Publication database
Optical coherence tomography (OCT) with 2 nm axial resolution using a compact laser plasma soft X-ray source
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.
Photochemistry and spectroscopy of small hydrated magnesium clusters Mg+(H2O)n, n = 1–5
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 D1–3 states (correlating with the 3s-3px,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 3px,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.
Photochemistry of glyoxylate embedded in sodium chloride clusters, a laboratory model for tropospheric sea-salt aerosols
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, [NanCln−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 [Nan−xCln−x−2HCOO]+ and [NanCln−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.
Photodissociation of Sodium Iodide Clusters Doped with Small Hydrocarbons
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.
Processing of ultra-hard materials with picosecond pulses: From research work to industrial applications
The ultrashort laser processing of the cutting tools and cutting inserts from tungsten carbide, ceramic and metal composites (CERMET), and polycrystalline diamond materials was demonstrated, and the ablation rates of mentioned ultra-hard materials were evaluated for a laser wavelength of 1064 and 532 nm. The optimal processing throughput was estimated. Laser manufacturing was performed with the five-axis computer numerical control (CNC) machine and scanner for beam translation with the high speed and the ultrashort ∼12 ps pulse duration high repetition rate laser source. The systematic approach was implemented in an experimental variation of process parameters that play a significant role in processing quality. By varying the laser fluence, pulse overlap, and layers’ count, different material removing rates can be achieved from 300 nm/layer to ∼18 μm/layer. The submicrometer removing rate involves a high precision control of the structure depth. It was demonstrated that only by a minor change of the processing parameters, the surface roughness of the material could be minimized down to Ra < 300 nm. Rough and smooth processing can be combined to optimize the structure processing throughput.
Quenching of the red Mn4+ luminescence in Mn4+-doped fluoride LED phosphors
Red-emitting Mn4+-doped fluorides are a promising class of materials to improve the color rendering and luminous efficacy of white light-emitting diodes (w-LEDs). For w-LEDs, the luminescence quenching temperature is very important, but surprisingly no systematic research has been conducted to understand the mechanism for thermal quenching in Mn4+-doped fluorides. Furthermore, concentration quenching of the Mn4+ luminescence can be an issue but detailed investigations are lacking. In this work, we study thermal quenching and concentration quenching in Mn4+-doped fluorides by measuring luminescence spectra and decay curves of K2TiF6:Mn4+ between 4 and 600 K and for Mn4+ concentrations from 0.01% to 15.7%. Temperature-dependent measurements on K2TiF6:Mn4+ and other Mn4+-doped phosphors show that quenching occurs through thermally activated crossover between the 4T2 excited state and 4A2 ground state. The quenching temperature can be optimized by designing host lattices in which Mn4+ has a high 4T2 state energy. Concentration-dependent studies reveal that concentration quenching effects are limited in K2TiF6:Mn4+ up to 5% Mn4+. This is important, as high Mn4+ concentrations are required for sufficient absorption of blue LED light in the parity-forbidden Mn4+ d–d transitions. At even higher Mn4+ concentrations (>10%), the quantum efficiency decreases, mostly due to direct energy transfer to quenching sites (defects and impurity ions). Optimization of the synthesis to reduce quenchers is crucial for developing more efficient highly absorbing Mn4+ phosphors. The present systematic study provides detailed insights into temperature and concentration quenching of Mn4+ emission and can be used to realize superior narrow-band red Mn4+ phosphors for w-LEDs.
Silk protein nanofibers for highly efficient, eco-friendly, optically translucent, and multifunctional air filters
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.
Spectral pulse shaping of a 5 Hz, multi-joule, broadband optical parametric chirped pulse amplification frontend for a 10 PW laser system
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.
Thomson scattering systems on C-2W field-reversed configuration plasma experiment
TAE Technologies’ newly constructed C-2W experiment aims to improve the ion and electron temperatures in a sustained field-reversed configuration plasma. A suite of Thomson scattering systems has been designed and constructed for electron temperature and density profile measurements. The systems are designed for electron densities of 1 × 1012 cm−3 to 2 × 1014 cm−3 and temperature ranges from 10 eV to 2 keV. The central system will provide profile measurements of Te and ne at 16 radial locations from r = −9 cm to r = 64 cm with a temporal resolution of 20 kHz for 4 pulses or 1 kHz for 30 pulses. The jet system will provide profile measurements of Te and ne at 5 radial locations in the open field region from r = −5 cm to r = 15 cm with a temporal resolution of 100 Hz. The central system and its components have been characterized, calibrated, installed, and commissioned. A maximum-likelihood algorithm has been applied for data processing and analysis.
Ultra-sensitive mid-infrared emission spectrometer with sub-ns temporal resolution
We evaluate the performance of a mid-infrared emission spectrometer operating at wavelengths between 1.5 and 6 μm based on an amorphous tungsten silicide (a-WSi) superconducting nanowire single-photon detector (SNSPD). We performed laser induced fluorescence spectroscopy of surface adsorbates with sub-monolayer sensitivity and sub-nanosecond temporal resolution. We discuss possible future improvements of the SNSPD-based infrared emission spectrometer and its potential applications in molecular science.