LUMINESCENCE OF COMMON MATERIALS:
APPLICATION TO NATIONAL SECURITY
Adjunct Professor Nigel A. Spooner 1,2
and Dr Barnaby W...
Overview:
 Luminescence Techniques for Defence & National Security
 Opportunistic Dosimetry: “New” Luminescence & “New”
...
Luminescence Detection of Radiation ExposureLuminescence Detection of Radiation Exposure
Does not rely on the detection of...
The population of trapped charge is proportional to the absorbed dose
Conduction Band


radiation
Valence Band
Tra...
Principal Steps in Luminescence AnalysisPrincipal Steps in Luminescence Analysis
Environmental radioactivity measurements ...
 Retrospective nuclear accident dosimetryRetrospective nuclear accident dosimetry
 Art authenticationArt authenticatio...
Motivation: Naturally-occurring materials are well-studied
 notably quartz and feldspar for luminescence dating
BUT – the...
A Key Goal is the testing and extension of protocols on newA Key Goal is the testing and extension of protocols on new
and...
Dosimetric Materials at Habitations:
 Ceramics
 Porcelain & tiles
 Bricks
 Pottery
 Mortar & Concrete
 Glass
 Salt
...
The Potential of Salt (NaCl) For
Retrospective Dosimetry
19 samples have been collected from around the world
 Australia,...
TL Emission Spectra
All samples were measured on the University of Adelaide “3D TL Spectrometer”
 No signal-of-formation ...
Signal Lifetime: by Variation of Heating Rate Method
0 100 200 300
0
5 10
3

0.01
Glow5n
Glow2n
Glow1bn
Glow05bn
Glow02n...
Sample
#
Provenance
OSL (after PH 150ºC)
(Cts/Gy/mg)
(1s shine)
IRSL (after PH 150ºC)
(Cts/Gy/mg)*25
(1s shine)
OSL
100 ...
The Photon-Counting Imaging System (PCIS)
- Quantitative TL and OSL Imagery
 Modified
Minisys reader
 High sensitivity
LN/CCD
detector
 Broad
spectrum high
capture optics
 Optical
stimulation
so...
PCIS Luminescence Imaging CapabilityPCIS Luminescence Imaging Capability
The bright inclusions are
mineral grains emitting...
TL from Australian Lake Salt crystals - PCIS Image
PCIS Image; False Colour,
Unprocessed Data.
No filters; 200-1050nm
spec...
OSL: 470 nm
Stimulation
UV emission: U
340 filter
1st sec Lightsum
=1.8 x 105 cts/Gy
Total Lightsum
~ 3 x 105 cts/Gy
TL 20...
Red/Near-IR TL (695-1050 nm)
Sample #3 (“Woolworths Homebrand”); 6 Gy beta dose
TL integrated from 200 – 300ºC; Schott RG ...
IPAS is a transdisciplinary institute incorporating physicists, chemists, biologists
and environmental scientists; Directo...
Principal IPAS Activity Areas
DSTO / Univ. of Adelaide
Centre of Expertise in Luminescence
(Part of IPAS)
Standing and Deployable Capability forStanding and Deployable Capability for
Detection of Prior Radiation ExposureDetectio...
Summary
New Material Example:
 Salt has high sensitivity to beta radiation: TL, OSL & IRSL detection
limits are < 1mGy us...
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Luminescence of common materials application to national security spooner

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Luminescence of common materials application to national security spooner

  1. 1. LUMINESCENCE OF COMMON MATERIALS: APPLICATION TO NATIONAL SECURITY Adjunct Professor Nigel A. Spooner 1,2 and Dr Barnaby W. Smith 1 1. Defence Science and Technology Organisation & 2. Institute for Photonics and Advanced Sensing School of Chemistry and Physics University of Adelaide
  2. 2. Overview:  Luminescence Techniques for Defence & National Security  Opportunistic Dosimetry: “New” Luminescence & “New” Materials  Example: Salt  Institute for Photonics and Advanced Sensing (IPAS) – DSTO/University of Adelaide Centre of Expertise in Luminescence
  3. 3. Luminescence Detection of Radiation ExposureLuminescence Detection of Radiation Exposure Does not rely on the detection of either Ionising Radiation or Radioisotopes - offers a unique capability in sanitised locations and in the post-event recovery phase Detection of cDetection of clearedleared ‘‘dirty bombdirty bomb’’ construction or storage sites.construction or storage sites. •• forensic analysis even whenforensic analysis even when freefree of isotopic contamination.of isotopic contamination. Support for UN weapons inspection efforts.Support for UN weapons inspection efforts. •• forensic analysis of bunkers, buildingsforensic analysis of bunkers, buildings and laboratories cleaned and refurnishedand laboratories cleaned and refurnished for nonfor non--nuclear cover activity.nuclear cover activity. Retrospective population exposureRetrospective population exposure assessment.assessment. •• measure ofmeasure of extent of the affected areaextent of the affected area.. •• quantification of radiation exposure over thequantification of radiation exposure over the affected areaaffected area PreventionPrevention DetectionDetection ResponseResponseRecoveryRecovery
  4. 4. The population of trapped charge is proportional to the absorbed dose Conduction Band   radiation Valence Band Trap Ea thermal or optical release light emission Luminescence MechanismLuminescence Mechanism - enabling quantitative dosimetry
  5. 5. Principal Steps in Luminescence AnalysisPrincipal Steps in Luminescence Analysis Environmental radioactivity measurements are alsoEnvironmental radioactivity measurements are also made to correct for the natural radiation backgroundmade to correct for the natural radiation background Including use of a NaI portable GammaIncluding use of a NaI portable Gamma--ray Spectrometry, hereray Spectrometry, here undergoing calibration at Geosciences Australia, Canberraundergoing calibration at Geosciences Australia, Canberra Then measured in the LaboratoryThen measured in the Laboratory PhotonPhoton--Counting Imaging System at ANUCounting Imaging System at ANU enables analysis of slices and potential rapidenables analysis of slices and potential rapid assessment of doseassessment of dose--depth profilingdepth profiling Chemically prepared … Sample cores are extracted from common building materials at suspect sites…
  6. 6.  Retrospective nuclear accident dosimetryRetrospective nuclear accident dosimetry  Art authenticationArt authentication  Detection of illicit food irradiationDetection of illicit food irradiation  Atomic bomb radiation effectsAtomic bomb radiation effects  Chronology of human evolutionChronology of human evolution  Geomorphology & Soil ScienceGeomorphology & Soil Science  MegafaunalMegafaunal extinction/climate changeextinction/climate change Luminescence TechniqueLuminescence Technique BUT: requires very experienced personnelBUT: requires very experienced personnel Numerous reported applications in the openNumerous reported applications in the open literature:literature:
  7. 7. Motivation: Naturally-occurring materials are well-studied  notably quartz and feldspar for luminescence dating BUT – these may not be present in many scenarios of interest  urban or industrial locations, vehicles Instead, Artificial materials may dominate  which ones can reveal prior exposure to ionising radiation? Many candidate materials exist but few are sufficiently well-studied to enable rapid use  entails compiling, validating and extending current know-how The complexity of the phenomena means extensive laboratory work is required to develop Standard Operating Procedures Extension to “New” Signals and Materials
  8. 8. A Key Goal is the testing and extension of protocols on newA Key Goal is the testing and extension of protocols on new and established materials, to develop Standard Operatingand established materials, to develop Standard Operating Procedures to enable rapid and flexible analysisProcedures to enable rapid and flexible analysis Example – Analysis of Brick Schematic diagram illustrating current standardised sectioning used to sample brick for depth-dose measurements Currently there are no standard protocols, however the Luminescence Dating community has a large and expanding literature on fired and unfired materials, and increasing effort in Radioepidemiology Key Goal – Standard Operating Procedures
  9. 9. Dosimetric Materials at Habitations:  Ceramics  Porcelain & tiles  Bricks  Pottery  Mortar & Concrete  Glass  Salt  Hard plastics (some?)  Gyprock  Mud-based insect nests  Carbonate materials (limestone, marble, calcite etc)  Quartz, Feldspar & Zircon grains Items carried by people, such as: • Glass (spectacles, watches etc) • Jewelry • Credit cards • Electronic components • Hard plastics (some?) • Some foodstuffs Opportunistic Dosimetry UtilisesUtilises materials that fortuitously occur in the incident environment, or are carried in by people Contrary to Luminescence Dating, Opportunistic Dosimetry can utilise signals lacking long-term stability. This eliminates many complications (from ambient environmental radiation and signals of formation), and in the CT context this biases against reporting False Positives
  10. 10. The Potential of Salt (NaCl) For Retrospective Dosimetry 19 samples have been collected from around the world  Australia, UK, Poland, USA, Canada etc. Types include:  Rock salt  Salt damp crystals  Domestic salt from evaporation of: sea water; saline lake water saline river water Our Analyses have included: 1. Emission Spectra 2. Kinetic Analysis 3. TL Sensitivity Changes During Heating 4. OSL & IRSL Dose Response 5. OSL & IRSL Pulse-Annealing Spectra 6. OSL & IRSL Sensitivity Summary 7. Imaged OSL, IRSL, TL
  11. 11. TL Emission Spectra All samples were measured on the University of Adelaide “3D TL Spectrometer”  No signal-of-formation was observed from any recent-age sample  Representative spectra are shown, measured at 2K/s; 2Gy beta dose Prominent TL peaks were seen in the mid-Temp range (150-280ºC), with emissions in UV: 380 nm (3.4 eV), Blue: 440 nm (2.8 eV), Red 590 nm (2.1 eV). (18) JFK Airport, USA (3) Woolworths Homebrand (10) Himalayan Rock Salt
  12. 12. Signal Lifetime: by Variation of Heating Rate Method 0 100 200 300 0 5 10 3  0.01 Glow5n Glow2n Glow1bn Glow05bn Glow02n Glow01n Glow005n Glow002n Glow001n Glow0002n T1Temperature (ºC) 0.1 deg/s 5 deg/s 0.02 deg/s 0.01 deg/s 0.002 deg/s 2 deg/s 0.2 deg/s 0.5 deg/s 1 deg/s 0.05 deg/s AreaNormalisedTL Sample #3; “Woolworths Homebrand” Salt chosen due to representative glow curve shape and strong Red TL emission 11 12 13 14 15 16 17 18 19 0.0027 0.0029 0.0031 0.0033 1/T Ln(Tmax 2 /B) 0.002 K/s 1.0 K/s 0.02 K/s 0.2 K/s 100ºC peak (5K/sec) Lifetime20ºC = 6.6 hours 200ºC peak (5K/sec) Lifetime20ºC = 0.64 ka 240ºC peak (5K/sec) E= 1.45 eV s= 7.9 x 1013 s-1 Lifetime20ºC = 3.9 ka Data for 100ºC peak Heating rates 5 K/s – 0.002 K/s
  13. 13. Sample # Provenance OSL (after PH 150ºC) (Cts/Gy/mg) (1s shine) IRSL (after PH 150ºC) (Cts/Gy/mg)*25 (1s shine) OSL 100 sec shine (Cts/Gy/mg) 11 Salt Damp Crystals | 48 ||| 5159 12 River Murray Salt Flakes (evap.) | 1602 |||||| 595 |||| 7735 1 Australian Lake Salt |||| |||||| |||||||||||| 13 Ramona's salt |||||| |||||| |||||||||||||| 3 Woolworth's HomeBrand Salt (evap. seawater) |||||| 11549 ||||||| 771 |||||||||||||| 29861 19 Sydney, Canada (Huston Texas) ||||||| |||| |||||||||||||| 16 Table Salt, UK, Silver Sachet |||||||||||| 26758 ||||||| 1028 |||||||||||||||||| 39637 14 Evap. Seawater ||||||| ||||| |||||||||||||||||| 15 Table Salt, UK Roadhouse, Blue Sachet ||||||||||| |||||||||| |||||||||||||||||| 18 JFK Airport, USA (Savannah Georgia) |||||||||||| ||||| ||||||||||||||||||||||| 20 Halifax Canada ||||||||||||||||| ||||| ||||||||||||||||||||||||||||||| 8 Evap. Seawater, SA ||||||||||||| ||||| ||||||||||||||||||||||||||||||| 9 Rock Salt (Poland) |||||||||||| |||||||||| ||||||||||||||||||||||||||||||||||| 10 Himalayan Crystal Salt ( 250Ma Rock Salt, Pakistan). |||||||||||||| ||||||||| ||||||||||||||||||||||||||||||||||||| 5 ISM Table Salt |||||||||||||||||||| |||||||| |||||||||||||||||||||||||||||||||||||||||||||| 7 Unbranded Table Salt |||||||||||||||||||||||| ||||||||| ||||||||||||||||||||||||||||||||||||||||||||||||||| |||||| 4 Coles Iodised Salt (evap. seawater) |||||||||||||||||||||||||| |||||||| ||||||||||||||||||||||||||||||||||||||||||||||||||| |||||||||||| 2 Saxa Cooking Salt (evap. seawater) ||||||||||||||||||||||||||||| ||||||||| ||||||||||||||||||||||||||||||||||||||||||||||||||| ||||||||||||||| 6 Water Softener Salt (unknown comp.) * |||||||||||||||||||||||||||||| 65862 |||||||||| 1088 ||||||||||||||||||||||||||||||||||||||||||||||||||| |||||||||||||||||||||||||| 173578
  14. 14. The Photon-Counting Imaging System (PCIS) - Quantitative TL and OSL Imagery
  15. 15.  Modified Minisys reader  High sensitivity LN/CCD detector  Broad spectrum high capture optics  Optical stimulation sources  Optical filtering capability  Integration electronics  Automation software systems Photon-Counting Imaging System (PCIS) Architecture
  16. 16. PCIS Luminescence Imaging CapabilityPCIS Luminescence Imaging Capability The bright inclusions are mineral grains emitting TL (acquired by natural irradiation over the 50 years since firing) Natural TL from 50 yearNatural TL from 50 year old house brickold house brick Aluminum Oxide ChipAluminum Oxide Chip Red TL integral measured from 130-260°C following 0.18 Gy dose (equates to 3 x 109 counts/Gy) QuantitativeQuantitative imaging of irradiated slices, including brick and concreteimaging of irradiated slices, including brick and concrete •• using a unique facility under development at the RSES, Australiausing a unique facility under development at the RSES, Australian National Universityn National University Irradiation Concrete slice (app. 5 mm square) after 20 Gy dose applied from direction as shown Concrete slice (app. 8 mm length) after 9 Gy dose applied from Z (above) direction
  17. 17. TL from Australian Lake Salt crystals - PCIS Image PCIS Image; False Colour, Unprocessed Data. No filters; 200-1050nm spectral range 20Gy beta dose; then TL measured at 2K/s The brightest grain shown here has emitted 5.7 x 107 counts The total light sum of all grains is approximately 4.2 x 108 counts Sensitivity is ~ 2 x 106 counts/Gy/mg for this salt sample
  18. 18. OSL: 470 nm Stimulation UV emission: U 340 filter 1st sec Lightsum =1.8 x 105 cts/Gy Total Lightsum ~ 3 x 105 cts/Gy TL 200ºC – 300ºC; 6 Gy beta dose; No filters (200 – 1050 nm) TL Lightsum = 1.6 x 108 counts. Corresponds to 2.5 x 107 cts/Gy Sample #3 (“Woolworths Homebrand”) 5 mg aliquot IRSL: 880 nm Stimulation Red emission: 3 mm BG 39 filter 1st sec Lightsum =2.8 x 105 cts/Gy Total lightsum ~ 2 x 106 cts/Gy
  19. 19. Red/Near-IR TL (695-1050 nm) Sample #3 (“Woolworths Homebrand”); 6 Gy beta dose TL integrated from 200 – 300ºC; Schott RG 695 filter TL Lightsum = 5.2 x 107 counts Corresponds to 1.7 x 106 cts/Gy/mg Reheat image (note heater plate incandescence and grain images)
  20. 20. IPAS is a transdisciplinary institute incorporating physicists, chemists, biologists and environmental scientists; Director Professor Tanya Monro New $80 million Integrated laboratories for research in Photonics and Sensing, University of Adelaide Nth. Tce campus Builds on University of Adelaide expertise in soft glass optical fibre research and silica fibre fabrication Aims to develop new technologies in areas including: 1. Fibre lasers (medicine & Defence) 2.2. Luminescence for detection of trace materials and environmentalLuminescence for detection of trace materials and environmental dosimetrydosimetry 3. “Smart” fibre sensors using surface chemistry techniques 4. Detection of viruses and cancer biomarkers (functionalised fibre sensors) 5. Evolutionary Biology & Photonics – assess impact of climate change on biodiversity IPAS Concept & Goals
  21. 21. Principal IPAS Activity Areas
  22. 22. DSTO / Univ. of Adelaide Centre of Expertise in Luminescence (Part of IPAS)
  23. 23. Standing and Deployable Capability forStanding and Deployable Capability for Detection of Prior Radiation ExposureDetection of Prior Radiation Exposure Principal method: Luminescence (TL or OSL) analyses of materialsPrincipal method: Luminescence (TL or OSL) analyses of materials (including brick, tiles, porcelain, drywall, concrete and sedime(including brick, tiles, porcelain, drywall, concrete and sediment) tont) to reveal radiation exposure in excess of natural backgroundreveal radiation exposure in excess of natural background DSTO / Univ. of Adelaide Centre of Expertise in Luminescence A Key Goal is the testing and extension of protocols on newA Key Goal is the testing and extension of protocols on new and established materials, to develop Standard Operatingand established materials, to develop Standard Operating Procedures enabling analysis rapidly and flexiblyProcedures enabling analysis rapidly and flexibly
  24. 24. Summary New Material Example:  Salt has high sensitivity to beta radiation: TL, OSL & IRSL detection limits are < 1mGy using 10 mg portions of sample  Salt appears a suitable material for Retrospective Dosimetry  Australian Luminescence Analysis capacity is currently focussed on the specialist technique of Optical Dating using OSL from Quartz  An emergency response will also require utilising less-studied materials  Well-defined SOPs for these materials are essential A key goal of the Centre of Expertise in Luminescence is theA key goal of the Centre of Expertise in Luminescence is the testing and extension of protocols on new and establishedtesting and extension of protocols on new and established materials, to develop Standard Operating Procedures andmaterials, to develop Standard Operating Procedures and enable rapid and flexible analysisenable rapid and flexible analysis

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