Cavity-enhanced optical feedback-assisted photo-acoustic spectroscopy with a 10.4 μm external cavity quantum cascade laser

An ultra-sensitive photo-acoustic spectrometer using a 10.4 μm broadly tunable mid-IR external cavity quantum cascade laser (EC-QCL) coupled with optical feedback to an optical power buildup cavity with high reflectivity mirrors was developed and tested. A laser optical power buildup factor of 181 was achieved, which corresponds to an intra-cavity power of 9.6 W at a wavelength of 10.4 μm. With a photo-acoustic resonance cell placed inside the cavity this resulted in the noise-equivalent absorption coefficient of 1.9 × 10^?10 cm^?1 Hz^?1/2, and a normalized noise-equivalent absorption of 1.1 × 10^?11 cm^?1 W Hz^?1/2. A novel photo-acoustic signal normalization technique makes the photo-acoustic spectrometer’s response immune to changes and drifts in the EC-QCL excitation power, EC-QCL to cavity coupling efficiency and cavity mirrors aging and contamination. An automatic lock of the EC-QCL to the cavity and optical feedback phase optimization permitted long wavelength scans within the entire EC-QCL spectral tuning range.     

Microdroplet evolution induced by a laser pulse

Interaction between high-power ultrashort laser pulse and giant clusters (microdroplets) consisting of 10⁹ to 10¹⁰ atoms is considered. The microdroplet size is comparable to the laser wavelength. A model of the evolution of a microdroplet plasma induced by a high-power laser pulse is developed, and the processes taking place after interaction with the pulse are analyzed. It is shown theoretically that the plasma is superheated: its temperature is approximately equal to the ionization potential of an ion having a typical charge. The microdroplet plasma parameters are independent of the pulse shape and duration. The theoretical conclusions are supported by experimental studies of x-ray spectra conducted at JAERI, where a 100-terawatt Ti-sapphire laser system was used to irradiate krypton and xenon microdroplets by laser pulses with pulse widths of 30 to 500 fs and intensities of 6×10¹⁶ to 2×10¹⁹W/cm².     

Enhanced soft X-ray emission from carbon nanofibers irradiated with ultra-short laser pulses

A comparative experimental study of the X-ray emission in the water-window spectral region has been performed using carbon nanofibers (CNFs) of different sizes and graphite plate targets, irradiated with ultra-short (Ti:sapphire) laser pulses. More than an order of magnitude enhancement in the X-ray yield is observed from CNFs of 60-nm diameter with respect to graphite targets. The X-ray emission from CNFs of 160-nm diameter was also high. The integrated X-ray yield of these carbon-based targets scales with the laser intensity (I _L) as I_L ^{~ 1.3-1.4}I_{\mathrm{L}}^{\sim 1.3-1.4} in the intensity range of 4×10¹⁶–4×10¹⁷ W/cm². The effect of the laser pulse duration on the X-ray emission from the CNFs was also studied by varying the pulse duration from 45 fs up to 3 ps at a constant fluence of 2×10⁴ J/cm². The optimum laser pulse duration for maximum X-ray emission increases with the diameter of the CNFs used. The results are explained from physical considerations of heating and hydrodynamic expansion of the CNF plasma in which resonance field enhancement takes place while passing through two times the critical density. The results add to the efforts towards achieving an efficient low-cost water-window X-ray source for microscopy.     

Miniature high-repetition-rate TEA CO2 laser with surface-wire-corona preionization

In this article, an experimental study of a miniature, sealed-off, high-repetition-rate transversely excited atmospheric-pressure (TEA) CO₂ laser with a kind of surface-wire-corona preionization (SWCP) is described. We have utilized an SWCP consisting of SiO₂ dielectric tube and a fine wire strained and attached to the dielectric surface. A BN ceramic material, which has an extremely low coefficient of thermal expansion of about 5 × 10⁻⁷/°C was employed as a supporter of the resonator. A measurement on emission spectra of SWCP has been reported. By applying SWCP to the TEA CO₂ laser, efficient laser operation at an overall efficiency of 9.8% with an output energy of 150 mJ has been achieved from a small discharge volume of 25 cm³ with an active length of 230 mm. At the pulse repetition frequency of 60 Hz, the TEM₀₀ mode of laser beam with pulse width of 60 ns was obtained.     

表面层对1 064 nm高反射镜损伤阈值影响

 采用电子束蒸发的方法制备了３种具有不同表面层材料及结构的中心波长为1 064 nm的零度高反镜,３种膜系表面层分别为1/4波长光学厚度的HfO₂,1/2波长光学厚度的SiO₂,以及1/4波长光学厚度的SiO₂。光谱测试表明：三者在1 064 nm处均有较高的反射率（高于99.8%）,利用热透镜的方法测量得到３个膜系辐照激光正入射情况下,薄膜对光的吸收比例分别为3.0×10^-6,5.0×10^-6和6.5×10^-6,其损伤阈值分别为32.5,45.2和28.4 J/cm²。并在膜层内部电场分布和膜层材料物理特性的基础上分析了３种不同表面层膜系吸收和损伤阈值差别的原因。     

Charge composition of a cluster plasma upon irradiation of large atomic clusters by the field of a superatomic femtosecond laser pulse

A theory is developed for calculating the charge composition of a cluster plasma produced upon irradiation of large atomic clusters by the field of a superatomic femtosecond laser pulse. The theory is based on the overbarrier process of a successive multiple internal ionization of atomic ions inside a cluster accompanied by the external field ionization. Collision ionization is also taken into account in the calculations. The theory is illustrated by the example of a cluster consisting of 10⁶ xenon atoms irradiated by a 50-fs laser pulse with a peak intensity of 2×10¹⁸ W/cm². In this case, the Xe²⁶⁺ ions dominate. The amounts of atomic xenon ions with multiplicity up to 31 are calculated.     

VUV generation by frequency tripling the third harmonic of a picosecond kHz Nd:YLF laser in xenon and mercury vapour

uv ^vac=351.165 nm) of a ps 1 kHz Nd:YLF laser system is frequency tripled in xenon and mercury vapour. About 4×10⁴ photons per pulse, i.e. 4×10⁷ photons/s, are generated in xenon yielding a conversion efficiency of η=3×10^-10. The unusual frequency tripling in xenon takes place in a positive dispersive wavelength region. It is shown that Kerr-induced dispersion in the atomic system and a fifth-order process rather than a third-order process can explain the frequency tripling. For comparison a four-wave mixing process is investigated in negative dispersive mercury vapour. Due to absorption of the generated VUV radiation in the autoionization region of mercury the observed effective efficiency is, in our experimental arrangement, even lower than in xenon. An analysis of the VUV generation with respect to absorption is given. Received: 1 September 1997     

Cavity-enhanced absorption: detection of nitrogen dioxide and iodine monoxide using a violet laser diode

We present an application of cavity-enhanced absorption spectroscopy with an off-axis alignment of the cavity formed by two spherical mirrors and with time integration of the cavity-output intensity for detection of nitrogen dioxide (NO₂) and iodine monoxide (IO) radicals using a violet laser diode at λ=404.278 nm. A noise-equivalent (1σ≡ root-mean-square variation of the signal) fractional absorption for one optical pass of 4.5×10^-8 was demonstrated with a mirror reflectivity of ∼0.99925, a cavity length of 0.22 m and a lock-in-amplifier time constant of 3 s. Noise-equivalent detection sensitivities towards nitrogen dioxide of 1.8×10¹⁰ molecule cm^-3 and towards the IO radical of 3.3×10⁹ molecule cm^-3 were achieved in flow tubes with an inner diameter of 4 cm for a lock-in-amplifier time constant of 3 s. Alkyl peroxy radicals were detected using chemical titration with excess nitric oxide (RO₂+NO→RO+NO₂). Measurement of oxygen-atom concentrations was accomplished by determining the depletion of NO₂ in the reaction NO₂+O→NO+O₂. Noise-equivalent concentrations of alkyl peroxy radicals and oxygen atoms were 3×10¹⁰ molecule cm^-3 in the discharge-flow-tube experiments. Received: 4 February 2003 / Revised version: 10 March 2003 / Published online: 12 May 2003 RID="*" ID="*"Corresponding author. Fax: +44-1865/275-410, E-mail: vlk@physchem.ox.ac.uk     

Wavenumber measurement of weak CO2 laser lines around 10.6 μm

An experimental method is described in which a tunable semiconductor diode laser and the regular CO₂ laser lines are utilized to measure the wavenumber of CO₂ laser lines to an accuracy of about ±5 × 10^?4 cm^?1. Twenty new CO₂ laser lines have been measured over the 943 to 951 cm^?1 region.     

Signal processing system in cavity enhanced spectroscopy

The paper presents a signal processing system used for nitrogen dioxide detection employing cavity enhanced absorption spectroscopy. In this system, the absorbing gas concentration is determined by the measurement of a decay time of a light pulse trapped in a cavity. The setup includes a resonance optical cavity, which was equipped with spherical and high reflectance mirrors, the pulsed diode laser (414 nm) and electronic signal processing system. In order to ensure registration of low-level signals and accurate decay time measurements, special preamplifier and digital signal processing circuit were developed. Theoretical analyses of main parameters of optical cavity and signal processing system were presented and especially signal-to-noise ratio was taken into consideration. Furthermore, investigation of S/N signal processing system and influence of preamplifier feedback resistance on the useful signal distortion were described. The aim of the experiment was to study potential application of cavity enhanced absorption spectroscopy for construction of fully optoelectronic NO₂ sensor which could replace, e.g., commonly used chemical detectors. Thanks to the developed signal processing system, detection limit of NO₂ sensor reaches the value of 0.2 ppb (absorption coefficient equivalent = 2.8 × 10⁻⁹ cm⁻¹).     

A quantum cascade laser-based optical feedback cavity-enhanced absorption spectrometer for the simultaneous measurement of CH4 and N2O in air

Optical feedback cavity-enhanced absorption spectroscopy (OF CEAS) has been demonstrated with a thermoelectrically cooled continuous wave distributed feedback quantum cascade laser (QCL) operating at wavelengths around 7.84 μm. The QCL is coupled to an optical cavity which creates an absorption pathlength greater than 1000 m. The experimental design allows optical feedback of infra-red light, resonant within the cavity, to the QCL, which initiates self-locking at each TEM₀₀ cavity mode frequency excited. The QCL linewidth is narrowed to below the mode linewidth, greatly increasing the efficiency of injection of light into the cavity. At the frequency of each longitudinal cavity mode, the absorption coefficient of an intracavity sample is obtained from the transmission at the mode maximum, measured with a thermoelectrically cooled detector: spectral line profiles of CH₄ and N₂O in ambient air were recorded simultaneously and with a resolution of 0.01386 cm^?1. A minimum detectable absorption coefficient of 5.5×10^?8 cm^?1 was demonstrated after an averaging time of 1 s for this completely thermoelectrically cooled system. The bandwidth-normalised limit for a single cavity mode is 5.6×10^?9 cm^?1?Hz^?1/2 (1σ).     

Measurement of the absolute Raman scattering cross sections of sulfur and the standoff Raman detection of a 6‐mm‐thick sulfur specimen at 1500 m

The absolute Raman scattering cross sections (σ_RS) for the 471, 217, and 153 cm⁻¹ modes of sulfur were measured as 6.0 ± 1.2 × 10⁻²⁷, 7.7 ± 1.6 × 10⁻²⁷, and 1.2 ± 0.24 × 10⁻²⁶ cm² at 815, 799, and 794 nm, respectively, using a 785‐nm pump laser. The corresponding values of σ_RS at 1120, 1089, and 1081 nm were determined to be 1.5 ± 0.3 × 10⁻²⁷, 1.2 ± 0.24 × 10⁻²⁷, and 1.2 ± 0.24 × 10⁻²⁷ cm² using a 1064‐nm laser. A temperature‐controlled, small‐cavity (2.125 mm diameter) blackbody source was used to calibrate the signal output of the Raman spectrometers for these measurements. Standoff Raman detection of a 6‐mm‐thick sulfur specimen located at 1500 m from the pump laser and the Raman spectrometer was made using a 1.4‐W, CW, 785‐nm pump laser. Copyright © 2010 John Wiley & Sons, Ltd.     

Rapidly tuning miniature TEA CO2 laser – rotating mirror and grating mechanism

In this research, directed toward using differential absorption lidar (DIAL) for measuring concentrations of pollutant gases, a device for rapidly tuning a transversely excited atmospheric-pressure (TEA) CO₂ laser is presented. It is shown that it is possible to utilize a rotating six-sided scanning mirror and a fixed diffraction grating to rapidly switch wavelength over randomly selected lasing transitions in the 9–11 μm region of the spectrum. The scanning mirror and an optical encoder are driven by a hysteresis synchronous motor at a speed of 1500 rpm. A surface-wire-corona preionization was utilized in a cavity. The laser system is highly automated with microprocessor-controlled laser line selection. Single-branch emission at two wavelengths with time interval ⩽10 ms has been obtained from a single cavity TEA CO₂ laser. An accurate line selection has been demonstrated in over 40 transitions at a pulse repetition frequency of up to 100 Hz. The laser energy at first-order couple output was up to 20 mJ per pulse and the pulse width is about 60 ns in an active volume of 36 cm³.     

Detection of C2H2 and HCl using mid-infrared degenerate four-wave mixing with stable beam alignment: towards practical in situ sensing of trace molecular species

A stable and convenient optical system to realize the forward phase-matching geometry for degenerate four-wave mixing (DFWM) is demonstrated in the mid-infrared spectral region by measuring DFWM signals generated in acetylene (C₂H₂) and hydrogen chloride (HCl) molecules by probing the fundamental ro-vibrational transitions. IR laser pulses tunable from 2900 cm^?1 to 3350 cm^?1 with a 0.025 cm^?1 linewidth were obtained using a laser system composed of an injection seeded Nd:YAG laser, a dye laser, and a frequency mixing unit. At room temperature and atmospheric pressure, a detection limit of 35 ppm (～ 9.5×10¹⁴ molecules/cm³) for C₂H₂ was achieved in a gas flow of a C₂H₂/N₂ mixture by scanning the P(11) line of the (010(11)⁰)–(0000⁰0⁰) band. The detection limit of the HCl molecule was measured to be 25 ppm (～6.8×10¹⁴ molecules/cm³) in the same environment by probing the R(4) line. The dependences of signal intensities on molecular concentrations and laser pulse energies were demonstrated using C₂H₂ as the target species. The variations of the signal line shapes with changes in the buffer gas pressures and laser intensities were recorded and analyzed. The experimental setup demonstrated in this work facilitates the practical implementation of in situ, sensitive molecular species sensing with species-specific, spatial and temporal resolution in the spectral region of 2.7–3.3 μm (3000–3700 in cm^?1), where various molecular species important in combustion have absorption bands.     

Laser-induced Alignment and Coulomb Explosion of CO2

实验研究了CO₂分子在飞秒强激光脉冲作用下的动力学过程,包括分子取向,隧穿电离和库仑爆炸,激光强度从1×10¹³W/cm²变化到6×10¹⁴W/cm². 当激光强度小于分子的电离阈值时,CO₂分子的非绝热转动激发形成一个相干转动波包,波包演化导致分子沿激光电场方向取向. 激光脉冲结束后,分子取向可以周期性地再现,利用另一束激光可以对取向结构进一步进行修饰. 当激光强度大于分子     

Energetic ion generation by Coulomb explosion in cluster gas and a low-density plastic foam with an intense femtosecond laser

The energy distributions of protons emitted from the Coulomb explosion of hydrogen clusters by an intense femtosecond laser have been experimentally obtained. Ten thousand hydrogen clusters were exploded, emitting 8.1-keV protons under laser irradiation of intensity 6 × 10¹⁶W/cm². The energy distributions are interpreted well by a spherical uniform cluster analytical model. The maximum energy of the emitted protons can be characterized by cluster size and laser intensity. The laser intensity scale for the maximum proton energy, given by a spherical cluster Coulomb explosion model, is in fairly good agreement with the experimental results obtained at a laser intensity of 10¹⁶–10¹⁷ W/cm² and also when extrapolated with the results of three-dimensional particle simulations at 10²⁰–10²¹ W/cm². Energetic proton generation in low-density plastic (C₅H₁₀) foam by intense femtosecond laser pulse irradiation has been studied experimentally and numerically. Plastic foam was successfully produced by a sol-gel method, achieving an average density of 10 mg/cm³. The foam target was irradiated by 100-fs pulses of a laser with intensity 1 × 10¹⁸ W/cm². A plateau structure extending up to 200 keV was observed in the energy distribution of protons generated from the foam target, with the plateau shape explained well by Coulomb explosion of lamella in the foam. The laser-foam interaction and ion generation were studied qualitatively by two-dimensional particle-in-cell simulations, which indicated that energetic protons are mainly generated by the Coulomb explosion. From the results, the efficiency of energetic ion generation in a low-density foam target by Coulomb explosion is expected to be higher than in a gas-cluster target.     

Study of gas detection based on integrated cavity output spectroscopy

A trace gases detection system based on integrated cavity output spectroscopy (ICOS) was developed, where a NIR tunable diode laser (TDL) was used as light source, an optical cavity composed by two plan-concave mirrors with reflection near 99.7% was used as the absorption cell. Trace water vapour (H₂O), carbon dioxide (CO₂), methane (CH₄), carbon monoxide (CO) and mixture of CO₂ and CO were tested by ICOS based on the characteristics absorption. The wavelength calibration, cavity transmission characteristics, quantitative measurement ability and sensitivity of the TDL-ICOS were also studied, and a evaluated minimum detectable sensitivity of 1.15 × 10^?7 cm^?1 was obtained when the system was used to CH₄ detection. The experiment results show that TDL-ICOS is expected to be a reliable and promising system for the detection of trace gases since it has some advantages such as real-time monitoring, simple device, easy operation, high sensitivity, good stability and quantitative ability.     

Decay and recondensation of electron-hole liquid in germanium under CO2 laser pulse irradiation: Investigation by microwave conductivity measurements

In microwave conductivity investigations of photoexcited germanium at low temperatures under CO₂ laser pulse irradiation the evaporation of EHL and e-h plasma formation have been observed. This plasma irreversibly vanishes at high CO₂ laser intensities I_CO2 >4 × 10⁵ W cm^?2 but recondenses at low intensities. It was found that complete and irreversible disappearance of EHL is due to the e-h plasma throw out to the crystal boundaries by phonon wind, generated in 10.6 μm radiation absorption whereas at I_CO2 > 10⁶ W cm^?2 it is connected with the crystal lattice heating over the condensation critical temperature. A theoretical analysis of the CO₂ laser produced phonon wind interaction with e-h plasma is briefly presented. By comparing with experimental data on recondensation process the phonon wind efficiency is estimated.     

Measurement of the absolute Raman scattering cross section of the 1584‐cm−1 band of benzenethiol and the surface‐enhanced Raman scattering cross section enhancement factor for femtosecond laser‐nanostructured substrates

The absolute Raman scattering cross section (σ_RS) for the 1584‐cm⁻¹ band of benzenethiol at 897 nm (1.383 eV) has been measured to be 8.9 ± 1.8 × 10⁻³⁰ cm² using a 785‐nm pump laser. A temperature‐controlled, small‐cavity blackbody source was used to calibrate the signal output of the Raman spectrometer. We also measured the absolute surface‐enhanced Raman scattering cross section (σ_SERS) of benzenethiol adsorbed onto a silver‐coated, femtosecond laser‐nanostructured substrate. Using the measured values of 8.9 ± 1.8 × 10⁻³⁰ and 6.6 ± 1.3 × 10⁻²⁴ cm² for σ_RS and σ_SERS respectively, we calculate an average cross‐section enhancement factor (EF) of 0.8 ± 0.3 × 10⁶. Copyright © 2009 John Wiley & Sons, Ltd.     

A comparative study of the ionic keV X-ray line emission from plasma produced by the femtosecond,picosecond and nanosecond duration laser pulses

We report here an experimental study of the ionic keV X-ray line emission from magnesium plasma produced by laser pulses of three widely different pulse durations (FWHM) of 45 fs, 25 ps and 3 ns, at a constant laser fluence of ∼1.5 × 10⁴ J cm^− 2. It is observed that the X-ray yield of the resonance lines from the higher ionization states such as H- and He-like ions decreases on decreasing the laser pulse duration, even though the peak laser intensities of 3.5 × 10¹⁷ W cm^− 2 for the 45 fs pulses and 6.2 × 10¹⁴ W cm^− 2 for the 25 ps pulses are much higher than 5 × 10¹² W cm^− 2 for the 3 ns laser pulse. The results were explained in terms of the ionization equilibrium time for different ionization states in the heated plasma. The study can be useful to make optimum choice of the laser pulse duration to produce short pulse intense X-ray line emission from the plasma and to get the knowledge of the degree of ionization in the plasma.