EP0746774A1

EP0746774A1 - Detection of explosive and narcotics by low power large sample volume nuclear quadrupole resonance (nqr)

Info

Publication number: EP0746774A1
Application number: EP92916035A
Authority: EP
Inventors: Michael L. 4337 Taney Avenue BUESS; Allen N. Garroway; Joel B. Miller
Original assignee: US Department of Navy
Current assignee: US Department of Navy
Priority date: 1991-07-16
Filing date: 1992-04-24
Publication date: 1996-12-11
Also published as: WO1993002365A1; CA2113558A1; CA2113558C; EP0746774A4; JP2002509601A

Abstract

The sensitive detection of explosives and narcotics by nuclear quadrupole resonance (NQR) is performed at low rf power by assuring that the rf field strength is larger than the local magnetic field. Additionally, it has been recognized that signal-to-noise ratio of a signal induced by a specimen of fixed size decreases by only the square root of the coil size. Thus, rather than scaling power linearly with coil size, as conventionally done to maintain the same rf field intensity, the power needs only be increased by the square root of the increased coil size to assure maintenance of the same signal to noise ratio. This technique permits the use of larger coils than previously used. The invention is useful for both volume coils and surface coils.

Description

DETECTION OF EXPLOSIVE AND NARCOTICS BY LOW POWER LARGE SAMPLE VOLUME NUCLEAR QUADRUPOLE RESONANCE (NQR)

Background of the Invention

Field of the Invention The present invention is directed generally to a method and an improved system for detecting nitrogenous explosives or narcotics by nuclear quadrupole resonance (NQR) , and more specifically, to a lower power method for detecting those materials.

Description of the Prior Art

In order to limit the unrestricted flow of explosives and narcotics, it is desired to detect sub-kilogram quantities of those materials in monitoring stations. Most military explosives and narcotics share common features: they are crystalline solids containing nitrogen. Presently, the explosive detections system and methods cannot reliably detect sub-kilogram quantities of military explosives against a background of more benign materials. In conventional vapor- based systems, dynamites and contaminated explosives may be detected. However, military explosives such as hexhydro-1,3,5- trinitro-s-triazene (commonly referred to as RDX and 2,2- bis[ (nitroxy)methyl]-l,3-propanediol, dinitrate (commonly referred to as PETN) are not reliably detected by the conventional vapor base systems especially when counter-measures are taken to reduce the effluent vapor and particles. Thermal neutron systems, which are ¹⁴N detectors, can detect relevant quantities of explosives. Unfortunately, conventional thermal neutron analysis systems frequently alarm on nitrogen- containing plastics. High false alarm rates are produced for inspected bags containing a few bomb equivalents of nitrogen in a benign form since the conventional thermal neutron analysis systems are sensitive only to the nuclear cross sections and not to any details of the particular chemical

SUBSTITUTE SHEET environment of the detected nitrogen nuclear. Hence the false alarm rate is inherently high, even with some spatial discrimination. Also, nuclear magnetic resonance (NMR) has been considered for detecting explosives. Because a large magnetic field is conventionally required for NMR, magnetically recorded data would be undesirable altered and other magnetizable materials could be damaged. Furthermore, the^' conventional non-vapor methods and systems are not suitable for inspecting people. The parent application of the present invention, Buess et al., DETECTION OF EXPLOSIVES BY NUCLEAR QUADRUPOLE RESONANCE, Ser. No. 07,704,744, Navy Case No. 72,625, filed May 23, 1991 (the entirety of which is incorporated herein by reference) , discloses a method and system for NQR detection of explosives. Recited advantages of NQR for explosives detection are:

(i) Specificity: the NQR resonant frequency of a quadrupolar nucleus in a crystalline solid is quite well- defined. Most explosives of interest contain nitrogen and are crystalline solids. Most nitrogen found in the contents of airline bags is in a polymeric form, with associated broad, weaker NQR resonances and generally at frequencies other than the characteristic frequencies of the explosive. NQR is sensitive to the chemical structure, rather than just the nuclear cross-section, as in the thermal neutron analysis approaches. For NQR, false alarms from other nitrogenous materials will be far less of a problem than in nuclear-based detection techniques.

(ii) Sensitivity: though NQR is not a very sensitive spectroscopy, the parent disclosure describes techniques to make the response more sensitive to the desired explosive and less sensitive to interfering signals. Sensitivity is a function of coil geometry and coil size. The invention described in the parent disclosure has demonstrated sensitivity to detect the equivalent of sub- kilogram quantities of explosive near a brief case-sized meanderline coil and substantially less explosives in a small solenoidal coil of 25 mm diameter in a few seconds. (iii) Localization: one of the novel features of the NRL approach is to localize the transmitting field and the receiver by a specialized surface coil, never previously used for NQR. One type of surface coil, the -meanderline¹ coil, localizes the sensitive inspection region to a well- defined region. Furthermore, the electrical and magnetic fields of the meanderline coil fall off very rapidly with^' distance, so that a person can be scanned by an NQR detector without depositing substantial rf power into the body.

Summary of the Invention

It is an object of the present invention to safely detect small quantities of nitrogenous explosives and narcotics within a large volume of material to be searched using low power techniques.

It is another object of the present invention to provide a system for detecting nitrogenous explosives and narcotics by nuclear quadrupole resonance over a large volume, at low power, less intense rf fields.

These and other objects are achieved by recognizing that the strength of the applied rf field need only be at least equal to the strength of the local magnetic field due to dipole-dipole interactions. A corollary of this principle is that the signal-to-noise ratio of a signal induced by a specimen of fixed size decreases by only the square root of the coil size, and using this recognition in the detection of explosives and narcotics by NQR. Thus, rather than scaling power linearly with coil size, as conventionally done to maintain the same rf field intensity, the power can be increased significantly less. Specifically, the power need only be increased by the square root of the increased coil size to assure maintenance of the same signal to noise ratio. This approach permits the use of larger coils than previously used.

The approach is useful for both volume coils and surface coils.

For example, a more conventional approach would require an rf peak power of about 6 MW for a 300 liter inspection volume. In contrast we have achieved detection with power

SUBSTITUTE SHEET levels of 400 watts. A 5 watt meanderline coil NQR explosives detector is feasible for use on people: the prior approach would have necessitated about a peak power of about 30 kW.

Detailed Description of the Preferred Embodiments

The technique utilized according to the present invention is pure nuclear quadrupolar resonance as taught in the previously mentioned Buess et al. patent application. Excitation and detection may be performed by any means known in the art, for example, a surface coil, such as a meanderline coil or a more conventional 'volume¹ coil such as a cylindrical or rectangular solenoid, a toroid, or a Helmholtz coil. Pure NQR is typically performed in zero magnetic field: no magnet is required.

As taught in the parent Buess et al. patent application the specimen is irradiated with a train of radio-frequency (rf) pulses whose frequency has been chosen to be near to the known ¹N NQR frequency of the explosive or narcotic. For example,

RDX has resonance lines near 1.8, 3.4 and 5.2 MHz, while

PETN-s NQR resonances are near 0.4, 0.5, and 0.9 MHz. Any irradiation sequence useful in NQR processes may be used according to the present invention. One preferred irradiation sequence is the strong off-resonance comb (SORC) , described in lainer et al., J. Mole. Struct. , 58 , 63 (1980), (the entirety of which is incorporated herein by reference) in which the pulse separations are less than the spin-spin relaxation time

T₂, producing about one-half of the equilibrium magnetization after every pulse.

Conventionally, intense rf magnetic fields are used to excite the NQR lines and generation of such intense fields requires substantial rf power with associated possibility of depositing unacceptable amounts of power into the scanned objects. Power deposition can have unfortunate consequences for scanning of baggage and small cargo, wherein at some suitably high power level, damage to electronics may occur by over voltage or local heating through electrostatic coupling of the electric field or inductive coupling to the magnetic field. For scanning people, rf power deposition, primarily by eddy current loss, can pose a problem at these frequencies (1-5 MHz) . A detailed discussion of the effects of rf power and field strength values on articles and persons and the acceptable levels of exposure to rf energy is unnecessary here and beyond the scope of this disclosure. It is sufficient to state that an advantage of the present approach that average^' and peak rf power levels can be reduced by orders of magnitude below those used in prior practice. An rf field strength of B₁ applied near the resonance frequency nutates the spins (for a spin 1=1 nucleus) through an angle of 2γB.,t_w, where γ is the magnetogyric ratio of the nuclear spin and t_H is the pulse width. For a fixed nutation angle, an intense pulse has a shorter duration and, correspondingly, excites a broader region of the spectrum. Conventionally, one excites the NQR resonance with a pulse sufficiently long to cause the spins to nutate through about 119°, giving a maximum magnetization. On commercial NQR spectrometers in a laboratory setting, the pulses required to obtain 119° tip angle typically have widths of 20-50 μs and cover a bandwidth l/t_H of 50-20 kHz. The rf field strength B., used in such cases is therefore 10-25 gauss.

As part of the present invention, it was recognized that the magnitude of the rf field strength need only be larger or equal to the magnitude of the local magnetic field strength due to dipole-dipole contributions. Hence the necessary rf field strength B_1rnιn is of the order of l/γT₂ where T₂ is the spin-spin relaxation time due to dipolar decoupling. Therefore, for example, the strong off resonance comb excitation will work quite satisfactorily at such low rf intensity. For RDX-based explosives, the present invention has successfully utilized rf fields as low as 0.7 G (0.07 mT) . (The width of the ^UN NQR line is also partly determined by inhomogeneous interactions due to distribution of the quadrupolar coupling constants, induced by strain, impurities and variations in temperature. Such an inhomogeneous contribution to the width is not as important as the homogeneous contribution from the dipole- dipole coupling.)

SUBSTITUTE SHEET Therefore, although the prior art applies an rf field of a strength that is at least 100 times greater in magnitude than that of the local magnetic field, the present invention achieves successful NQR detection of nitrogenous explosives and narcotics by using a rf field strength to local field strength ratio of from 1 or about 1 to about 50, preferably as close as possible to 1. Typically, a ratio of about 2 to about 30, more^' typically a ratio of about 2 to about 20, and most typically a ratio of about 2 to about 10 is used. A second, related aspect of the present invention is the use of large volume sample coils: since only rather modest rf field strengths are required, a fixed rf power can irradiate a much larger volume by the present method. In a coil of effective volume V and quality factor Q, a pulse of power P creates a rf field strength B₁ proportional to (PQ/Vv₀)¹², where v₀ is the carrier frequency. By the principle of reciprocity, the signal-to-noise ratio obtainable from a given amount of sample will scale with the strength of B., per unit current. Hence, provided there is sufficient power to irradiate the NQR line, a specimen of fixed size will induce a signal which scales as (coil volume)^"12. For example the penalty in signal- to-noise ratio increasing coil volume by a factor of 15000 on comparing a 20 cm³ coil to a 300 liter coil volume is about 120. Thus, according to the present invention, one can irradiate, for example, a volume of about 300 liters and detect significant quantities of explosive in a reasonably short time with an rf peak power of 400 watts, the same peak power conventionally employed on a small 20 cm³ coil system. If one followed the more prior art approach of maintaining the same rf field intensity B_1f one would need to scale the power linearly with coil volume, necessitating an rf peak power of 6 MW for the 300 liter system, in contrast to the 400 watts used according to the present invention. In the present invention, the scaling of peak power with size can be significantly less than linear.

As the NQR transitions are induced by rf pulses, discussion so far has centered on the pulse or peak power which creates the (peak) rf magnetic field intensity. Peak power

SUBSTITUTE SHEET dictates not only the necessary power requirement of the rf transmitter, but also determines the peak voltages induced in the specimen. One must also be concerned with average power which also places some requirements on the rf transmitter and also determines the maximum power which is deposited into the scanned object. (It must be noted that most of the rf energy is dissipated in the coil by resistive losses, with only a^' fraction dissipated in the specimen through dielectric or eddy current losses. Furthermore, where power dissipation in the specimen may be a problem, there are other well-known rf shielding techniques which can reduce the fraction of the rf power actually dissipated in the specimen.) To appreciate the advantages of the present invention, consider scaling up the coil volume while keeping the rf peak power essentially fixed. For simplicity of argument, keep the nutation angle about the same in the large volume coil as in the small coil. Hence the rf pulse length will need to be increased in direct proportion to (coil volume)¹², and so the average power will increase by that same factor, provided the same pulse spacing is maintained. That is, the scaling of average power with size can be significantly less than linear, and in particular, may be between as low as proportionate to the square root of coil volume without significantly decreasing the signal to noise ratio. In the SORC sequence a typical rf pulse duty factor with short pulses spaced closer than the spin-spin relaxation time T₂ might be 0.2% for a small volume coil. To maintain the same nutation angle and the same spacing between pulses, a duty cycle of about 25% is then required for the 300 liter coil. For operating conditions with a peak power of 400 w, the average power dissipated in the small coil would be 0.8 W and, by the present invention, only 100 W in the 300 liter coil, far less than the 6 kW average power which would be dictated by maintaining the large rf magnetic field in the large sample coil. While the above description has focused on "volume coils", for the sake of simplicity, other types of coils, such as the circular surface coil, the pancake coil, the meanderline and other variants, may be successfully used in conjunction with the principles of the present invention.

SUBSTITUTE SHEET The improvement offered by the present invention to that disclosed in the parent patent application is that very large sample volumes can be inspected for explosives or narcotics by NQR, without a proportional increase in peak power or average power levels. In practice, suitcase-sized sample volumes can be inspected at rather modest peak and average rf power levels. Furthermore, this approach makes feasible the examination of^' people by large surface coils, such as the meanderline, or even ^■volume¹ coils such as a solenoid, as indicated below.

Obviously, many modifications and variations of the present invention are possible in light of the above teachings. It is therefore to be understood that, within the scope of the appended claims, the invention may be practiced otherwise than as specifically described.

SUBSTITUTE SHEET

Claims

ClaimsWhat is claimed is:

1. A method for detecting a class of explosives and narcotics^' containing nitrogen in a specimen by nuclear quadrupole resonance, comprising the steps of: (a) generating a train of radio frequency pulses having a predetermined frequency;

(b) transmitting said train of radio frequency pulses to a coil;

(c) irradiating the specimen with an rf field of predetermined strength in response to said train of radio frequency pulses transmitted to said coil at said step (b) , said specimen having a local magnetic field due to dipole- dipole contributions;

(d) detecting an integrated nitrogen signal in response to irradiating the specimen at said step (c) ;

(e) receiving said integrated nitrogen signal detected at said step (d) ;

(f) comparing said integrated nitrogen signal to a predetermined threshold value; and (g) signalling when said integrated nitrogen signal exceeds said predetermined threshold value; wherein the strength of said predetermined rf field and said local magnetic field is at a ratio of about 1:1 to about

50:1.

2. The method of claim 1, wherein the ratio of the strength of said magnetic field to the strength of said local field is about 1:1 to about 30:1.

3. The method of claim 2, wherein the ratio of the strength of said magnetic field to the strength of said local field is about 1:1 to about 20:1.

SUBSTITUTE SHEET

4. The method of claim 3, wherein the ratio of the strength of said magnetic field to the strength of said local field is about 2:1 to about 20:1.

5. The method of claim 3, wherein the ratio of the strength of said magnetic field to the strength of said local field is about 1:1 to about 10:1.

6. The method of claim 5, wherein the ratio of the strength of said magnetic field to the strength of said local field is about 2:1 to about 10:1.

7. A method according to Claim 1, wherein said step (a) generates said predetermined frequency of said train of radio frequency pulses to be near to a ¹⁴N NQR frequency of the type of explosive or narcotic to be detected.

8. A method according to Claim 1, wherein said step (a) generates said train of radio frequency pulses comprising a strong off-resonance comb of radio frequency pulses.

9. A method according to claim 1, wherein said coil is a meanderline surface coil for detecting the class of explosives and narcotics in the specimen at predetermined areas.

10. A method according to claim 1, wherein said coil comprises a localized coil for detecting the class of explosives and narcotics in the specimen at predetermined regions.

11. A method according to Claim 1, wherein said coil comprises a solenoidal coil for detecting the class of explosives and narcotics in the entire specimen.

12. A method according to Claim 1, wherein said coil comprises a toroidal coil for detecting the class of explosives and narcotics in the specimen at predetermined regions.

13. In a system for detecting a class of explosives and narcotics containing nitrogen in a specimen by nuclear quadrupole resonance, said system including: a first coil of predetermined size for irradiating the specimen with a train of radio frequency pulses of predetermined average power and frequency and detecting an integrated nitrogen signal in response to irradiating the^' specimen; pulse generating means for generating said train of radio frequency pulses; coupling means for transmitting said train of radio frequency pulses to said first coil and receiving said integrated nitrogen signal from said first coil; comparing means for comparing said integrated nitrogen signal to a predetermined threshold value; and an alarm for signalling when said integrated nitrogen signal exceeds said predetermined threshold value; the improvement wherein a second coil of a predetermined size larger than said first coil is substituted for said first coil, and said pulse-generating means is adapted so that the predetermined average power of said train of rf pulses generated thereby causes said first coil to irradiate said specimen with a train of rf pulses of an average power increased with respect to the predetermined average power irradiated by said first coil significantly less than in direct proportion to the linear increase in volume of said second coil with respect to said first coil.

14. The system of claim 9, wherein said pulse-generating means is adapted so that the predetermined average power of said train of rf pulses generated thereby causes said first coil to irradiate said specimen with a train of rf pulses of a average power increased with respect to the predetermined average power irradiated by said first coil in direct proportion to about the square root of the increase in coil volume.

15. A system for detecting a class of explosives and narcotics containing nitrogen in a specimen having a local magnetic field

SUBSTITUTE SHEET due to dipole-dipole contributions, by nuclear quadrupole resonance, said system including: a coil of predetermined size for irradiating the specimen with a train of radio frequency pulses of predetermined frequency and detecting an integrated nitrogen signal in response to irradiating the specimen; pulse generating means for generating said train of radio frequency pulses; coupling means for transmitting said train of radio frequency pulses to said coil and receiving said integrated nitrogen signal from said coil; comparing means for comparing said integrated nitrogen signal to a predetermined threshold value; and an alarm for signalling when said integrated nitrogen signal exceeds said predetermined threshold value; wherein said pulse-generating means causes said coil to irradiate said specimen with an rf field having a strength which is from about equal to the strength of the local magnetic field of said sample up to about 50 times the strength of the local magnetic field of the specimen.

16. The system of claim 15, wherein said pulse-generating means causes said coil to irradiate said specimen with an rf field having a strength which is from about equal to the strength of the local magnetic field of said sample up to about 30 times the strength of the local magnetic field of the specimen.

17. The system of claim 16, wherein said pulse-generating means causes said coil to irradiate said specimen with an rf field having a strength which is from about equal to the strength of the local magnetic field of said sample up to about 20 times the strength of the local magnetic field of the specimen.

18. The system of claim 17, wherein said pulse-generating means causes said coil to irradiate said specimen with an rf field having a strength which is from about equal to the strength of the local magnetic field of said sample up to about

SUBSTITUTE SHEET 10 times the strength of the local magnetic field of the specimen.

SUBSTITUTE SHEET