Influence of the laser pulse duration on spectrochemical analysis of solids by laser-induced plasma spectroscopy

Quantitative analysis of aluminum and copper alloys by means of laser-induced plasma spectroscopy (LIPS) has been investigated for three representative laser pulse durations (80 fs, 2 ps, and 270 ps). The experiments were carried out in air at atmospheric pressure with a constant energy density of 20 J/cm2. Because the decay rate of the spectral emission depends on the laser pulse duration, the optimum detection requires an optimization of the temporal gating acquisition parameters. LIPS calibration (sensitivity and nonlinearity) and the limit of detection (LOD) are discussed in detail. While the LOD of minor elements embedded in alloy samples obtained by sub-picosecond or sub-nanosecond laser pulses are both time and element dependent, provided an appropriate temporal window is chosen, the optimum LODs (several parts per million (ppm)) prove to be independent of the laser pulse duration. Finally, it is found that for elements such as those detected here, gated LIPS spectra using picosecond or sub-picosecond laser pulses provide much better LOD values than non-gated spectra.     

Tunable distributed feedback lasing with a threshold in the nanojoule range in an organic guest-host polymeric waveguide

Tunable distributed feedback lasing was achieved in a guest-host polymeric waveguide using holographic dynamic gratings. Tris(8-quinolinolato)aluminum (Alq) as a host and 4-(dicyanomethylene)-2-methyl-6-(4-dimethylaminostyryl)-4H-pyran (DCM) as a guest emitter were dispersed in poly(N-vinyl carbazole) (PVCz) matrix. Emission of both the TE(0) and the TM(0) modes was measured. Effective energy transfer from PVCz to DCM through Alq assisted in the reduction of the threshold of laser emission. The threshold of 38 nJ/pulse was measured for first-order lasing and that of 53 nJ/pulse for second-order lasing.     

Angular diagram of broadband emission of millimeter-sized water droplets exposed to gigawatt femtosecond laser pulses

We report on the experiments on the interaction of gigawatt femtosecond laser pulses with suspended millimeter-sized water droplets. The transparent droplets experienced laser-induced breakdown and explosive boiling up and emitted a broadband radiation. This radiation covers the spectral range from 450 to 1100?nm and consists of the spectrum of laser pulse scattered and transformed by the droplet due to self-phase modulation and plasma emission produced in water during photoionization. The droplet emission spectrum showed remarkable broadening at all viewing angles and is maximal in the direction of the laser exit from the droplet. The enlargement of the droplet results in additional spectral spreading of the emitted radiation. The depth and amount of laser pulse spectral self-transformations upon propagation through the water droplet are simulated by means of numerical calculations.     

脉冲激光光谱测试仪的设计

设计了一种基于ISP技术的线阵CCD的驱动电路和高速脉冲光谱数据采集卡,建立了一套智能化脉冲激光光谱测试系统。该系统主要由分光系统、CCD传感器、光脉冲同步信号发生器、数据采集卡及计算机等部分组成。CCD将光强信号转换为电信号输出,经A/D转换器转换后的数字信号存入数据采集卡的帧存储器中,由计算机控制进行光谱数据的分析、处理。提出了用重心法对脉冲激光器的重复频率进行评估的方法,使测量精度达到了亚像素级。对系统所用脉冲激光器谱线峰值波长的复现性进行了测量,其标准差为0.0327nm。     

The effect of a UV preionization pulse on short-wave radiation output from a laser-produced-plasma source with a Xe gas-jet target

Experiments aimed to raise the emissivity of a laser-produced plasma source with a Xe gas target in the far-UV spectral range are described. In these experiments, the main pulse of the IR Nd:YAG laser was preceded by a pre-ionization pulse of a UV KrF excimer laser. The consequences of applying the prepulse and its influence on the short-wavelength emission intensity were traced up to main-pulse delays of about 5 μs with respect to the prepulse. It is supposed that the main mechanism by which the prepulse affects the evolution of the plasma and its emission intensity is related to the density waves excited in the gas target by this pulse.     

Intrapulse temporal and wavelength shifts of a high-power 2.1-µm Ho:YAG laser and their potential influence on atmospheric lidar measurements

A high-power, flash-lamp-pumped, Q-switched Ho:YAG laser has been developed to produce up to 150 mJ in a 100-ns Q-switched pulse. The Ho laser was initially used in a direct detection lidar-differential absorption lidar (DIAL) system to measure vertical density profiles of aerosols and water vapor in the atmosphere. It was found, however, that the Ho laser operated simultaneously on two closely spaced spectral emission wavelengths (2.090 and 2.097 μm) and that the distribution of energy between the two wavelengths could change significantly on time scales of several seconds to minutes. Such intrapulse temporal and wavelength shifts were found to alter the atmospheric lidar return significantly because one of the laser lines coincided with a water vapor absorption line in the atmosphere. This laser spectral output problem was overcome by the use of intracavity étalons that controlled the laser spectral-temporal characteristics but reduced the laser output energy to approximately 75 mJ/pulse in a 100-ns pulse length. These results are important as they serve to point out the difficulties of developing and using a high-power 2.1- μm Ho laser for atmospheric lidar when high-resolution spectral and temporal characteristics can significantly influence the lidar return and be misinterpreted as resulting from atmospheric signals.     

Upconversion luminescence properties of nanocrystallite MgAl2O4 spinel doped with Ho3+ and Yb3+ ions

The upconversion luminescence spectra of nanocrystallite MgAl₂O₄ doped with 1% of Ho³⁺ and 5% of Yb³⁺ ions after excitation at 980 nm were measured. Influence of excitation regime either continuous or pulse on upconversion mechanisms was shown. For continuous wave (CW) laser excitation upconversion process is due to phonon assisted Excited State Absorption (ESA). For pulse laser excitation upconversion emission is due to Energy Transfer Upconversion (ETU).     

Time-resolved spectral and spatial description of laser-induced breakdown in air as a pulsed, bright, and broadband ultraviolet-visible light source

The optical breakdown induced in air at atmospheric pressure by Nd:YAG Q-switched laser pulses is studied in terms of the spectral features of the emitted radiation in the wavelength range 180-850 nm during the first 200 ns after the laser pulse onset. During the plasma build up, radiation emission features intense, broadband, and structureless ultraviolet-visible spectra before the appearence of atomic lines on the microsecond scale. Also, the emitting plasma kernel, imaged during the buildup and decay stages in the early tens of nanoseconds, turns out to have a size of ~0.3 mm and a volume of ~0.02 mm(3). The coupling of direct emission data and broadband absorption measurements allowed us to retrieve peak values of electron temperature above 100,000 K and of an optical depth of the order of unity, under the assumptions of local thermodynamic equilibrium and a homogeneous kernel. The simultaneous occurrence of such temporal, spatial, and spectral features of the plasma kernel suggests its exploitation as a pulsed, bright, and broadband ultraviolet-visible light source.     

Effects of sample temperature in femtosecond single-pulse laser-induced breakdown spectroscopy

As much as tenfold atomic emission enhancements have been observed in experiments combining nanosecond (ns) and femtosecond (fs) laser pulses in an orthogonal dual-pulse configuration for laser-induced breakdown spectroscopy (ns-fs orthogonal dual-pulse LIBS). In the examination of one of several potential sources of these atomic emission enhancements (sample heating by a ns air spark), minor reductions in atomic emission and as much as 15-fold improvements in mass removal have been observed for fs single-pulse LIBS of heated brass and aluminum samples. These results suggest that, although material removal with a high-powered, ultrashort fs pulse is temperature dependent, sample heating by the ns air spark is not the source of the atomic emission enhancements observed in ns-fs orthogonal dual-pulse LIBS.     

The influence of coatings on subsurface mechanical properties of laser peened 2011-T3 aluminum

High power Q-switched laser systems are currently being developed for use in a process known as laser shock processing or laser peening which results in significantly improved fatigue properties in aluminum components. An ablative, sacrificial coating such as paint or metal foil is used to protect the aluminum component from surface melting by the laser pulse, which adversely affects fatigue life. This paper, using nano-indentation, analyzes the effect of the paint and foil coatings on the shock wave propagation into the aluminum specimen and the resulting change in mechanical properties versus depth. Near the surface, hardness was found to be increased by the laser peening, however this process decreased the measured elastic modulus. The laser pulse energy density and properties of the foil including its adhesion to the aluminum alloy were found to influence the change in surface mechanical properties.     

Two- and three-photon absorption and frequency upconverted emission of silicon quantum dots

In this communication, we present the experimental results of two- and three-photon excitation studies on silicon quantum dots (QDs) in chloroform (as well as in water) by using femtosecond laser pulses with wavelengths of 778 and 1335 nm and a pulse duration approximately 160 fs. The photoluminescence spectral distributions are nearly the same upon one-, two-, and three-photon excitation. With one- and two-photon excitation, the temporal relaxation measurements of photoluminescence emission manifest the same multiexponential decay behavior in the time range from 0.05 ns to 15 mus, characterized by three successive decay constants: 0.75 ns, 300 ns, and 5 mus, respectively. Finally, the two-photon absorption spectrum in the spectral range of 650-900 nm and the three-photon absorption spectrum in the spectral range of 1150-1400 nm have been measured.     

Polarization and phase control of remote surface-plasmon-mediated two-photon-induced emission and waveguiding

We report here on the control of remote surface-plasmon-mediated two-photon-induced luminescence of dendritic silver nanoparticle aggregates as observed by femtosecond laser microscopy. With a focal spot diameter approximately 1 microm, polarized remote emission has been observed 99 microm from the focal spot. We show control over the regions of emission by changing the polarization of the incident beam and by changing the spectral phase of the laser pulse.     

Comparison of nonintensified and intensified CCD detectors for laser-induced breakdown spectroscopy

The performance and sensitivity of an intensified CCD array system and a nonintensified CCD array detector system are compared for laser-induced breakdown spectroscopy (LIBS). LIBS measurements were recorded in a calcium-based aerosol-seeded gas stream at ambient pressure. The signal-to-noise ratio based on the 393.37-nm calcium emission line was calculated as a function of detector delay with respect to the plasma-initiating laser pulse. Both ensemble-averaging and single-shot spectral analyses were performed. For all conditions, the intensified CCD system provided an enhanced signal-to-noise ratio compared with the nonintensified CCD system.     

Temperature-Dependent Polarization Effects in Ce:LiLuF

We report on tuned-laser, pump-probe-gain, and fluorescence yield studies of the effect that crystal temperature plays on the polarized emission characteristics of Ce:LiLuF. It was found that varsigma-polarized emission at the 327-nm fluorescence spectra peak is characterized by smaller laser pulse buildup times, higher small-signal gains, and smaller output powers than the pi-polarized 327-nm emission. We concluded that excited-state absorption (ESA) (and the resultant formation of color centers) is more severe for varsigma-polarized emission than for pi-polarized emission in this spectral region. We postulate that the enhancement in laser performance and crystal fluorescence observed with crystal cooling is due to narrowing of the ESA absorption band that reduces the probability of ESA and color-center formation.     

Elastic light scattering from single microparticles on a femtosecond time scale

Experimentally measured and theoretically calculated elastic light-scattering spectra from single microparticles illuminated by 100-fs pulses are presented. Although in the theoretical calculation only a single incoming femtosecond laser pulse was used, the spectral behavior of scattered light shows all the features seen in the experimental spectrum from many femtosecond pulses, including morphology-dependent resonances (MDR's). The good agreement between experimental and theoretical elastic light-scattering data has stimulated a theoretical investigation of the time-dependent behavior of the elastically scattered light from a single microparticle on a femtosecond time scale. Since the spatial pulse length of the incoming laser pulse is smaller than the particle circumference, the temporal behavior of reflection, diffraction, refraction, and coupling into MDR's can be distinguished. Since the time-dependent scattering is strongly dependent on particle size, refractive index, and pulse chirp, it may be possible to encode several bits of information into a single laser pulse and therefore to increase optical data communication rates.     

Sub-wavelength ripples in fused silica after irradiation of the solid/liquid interface with ultrashort laser pulses

Laser-induced backside wet etching (LIBWE) is performed using ultrashort 248?nm laser pulses with a pulse duration of 600?fs to obtain sub-wavelength laser-induced periodic surface structures (LIPSS) on the back surface of fused silica which is in contact with a 0.5?mol?l(-1) solution of pyrene in toluene. The LIPSS are strictly one-dimensional patterns, oriented parallel to the polarization of the laser radiation, and have a constant period of about 140?nm at all applied laser fluences (0.33-0.84?J?cm(-2)) and pulse numbers (50-1000 pulses). The LIPSS amplitude varies due to the inhomogeneous fluence in the laser spot. The LIPSS are examined with scanning electron microscopy (SEM) and atomic force microscopy (AFM). Their power spectral density (PSD) distribution is analysed at a measured area of 10?μm × 10?μm. The good agreement of the measured and calculated LIPSS periods strongly supports a mechanism based on the interference of surface-scattered and incident waves.     

Analysis of dioxins by gas chromatography/resonance-enhanced multiphoton ionization/mass spectrometry using nanosecond and picosecond lasers

Dioxins in a soil sample were measured using gas chromatography/resonance-enhanced multiphoton ionization/time-of-flight mass spectrometry coupled with different types of laser sources. The fourth-harmonic emission (266 nm) of a nanosecond Nd:YAG laser (1 ns) provided low ionization efficiency, especially for highly chlorinated dioxins/dibenzofurans (CDDs/CDFs). The ionization efficiency was improved using the fourth-harmonic emission (266 nm) of a picosecond Nd:YAG laser (4 ps), due to shorter singlet excited-state lifetimes. It was, however, difficult to efficiently ionize hepta-CDD and octa-CDD/CDF, because of their shorter lifetimes, which were induced by stronger spin-orbit coupling that led to efficient relaxation of the excited molecule to triplet levels. The ionization efficiency was substantially improved using the fifth-harmonic emission (213 nm) of the picosecond Nd:YAG laser (4 ps), in which the analyte molecule that was relaxed to triplet levels was efficiently ionized using a photon with sufficient energy for ionization, although the pulse energy obtained at 213 nm was only one-third of the pulse energy obtained at 266 nm. The limits of detection achieved for 17 toxic polychlorinated dibenzo-p-dioxins/polychlorinated dibenzofurans (PCDDs/PCDFs) were 0.41-45 pg. The analytical instrument developed in the present study performed sufficiently well for the practical trace analysis of dioxins in soil samples.     

Laser-ablated volume and depth as a function of pulse duration in aluminum targets

The ablated depth and volume per laser pulse from an aluminum target were measured for pulse durations that ranged from 80 fs to 270 ps at an average fluence of approximately 100 J/cm2 and a wavelength of 0.8 microm. The ablated volume showed a flat maximum for subpicosecond pulses and a minimum for approximately 6 ps. The crater diameters were rather constant up to pulse durations of approximately 6 ps and increased for larger pulse durations. As a result, the ablated depth also showed a plateau for subpicosecond pulses but decreased monotonically with pulse duration. A physical interpretation of these results and their consequences for laser applications are discussed.     

Frequency Spectral Measurements of a Pulsed,TE CO2

Abstract

Experimental measurements of the intra-pulse chirp and temporal coherence from a Joule class TE CO₂ laser incorporating LAWS transmitter design features are presented. Digitized quadrature data (I and Q) from our ground-based coherent Doppler lidar system utilizing return signals off a hard target in the telescope far field are processed using fast Fourier transform and pulse pair techniques to obtain laser pulse frequency spectral components (offset frequency and spectral width) and high-resolution (～ 50 ns/sample) frequency chirp profiles. Less than 300 kHz of frequency chirp is observed in the first 3·5 μs of the laser pulse which contains approximately 90% of the pulse energy. Spectral width of the laser pulse, including both chirp and transform limited components, are measured to be less than 300 kHz full width at half maximum.     

Simple autocorrelator for ultraviolet pulse-width measurements based on the nonlinear photoelectric effect

An optical pulse-width measurement in the ultraviolet spectral region has been performed in a simple manner by introducing into the second-order autocorrelator a nonlinear response of the optical detector based on the two-photon photoelectric effect. The pulse widths of the third, fourth, and fifth harmonics of a mode-locked Nd:YAG laser were measured by the use of a photomultiplier with a cesium iodide photocathode with a minimum required pulse energy of 10 nJ and a power density of 10 kW/cm(2). The effect of transient interband optical excitation with different photon energies on the intensity correlation profile was also studied for the case of a copper iodide photocathode, and the result provides a background-free intensity correlation in a part of the ultraviolet spectral region.