology that can non-invasively visualize ocular structures in animal eyes. This report describes an integrated multimodality imaging system that combines PAM, optical coherence tomography (OCT), and fluorescence microscopy (FM) to evaluate angiogenesis in larger animal eyes. High-resolution in vivo imaging was performed in live rabbit eyes with vascular endothelial growth factor (VEGF)-induced retinal neovascularization (RNV). The results demonstrate that our multimodality imaging system can non-invasively visualize RNV in both albino and pigmented rabbits to determine retinal pathology using PAM and OCT and verify the leakage of neovascularization using FM and fluorescein dye. This work presents high-resolution visualization of angiogenesis in rabbits using a multimodality PAM, OCT, and FM system and may represent a major step toward the clinical translation of the technology.

We present optical coherence tomography (OCT) with 2 nm axial resolution using broadband soft X-ray radiation (SXR) from a compact laser plasma light source. The laser plasma was formed by the interaction of nanosecond laser pulses with a gaseous target in a double stream gas puff target approach. The source was optimized for efficient SXR emission from the krypton/helium gas puff target in the 2 to 5 nm spectral range, encompassing the entire “water-window” spectral range from 2.3 nm to 4.4 nm wavelength. The coherence parameters of the SXR radiation allowed for the OCT measurements of a bulk multilayer structure with 10 nm period and 40% bottom layer thickness to period ratio, with an axial resolution of about 2 nm and detect multilayer interfaces up to a depth of about 100 nm. The experimental data are in agreement with OCT simulations performed on ideal multilayer structure. In the paper, detailed information about the source, its optimization, the optical system, OCT measurements and the results are presented and discussed.

Hydrated singly charged magnesium ions Mg⁺(H₂O)_n, n ≤ 5, in the gas phase are ideal model systems to study photochemical hydrogen evolution since atomic hydrogen is formed over a wide range of wavelengths, with a strong cluster size dependence. Mass selected clusters are stored in the cell of an Fourier transform ion cyclotron resonance mass spectrometer at a temperature of 130 K for several seconds, which allows thermal equilibration via blackbody radiation. Tunable laser light is used for photodissociation. Strong transitions to D_1–3 states (correlating with the 3s-3p_x,y,z transitions of Mg⁺) are observed for all cluster sizes, as well as a second absorption band at 4–5 eV for n = 3-5. Due to the lifted degeneracy of the 3p_x,y,z energy levels of Mg⁺, the absorptions are broad and red shifted with increasing coordination number of the Mg⁺ center, from 4.5 eV for n = 1 to 1.8 eV for n = 5. In all cases, H atom formation is the dominant photochemical reaction channel. Quantum chemical calculations using the full range of methods for excited state calculations reproduce the experimental spectra and explain all observed features. In particular, they show that H atom formation occurs in excited states, where the potential energy surface becomes repulsive along the O⋯H coordinate at relatively small distances. The loss of H₂O, although thermochemically favorable, is a minor channel because, at least for the clusters n = 1-3, the conical intersection through which the system could relax to the electronic ground state is too high in energy. In some absorption bands, sequential absorption of multiple photons is required for photodissociation. For n = 1, these multiphoton spectra can be modeled on the basis of quantum chemical calculations.

Although marine aerosols undergo extensive photochemical processing in the troposphere, a molecular level understanding of the elementary steps involved in these complex reaction sequences is still missing. As a defined laboratory model system, the photodissociation of sea salt clusters doped with glyoxylate, [Na_nCl_n−2(C₂HO₃)]⁺, n = 5–11, is studied by a combination of mass spectrometry, laser spectroscopy and ab initio calculations. Glyoxylate acts as a chromophore, absorbing light below 400 nm via two absorption bands centered at about 346 and 231 nm. Cluster fragmentation dominates, which corresponds to internal conversion of the excited state energy into vibrational modes of the electronic ground state and subsequent unimolecular dissociation. Photochemical dissociation pathways in electronically excited states include CO and HCO elimination, leading to [Na_n−xCl_n−x−2HCOO]⁺ and [Na_nCl_n−2COO˙]⁺ with typical quantum yields in the range of 1–3% and 5–10%, respectively, for n = 5. The latter species contains CO₂˙⁻ stabilized by the salt environment. The comparison of different cluster sizes shows that the fragments containing a carbon dioxide radical anion appear in a broad spectral region of 310–380 nm. This suggests that the elusive CO₂˙⁻ species may be formed by natural processes in the troposphere. Based on the photochemical cross sections obtained here, the photolysis lifetime of glyoxylate in a dry marine aerosol is estimated as 10 h. Quantum chemical calculations show that dissociation along the C–C bond in glyoxylic acid as well as glyoxylate embedded in the salt cluster occurs after reaching the S₁/S₀ conical intersection, while this conical intersection is absent in free glyoxylate ions.

Marine aerosols consist of a variety of compounds and play an important role in many atmospheric processes. In the present study, sodium iodide clusters with their simple isotope pattern serve as model systems for laboratory studies to investigate the role of iodide in the photochemical processing of sea-salt aerosols. Salt clusters doped with camphor, formate and pyruvate are studied in a Fourier transform ion cyclotron resonance mass spectrometer (FT-ICR MS) coupled to a tunable laser system in both UV and IR range. The analysis is supported by ab initio calculations of absorption spectra and energetics of dissociative channels. We provide quantitative analysis of IRMPD measurements by reconstructing one-photon spectra and comparing them with the calculated ones. While neutral camphor is adsorbed on the cluster surface, the formate and pyruvate ions replace an iodide ion. The photodissociation spectra revealed several wavelength-specific fragmentation pathways, including the carbon dioxide radical anion formed by photolysis of pyruvate. Camphor and pyruvate doped clusters absorb in the spectral region above 290 nm, which is relevant for tropospheric photochemistry, leading to internal conversion followed by intramolecular vibrational redistribution, which leads to decomposition of the cluster. Potential photodissociation products of pyruvate in the actinic region may be formed with a cross section of <2×10⁻²⁰ cm², determined by the experimental noise level.

New types of air filter technologies are being called because air pollution by particulate matters (PMs) and volatile organic compounds has raised serious concerns for public health. Conventional air filters have limited application and poor degradability and they become non-disposable wastes after use. Here, we report a highly efficient, eco-friendly, translucent, and multifunctional air purification filter that is highly effective for reducing air pollution, protecting the environment, and detecting hazardous chemical vapors encountered in everyday life. Uniform silk protein nanofibers were directly generated on a window screen by an electrospinning process. Optical properties (translucence and scattering) of the silk nanofibrous air filters (SNAFs) are advantageous for achieving viewability and controlling the room temperature. Air filtration efficiencies of the fabricated SNAFs could reach up to 90% and 97% for PMs with sizes under 2.5 and 10 μm, respectively, exceeding the performances of commercial semi-high-efficiency particulate air (semi-HEPA) filters. After use, the SNAFs could be naturally degraded. Furthermore, we demonstrate the ability of SNAFs impregnated with organic dyes to sense hazardous and volatile vapors encountered in everyday life.

We present a broadband optical parametric chirped pulse amplification (OPCPA) system delivering 4 J pulses at a repetition rate of 5 Hz. It will serve as a frontend for the 1.5 kJ, <150 fs, 10 PW laser beamline currently under development by a consortium of National Energetics and Ekspla. The spectrum of the OPCPA system is precisely controlled by arbitrarily generated waveforms of the pump lasers. To fully exploit the high flexibility of the frontend, we have developed a 1D model of the system and an optimization algorithm that predicts suitable pump waveform settings for a desired output spectrum. The OPCPA system is shown to have high efficiency, a high-quality top-hat beam profile, and an output spectrum demonstrated to be shaped consistently with the theoretical model.