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Title: Advanced Ultrafast Spectroscopy for Chemical Detection of Nuclear Fuel Cycle Materials

Abstract

The development of new signatures and observables from processes related to proliferation activities are often related to the development of technologies. In our physical world, the intensity of observables is linearly related to the input drivers (light, current, voltage, etc.). Ultrafast lasers with high peak energies, opens the door to a new regime where the intensity of the observables is not necessarily linear with the laser energy. Potential nonlinear spectroscopic applications include chemical detection via remote sensing through filament generation, material characterization and processing, chemical reaction specificity, surface phenomena modifications, X-ray production, nuclear fusion, etc. The National Security Directorate laser laboratory is currently working to develop new tools for nonproliferation research with femtosecond and picosecond lasers. Prior to this project, we could only achieve laser energies in the 5 nano-Joule range, preventing the study of nonlinear phenomena. To advance our nonproliferation research into the nonlinear regime we require laser pulses in the milli-Joule (mJ) energy range. We have procured and installed a 35 fs-7 mJ laser, operating at one-kilohertz repetition rate, to investigate elemental and molecular detection of materials in the laboratory with potential applications in remote sensing. Advanced, nonlinear Raman techniques will be used to study materials of interestmore » that are in a matrix of many materials and currently with these nonlinear techniques we can achieve greater than three orders of magnitude signal enhancement. This work studying nuclear fuel cycle materials with nonlinear spectroscopies will advance SRNL research capabilities and grow a core capability within the DOE complex.« less

Authors:
 [1];  [1];  [1]
  1. Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)
Publication Date:
Research Org.:
Savannah River Site (SRS), Aiken, SC (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1395974
Report Number(s):
SRNL-STI-2017-00636
TRN: US1800075
DOE Contract Number:
AC09-08SR22470
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL PROTECTION; NUCLEAR FUELS; LASERS; FUEL CYCLE; X RADIATION; SPECTROSCOPY; NATIONAL SECURITY; REMOTE SENSING

Citation Formats

Villa-Aleman, E., Houk, A., and Spencer, W. Advanced Ultrafast Spectroscopy for Chemical Detection of Nuclear Fuel Cycle Materials. United States: N. p., 2017. Web. doi:10.2172/1395974.
Villa-Aleman, E., Houk, A., & Spencer, W. Advanced Ultrafast Spectroscopy for Chemical Detection of Nuclear Fuel Cycle Materials. United States. doi:10.2172/1395974.
Villa-Aleman, E., Houk, A., and Spencer, W. 2017. "Advanced Ultrafast Spectroscopy for Chemical Detection of Nuclear Fuel Cycle Materials". United States. doi:10.2172/1395974. https://www.osti.gov/servlets/purl/1395974.
@article{osti_1395974,
title = {Advanced Ultrafast Spectroscopy for Chemical Detection of Nuclear Fuel Cycle Materials},
author = {Villa-Aleman, E. and Houk, A. and Spencer, W.},
abstractNote = {The development of new signatures and observables from processes related to proliferation activities are often related to the development of technologies. In our physical world, the intensity of observables is linearly related to the input drivers (light, current, voltage, etc.). Ultrafast lasers with high peak energies, opens the door to a new regime where the intensity of the observables is not necessarily linear with the laser energy. Potential nonlinear spectroscopic applications include chemical detection via remote sensing through filament generation, material characterization and processing, chemical reaction specificity, surface phenomena modifications, X-ray production, nuclear fusion, etc. The National Security Directorate laser laboratory is currently working to develop new tools for nonproliferation research with femtosecond and picosecond lasers. Prior to this project, we could only achieve laser energies in the 5 nano-Joule range, preventing the study of nonlinear phenomena. To advance our nonproliferation research into the nonlinear regime we require laser pulses in the milli-Joule (mJ) energy range. We have procured and installed a 35 fs-7 mJ laser, operating at one-kilohertz repetition rate, to investigate elemental and molecular detection of materials in the laboratory with potential applications in remote sensing. Advanced, nonlinear Raman techniques will be used to study materials of interest that are in a matrix of many materials and currently with these nonlinear techniques we can achieve greater than three orders of magnitude signal enhancement. This work studying nuclear fuel cycle materials with nonlinear spectroscopies will advance SRNL research capabilities and grow a core capability within the DOE complex.},
doi = {10.2172/1395974},
journal = {},
number = ,
volume = ,
place = {United States},
year = 2017,
month = 9
}

Technical Report:

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  • A workshop on 'Decay Spectroscopy at CARIBU: Advanced Fuel Cycle Applications, Nuclear Structure and Astrophysics' will be held at Argonne National Laboratory on April 14-16, 2011. The aim of the workshop is to discuss opportunities for decay studies at the Californium Rare Isotope Breeder Upgrade (CARIBU) of the ATLAS facility with emphasis on advanced fuel cycle (AFC) applications, nuclear structure and astrophysics research. The workshop will consist of review and contributed talks. Presentations by members of the local groups, outlining the status of relevant in-house projects and availabile equipment, will also be organized. time will also be set aside tomore » discuss and develop working collaborations for future decay studies at CARIBU. Topics of interest include: (1) Decay data of relevance to AFC applications with emphasis on reactor decay heat; (2) Discrete high-resolution gamma-ray spectroscopy following radioactive decya and related topics; (3) Calorimetric studies of neutron-rich fission framgents using Total ABsorption Gamma-Ray Spectrometry (TAGS) technique; (4) Beta-delayed neutron emissions and related topics; and (5) Decay data needs for nuclear astrophysics.« less
  • A preliminary study by a group of experts at ORNL has generated and evaluated a number of aqueous and non-aqueous flowsheets for recovering transuranium actinides from LWR fuel for use as fuel in an LMR and, at the same time, for transmutation of the wastes to less hazardous materials. The need for proliferation resistance was a consideration in the flowsheets. The current state of development of the flowsheets was evaluated and recommendations for additional study were made. 3 refs., 6 figs.
  • Fuel cycle studies reported include development of centrifugal contactors for Purex processes. Tricaprylmethyl-ammonium nitrate and di-n-amyl-n-amylphosphonate are being evaluated as Thorex extractants. Dispersion of uranium and plutonium by fires, and mechanisms for subdividing and dispersing liquids and solids were reviewed. In the pyrochemical and dry processing program, a facility for testing containment materials is under construction; a flowsheet for carbide fuel processing has been designed and studies of carbide reactions in bismuth are underway; salt transport processes are being studied; process-size refractory metal vessels are being fabricated; the feasibility of AIROX reprocessing is being determined; the solubility of UO/sub 2/,more » UO/sub 2/ + fission products, and PuO/sub 2/ in molten alkali metal nitrates, has been investigated; a flowsheet was developed for reprocessing actinide oxides in molten salts; preparation of Th-U carbide from the oxide is being studied; new flowsheets based on the Dow Aluminum Pyrometallurgical process for reprocessing of spent uranium metal fuel have been prepared; the chloride volitility processing of thorium-based fuels is being studied; the reprocessing of (Th,U)O/sub 2/ solid solution in KCl-LiCl-ThCl/sub 4/-Th is being studied; and a flowsheet for processing spent nuclear fuel in molten tin has been constructed. Leach rates of simulated encapsulated waste forms in a metal matrix were studied. Nine criteria for handling waste cladding hulls were established. Strontium and tin migration in glauconite columns was measured. Radioactive Sr in a stream of water moved through oolitic limestone as rapidly as water, but in a stream of water equilibrated with the limestone, Sr moved through the limestone one-tenth as fast. Migration of trace quantities of Cs and I through kaolinite was studied. 88 figures, 53 tables.« less
  • This report provides a summary of work completed in FY-94 by FSU to develop and investigate the feasibility of using Raman spectroscopy with Hanford tank waste materials. Raman performance impacts from sample morphology, including the effects of absorption, particle size, density, color and refractive index, are discussed. An algorithm for relative species concentration measurement from Raman data is presented. An Algorithm for applying Raman to tank waste core screening is presented and discussed. A library of absorption and Raman spectra are presented that support this work.
  • Metallographic studies and compositional analyses of the various materials exposed in the fluid-bed combustor environment are continuing. The severe wastage of the bed-cooling tubes is considered to have serious implications for the commercial application of the concept of burning coal with limestone in a fluid-bed combustor. It is recommended that the problem be investigated in greater depth than can be done in the current program.