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At least 109 records · Page 6

Spectral dependence of third-order nonlinear optical properties in InN

We report on the nonlinear optical properties of InN measured in a wide near-infrared spectral range with the femtosecond Z-scan technique. The above-bandgap nonlinear absorption in InN is found to originate from the saturation of absorption by the band-state-filling and its cross-section increases drastically near the bandgap energy. With below-bandgap excitation, the nonlinear absorption undergoes a transition from saturation absorption (SA) to reverse-SA (RSA), attributed to the competition between SA of band-tail states and two-photon-related RSA. The measured large nonlinear refractive index of the order of 10{sup −10} cm{sup 2}/W indicates InN as a potential material for all-optical switching and related applications.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Saturated two-photon absorption of single-frequency radiation in gaseous media

A saturated nonresonant two-photon absorption (TPA) theory of quasi-monochromatic radiation by an atom is developed in a model of a three-level cascade quantum system. It is shown that doubled-frequency radiation, arising from a multipole interaction of radiation with the dipole-forbidden transition, experiences spatial oscillations at arbitrary intensities of the pump. The influence of the total phase of the waves with the initial and doubled frequencies on TPA is considered under conditions of ring frequency mixing in a medium.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

The application of far IR lasers to the investigation of the optical properties of materials

The effect of diffusion on the saturation and absorption properties of molecular gases is considered. The analysis starts with a simple derivation of the multi-level rate equations. Incorporating the diffusion term, calculations are carried out both for the homogeneous and inhomogeneous broadening cases. Both graphical and analytical solutions are obtained for the absorption coefficient and the saturation intensity. It is shown that the effect of diffusion is characterized by a diffusion function, which varies inversely with the radius of the beam at low pressures and small beam sizes. The analysis is done in terms of two parameters k1a and k2a, which are simple functions of the intensity of the beam I, the effective relaxation rate w, and the effective diffusion constant D the a is designated as the radius of the beam.

Stafsudd, O. M.↗

Scattering and Radiative Properties of Morphologically Complex Carbonaceous Aerosols: A Systematic Modeling Study

This paper provides a thorough modeling-based overview of the scattering and radiative properties of a wide variety of morphologically complex carbonaceous aerosols. Using the numerically-exact superposition T-matrix method, we examine the absorption enhancement, absorption Angstroem exponent (AAE), backscattering linear depolarization ratio (LDR), and scattering matrix elements of black-carbon aerosols with 11 different model morphologies ranging from bare soot to completely embedded soot-sulfate and soot-brown carbon mixtures. Our size-averaged results show that fluffy soot particles absorb more light than compact bare-soot clusters. For the same amount of absorbing material, the absorption cross section of internally mixed soot can be more than twice that of bare soot. Absorption increases as soot accumulates more coating material and can become saturated. The absorption enhancement is affected by particle size, morphology, wavelength, and the amount of coating. We refute the conventional belief that all carbonaceous aerosols have AAEs close to 1.0. Although LDRs caused by bare soot and certain carbonaceous particles are rather weak, LDRs generated by other soot-containing aerosols can reproduce strong depolarization measured by Burton et al. for aged smoke. We demonstrate that multi-wavelength LDR measurements can be used to identify the presence of morphologically complex carbonaceous particles, although additional observations can be needed for full characterization. Our results show that optical constants of the host/coating material can significantly influence the scattering and absorption properties of soot-containing aerosols to the extent of changing the sign of linear polarization. We conclude that for an accurate estimate of black-carbon radiative forcing, one must take into account the complex morphologies of carbonaceous aerosols in remote sensing studies as well as in atmospheric radiation computations.

carbonaceous aerosols; scattering matrix; polariza↗

Measuring the Density Fields around Bright Quasars at z ~ 6 with XQR-30 Spectra

Measuring the density of the intergalactic medium using quasar sight lines in the epoch of reionization is challenging due to the saturation of Ly α absorption. Near a luminous quasar, however, the enhanced radiation creates a proximity zone observable in the quasar spectra where the Ly α absorption is not saturated. In this study, we use 10 high-resolution ( R ≳ 10,000) z ~ 6 quasar spectra from the extended XQR-30 sample to measure the density field in the quasar proximity zones. We find a variety of environments within 3 pMpc distance from the quasars. We compare the observed density cumulative distribution function (CDF) with models from the Cosmic Reionization on Computers simulation and find a good agreement between 1.5 and 3 pMpc from the quasar. This region is far away from the quasar hosts and hence approaching the mean density of the universe, which allows us to use the CDF to set constraints on the cosmological parameter σ 8 = 0.6 ± 0.3. The uncertainty is mainly due to the limited number of high-quality quasar sight lines currently available. Utilizing the more than 200 known quasars at z ≳ 6, this method will allow us to tighten the constraint on σ 8 to the percent level in the future. In the region closer to the quasar within 1.5 pMpc, we find that the density is higher than predicted in the simulation by 1.23 ± 0.17, suggesting that the typical host dark matter halo mass of a bright quasar ( M 1450 < -26.5) at z ~ 6 is .

79 ASTRONOMY AND ASTROPHYSICS↗

Dependence of the Two-Photon Absorption Coefficient of Steel on the Pulse Duration During Its Ablation by Femto- and Picosecond Laser Pulses

The dependences of the depth of single-pulse ablation of the steel surface on the energy density of ultrashort laser pulses (0.3–12 ps) with a wavelength of 515 nm have the form different from the usual logarithmic one for linear absorption of radiation. Since the density of states of free conduction electrons in the s band is low, and the d band of strongly bound electrons with a high density of states is located around the Fermi level, these dependences have been approximated within the two-photon absorption model. The two-photon absorption coefficient increases almost linearly with the duration of laser pulses, which indicates the saturation of absorption and allows estimating the corresponding parameters of the electronic subsystem. © 2019, Pleiades Publishing, Inc.

60 APPLIED LIFE SCIENCES↗

Investigation of laser-induced iodine fluorescence for the measurement of density in compressible flows

Laser induced fluorescence is an attractive nonintrusive approach for measuring molecular number density in compressible flows although this technique does not produce a signal that is directly related to the number density. Saturation and frequency detuned excitation are explored as means for minimizing the quenching effect using iodine as the molecular system because of its convenient absorption spectrum. Saturation experiments indicate that with available continuous wave laser sources of Gaussian transverse intensity distribution only partial saturation could be achieved in iodine at the pressures of interest in gas dynamics. Using a fluorescence lineshape theory, it is shown that for sufficiently large detuning of a narrow bandwidth laser from a molecular transition, the quenching can be cancelled by collisional broadening over a large range of pressures and temperatures. Experimental data obtained in a Mach 4.3 underexpanded jet of nitrogen seeded with iodine for various single mode argon laser detunings from a strong iodine transition at 5145 A are discussed.

Mcdaniel, J. C., Jr.↗

Intrinsic Absorption and Reddening in Seyfert 1 Galaxies

We discuss the origin of the ``dusty lukewarm absorber'', which we previously identified in the reddened Seyfert 1 galaxies NGC 3227 and Akn 564. This absorber is characterized by saturated UV absorption lines (C IV, N V) near the systemic velocity of the host galaxy, and is likely responsible for reddening both the continuum and the emission lines (including those from the narrow-line region) from these Seyferts. From a large sample of Seyfert 1 galaxies, we find that continuum reddening (as measured by UV color) tends to increase with inclination of the host galaxy. Furthermore, reddened, inclined Seyfert galaxies observed at moderate to high spectral resolution all show evidence for dusty lukewarm absorbers. We suggest that these absorbers lie in the plane of the host galaxy at distances greater than about 100 pc from the nucleus, and are physically distinct from the majority of intrinsic absorbers that are outflowing from the nucleus.

Crenshaw, D. M.↗

Material/element-dependent fluorescence-yield modes on soft X-ray absorption spectroscopy of cathode materials for Li-ion batteries

Here, we evaluate the utilities of fluorescence-yield (FY) modes in soft X-ray absorption spectroscopy (XAS) of several cathodematerials for Li-ion batteries. In the case of total-FY (TFY) XAS for LiNi 0.5 Mn 1.5 O 4 , the line shape of the Mn L 3 -edge XAS was largely distorted by the self-absorption and saturation effects, while the distortions were less pronounced at the Ni L 3 edge. The distortions were suppressed for the inverse-partial-FY (IPFY) spectra. We found that, in the cathodematerials, the IPFY XAS is highly effective for the Cr, Mn, and Fe L edges and the TFY and PFY modes are useful enough for the Ni L edge which is far from the O K edge.

36 MATERIALS SCIENCE↗

Coupling to rotational manifolds to improve gas-phase pump–probe spectroscopic models

The physical picture of gas-phase optical transitions is normally presented as an isolated two-level system balanced by upward and downward processes. Isolated models assume a phenomenological treatment of collisional dephasing but do not strictly account for collisional population exchange with the rotational baths. While this assumption is valid under low-intensity conditions, where excitation is rate-limiting, isolated models can deviate from Beer’s Law at sufficient pressures and monochromatic intensities when both collisional broadening and power broadening are comparable to (or greater than) lifetime broadening, which are not uncommon conditions for cavity enhanced spectroscopies in the mid-IR spectral range. Although this problem has been addressed by rate-equation models for linear absorption measurements, a general treatment for multi-level quantum mechanical models suitable for non-linear absorption measurements (two-photon/two-color/pump–probe) is lacking. Isolated models require physical parameter inputs that disagree with expected values by at least an order of magnitude. These non-physical models undermine the ability to predict non-linear signal strengths under untested conditions and thereby limit the potential to optimize the sensitivity of non-linear spectroscopies and to expand their analytical applications (e.g., new analytes and/or buffer gases, changes in cavity free-spectral-range, changes in intracavity powers or wavelengths, and accurate investigation of physical phenomena). In this study, we derive bath-coupled models for gaseous pump–probe spectroscopy by application of the quantum Lindblad equation and detailed balance. Bath-coupled models are shown to fit data consistently across variations in intensity and agree with all physically expected values.

Cavity ring-down spectroscopy↗

Frequency measurements and self-broadening of sub-Doppler transitions in the v1 + v3 band of C 2 H 2

Here, frequency comb-referenced measurements of sub-Doppler laser saturation dip absorption lines in the v1 + v3 band of acetylene near 1:5 μm are reported. These measurements include transitions involving higher rotational levels than previously frequency measured in this band. The accuracy of the measured frequencies is typically better than 10 kHz. Measurements of the observed sub-Doppler line widths as a function of pressure showed that the self pressure-broadening coefficients are about 3.5 times larger than those derived from conventional pressure broadening of unsaturated Doppler-limited spectra. This is attributed to the contribution of velocity-changing collisions to the total dephasing rate in the low pressure sub-Doppler measurements. At higher pressures, when the homogeneous broadening becomes comparable to the typical Doppler shift per elastic collision, the velocity changing collisions cease to contribute significantly to the incremental pressure broadening. Lastly, a time-dependent soft collision model is developed to illustrate the transition between low and high pressure regimes of sub-Doppler pressure-broadening.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Resonant and Nonresonant Nonlinear Absorption in Colloidal Core/Shell Semiconductor Nanoplatelets

Nonlinear absorption of colloidal solution of core/shell CdSe/CdS nanoplatelets (NPLs) in the case of resonant and nonresonant stationary excitation of the electron/light-hole and electron/heavy-hole exciton transitions was investigated. We have revealed the induced bleaching simultaneously of both exciton transitions. The peculiarities of the nonlinear change in absorption were associated with saturation of exciton transitions absorption due to phase space filling, energy up- and down-conversion mechanisms.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Tagging CO 2 to Enable Quantitative Inventories of Geological Carbon Storage

In the wake of concerns about the long term integrity and containment of sub-surface CO 2 sequestration reservoirs, many efforts have been made to improve the monitoring, verification, and accounting methods for geo-sequestered CO 2 . Our project aimed to demonstrate the feasibility of a system designed to tag CO 2 with carbon isotope 14 C immediately prior to sequestration to a level that is normal on the surface (one part per trillion). Because carbon found at depth is naturally free of 14 C, this tag would easily differentiate pre-existing carbon from anthropogenic injected carbon and provide an excellent handle for monitoring its whereabouts in the subsurface. It also creates an excellent handle for adding up anthropogenic carbon inventories. Future inventories in effect count 14 C atoms. Accordingly, we have developed a 14 C tagging system suitable for use at the part-per-trillion level. This system consists of a gas-exchange apparatus to make disposable cartridges ready for controlled injection into a fast flowing stream of pressurized CO 2 . We built a high-pressure injection and tagging system, and a 14 C detection system. The disposable cartridge and injection system have been successfully demonstrated in the lab with a high-pressure flow reactor, as well as in the field at the CarbFix CO 2 sequestration site in Iceland. The laser-based 14 C detection system originally conceived has been shown to possess inadequate sensitivity for ambient levels. Alternative methods for detecting 14 C, such as saturated cavity absorption ringdown spectroscopy and scintillation counting, may still be suitable.

anthropogenic carbon↗

Scattered light in the echelle modes of the Goddard High Resolution Spectrograph aboard the Hubble Space Telescope. II - Analysis of in-flight spectroscopic observations

We report on an analysis of observations made with the GHRS aboard the HST for the purpose of calibrating the effects of scattered light. The data were obtained during the first 2 years of flight operations as part of the Science Verification, Science Assessment Observations, and Guaranteed Time Observations programs. Both the general level of background light near the spectra and the filling-in of the cores of saturated interstellar absorption lines have been determined as functions of grating, order, wavelength, and aperture. The behavior is in accordance with our detailed analysis of prelaunch laboratory data and validates both the observing procedures and the data reduction developed on the basis of that experience. We present and discuss the use of a background (scattered light) removal algorithm designed to produce net spectra properly corrected for the effects of grating scattered light. The coefficients of the scattered light removal algorithm have been determined, and recommended numerical values are presented.

Cardelli, Jason A.↗

An Efficient Single Frequency Ho:YLF Laser for IPDA Lidar Applications

A highly efficient, versatile, single frequency 2-micron pulsed laser can be used in a pulsed Differential Absorption Lidar (DIAL) / Integrated Path Differential Absorption (IPDA) instrument to make precise, high-resolution measurements to investigate sources and sinks of CO2. For a direct detection IPDA lidar, the desired 2 m Ho:YLF laser should generate 30-40 mJ pulses at the repetition rate of 100 to 200 Hz, with short pulse length (<100 ns) and better than 2% wall plug efficiency. A Tm fiber laser in-band pumped Ho:YLF laser has been developed to meet this technical challenge. This Ho:YLF laser is designed in a four mirror ring resonator with bow tie configuration, which helps to obtain high beam quality. It is end-pumped by a 40 W linearly polarized Tm fiber laser at 1.94μm. The resonator length is 1.10 meters with output coupler reflectivity at 45%. The laser crystal size is 3 x 3 x 60 mm (w, h, l) with a doping concentration of 0.5% Holmium. The laser beam and pump beam are mode-matched in the active medium. Thus, the pump and laser beams have the same confocal parameters. Mode-matching is also helpful for operating the laser in a single transverse mode. The laser beam waist is slightly less than 0.5 mm at the center of the laser crystal. Based on quasi-four level modeling, pump absorption and saturation depend on laser intensity. Laser amplification and saturation also depend on the pump intensity in the crystal. The laser is injection seeded to obtain the single frequency required by an IPDA lidar measurement. The seed beam is entered into the resonator through an output coupler. The laser is mounted on a water cooled optical bench for stable and reliable operation. The size of the optical bench is 22.16 x 9.20 x 1.25 inches. It is stiffened so that the laser can be operated in any orientation of the optical bench. This packaged Ho:YLF laser is designed for either mobile trailer or airborne platform operation. The engineering prototype Ho:YLF laser has been fully characterized to demonstrate laser performance. Figure 1 shows the laser output power as a function of pump power at different pulse repetition rates from 100 Hz to 333 Hz. The threshold of the laser is less than 14 W. The slope efficiencies are 28%, 40%, 41% and 43% for pulse repetition rates of 100, 200, 250 and 333 Hz, respectively. Maximum power increases with the pulse repetition rate. Output power of 4.2 W, 6 W, 6.7 W, and 7.7 W is achieved for pulse repetition rates of 100, 200, 250 and 333Hz, respectively. This represents the optical conversion efficiency of 16.7%, 22.4%, 23.7%, and 26.5% at these various pulse repletion rates. It is the most efficient and compact Ho:YLF laser demonstrated in the high pulse energy (>20mJ) and moderate pulse repetition rate (100's Hz) operation range. As shown in Figure 1, the maximum pulse energy at 100 Hz is 42 mJ. This is limited due to optical damage. The laser stability is characterized and found to be very stable. A relative pulse energy standard deviation of 2% was measured. The beam quality of the Ho:YLF was measured by a Spiricon infrared laser beam camera. Figure 2 shows the beam profile image of the laser. Both the X-profile of the beam (horizontal direction) and the Y-profile of the beam (vertical direction) are well fitted by a Gaussian profile. The qualitative beam quality measurement shows excellent beam quality in both axis. The M-square value for the laser beam is measured at 1.06 and 1.09 for the x and y axis respectively.-

Yu, J.↗

Electronic absorption band broadening and surface roughening of phthalocyanine double layers by saturated solvent vapor treatment

Variations in the electronic absorption (EA) and surface morphology of three types of phthalocyanine (Pc) thin film systems, i.e. copper phthalocyanine (CuPc) single layer, zinc phthalocyanine (ZnPc) single layer, and ZnPc on CuPc (CuPc/ZnPc) double layer film, treated with saturated acetone vapor were investigated. For the treated CuPc single layer film, the surface roughness slightly increased and bundles of nanorods were formed, while the EA varied little. In contrast, for the ZnPc single layer film, the relatively high solubility of ZnPc led to a considerable shift in the absorption bands as well as a large increase in the surface roughness and formation of long and wide nano-beams, indicating a part of the ZnPc molecules dissolved in acetone, which altered their molecular stacking. For the CuPc/ZnPc film, the saturated acetone vapor treatment resulted in morphological changes in mainly the upper ZnPc layer due to the significantly low solubility of the underlying CuPc layer. The treatment also broadened the EA band, which involved a combination of unchanged CuPc and changed ZnPc absorption.

36 MATERIALS SCIENCE↗