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WO1999049311A2 - Procede et dispositif permettant de detecter, de localiser et d'analyser des composes chimiques par activation de particules subatomiques - Google Patents

Procede et dispositif permettant de detecter, de localiser et d'analyser des composes chimiques par activation de particules subatomiques Download PDF

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Publication number
WO1999049311A2
WO1999049311A2 PCT/US1999/003491 US9903491W WO9949311A2 WO 1999049311 A2 WO1999049311 A2 WO 1999049311A2 US 9903491 W US9903491 W US 9903491W WO 9949311 A2 WO9949311 A2 WO 9949311A2
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Prior art keywords
detector
detecting
particle
act
subatomic
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WO1999049311A3 (fr
Inventor
Bogdan C. Maglich
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HIENERGY MICRODEVICES Inc
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HIENERGY MICRODEVICES Inc
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Priority to AU49516/99A priority Critical patent/AU4951699A/en
Priority to EP99933468A priority patent/EP1071948A2/fr
Priority to CA002321063A priority patent/CA2321063A1/fr
Priority to JP2000538230A priority patent/JP2002507746A/ja
Publication of WO1999049311A2 publication Critical patent/WO1999049311A2/fr
Publication of WO1999049311A3 publication Critical patent/WO1999049311A3/fr
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    • G—PHYSICS
    • G01—MEASURING; TESTING
    • G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
    • G01N23/00—Investigating or analysing materials by the use of wave or particle radiation, e.g. X-rays or neutrons, not covered by groups G01N3/00 – G01N17/00, G01N21/00 or G01N22/00
    • G01N23/22—Investigating or analysing materials by the use of wave or particle radiation, e.g. X-rays or neutrons, not covered by groups G01N3/00 – G01N17/00, G01N21/00 or G01N22/00 by measuring secondary emission from the material
    • G01N23/221—Investigating or analysing materials by the use of wave or particle radiation, e.g. X-rays or neutrons, not covered by groups G01N3/00 – G01N17/00, G01N21/00 or G01N22/00 by measuring secondary emission from the material by activation analysis
    • G01N23/222—Investigating or analysing materials by the use of wave or particle radiation, e.g. X-rays or neutrons, not covered by groups G01N3/00 – G01N17/00, G01N21/00 or G01N22/00 by measuring secondary emission from the material by activation analysis using neutron activation analysis [NAA]

Definitions

  • the present invention relates to the field of chemical compound detection and analysis, specifically to the detection, identification, and spatial location of explosives, nerve agents, contraband, and other chemical compounds using subatomic particle activation.
  • X-ray analysis can only provide information about an object's shape or location, and are not useful in large area searches (such as for land mines buried in the field or searches of large containerized cargo).
  • prior art contraband detection devices based on gamma ray spectrum analysis are not able to determine quantitative elemental composition of the interrogated object. Rather, they can detect only the presence (or dominance) of certain elements that are potentially indicative of contraband, thus providing an 'alert' signal.
  • This alert signal in turn requires intrusive inspection of the interrogated object, and results in a false alarm rate which, while reduced from that of X ray contraband detectors, is still quite high (over 90% by some estimates).
  • High Purity Germanium Detectors HPGD have an energy resolution on the order of 0.1-0.3%; however, their dead time, determined by their charge collection time, is roughly 200 ns. Such dead time was considered incompatible with the aforementioned requirement of high temporal resolution.
  • Another critical performance criterion of chemical detection systems is detection speed, or discovery time.
  • detection speed For such a detection system to be practical, it must be able to detect and recognize a predetermined quantity of contraband in a short period of time. For example, detection of 1 Kg of explosive within about 1 second would practically allow for the use of the system in most any application.
  • this level of performance requires a high data accumulation rate: at least 10,000 gamma events must be fully measured and processed per second (after rejecting associated "noise") in order to have a large enough statistical sample to recognize the explosive by gamma ray analysis.
  • CRi instantaneous counting rate in detector 1
  • CR 2 instantaneous counting rate in detector 2
  • the present invention satisfies the aforementioned needs by providing an improved apparatus for the detection, location, and chemical-specific analysis of chemical compounds with the purpose of non-intrusive identification as either explosives, nerve agents, chemical weapons, and contraband, as well as a method of operating the same, with high energy, temporal, and spatial resolution, and high detection speed. Additionally, a system and method for the standardized measurement of the efficacy of this apparatus and other existing detection/analysis devices is disclosed.
  • an improved chemical compound detection, retrieval, location, and analysis apparatus is disclosed.
  • an excitation beam containing one or more atomic species is used to bombard one or more specially constructed targets, thereby generating streams of subatomic particles which emanate from the target(s) in substantially opposite directions.
  • neutrons and alpha particles emanating from the target(s) i.e., "tagged fast neutrons" are utilized, although it can be appreciated that other particles or emissions may conceivably be used.
  • the object or area being examined is exposed to the generated neutron flux, the energetic neutrons of which interact with the nuclei atoms (in this case carbon, nitrogen, or oxygen, though others may be chosen) of any explosives, chemical weapons/nerve agents, or contraband within the subject thereby generating prompt quanta in the form of gamma rays.
  • One or more gamma detectors are located relative to the subject being examined to detect these emitted quanta, which are subsequently analyzed to identify the elemental atomic proportions resident in the test subject.
  • one or more scintillation (or comparable) detectors are placed within the solid angle of the alpha particle flux in order to detect alpha particles in coincidence with the gamma events detected by the aforementioned gamma detectors, thereby further permitting spatial positioning.
  • a magnetic field or electric field in order to permit the excitation of more than one target.
  • multiple (but spatially discrete) neutron and alpha particle streams are generated, thereby bombarding the subject being examined with neutrons from different relative angles.
  • beam "separation" may be accomplished without any applied field by generating a spatially broad beam and having it intersect multiple targets. This use of multiple neutron/alpha streams (or a single broad beam) and corresponding alpha/gamma detectors permits an even more accurate spatial location of the organic compound within the test subject
  • an improved chemical compound location apparatus and method Utilizing the general technique of particle induced prompt gamma emission described above, one or more gamma detectors are placed in known physical proximity to the test subject. One or more alpha particle detectors are placed in general proximity to the target(s) as well. The timing difference (nanosecond time frame) between the alpha particle detection event and the induced prompt gamma detection event provides a coarse determination of the axial (i.e., line-of sight or "Z-axis") distance between the activated chemical compound and the target, based on known neutron and alpha particle velocities, circuit and detector-induced delays, and excitation beam pulse duration.
  • axial i.e., line-of sight or "Z-axis
  • an improved coincidence detection apparatus and method is disclosed.
  • An array of alpha particle detectors is formed in general proximity to the neutron- generating target(s) previously described.
  • individual prompt gamma events relating to specific elemental gamma "lines” that are characteristic of certain "signature” elements associated with explosives
  • individual detection events within the alpha detector array thereby fixing the spatial position of the gamma emitter within the test subject, and permitting a greatly enhanced rate of event processing due to parallelism.
  • Germanium crystal detectors are used to detect prompt gamma events within the test subject.
  • the Germanium detectors provide enhanced gamma energy resolution, thereby allowing discrimination of the multiple C:N:O (or other elements) spectral lines from the "background" of hundreds of other gamma lines.
  • the high-resolution gamma spectrum is decomposed into a binary representation, with each line assigned a different binary value ("bin") representing its gamma energy level.
  • Known lines (bins) associated with carbon, nitrogen, and oxygen for the chosen type/energy of incident particle stream are then further processed, with other unrelated lines being filtered out. In this fashion, the computational burden on attached signal or data processing equipment is greatly reduced since only relevant C:N:O peaks survive the filtration stage.
  • an improved method for identifying chemical compounds using particle activation is disclosed.
  • the filtered gamma detector output signal described in the preceding paragraph is input to a signal processing apparatus running an improved explosive/chemical weapon/nerve agent/contraband identification and classification algorithm.
  • This algorithm is based on the well known "Dalitz Triangle,” and identifies the activated chemical compound (if it is an explosive, chemical weapon, nerve agent, or contraband substance) within the test subject through calculation of the relative proportions of C:N:O (or other elements) as provided by the filtered gamma spectra.
  • Statistical weighting and error analysis may also be employed to evaluate the resultant data.
  • an improved system and method for measuring the efficacy (figure of merit) of a particle activation-based detection/analysis system and calibrating same is disclosed.
  • a discovery time constant (T d ) is mathematically defined which is a measure of the time required to perform a chemically specific identification of a certain mass of chemical compound at a certain distance from the particle source, and certain distance between the chemical compound and gamma detector(s), with a prescribed statistical confidence level about the relevant point on the aforementioned Dalitz triangle.
  • a baseline system T is then generated thereby providing a basis for comparison for actual data received from the operating system when analyzing specimens of varying mass under varying test conditions.
  • T d values measured under such varying test conditions are then used to generate correction factors for the system which are useful in calibration and field testing. Furthermore, experimentally generated values of T d for one system are then compared to those of another system in order to determine the relative efficacy of the two systems under various operating conditions.
  • Fig. 1 is a side view of a first embodiment of the chemical compound detection and analysis apparatus of the present invention.
  • Fig. 2a is a perspective view of the apparatus of the present invention adapted for use in examining airport baggage handling cars.
  • Fig. 2b is a perspective view of the apparatus of the present invention adapted for use on a land mobile vehicle.
  • Fig. 3 is a perspective view of a first embodiment of an alpha particle detector array according to the present invention.
  • Fig. 4 is a side view of a second embodiment of the chemical compound detection and analysis apparatus of the present invention, utilizing multiple targets and an applied magnetic field.
  • Fig. 5 is a side view of a third embodiment of the chemical compound detection and analysis apparatus of the present invention, utilizing multiple targets and a single, spatially broadened beam.
  • Fig. 6 is a perspective view of a dual-source neutron activation apparatus according to the present invention.
  • Fig. 7 is a perspective view of a fourth embodiment of the chemical compound detection and analysis apparatus of the present invention, as might be attached to a land-mobile vehicle useful for land mine or buried explosives detection.
  • Fig. 8 is a block diagram illustrating one embodiment of the gamma spectrum analog-to- digital conversion and filtration process of the present invention.
  • Fig. 9 is a prompt gamma ray emission spectrum obtained from a typical prior art fast neutron activation detection system.
  • Fig. 10 is a prompt gamma ray emission spectrum (background subtracted) obtained by irradiating a urea test specimen with fast neutrons and detecting prompt gamma emissions using a Germanium crystal detector gated at 40 ns.
  • Fig. 11 is a prompt gamma ray emission spectrum (no background subtraction) obtained by irradiating a urea test specimen with fast neutrons and detecting prompt gamma emissions using a Germanium crystal detector gated at approximately 6 ns.
  • Figs. 12a and 12b are sample prompt gamma ray spectra showing the peak and three discrete bandwidths analyzed as part of one embodiment of the chemical identification method of the present invention.
  • Fig. 13 is a graph illustrating the method of gamma event rise time measurement according to the present invention.
  • Fig. 14 is a bar graph of a digitized spectrum showing the relative constituent elements and concentrations of several common chemical compounds.
  • Figs. 15a and 15b are diagrams of the C:H:O and C:N:O Dalitz triangles, respectively, showing a variety of common chemical compounds.
  • Fig. 16 is a block diagram of the method disclosed in the present invention for evaluating and calibrating FNA devices using the discovery time constant T .
  • Fig. 1 shows a first embodiment of the particle detection and analysis apparatus of the present invention.
  • an accelerated beam 10 containing one or more subatomic species here, various ionized isotopes of hydrogen including deuterium and tritium
  • subatomic species here, various ionized isotopes of hydrogen including deuterium and tritium
  • a conventional or advanced charged particle accelerator of the type well known in the art such as the Model A-711 accelerator manufactured by the MF Physics Corporation, is used as the source 15 although a variety of different such sources may be used with equal success.
  • the source 15 is operated in a continuous direct current (i.e., DC) mode such that excitation particles are incident on the target(s) continually which may or may not be modulated into "long" (0.1 to 10 sec.) discrete time intervals, although other schemes may be used.
  • long is used with respect to the coincidence resolving times described later herein, which are on the order of 1 to 100 nanoseconds.
  • neutrons and alpha particles are generated from the target(s) in the present embodiment, other subatomic particles or emissions with desirable properties may also feasibly be used to produce the desired result within the test subject.
  • the object or area being examined 20 is exposed to the generated fast neutron flux 14, the energetic neutrons of which interact with the carbon, nitrogen, or oxygen bearing (C:N:O) molecules of any explosives, chemical weapons/nerve agents, or contraband 22 within the subject 20 thereby generating prompt quanta in the form of gamma rays 24 which are characteristic of C, N, and O and are know as "signatures" of the aforementioned substances. It is further noted that the energies of these gamma rays 24 have substantially discrete values.
  • One or more high-resolution gamma detectors 26 of the type well known in the art are placed relative to the subject being examined 20 to detect these emitted quanta, which are subsequently analyzed to identify the molecules resident in the test subject.
  • one or more scintillation (or comparable) detectors 28 of the type well know in the art are placed within the solid angle of the alpha particle flux 16 in order to detect alpha particles in coincidence with the gamma events detected by the aforementioned gamma detectors 26, thereby permitting two separate determinations: 1) that of the gamma-alpha simultaneous timing (rejecting non-synchronous events), and 2) spatial positioning.
  • High purity (80%) germanium detectors of the N-type (neutron resistant) produced by ORTEC Corporation are used as the gamma detectors 26 in the present embodiment.
  • Germanium crystal detectors are preferred (as further described below), it can be appreciated that other types of high-resolution detectors, for example those utilizing Xenon, may be used to accomplish the desired functionality of coincident alpha and prompt gamma detection for both the timing and spatial location of the chemical compound within the test subject.
  • the targets 18 of the present embodiment are constructed of a scandium titride layer deposited on a copper (Cu) substrate, both substances which are well known in the material sciences, the targets having the desirable property of generating a stream of neutrons (neutrally charged nucleons) and alpha particles (ionized helium nuclei) when properly excited by the incident deuteron/tritium ion beam 10. It can be appreciated, however, that other types of targets and materials may be used in this application.
  • Neutrons are created in the target(s) according to the following exemplary reactions: iH 2 + iH 3 - 2 He 4 + on 1 + 14 MeV
  • the energy of the incident deuteron/tritium ion beam 10 must be sufficient to overcome any coulombic interaction with the positively charged nuclei of the target material atoms. Deuteron/tritium ion energies of 0.05 MeV or greater have been found sufficient for this purpose.
  • Fast neutrons having energies on the order of 14 Mev are utilized to bombard the test subject 18 in the present embodiment due to their desirable scattering properties (i.e., inelastic scattering with nuclei) and ability to penetrate significant thicknesses of common substances such as steel, soil, sand, lead, earth, and slabs of water up to approximately 50 cm in thickness (1/e interaction length).
  • the cross section (in mbarns) for gamma production in C, N, and O by 14 MeV neutrons is nearly independent of the neutron energy at that energy level; thus, the relative concentrations of these elements can be obtained to a high degree of accuracy without knowing the actual collision energy.
  • neutron energy levels other than 14 MeV may be used based in the present invention on the desired system operating characteristics.
  • the neutron and alpha particle beams 14, 16 released by the target are distributed spatially throughout a given solid angle ⁇ (measured in steradians) which is related to the angle of incidence of the charged particle beam to the target, the axis of each beam (corresponding to the highest neutron or alpha particle flux) being substantially co-linear with the other, yet opposite in direction relative to the target 18 (see Fig. 1).
  • Each target may be either fixed or independently steerable (adjustable) in relation to the excitation beam 10 and test subject 20 via a conventional electromechanical positioning device 21, although it can be appreciated that any variety of arrangements may be used.
  • Such positioning devices may be manually controlled, or alternatively automatically controlled via inputs such as those from the signal processing components described later herein. In this fashion, the resulting neutron and alpha particle beams 14, 30 may be adjusted to provide the desired neutron/alpha flux in a given solid angle, such as for scanning purposes.
  • alpha particle detection is accomplished via an array 34 of scintillation or comparable detector elements 36 having a known spatial relationship to each other.
  • Fig. 3 shows an exemplary configuration consisting of a square array (8x8) of 64 discrete detector elements. Each of the 64 detector elements is viewed by one photomultiplier ("PM") tube or by one of the 64 "segmented anodes" built into one large PM tube, each anode acting as an independent counter.
  • This array 34 is placed in a known position relative to the target(s) such that each detector element subtends a given solid angle ⁇ with respect to its associated target 18.
  • borated polyethylene elements 38 are used to shield personnel and equipment adjacent to the apparatus from the deuteron/neutron/alpha radiation generated within the system, and further to collimate the neutron beam 14 generated by the target(s) if desired as shown in Fig. 1.
  • the present embodiment may be adapted to a variety of different applications and geometries including, inter alia, land mine detection and identification, artillery shell analysis, or as shown in Fig. 2a, analysis of airport baggage carriers for contraband.
  • the present invention may be readily adapted to a land mobile vehicle of the type well known in the mechanical arts (Fig. 2b) which is either controlled directly by an operator, or remotely controlled in order to facilitate surveying large portions of terrain with relative efficiency.
  • the excitation beam produced by the aforementioned source 15 contains a plurality of atomic species including deuterons and tritium ions, each having different atomic mass number.
  • a charged particle passing through a magnetic field experiences a deflecting force, the magnitude and direction of which is determined by the particle's charge and mass, and the strength and direction of the magnetic field vector at that given location.
  • particles of different atomic mass but of the same kinetic energy can be deflected along curved paths of different radii utilizing the same magnetic field.
  • two atomic species are deflected using a perpendicular magnetic field 40 in such a manner as to permit impact of the different species on two different targets 18.
  • the magnetic field is generated through use of a conventional or superconducting electromagnet 42 of the type well know in the art which is placed in direct proximity to the excitation beam path 10, although other methods and arrangements (such as electrostatic depletion) may be utilized with equal success.
  • the charged excitation particles strike two spatially disparate targets of the same construction as previously described, thereby permitting both resulting fast neutron beams 14 to be directed toward the same test object or area simultaneously.
  • This "binocular" apparatus permits enhanced spatial resolution of the gamma-emitting chemical compound within the test subject via triangulation; i.e., the emission location is fixed by computing the intersection of two lines (or subtended solid angles) within the test subject 20. This way, the usual determination of the Z-axis coordinate by measuring time-of-flight of each neutron is avoided and precise X,Y,Z values are obtained directly. Spatial resolution on the order of 1 cm or less is practically achievable using, inter alia, the binocular apparatus of the present invention.
  • the excitation beam 10 may be split into multiple beams and directed into multiple targets using (i) an electrostatic septum, as is well known in the field of particle physics, or (ii) by broadening the beam spatially and utilizing multiple targets to intersect a fraction of the beam, as shown in Fig. 5.
  • the beam 10 may be comprised of one or multiple species.
  • two or more deuteron sources 15 are utilized to excite a plurality of targets 18, thereby inducing the emission of neutrons for the targets.
  • This embodiment obviates the need for the application of the aforementioned magnetic field 40 (and the supporting structure necessary to generate such field) or broad particle beam.
  • the multiple deuteron sources 15 are physically placed so as to optimize the ability of the device to spatially locate the chemical compound(s) of interest within the test subject 20, and are similarly operated in either a continuous ("long") or modulated mode (such modulated pulses being substantially coincident or staggered in time, depending on the desired properties of the system).
  • FIG. 7 another embodiment of the chemical compound detection, location, and analysis apparatus of the present invention is shown.
  • a plurality of gamma detectors 26 are placed in known physical proximity to the test subject, and one or more alpha particle detectors (not shown) are placed in general proximity to the target(s).
  • the target is excited by a DC deuteron pulse of known duration (typically 0.1 to 20 sec), and the timing difference between a given alpha particle detection event (or series of events) as detected by the alpha detectors 28 and the induced prompt gamma event(s) detected by the gamma detectors 26 is measured to provide a coarse determination of the axial (i.e., line-of sight, or "Z-axis") distance 44 between the activated chemical compound and the target 18.
  • axial i.e., line-of sight, or "Z-axis
  • Such determination is performed by a digital signal processor (or microprocessor) running an algorithm in the present embodiment; although other arrangements may be used.
  • a digital signal processor or microprocessor running an algorithm in the present embodiment; although other arrangements may be used.
  • Known neutron and alpha particle velocities, electronically-induced detection delays, prompt gamma emission delays, and excitation beam pulse duration are considered in order to produce this coarse estimate.
  • Further refinement of the coarse axial position previously calculated, as well as an off-axis (i.e., "X-Y") position determination are provided through subsequent multi-node geometric analysis (using any number of lines of position, such as triangulation) of data provided by the aforementioned gamma detector array 26.
  • the location of a prompt gamma emitter i.e., chemical compound
  • This arrangement also has the advantages of not having to measure neutron time-of-flight (TOF) or neutron emission/incidence angle.
  • An array of alpha particle detectors such as that shown in Fig. 3 and previously described herein is formed in general proximity to the neutron-generating target(s) previously described.
  • Pre-selected individual gamma spectral lines are electronically correlated with each alpha detector array element 36 by the analyzer 39 to form a plurality of parallel coincidence circuits.
  • gamma detection events remaining in the post-filtration gamma spectrum are correlated with alpha detection events for each alpha detector array element using a nominal 10 msec, gating window.
  • approximately twenty (20) different discrete gamma lines from one gamma counter 37 and detector 26 are selected and electronically placed in coincidence with signals from each of the 64 elements of the alpha detector array 34.
  • This arrangement produces a large number of parallel coincidence channels.
  • a set of four gamma detectors 26 and 64 alpha detector elements 36 are used.
  • This highly parallel coincidence circuit structure of the present invention permits the processing of a substantially increased number of prompt gamma events, since only those events correlating to the desired twenty or so spectral lines (C:N:O in the present embodiment) need be correlated to events detected by the alpha array 34, and such events are processed with a high degree of parallelism.
  • a higher incident neutron flux 14 (on the order of 10 9 to 10 n n s-4pi) may be used as compared to prior art systems using detector-detector coincidence (and maximum neutron fluxes on the order of 10 6 n/s-4pi), and significantly less time is ultimately required to identify and analyze a given compound under the same test conditions.
  • precise gamma energy determination is important in the present invention in order to identify the parent atom of gamma rays chosen for analysis.
  • Several factors influence the selection of gamma ray peaks and spectral lines used for the analysis. These factors include (i) gamma energy; (ii)cross section; (iii) cascade vs.
  • 38,400 coincidence circuits are formed.
  • each coincidence circuit in the present embodiment is provided a parallel coincidence circuit with an artificially imposed delay to account for the aforementioned "accidental" coincidences. This amounts to an additional 19,200 coincidence circuits.
  • the total number of coincidence circuits used in this second embodiment is 38,400 (19,200 + 19,200).
  • Figs. 9 through 14 an improved gamma ray detection, filtration, and analysis apparatus and method is described.
  • high purity Germamum (Ge) crystal detectors (HPGDs) 26 are used to detect prompt gamma ray emitted from within the test subject.
  • the Germanium detectors provide enhanced gamma energy resolution (on the order of 0.1%) unlike the more common Sodium Iodide detectors (6-10%) typically used in prior art systems, thereby allowing discrimination of the multiple C:N:O or other spectral "lines”.
  • Fig. 9 illustrates a typical gamma spectrum obtained using a prior art Nal detector.
  • the high-resolution gamma spectrum 50 produced from the Ge detectors of the present invention provide greatly enhanced energy resolution, as evidenced by the narrow spectral peaks or lines illustrated in Figs. 10 and 11.
  • the gamma spectrum 50 is electronically converted to a digital representation (Fig. 14) using a conventional analog-to-digital (A/D) converter 31 of the type well know in the electronic arts.
  • A/D analog-to-digital
  • Each spectral line 52 is assigned a discrete binary value ("bin") representing its gamma energy level.
  • spectral lines (bins) associated with carbon, nitrogen, and oxygen for the chosen type/energy of incident particle stream are then identified as decribed in Appendix A and further processed, while other unrelated lines 54 are electronically filtered (using, for example, a conventional digital filter) 33.
  • three (3) coincidence circuits are used per each line.
  • amplitudes of each of the aforementioned approximately 20 spectral lines associated with C:N:O are determined through analysis of three equal 4 KeV bandwidths within the spectral line; namely, one "peak" bandwith and two "shoulder” bandwidths (see Figs. 12a and 12b).
  • the peak-to-shoulder difference(s) are used to determine the amplitude of the peak for purposes of further analysis in the Dalitz plot.
  • Germanium detectors characteristically have a slower response time than other types of detectors (such as Sodium Iodide crystal), thereby having a correspondingly lower temporal resolution.
  • HPGDs can process a maximum event rate (including random events) on the order of 50,000 counts/sec. This slower response rate is compensated for in the present invention through the use of electronic processing of signals from the detector which effectively varies the response time constant to a lower value.
  • that portion of the HPGD signal corresponding to a fraction of the rise time of the gamma event is used to determine the time resolution.
  • This rise time is typically in the range of 1.5 to 4 ns, and is measured from a point 10% above the baseline prior to the event to a point 10% below the peak value of the event, as shown in Fig. 13.
  • the rise time signal processing is accomplished via a constant fraction discriminator (CFD) which is well known in the signal processing and nuclear detection arts.
  • CFD constant fraction discriminator
  • Charge collection in the present embodiment is further stopped electronically ("gated") at 20 ns.
  • the effective maximum count rate of the Ge detector is substantially increased, since the detector "dead time” is reduced, and temporal resolution increased.
  • Figs. 10 and 11 are exemplary gamma spectra which depict the effect of gating on spectra obtained from a given sample of a chemical compound.
  • FIG. 10 illustrates a gamma spectrum obtained from a urea specimen using a nominal 40 ns gating interval, and background subtraction. Background subtraction is performed in the present embodiment using the method described in Appendix D hereto, with reference to Fig. 12b.
  • Fig. 11 illustrates a gamma spectrum of the same urea specimen taken using a 5.9 ns gating interval, with no background subtraction (background subtraction is precluded in the spectrum of Fig. 11 due to the narrow gate).
  • SNR signal-to-noise ratio
  • Figs. 15a and 15b an improved method for identifying chemical compounds using particle activation is described.
  • the filtered digital gamma detector output signal described in the preceding paragraph is input to a signal processing apparatus (such as the aforementioned digital signal processor) running an improved identification/classification algorithm that reduces a three-dimensional problem to a two-dimensional representation.
  • This algorithm is based on the well known "Dalitz Triangle" 60, 62, which correlates the concentrations of three elements within a compound. See Appendix F. Specifically, the length of the normal to each side of the equilateral triangle 60, 62 is proportional to the square of the atomic density of each of the three elements.
  • the algorithm of the present invention takes the filtered digital gamma spectrum 56 which is collected over a given integration interval, computes the relative proportions of the constituent elements based on the binary representations of amplitude of the spectral lines (which correlates to the number of prompt gamma events detected), and mathematically generates a vector 64 normal to the appropriate side of the triangle for each element being analyzed. See Fig. 15b.
  • the point of intersection 66 (or closest point of approach) for all three normal vectors is calculated using well known geometric techniques, thereby defining a single point or range.
  • This point/range is then compared to a "library" of points/ranges associated with various known chemical compounds of interest (such as may be stored in tabular form within a conventional random access memory (RAM)) to identify the compound detected.
  • a "library" of points/ranges associated with various known chemical compounds of interest such as may be stored in tabular form within a conventional random access memory (RAM)
  • Subsequent spectra collected from the gamma detectors over a given sample period are then used to statistically increase the confidence level of the identification result.
  • Statistical error bands 68 (such as a given number of standard deviations on a normal or Gaussian distribution) may be used to establish confidence criteria.
  • Such data may also be displayed visually to the system operator, thereby providing him a visual indication of the confidence of a given analysis.
  • the Dalitz triangle may be displayed in graphical form, with the library of known chemical compounds displayed as discrete points within the triangle 60,62.
  • T d a discovery time constant
  • This time constant is a measure of the time required to perform a chemically specific identification of a certain mass of chemical compound at a certain distance from the particle source (target), and certain distance between the chemical compound and gamma detector(s), with a prescribed statistical confidence level about the relevant point on the aforementioned Dalitz triangle 60,62.
  • the relevant distances to the chemical compound and detector(s) are measured or calculated, and the mass M determined as shown in step 702 of Fig. 16.
  • the desired confidence level is selected in step 704. This confidence level is mathematically determined through statistical analysis of the spectral data produced on successive operation of the system during a given testing interval, as previously described.
  • step 706 The known mass of a given chemical compound is then analyzed in step 706, thereby experimentally determining T d for this set of constraints.
  • step 708 the time constant is optionally normalized. For example, the system may require 5 seconds to identify a 1 kg sample compound to a 95% level of confidence at a detector/sample distance of 1 meter in dry air at STP; this nominal or "baseline" value may be normalized to 1 second if desired.
  • steps 710 and 712 the mass and/or environmental test factors (such as location of the mass, relative humidity, etc.) are varied and the discovery time again measured under these new conditions.
  • steps 710, 712 may be repeated a number of times when, for example, incrementally varying one parameter, or varying many parameters at once, as described further below.
  • correction or calibration factors are calculated for the system in step 714. For example, if the system was normalized using a 1 kg mass in dry air at STP, operation of the system in humid air at lower temperature (assuming comparable mass and detector geometry) would produce a higher value of Td. This higher value of T d is then ratioed with the nominal T d to produce a correction factor for operation of the system in humid/low temperature environments. Tables or curves may also be constructed detailing the response of the system as a function of varying system parameters and test conditions, or salient combinations of parameters.
  • experimentally generated values of T for one system may also be compared to those generated for another system in order to determine the relative efficacy (merit) of the two systems at chemical identification and location.
  • This method is very useful in standardizing the comparison of two systems of differing operating principle; at present, no system of comparison exists, hence manufacturer's claims of performance can not be directly compared.
  • Such "figures of merit” may be developed as a function of various critical parameters (such as ambient temperature, humidity, interposed shielding, etc.) to assist in determining the best instrument/technique (or combination thereof) to apply in a given testing or field application.
  • the gamma energy peaks produced during the inelastic collision between fast neutrons and various atomic nuclei have a typical energy range of 0.100 to 18 MeV.
  • the general contention in explosive detection has always been to detect the major components of explosives; that is, carbon, nitrogen, and oxygen. Therefore, the following discussion will focus on the gamma ray spectra of these constituent elements. It should be noted, however, that this principal is potentially applicable to many other elements including chlorine, phosphorus, and sulfur.
  • HPGDs Size and efficiency limitations of HPGDs limit the upper range of detectable gamma energies. For example, based on laboratory measurements with at 45% efficient N-type HPGD, a ceiling of 5.5 - 6.2 MeV prohibited the use of any gamma peaks about 6.129 MeV. The gamma energy peak selection process was therefore limited to gamma counts emanating below 6.2 MeV. The 5.104 photo-peak of nitrogen produced 49 counts ⁇ 14 using this detector. In comparison, an 81% N-type detector produced an energy ceiling of 7 MeV, with the equivalent 5.104 nitrogen photo-peak (using equivalent neutrons) producing 197 counts ⁇ 21.
  • the floor for gamma peak selection is at least in part based on the identity of interrogated material, and is on the order of 1.6 ⁇ .5 MeV for most applications.
  • the probability of inducing a specific gamma ray depends on the binding forces within the nucleus of each atom. This probability is the atomic cross section or size (effective) for the production of gamma rays and is measured in barns (10 "24 cm). Established cross sections for carbon, nitrogen, and oxygen are used to establish a ratio between the number of carbon, nitrogen, and oxygen atoms.
  • Carbon is somewhat unique with respect to the present analysis.
  • Nitrogen and oxygen have many photo-peaks from 1.6 to 7.2 MeV.
  • the cross-section of the oxygen photo-peak at 6.129 MeV is 101 mb.
  • Nitrogen has three detectable photo-peaks at 2.312, 3.948, and 5.104 MeV with cross sections of 7.8, 3.5, and 31 mb, respectively.
  • the minimum detectable cross section of a photo-peak is 5 mb (cascades often increase the observable cross section of photo-peaks, see section A.3 below).
  • cascade effects increase the number of possible energy peaks.
  • Cascade effects are excitations of energy level that are not sufficient enough to cause a direct drop to the lowest energy state; and as a result, cascade peaks are produced from the systematic drop of photons from excited energy states to more stable ones.
  • the 2.748 MeV oxygen cascade is produced by the excitation of the 8.,872 MeV photo-peak and its subsequent drop to the 6.129 MeV energy level. The photon then drops from the 6.129 MeV (second photo-peak) to the ground state.
  • the excitation of higher energy levels produce more gamma energy peaks and hence a greater probability of detection.
  • data for cascade cross sections are not readily available.
  • Cascade peaks represent over 50% of the total spectrum for oxygen and nitrogen. In order to maximize count rate, it is prudent to utilize cascade peaks to avoid the problems addressed by gamma energies outside the 1.6 to 7.2 MeV range, avoid the use of low cross section peaks, and finally circumvent the problem of proximity and overlap.
  • Proximity of gamma ray peaks is the simpler of the two cases.
  • One of the advantages of using HPGe detectors is its increased resolution (on the order of 0.1%) at 622 KeV. For instance, a HPGe detector can discriminate between a 5.156 MeV aluminum signal from a 5.104 MeV nitrogen signal. Nal detectors have resolution of roughly 10% at 722 KeV and cannot discern between many peaks in the spectrum. Proximity is an indication of the increased resolving power of the HPGD and is treated as an important tool for discrimination.
  • A.5 Single/Double Escape Peaks Another important factor in determining which gamma energies are used for analysis is the production of single and double escape peaks. Pair production is the result of electron/positron annihilation with the concomitant release of 511 KeV (0.5MeV) quanta in roughly opposite directions. This process occurs in the matrix of the crystal lattice and is a function of the detector size.
  • the most prominent single escape peak is from the oxygen 6.129 MeV peak.
  • One sharp peak is produced 0.511 MeV lower at 5.618 MeV.
  • a second escape peak is also produced 1.022 MeV downstream at 5.107 MeV.
  • the nitrogen photo-peak at 5.104-5.107 peak is greater in intensity than the 5.618 MeV peak; this is a clear indication that there is a signal from nitrogen as well as oxygen.
  • the cross section of the first and double escape peaks are 70% and 31% of the 6.129 MeV peak.
  • the net number of counts in the 5.107 MeV double escape, contributed from oxygen at 6.129 MeV is 31% of net counts in 6.129 MeV oxygen photo-peak.
  • N may arise from a variety of sources including air surrounding the test specimen and apparatus; in one m 3 of air, there is 925 grams of nitrogen and substantial oxygen.
  • the mass of the urea test sample is also known (5 kg in the present example) it is also possible to calculate the ratio of "moles of sample” to "moles of noise" (molecular weight of air ⁇ 29/gmole and urea 60.1 g/mole); specifically 6.87%.
  • Equation B.l yields a correction value of 5.36% for nitrogen and 1.44% for oxygen. In other words, the net peak counts have to be corrected to account for extraneous signals from nitrogen and oxygen in air.
  • relative detector efficiency i.e., that efficiency relative to a particular chosen energy value
  • relative efficiency is that only a quantitative atometric ratio of elements is needed, and not atomic content from one species outright. For instance, one does not have to solve implicitly for n (atomic density). Instead, if the ratio of atomic density is used, one may set C:N:O equal to the ratio of i to « 2 where the detector efficiencies are relative to each other. Table C.I lists experimental numerical values of the relative efficiency of a 80% N-type HPGe.
  • relative efficiency in Table C.I is based on the 2,300 KeV value.
  • the ratio of relative intensity increases 45% from 2,300 KeV to 4,400 KeV and 9% from 4,400 KeV to 5,100 KeV.
  • ROI Regions of Interest
  • the background on the upstream (lower energy) side of the peak is calculated as the average of the first three channels of the ROI.
  • the channel number for this background point is the middle channel of the three points.
  • Background on the downstream (higher energy) channel side of the peak is calculated as the average of the last three channels of the ROI.
  • the channel number for this background point is also the middle channel of these latter three points.
  • the two background points on each side of the peak form the end points of the straight-line background.
  • a g the gross counts in the ROI
  • a ag the gross counts in the ROI
  • the error in the net adjusted area is the square root of the sum of the squares of the error in the adjusted gross area and the weighted error of the adjusted background.
  • the background error is weighted by the ration of the adjusted peak width to the number of the channels used to calculate the adjusted background.
  • gamma information is gathered using an average value of peak width, location, and energy (Appendix A).
  • the gamma lines are systematically chosen for background subtraction (Appendix D). Each gamma line is subjected to numerous fitting routines until the lowest error value is repeated. Finally, corrections are made for extraneous noise, detector efficiency, and gamma attenuation (Appendix C).
  • the aforementioned data for one element are related to the number of gamma counts of another — such as carbon to oxygen — from the following established formula:
  • r eff , ⁇ a bs and v abS are detector efficiency, gamma and neutron attenuation factors, respectively, and ⁇ is the cross section.
  • r eff includes solid angle subtended by the detector at 0.25 m (according to the relevant IEEE standard).
  • the number of neutrons was calculated using the ratio of alpha to neutron counting rate:
  • n atomic density
  • V volume
  • the cross product of atomic density and volume is atoms (n).
  • Equation E.l may be rewritten to cancel out factors in the following form:
  • Equation E.5 can be solved for n.
  • Equation E.6 Determination of the C:N:O ratio is based on Equation E.6.
  • ⁇ atten is a reciprocal because its effects decrease gamma value below 2,300 KeV and increase values above 2,300 KeV.
  • E.6 may be written as follows:
  • nnurog n (76.5 x 1.57)/(32 x 1.31 ) (Eqn. E.8)
  • noxygen (127 x 1.41)/(101 x 1.74) (Eqn. E.10)
  • the Dalitz Plot (or "A-plot") is a two dimensional graphical representation of three dimensions of information; namely, the carbon, nitrogen and oxygen ratio of explosives and other contraband. See Figs. 15a and 15b above.
  • the normalized atomic densities of carbon, C, and oxygen, O' are represented by perpendicular distances-squared from the other two sides of the triangle.
  • This information may easily be translated into an A-plot by the following steps (using urea as an example):

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Abstract

Dispositif et procédé permettant de détecter, de localiser et d'analyser, par activation de particules subatomiques, des composés chimiques contenus dans un objet à tester. Une source d'excitation excite une cible de façon à produire simultanément des faisceaux dont chacun est constitué de certaines espèces subatomiques, tels que neutrons rapides et particules alpha. L'objet à tester (et les composés chimiques qu'il contient) est irradié par les neutrons rapides, ce qui stimule l'émission de rayons gamma instantanés. Des détecteurs gamma et alpha sont positionnés par rapport à l'objet à tester et à la cible de façon à détecter les rayons gamma instantanés et les particules alpha émis en coïncidence substantielle, et la relation physique connue entre les faisceaux est utilisée pour localiser spatialement le composé chimique activé. Les spectres d'énergie dérivés des détecteurs gamma sont filtrés de façon à éliminer tous les artefacts spectraux non pertinents, ce qui 1) permet de créer une pluralité de canaux de coïncidence parallèles ; 2) diminue le traitement de signaux ultérieur nécessaire ; et 3) augmente globalement la précision et le rendement des processus d'identification et d'analyse du composé chimique. L'invention concerne également un mode de réalisation multifaisceau/multicible, qui permet une localisation spatiale encore plus précise. Elle concerne aussi un procédé qui permet d'étalonner et d'évaluer l'efficacité du système avec divers paramètres d'analyse.
PCT/US1999/003491 1998-02-18 1999-02-17 Procede et dispositif permettant de detecter, de localiser et d'analyser des composes chimiques par activation de particules subatomiques Ceased WO1999049311A2 (fr)

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AU49516/99A AU4951699A (en) 1998-02-18 1999-02-17 Method and apparatus for detecting, locating, and analyzing chemical compounds using subatomic particle activation (atometry)
EP99933468A EP1071948A2 (fr) 1998-02-18 1999-02-17 Procede et dispositif permettant de detecter, de localiser et d'analyser des composes chimiques par activation de particules subatomiques
CA002321063A CA2321063A1 (fr) 1998-02-18 1999-02-17 Procede et dispositif permettant de detecter, de localiser et d'analyser des composes chimiques par activation de particules subatomiques
JP2000538230A JP2002507746A (ja) 1998-02-18 1999-02-17 亜原子粒子による活性化法を用いた、化合物の検出、位置決めおよび分析の方法および装置

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EP1448980A4 (fr) * 2001-06-18 2006-11-02 Hienergy Microdevices Inc Procede et appareil de microscopie neutronique a imagerie stoechiometrique
WO2016036264A1 (fr) 2014-09-07 2016-03-10 Uniwersytet Jagielloński Dispositif et procédé de détection non effractive de matières dangereuses dans l'environnement aquatique

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JP5366394B2 (ja) * 2007-12-21 2013-12-11 ハミルトン・サンドストランド・コーポレイション 試料に含まれる化合物を検出するシステムおよび方法

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US5323004A (en) * 1989-05-08 1994-06-21 Scientific Innovations, Inc. Nuclear resonances in activation analysis, and particularly, its application to detection of nitrogen based explosives in luggage
US5098640A (en) * 1990-01-10 1992-03-24 Science Applications International Corporation Apparatus and method for detecting contraband using fast neutron activation
US5200626A (en) * 1990-03-28 1993-04-06 Martin Marietta Energy Systems, Inc. Hidden explosives detector employing pulsed neutron and x-ray interrogation
US5247177A (en) * 1990-04-09 1993-09-21 The State Of Israel, Atomic Energy Commission, Soreq Nuclear Research Center Detection of nitrogenous material
GB9301983D0 (en) * 1993-02-02 1993-03-17 Atomic Energy Authority Uk Analysis using neutrons
US5557108A (en) * 1993-10-25 1996-09-17 T+E,Uml U+Ee Mer; T+E,Uml U+Ee May O. Integrated substance detection and identification system
JPH10510621A (ja) * 1994-10-31 1998-10-13 ロックヒード マーティン スペシャルティー コンポネンツ インク． 中性子問合せ及びｘ線撮像の組合せを用いた、爆発物を検出するための検査システム及び空間解像技術
US5784430A (en) * 1996-04-16 1998-07-21 Northrop Grumman Corporation Multiple station gamma ray absorption contraband detection system
DE19622758A1 (de) * 1996-06-07 1997-12-11 Philips Patentverwaltung Verfahren zur Detektion eines Körpers innerhalb eines Untersuchungsbereichs und Anordnung zur Durchführung des Verfahrens

Cited By (2)

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Publication number Priority date Publication date Assignee Title
EP1448980A4 (fr) * 2001-06-18 2006-11-02 Hienergy Microdevices Inc Procede et appareil de microscopie neutronique a imagerie stoechiometrique
WO2016036264A1 (fr) 2014-09-07 2016-03-10 Uniwersytet Jagielloński Dispositif et procédé de détection non effractive de matières dangereuses dans l'environnement aquatique

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