SEARCH · Engineering Papers
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Direct comparisons are made between an active laser-based swept-wavelength ECQCL and passive LWIR hyperspectral imager for dynamic chemical plume detection at a standoff distance of 1.5 km in complex terrain
We irradiate a ZnTe single crystal with 10-fs laser pulses at a repetition rate of 80 MHz and investigate its resulting gradual modification by means of coherent-phonon spectroscopy. We observe the emergence of a phonon mode at about 3.6 THz whose amplitude and lifetime grow monotonously with irradiation time. The speed of this process depends sensitively on the pump-pulse duration. Our observations strongly indicate that the emerging phonon mode arises from a Te phase induced by multiphoton absorption of incident laser pulses. A potential application of our findings is laser-machining of microstructures in the bulk of a ZnTe crystal, a highly relevant electrooptic material.
Experiments accessing extreme conditions at x-ray free electron lasers (XFELs) involve rapidly evolving conditions of temperature. Here, we report time-resolved, direct measurements of temperature using spectral streaked optical pyrometry of x-ray and optical laser-heated states at the High Energy Density instrument of the European XFEL. This collection of typical experiments, coupled with numerical models, outlines the reliability, precision, and meaning of time dependent temperature measurements using optical emission at XFEL sources. Dynamic temperatures above 1500 K are measured continuously from spectrally- and temporally-resolved thermal emission at 450–850 nm, with time resolution down to 10–100 ns for 1–200 μs streak camera windows, using single shot and integrated modes. Targets include zero-pressure foils free-standing in air and in vacuo, and high-pressure samples compressed in diamond anvil cell multi-layer targets. Radiation sources used are 20-fs hard x-ray laser pulses at 17.8 keV, in single pulses or 2.26 MHz pulse trains of up to 30 pulses, and 250-ns infrared laser single pulses. A range of further possibilities for optical measurements of visible light in x-ray laser experiments using streak optical spectroscopy are also explored, including for the study of x-ray induced optical fluorescence, which often appears as background in thermal radiation measurements. We establish several scenarios where combined emissions from multiple sources are observed and discuss their interpretation. Challenges posed by using x-ray lasers as non-invasive probes of the sample state are addressed.
A laser-induced air breakdown plasma is a dynamical system and its fundamental parameters change significantly during its lifetime. The temporal evolution of the spectral features from an air plasma shows emission from bremsstrahlung followed by discrete electronic transitions from ions, atoms, and rotational and vibrations bands from molecules. The molecular band emission from air plasma typically appears at times ≳5 μs and persists for 100s of μs. Here, an evaluation is made on the temperature evolution and speciation in a laser-produced air plasma. The air plasmas are generated by focusing 1064 nm, 6 ns pulses from an Nd:YAG laser. High-resolution emission spectra of various molecules such as N 2 , N 2 + , CN, OH, NH, NO are acquired for fits to spectral models. Fitting of atomic and molecular emission features permits tracking of the air spark temperature evolution from 1 to 200 µs. Though the excitation and molecular temperatures show good overlap at times ≲10 μs, the molecular temperatures obtained from different species show a discontinuity at times ~ 30 μs and this is related to shock collapse and subsequent changes in hydrodynamics and chemistry of the plume. The fitting of multiple species in broadband spectra has permitted calculation of the relative concentrations of various molecules as a function of temperature that provides insight into the air spark speciation. Finally, the measured mole fractions from laser-induced air plasma are within a factor of 2 - 6 of the values estimated by speciation model under the assumption of thermal and chemical equilibrium across the temperature ranges studied and probable reasons for the observed deviation are described.
We report on the linewidth narrowing of a room-temperature mid-infrared quantum cascade laser by phase-locking to a difference-frequency-generated radiation referenced to an optical frequency comb synthesizer. A locking bandwidth of 250 kHz, with a residual rms phase-noise of 0.56 rad, has been achieved. The laser linewidth is narrowed by more than 2 orders of magnitude below 1 kHz, and its frequency is stabilized with an absolute traceability of 2 Multiplication-Sign 10{sup -12}. This source has allowed the measurement of the absolute frequency of a CO{sub 2} molecular transition with an uncertainty of about 1 kHz.
Laser-Induced Breakdown Spectroscopy or LIBS is a rapid, in-situ analytical technique where a laser of known energy is pulsed at the surface of an analyte. The laser pulse rapidly heats a localized area to many thousand degrees Kelvin, ablating part of the analyte and turning it into a plasma. As the plasma cools, excited atoms return to a ground state with known emission energies. This emitted energy is captured by various spectrometers and provides a spectrum of the emitted energies and intensities. This spectrum can be analyzed to provide the elemental composition of a sample by using known emission lines and relative abundance. ElementLIBS was developed for the SciAps hand-held LIBS model Z300 but will work with any model that provides a LIBS spectrum of similar resolution. The Z300 has an integrated resolution of 1/30 nm with a range of approximately 180nm – 960nm, providing an output spectrum of 23431 pixels across three spectrometers. These criteria are only provided as a reference, as the software was designed to work with any size spectrum, provided the input file is of the correct format and the models were developed using the same framework. If spectra of varying dimensions are used, the software will fail without warning and unusual events could occur.
A metal-semiconductor heterojunction is investigated by Auger and photoelectron spectroscopy to characterize the structural and electronic properties of the metallic film and to obtain the time-resolved electronic response induced by femtosecond laser excitation of the semiconductor material. The 3.5 monolayer (ML) Zn films deposited on p-type Si(100) at liquid nitrogen temperature grows in a layer-by-layer fashion. Electronic structure measurements by extreme ultraviolet (XUV) photoelectron spectroscopy indicate that the films are metallic in nature, creating a Schottky barrier at the 3.5 ML Zn/p-Si(100) interface. Utilizing a 35 fs, 800 nm pump pulse at a pump intensity of (2.5-6) × 10 9 W/cm 2 to excite the Si and a time-delayed extreme ultraviolet pulse to probe the Zn, we observed large transient surface photovoltage shifts of 0.3-2.2 eV at carrier densities of (1.5-4.5) × 10 20 cm -3 . Three shifts are determined the Zn 3d core level, the photoemission onset, and the metallic Fermi level. The photovoltages increase with laser excitation intensity, and the Zn 3d core level exhibits the largest binding energy shifts due to pronounced screening of the core level. The large observed shifts are rationalized on the basis of the energetics of band flattening and carrier accumulation in the metallic layer of the Zn/p-Si(100) heterojunction at high carrier densities. The observed carrier recombination dynamics are biexponential in character, with similar time constants for both the Zn 3d and photoemission onset binding energy shifts. The Zn 3d core level shifts are also found to be sensitive to the electron temperature. These results show that core-level photoemission can be used to monitor valence electron dynamics, allowing separation of charge dynamics in heterojunctions and solids composed of multiple elements.
A novel method of determining the total uncertainty in the integrated intensity of fitted emission lines in multi-peaked emission spectra is presented. The proposed method does not require an assumption of the type of line profile to be specified. The absolute difference between a fit and measured spectrum defines the uncertainty of the integrated signal intensity and is subsequently decomposed to determine the uncertainty of each peak in multi-line fits. Decomposition relies on tabulating a weighting factor which describes how each peak contributes to the total integral uncertainty. Applications of this method to quantitative approaches in laser-induced breakdown spectroscopy analysis are described.
Through computer simulation on experimentally acquired optical spectra, uranium isotopic analysis by laser ablation molecular isotopic spectrometry and laser induced breakdown spectroscopy were studied. The use of only one spectral feature, either the strong UO band at 593.55 nm or the nearby U I 593.382 nm line, are similar in precisions (~ 1.5% in absolute 235 U abundances). Precision improves to 0.72% with the use of a group of U atomic lines from 591.6 to 596.5 nm. The use of both molecular bands and atomic lines further advances the precision to 0.42% and compares well with the U II 424.437 nm single-line benchmark (0.48% precision).
The development of interband cascade lasers (ICLs) has made the strong C-H transitions in the 3 μm spectral region increasingly accessible. We present the demonstration of a single mode distributed feedback ICL coupled to a V-shaped optical cavity in an optical feedback cavity-enhanced absorption spectroscopy (OF-CEAS) experiment. We achieved a minimum detectable absorption coefficient, α{sub min}, of (7.1±0.2)×10{sup −8} cm{sup −1} for a spectrum of CH{sub 4} at 3.24 μm with a two second acquisition time (100 scans averaged). This corresponds to a detection limit of 3 ppb CH{sub 4} at atmospheric pressure, which is comparable to previously reported OF-CEAS instruments with diode lasers or quantum cascade lasers. The ability to frequency lock an ICL source in the important 3 μm region to an optical cavity holds great promise for future spectroscopic applications.
The electron affinity (EA), the energy released when a neutral atom binds an additional electron, is a fundamental property of atoms that is governed by electron-electron correlations and is strongly related to an element’s chemical reactivity. However, conventional techniques for EA determination lack the experimental sensitivity to probe very scarce samples. As a result, the EA for the heaviest elements of the periodic table is entirely uncharted. Here, we present a novel technique to determine EAs through Laser Photodetachment Threshold Spectroscopy, performed in an electrostatic ion beam trap to increase the samples’ exposure to laser photons and, thus, improve the experimental signal sensitivity by three orders of magnitude. Moreover, the additional exposure time allows the use of lower-power continuous-wave narrow-band lasers that reduce uncertainties associated with broadening effects induced by the laser bandwidth. By applying this technique, we measure the EA of 35 Cl to be 3.612720(44) eV, achieving state-of-the-art precision while employing five orders of magnitude fewer anions. The demonstrated sensitivity paves the way for systematic EA measurements across isotopic chains - including isotope shifts and hyperfine splittings - and ultimately for the first direct determination of electron affinities in superheavy elements.
This report describes in chronological detail the development of the Spaceborne Photonics Institute as a sustained research effort at Hampton University in the area of optical physics. This provided the research expertise to initiate a PhD program in Physics. Research was carried out in the areas of: (1) modelling of spaceborne solid state laser systems; (2) amplified spontaneous emission in solar pumped iodine lasers; (3) closely simulated AM0 CW solar pumped iodine laser and repeatedly short pulsed iodine laser oscillator; (4) a materials spectroscopy and growth program; and (5) laser induced fluorescence and atomic and molecular spectroscopy.
In the present work, the optical emission spectra of silver (Ag) plasma have been recorded and analyzed using the laser induced breakdown spectroscopy technique. The emission line intensities and plasma parameters were investigated as a function of lens to sample distance, laser irradiance, and distance from the target surface. The electron number density (n{sub e}) and electron temperature (T{sub e}) were determined using the Stark broadened line profile and Boltzmann plot method, respectively. A gradual increase in the spectral line intensities and the plasma parameters, n{sub e} from 2.89 × 10{sup 17} to 3.92 × 10{sup 17 }cm{sup −3} and T{sub e} from 4662 to 8967 K, was observed as the laser irradiance was increased 2.29 × 10{sup 10}–1.06 × 10{sup 11} W cm{sup −2}. The spatial variations in n{sub e} and T{sub e} were investigated from 0 to 5.25 mm from the target surface, yielding the electron number density from 4.78 × 10{sup 17} to 1.72 × 10{sup 17 }cm{sup −3} and electron temperature as 9869–3789 K. In addition, the emission intensities and the plasma parameters of silver were investigated by varying the ambient pressure from 0.36 to 1000 mbars.
Raman and photoluminescence spectra of nanostructured ZnO films with adsorbed C60 molecules were studied. The possibility of intensive C60–ZnO electronic coupling forming in this composite was investigated. It is shown that such an electron coupling can be significantly enhanced by irradiating the composite with high intensity UV laser radiation (λ = 325 nm).
The effects of laser wavelength and argon ambient gas pressure on ionic and atomic emission from aluminum and copper metal plasmas has been studied. The plasmas were generated using metal targets excited with a Q-switched Nd:YAG laser operating at the first fundamental (1064 nm), second (532 nm), third (355 nm), and fourth harmonics (266 nm) with repetition rate up to 10 Hz. The spectroscopic analysis of the plasma plume emission revealed that the intensities and signal-to-noise (S/N) ratio of various neutral and ion spectral lines, small components, and trace impurities increase sharply when the fourth laser harmonic is used at a wavelength of 266 nm. Based on LTE assumption, the electron excitation temperature (T{sub e}) and electron number density (N{sub e}) of the produced plasma have been estimated from the Boltzmann plot using neutral spectral lines of Al I at 256.8, 257.5, 309.3, and 396.15 nm and Cu I at 427.58, 510.59, 570.07, and 578.58 nm and from Stark broadening width profile of Al II at 281.6 nm and Cu I at 324.75 nm, respectively. The variations of T{sub e}, N{sub e}, and emission intensities of metals as a function of laser irradiance of different laser wavelengths at 1064, 532, 355, and 266 nm were studied. The effect of the argon ambient gas pressure on the plasma parameters was also studied. The diagnostics of the produced metal plasma was undertaken using laser induced breakdown spectroscopy (LIBS).
We have studied the structure of enzymes and the chemistry at the catalytic sites, intensively and have acquired an understanding of the atomic-scale chemistry which requires a new approach beyond steady state X-ray crystallography and X-ray spectroscopy at cryogenic temperatures. Following the dynamic changes in the geometric and electronic structure of metallo-enzymes at ambient conditions, while overcoming the severe X-ray-induced changes to the redox active catalytic center, is key for deriving reaction mechanisms. Such studies become possible by the intense and ultra-short femtosecond (fs) X-ray pulses from an X-ray free electron laser (XFEL) by acquiring a signal before the sample is destroyed. Our review describes the recent and pioneering uses of XFELs to study the protein structure and dynamics of metallo-enzymes using crystallography and scattering, as well as the chemical structure and dynamics of the catalytic complexes (charge, spin, and covalency) using spectroscopy during the reaction to understand the electron-transfer processes and elucidate the mechanism.
How materials evolve at thermal equilibrium and under external excitations at small length and time scales is crucial to the understanding and control of material properties. X-ray photon correlation spectroscopy (XPCS) at X-ray free electron laser (XFEL) facilities can in principle capture dynamics of materials that are substantially faster than a millisecond. However, the analysis and interpretation of XPCS data is hindered by the strongly fluctuating X-ray intensity from XFELs. Here we examine the impact of pulse-to-pulse intensity fluctuations on sequential XPCS analysis. We show that the conventional XPCS analysis can still faithfully capture the characteristic time scales, but with substantial decrease in the signal-to-noise ratio of the g2 function and increase in the uncertainties of the extracted time constants. We also demonstrate protocols for improving the signal-to-noise ratio and reducing the uncertainties.
We present a detailed investigation of the temporal evolution of line and continuum emissions in laser-induced breakdown spectroscopy (LIBS) of gaseous uranium hexafluoride (UF 6 ), focusing on the spectral region near 646 nm. Spectral emission features, signal-to-background ratios (SBRs) of selected uranium lines, and spectral linewidths were examined under varying UF 6 pressures (15–60 Torr) and laser pulse energies (10–60 mJ). Higher pressures and pulse energies enhanced continuum emission and reduced SBRs but did not cause significant spectral congestion. Additional studies with the use of different laser systems, including nanosecond-pulsed Nd:YAG lasers (at fundamental and various harmonics) and a femtosecond-pulsed Ti:sapphire laser, revealed long-lived plasma continua in all cases. This persistent continuum is attributed to a pseudo-continuum from overlapping molecular emissions, as its intensity scales linearly with electron number density, deviating from the expected quadratic dependence of classical ion–electron interactions for free-free and free-bound continuum emission. Based on plasma persistence time, SBR, U II/U I intensity ratios, and electronic excitation temperature, no fundamental advantage was found for femtosecond-pulsed lasers over conventional nanosecond-pulsed ones for UF 6 enrichment assay with direct LIBS measurement.