Spectroscopic trace-gas sensor with rapidly scanned wavelengths of a pulsed quantum cascade laser for in situ NO monitoring of industrial exhaust systems

Development of a pulsed quantum cascade laser (QCL)-based spectroscopic trace-gas sensor for sub-part-per-million detection of nitric oxide (NO) and capable of monitoring other molecular species such as CO₂, H₂O, and NH₃ in industrial combustion exhaust systems is reported. Rapid frequency modulation is applied to the QCL to minimize the influence of fluctuating non-selective absorption. A novel method utilizes only a few laser pulses within a single wavelength scan to probe an absorption spectrum at precisely selected optical frequencies. A high-temperature gas cell was used for laboratory evaluation of the NO sensor performance. A noise-equivalent sensitivity (1) of 100 ppb × m/ at room temperature and 200 ppb × m/ at 630 K was achieved by measuring the NO R(6.5) absorption doublet at 1900.075 cm^–1.     

Photorefractive measurements on electron-irradiated semi-insulating GaAs

We present photorefractive measurements at 1.06 m and 1.3 m performed in electron-irradiated GaAs. Irradiation with electrons of kinetic energies 1 MeV introduces intrinsic electrically active defects which modify the Fermi-level position and allow to modify the electron-hole competition mechanism of the photorefractive effect. Furthermore, it is shown that the optical absorption in the 1.3–1.5 m spectral range can be increased, which might allow to enlarge the useful spectral range of GaAs towards optical telecommunication windows. The native and irradiation-induced defects are assessed by electron paramagnetic resonance and optical absorption spectroscopy conducted at T=300 K and 77 K. The direct influence of an irradiation-induced mid-gap defect on the photorefractive effect is experimentally and theoretically demonstrated.     

Potentiality of the photothermal surface-displacement technique for precisely performed absorption measurement of optical coatings

The influence of sample properties on the measured signal has to be investigated, so that measurements of the optical absorption in thin-film coatings by means of the photothermal surface-displacement technique may be precisely performed. Carrying out simultaneously absorption measurements on metal coatings at =10.6 m by using laser calorimetry as well as the surface-displacement technique, the aforementioned influence and the validity of assumptions of the theoretical model, respectively, can be proven. It can be demonstrated that, in contrast to the model, thermophysical coating properties contribute to the probed surface displacement.     

Optical limiting with higher fullerenes

Optical limiting has been investigated for higher fullerenes and compared with C₆₀. The transmission through an aperture placed after solutions of C₇₆, C₇₈, and C₈₄ in tetrahydronaphthalene was measured using Q-switched laser pulses with a wavelength of 532 nm and a pulse width of 8 ns FWHM. Unlike C₆₀, the transmission for these higher fullerene solutions decreased linearly with increasing optical pulse energy. We attribute the linearized optical limiting response to self-defocusing of the optical beam and the absence of excited-state absorption. The ground state absorption spectra for the higher fullerenes suggest their use for optical limiting in the near infrared, and the C₈₄-tetrahydronaphthalene solution was found to be an optical limiter at 1.064 m.     

Physical properties of GaAs on glass

Physical properties of GaAs layers grown by molecular beam epitaxy on glass substrates are investigated by Raman light scattering, Photothermal Deflection Spectroscopy (PDS), optical absorption and Scanning Electron Microscopy (SEM) measurements. The results indicate that the layers are polycrystalline and strain-free. Raman spectra exhibit GaAs-TO and LO modes at 260 and 283 cm^–1, respectively. The peaks are shifted by about 10 cm^–1 with respect to bulk GaAs which we attribute to local heating effects induced by laser excitation. The phonon lines are strong and have a bandwidth of about 5 to 8 cm^-1 indicating a good crystalline quality. However, neither photoluminescence nor the Hall effect could be observed that is suggestive of the presence of a large number of electronic defects. SEM micrographs taken from the surface and the interface exhibit a granular structure with the polycrystal sizes of well under 1 m. PDS results show about 10¹⁸ cm^–3 defects and some disorder at the band gap.     

Surface roughness effect on optical absorptivity of metals

The white light (3700 K) optical absorptivity has been measured, using a calorimetric method, for a series of rough cold-worked metal surfaces. Results show a strong maximum (30%) in absorptivity vs roughness. The depth variance of surface imperfections (from 20 to 700 nm) has been determined by measuring infrared reflectance of the samples.     

Incubation/ablation patterning of polymer surfaces with sub-μm edge definition for optical storage devices

By exposure to low fluence UV laser radiation, the optical absorption coefficient of subsurface polymer material can be increased (incubation) with spatial control, using a suitable contact mask, proper imaging of the mask, or laser direct writing. Spatially selective ablation of polymethylmethacrylate (PMMA) is then achieved with large area XeCl excimer laser pulses at 308 nm. In this way, the transfer of spatial information to the material can be decoupled from the high laser fluence removal (ablation) step. The advantages are: The mask is exposed to only low fluence laser radiation — damage is avoided. Since the mask can be removed before the ablation step, mask contamination by the ablated plume cannot occur. Using this incubation/ablation method, PMMA surfaces can be patterned (248 nm/308 nm) with submicrometer spatial control and edge contrasts better than 0.2 m. This has impact on optical storage technology and laser surface processing techniques in general. The smallest single structure obtained was somewhat smaller than 0.5 m in diameter up to now, given by the mask.Presented at Laserion '91, June 12–14, 1991     

Effect of radiation dose on the size of bismuth particles produced by radiolysis

Colloidal bismuth is formed in -irradiated solutions , containing BiO⁺, 0.2 M propanol-2 and 2×10^-2 M of polyacrylic acid. Radiolytic reduction of these solutions produces long-lived bismuth clusters which are stabilized on the polymer chains. The clusters have a distinct absorption band at 350 nm with a tentatively assigned to or structures. With continued irradiation, the clusters coalesce into colloidal particles of 5 nm diameter. The absorption spectra of Bi oligomers and colloidal particles are reported as well as the optical changes accompanying their formation.     

Slow-light enhanced light–matter interactions with applications to gas sensing

Optical gas detection in microsystems is limited by the short micron scale optical path length available. Recently, the concept of slow-light enhanced absorption has been proposed as a route to compensate for the short path length in miniaturized absorption cells. We extend the previous perturbation theory to the case of a Bragg stack infiltrated by a spectrally strongly dispersive gas with a narrow and distinct absorption peak. We show that considerable signal enhancement is possible. As an example, we consider a Bragg stack consisting of PMMA infiltrated by O₂. Here, the required optical path length for visible to near-infrared detection (760 nm) can be reduced by at least a factor of 10², making a path length of 1 mm feasible. By using this technique, optical gas detection can potentially be made possible in microsystems.     

Anisotropy of photocurrent for two-photon absorption photodetector made of hemispherical silicon with $(\overline{1}10)$ plane

We fabricated a hemispherical nearly-intrinsic Si-based photodetector with ( plane. The photocurrent generated from the detector under a continuous wave laser at the wavelength of 1.3 μm was observed. The photocurrent shows a quadratic dependence on the incident optical power. The dependence of the photocurrent on the azimuth of the incident optical field is consistent with the anisotropy of the two-photon absorption in Si crystals. The ratio of the two nonzero independent components of the third-order susceptibility of silicon is obtained to be 0.42 from the observed result of the anisotropy of the photocurrent.     

Optical properties of CdIn2Se4 thin films

The optical constants (the refractive index n, the absorption index k, and the absorption coefficient ) of CdIn₂Se₄ thin films were determined in the spectral range of 500–2000 nm. Graphical representation of log() as a function of log(1/) shows two distinct, linear parts indicating the existance of both direct and indirect optical transitions. The corresponding forbidden energy gaps E _g ^d and E _g ^Emphasis>d were determined. The effect of both annealing temperature as well as the substrate temperature on the optical constants of CdIn₂Se₄ thin films was also investigated.     

Anisotropy of infrared optical absorption in layered superconductors

We analyze the problem of infrared optical absorption in a clean layered London superconductor in the vicinity of the gap =2. We conclude that absorption of light with wave vectorqc is enhanced over ordinary Drude absorption (qc) due to resonance absorption (Landau damping). Experimental absorption studies with qc might therefore improve chances to observe a superconducting gap in the high-T _c superconductors.     

Anomalous linewidths and peak-height ratios in137Ba hyperfine lines

We have investigated several effects of optical pumping in the hyperfine spectrum of the6s6p ¹ P ₁6s ^{2 1} S ₀ transition in¹³⁷Ba. Most of these effects are explained by absorption strength changes which occur because of redistribution of population among magnetic substates. At very low laser intensities, no redistribution effects are observed. At higher intensities, it is possible to either empty the magnetic substates that are accessible to optical excitation, or to redistribute the population among these states until a steady-state condition is achieved. The first case results in the familiar disappearance of a hyperfine line. The less familiar second case can result in peak-height ratios in the Ba¹ P ₁¹ S ₀ hyperfine spectrum that differ by almost a factor of three from the low-intensity case. In this second case, the observed linewidth can either broaden or narrow, depending on whether redistribution decreases or increases absorption strength. At high intensities, saturation effects dominate and branching to intermediateD states becomes apparent. We report here the result of a numerically integrated rate equation model which shows good agreement with our experiments.     

A tunable light source in the 370 nm range based on an optically stabilized,frequency-doubled semiconductor laser

A tunable harmonic output power of 18 W at a wavelength of =370 nm is obtained by resonance-enhanced frequency doubling of an optically-stabilized semiconductor laser. A commercially available AlGaAs laser diode which emits a maximum power of 10 mW at =740 nm is operated in an extended-cavity configuration. Dispersion prisms are used in the extended cavity to obtain longitudinal-mode selection with low loss of optical power. The output is focussed into an optically isolated high-finesse ring resonator which contains a LiIO₃ crystal for second-harmonic generation. One potential application of this laser source is the optical excitation and laser cooling of ytterbium in an ion trap. In a related demonstration experiment, the frequency-doubled diode laser is applied to excite the =369.5 nm ² S _1/2-² P _1/2 transition of ytterbium ions in a hollow-cathode discharge.     

Ab initio investigations on the electronic structure and optical properties of HX-ZnO

First-principles ultrasoft pseudopotential method is applied to study HX ZnO, which has a novel graphite like hexagonal structure transformed from wurtzite (WZ) phase under tensile stress along direction or compressive stress along [0001] direction. The electronic structure and optical properties, including dielectric function, reflectivity and absorption coefficient, of HX ZnO are calculated and compared with those of WZ ZnO under the given uniaxial stress. It is found that HX ZnO is an indirect semiconductor, being different from WZ ZnO. HX ZnO has a dielectric response different from WZ ZnO at ambient conditions or under the given uniaxial stress, especially in the case of E∥c. Similar variation is also observed in the reflectivity and absorption coefficient. The variation in the optical properties is attributed to the additional ZnO bond along c-axis HX ZnO.     

High-power source of coherent picosecond light pulses tunable from 0.41 to 12.9 μm

We report a high-power source of coherent picosecond light pulses based on optical parametric generation and amplification in LiB₃O₅ and AgGaS₂ crystals. The spectral range of this continuously tunable source covers the visible, near-infrared and medium-infrared spectrum from 0.41 to 12.9 m. An optical parametric generator and amplifier, consisting of two type-I phase-matched LiB₃O₅ crystals and a diffraction grating, is pumped by the third harmonic of a picosecond Nd:YAG laser and provides spectrally narrow, high-power pulses from 0.41 to 2.4 m. Energy conversion efficiencies up to 16 percent are achieved. The pulse duration is about 14 ps, the bandwidth between 10 and 30 cm^–1. The tuning range is extended to 12.9 m by mixing the infrared output between 1.16 and 2.13 m with the fundamental of the Nd:YAG laser in type-I-phase-matched AgGaS₂ crystals. Up to 25 percent of the pulse energy at 1.064 m is converted into parametric infrared pulses. Bandwidths between 3 and 8 cm^–1 and a pulse duration of approximately 19 ps are measured for these pulses. We also observe a retracing behaviour in the tuning curve of AgGaS₂ not reported before.     

Determination of the absorption coefficient of solids in the short-wave region of the millimeter band

A technique for measuring the absorption coefficient of solids in the short-wave region of the millimeter band is described. The absorption coefficients of six materials were measured at a wavelength = 2mm.The authors express their gratitude for the interest of Academician A. M. Prokhorov, in whose laboratory this work was done. The authors also wish to thank E. A. Vinogradov for his assistance.     

Light absorption in laser-heated cavities

The absorption of laser light in 0.25–1 mm diameter gold cavities, irradiated for the purpose of generating high-temperature blackbody radiation with intense laser radiation of either =0.44 m or =1.3 m wavelength, was investigated. For =0.44 m radiation the absorption exceeded 0.9 for all conditions, but dropped to only 0.3 for the smallest cavities irradiated at =1.3 m. Entrance hole and cavity filling with plasma seems important for the understanding of the observations.     

λ=2537 Å line from a low-pressure mercury discharge lamp emission profile and line absorption by a gas containing a mercury vapor

By measuring the emission-line intensity of Hgi =2537 Å (6³ P6¹ S) from a low-pressure mercurcury lamp, we have determined the dependence of the upper-level population on the discharge current and the mercury vapor density. From the radial profile of the intensity the spatial distribution function of the population has been determined to be the zero-th order decay mode for the trapped radiation. Line absorption by mercury vapor in a cell has been measured with various mercury densities and Lorentzian widths. The results are consistent with the upper-level population distribution as determined above. On the basis of these findings we calculate the emission-line profile and its change during the absorption in the absorption cell. The amount of absorption at an arbitrary depth of the absorption cell is calculated, and the optimum cold-spot temperature of the lamp of 40–50°C is suggested for the maximum absorption under the typical condition of the photo-CVD experiment.