Publication database
The importance of relativistic effects on two-photon absorption spectra in metal halide perovskites
Despite intense research into the optoelectronic properties of metal halide perovskites (MHPs), sub-bandgap absorption in MHPs remains largely unexplored. Here we recorded two-photon absorption spectra of MHPs using the time-resolved microwave conductivity technique. A two-step upward trend is observed in the two-photon absorption spectrum for methylammonium lead iodide, and some analogues, which implies that the commonly used scaling law is not applicable to MHPs. This aspect is further confirmed by temperature-dependent conductivity measurements. Using an empirical multiband tight binding model, spectra for methylammonium lead iodide were calculated by integration over the entire Brillouin zone, showing compelling similarity with experimental results. We conclude that the second upward trend in the two-photon absorption spectrum originates from additional optical transitions to the heavy and light electron bands formed by the strong spin-orbit coupling. Hence, valuable insight can be obtained in the opto-electronic properties of MHPs by sub-bandgap spectroscopy, complemented by modelling.
Thermochemical writing with high spatial resolution on Ti films utilising picosecond laser
In this paper, we investigate the local oxidation of titanium thin films under the action of picosecond laser pulses. Periodical structures were recorded by the multi-beam interference scheme utilizing various numbers of laser beams, and the relationship between spatial resolution and the contrast of the structures was studied. The Raman spectra of the laser processing regions confirmed the oxidation even under the action of a single picosecond pulse. An analytical simulation of titanium film oxidation in the interference field was provided, and obtained results are correlated with the experimental data. The results of theoretical modeling show that the thermochemical effects of picosecond laser pulses allow recording periodic structures with a period of 0.65 lines per μm. The demonstrated results are important in the adaptation of technological laser systems for the manufacture of diffractive optical elements.
Third-order nonlinear optical properties of phycobiliproteins from cyanobacteria and red algae
Second hyperpolarizability (γ) measurements as well as third harmonic generation (THG) imaging was performed to determine if phycobiliproteins contribute to cyanobacteria THG, and to establish if phycobiliproteins are suitable dyes for THG microscopy. Three phycobiliproteins and one phycobilin were investigated via THG ratio γ measurements, revealing phycocyanobilin has ~7× higher γ than β-carotene, a standard THG dye. Phycobiliproteins also had large γ values, showing they are promising THG dyes. Stoichiometric summations of phycobilin γ values revealed they are the dominant source of THG signal from phycobiliproteins. THG imaging was performed to demonstrate phycobiliproteins and phycobilins can be useful THG dyes.
Vibrational Relaxation Lifetime of a Physisorbed Molecule at a Metal Surface
Previous measurements of vibrational relaxation lifetimes for molecules adsorbed at metal surfaces yielded values of 1–3 ps; however, only chemisorbed molecules have been studied. We report the first measurements of the vibrational relaxation lifetime of a molecule physisorbed to a metal surface. For CO(υ=1) adsorbed on Au(111) at 35 K the vibrational lifetime of the excited stretching mode is 49±3 ps. The long lifetime seen here is likely to be a general feature of physisorption, which involves weaker electronic coupling between the adsorbate and the solid due to bonding at larger distances.
Advanced laser scanning for highly-efficient ablation and ultrafast surface structuring: experiment and model
Ultra-short laser pulses are frequently used for material removal (ablation) in science, technology and medicine. However, the laser energy is often used inefficiently, thus, leading to low ablation rates. For the efficient ablation of a rectangular shaped cavity, the numerous process parameters such as scanning speed, distance between scanned lines, and spot size on the sample, have to be optimized. Therefore, finding the optimal set of process parameters is always a time-demanding and challenging task. Clear theoretical understanding of the influence of the process parameters on the material removal rate can improve the efficiency of laser energy utilization and enhance the ablation rate. In this work, a new model of rectangular cavity ablation is introduced. The model takes into account the decrease in ablation threshold, as well as saturation of the ablation depth with increasing number of pulses per spot. Scanning electron microscopy and the stylus profilometry were employed to characterize the ablated depth and evaluate the material removal rate. The numerical modelling showed a good agreement with the experimental results. High speed mimicking of bio-inspired functional surfaces by laser irradiation has been demonstrated.
Characterization and calibration of the Thomson scattering diagnostic suite for the C-2W field-reversed configuration experiment
The new C-2W Thomson scattering (TS) diagnostic consists of two individual subsystems for monitoring electron temperature (Te) and density (ne): one system in the central region is currently operational, and the second system is being commissioned to monitor the open field line region. Validating the performance of the TS’s custom designed system components and unique calibration of the detection system and diagnostic as a whole is crucial to obtaining high precision Te and ne profiles of C-2W’s plasma. The major components include a diode-pumped Nd:YAG laser which produces 35 pulses at up to 20 kHz, uniquely designed collection lenses with a fast numerical aperture, and uniquely designed polychromators with filters sets to optimize a Te ranging from 10 eV to 2 keV. This paper describes the design principles and techniques used to characterize the main components of the TS diagnostic on C-2W, as well as the results of Rayleigh scattering calibrations performed for the whole system response.
Charge carrier transport in polycrystalline CH3NH3PbI3 perovskite thin films in a lateral direction characterized by time-of-flight photoconductivity
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 (Ea). It was found that the Ea estimated from the slope of a mobility-temperature dependence is in the range of ∼56–70 meV. The factors contributing to Ea 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.
Compact diffractive optics for THz imaging
We present a compact diffractive silicon-based multilevel phase Fresnel lens (MPFL) with up to 50 mm in diameter and a numerical aperture up to 0.86 designed and fabricated for compact terahertz (THz) imaging systems. The laser direct writing technology based on a picosecond laser was used to fabricate diffractive optics on silicon with a different number of phase quantization levels P reaching an almost kinoform spherical surface needed for efficient THz beam focusing. Focusing performance was investigated by measuring Gaussian beam intensity distribution in the focal plane and along the optical axis of the lens. The beam waist and the focal depth for each MPFL were evaluated. The influence of the phase quantization number on the focused beam amplitude was estimated, and the power transmission efficiency reaching more than 90% was revealed. The THz imaging of less than 1 mm using a robust 50 mm diameter multilevel THz lens was achieved and demonstrated at 580 GHz frequency.
Conversion efficiency of a laser-plasma source based on a Xe jet in the vicinity of a wavelength of 11 nm
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 blue-phosphorescent organic light-emitting devices involves exciton-induced generation of polaron pair within emitting layers
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.