Dependence of Laser-induced Breakdown Spectroscopy Results on Pulse Energies and Timing Parameters Using Soil Simulants

The  dependence of some LIBS detection capabilities on lower pulse energies (&lt;100  mJ) and timing parameters were examined using synthetic silicate ...

Alvernia University

We have developed a miniature fiber-optic probe with no focusing optics for in situ analysis of volatile organic compounds (VOCs). The probe uses an optical fiber to transmit a laser pulse to a vapor sample causing it to ionize adjacent to the fiber tip through a resonance-enhanced multiphoton ionization (REMPI) process. The distal end of the optical fiber is contained co-axially within 2-mm-inner-diameter stainless steel tubing that serves as an electrode. The electrode is biased at a high positive potential to collect electrons. The current generated is shown to be proportional over about two orders of magnitude to the concentration of the species ionized. Visible wavelength REMPI spectroscopy is used to determine probe sensitivities of 20 ppb (benzene) and 43 ppb (toluene). Designing the probe without focusing optics specifies an achromatic ionization region constant in size and position as the laser wavelength is scanned, which simplifies data collection and reduction. Focusing achromatic systems are discussed and the potential signal improvement is estimated.

A non-lensed fiber-optic resonance-enhanced multiphoton ionization probe.

Emissions from a laser-induced breakdown spectroscopy (LIBS) plasma were examined in the region from 750 nm to 2000 nm. A Nd:YAG laser at 532 nm and 75 mJ per pulse were used to initiate the plasma. The detector was an InGaAs 1024 element diode array cooled to -100 degrees C. An f/4 spectrometer with gratings blazed for this region was used as the dispersive element. Survey spectra of soils, uranium, and other selected samples were taken in air and in a flow cell purged with argon at a local pressure of 0.84 x 10(5) Pa. Strong infrared lines of neutral aluminum, carbon, potassium, silicon, sulfur, and uranium, as well as once ionized lines of calcium, were observed out to 1670 nm. For potassium, the detection limits of the infrared (IR) system were compared with those obtained from a standard intensified charge-coupled device (ICCD) spectrometer arrangement, using the 766-770 nm doublet. Detection limits with the IR system were twice as high as those obtained from the ICCD detector.

Laser-induced breakdown spectra in the infrared region from 750 to 2000 nm using a cooled InGaAs diode array detector.

The goal of this work is a detailed study of uranium detection by laser-induced breakdown spectroscopy (LIBS) for application to activities associated with environmental surveillance and detecting weapons of mass destruction (WMD). The study was used to assist development of LIBS instruments for standoff detection of bulk radiological and nuclear materials and these materials distributed as contaminants on surfaces. Uranium spectra were analyzed under a variety of different conditions at room pressure, reduced pressures, and in an argon atmosphere. All spectra displayed a high apparent background due to the high density of uranium lines. Time decay curves of selected uranium lines were monitored and compared to other elements in an attempt to maximize detection capabilities for each species in the complicated uranium spectrum. A survey of the LIBS uranium spectra was conducted and relative emission line strengths were determined over the range of 260 to 800 nm. These spectra provide a guide for selection of the strongest LIBS analytical lines for uranium detection in different spectral regions. A detection limit for uranium in soil of 0.26% w/w was obtained at close range and 0.5% w/w was achieved at a distance of 30 m. Surface detection limits were substrate dependent and ranged from 13 to 150 microg/cm2. Double-pulse experiments (both collinear and orthogonal arrangements) were shown to enhance the uranium signal in some cases. Based on the results of this work, a short critique is given of the applicability of LIBS for the detection of uranium residues on surfaces for environmental monitoring and WMD surveillance.

Detection of uranium using laser-induced breakdown spectroscopy.

We present spectra of depleted uranium metal from laser plasmas generated by nanosecond Nd:YAG (1064 nm) and femtosecond Ti:sapphire (800 nm) laser pulses. The latter pulses produce short-lived and relatively cool plasmas in comparison to the longer pulses, and the spectra of neutral uranium atoms appear immediately after excitation. Evidence for nonequilibrium excitation with femtosecond pulses is found in the dependence of spectral line intensities on the pulse chirp.

Comparative study of femtosecond and nanosecond laser-induced breakdown spectroscopy of depleted uranium.

The development of field-deployable instruments to monitor radiological, nuclear, and explosive (RNE) threats is of current interest for a number of assessment needs such as the on-site screening of suspect facilities and nuclear forensics. The presence of uranium and plutonium and radiological materials can be determined through monitoring the elemental emission spectrum using relatively low-resolution spectrometers. In addition, uranium compounds, explosives, and chemicals used in nuclear fuel processing (e.g., tributyl-phosphate) can be identified by applying chemometric analysis to the laser-induced breakdown (LIBS) spectrum recorded by these spectrometers. For nuclear forensic applications, however, isotopes of U and Pu and other elements (e.g., H and Li) must also be determined, requiring higher resolution spectrometers given the small magnitude of the isotope shifts for some of these elements (e.g., 25 pm for U and 13 pm for Pu). High-resolution spectrometers will be preferred for several reasons but these must fit into realistic field-based analysis scenarios. To address the need for field instrumentation, we evaluated a previously developed field-deployable hand-held LIBS interrogation probe combined with two relatively new high-resolution spectrometers (Î»/Î”Î» ~75,000 and ~44,000) that have the potential to meet field-based analysis needs. These spectrometers are significantly smaller and lighter in weight than those previously used for isotopic analysis and one unit can provide simultaneous wide spectral coverage and high resolution in a relatively small package. The LIBS interrogation probe was developed initially for use with low resolution compact spectrometers in a person-portable backpack LIBS instrument. Here we present the results of an evaluation of the LIBS probe combined with a high-resolution spectrometer and demonstrate rapid detection of isotopes of uranium and hydrogen and highly enriched samples of (6)Li and (7)Li.

Monitoring uranium, hydrogen, and lithium and their isotopes using a compact laser-induced breakdown spectroscopy (LIBS) probe and high-resolution spectrometer.

Rosemarie C. Chinni

Department of Math and Sciences

Alvernia University

Dependence of Laser-induced Breakdown Spectroscopy Results on Pulse Energies and Timing Parameters Using Soil Simulants

Rosemarie C. Chinni

.css-o250i3{font-size:18px;font-family:Open Sans,sans-serif;line-height:21.6px;}Department of Math and Sciences

Alvernia University

Dependence of Laser-induced Breakdown Spectroscopy Results on Pulse Energies and Timing Parameters Using Soil Simulants

Department of Math and Sciences