WO1997029356A1 - Procede et appareil de telemesure de densite - Google Patents

Procede et appareil de telemesure de densite Download PDF

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Publication number
WO1997029356A1
WO1997029356A1 PCT/US1997/002224 US9702224W WO9729356A1 WO 1997029356 A1 WO1997029356 A1 WO 1997029356A1 US 9702224 W US9702224 W US 9702224W WO 9729356 A1 WO9729356 A1 WO 9729356A1
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Prior art keywords
detectors
temperamre
source
density
photons
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PCT/US1997/002224
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English (en)
Inventor
Andrzej K. Drukier
Peter Volkovitsky
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Biotraces, Inc.
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Priority to EP97906575A priority Critical patent/EP0879410A1/fr
Priority to AU21230/97A priority patent/AU2123097A/en
Publication of WO1997029356A1 publication Critical patent/WO1997029356A1/fr
Priority to NO983601A priority patent/NO983601D0/no

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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
    • G01N23/02—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 transmitting the radiation through the material
    • G01N23/06—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 transmitting the radiation through the material and measuring the absorption
    • G01N23/12—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 transmitting the radiation through the material and measuring the absorption the material being a flowing fluid or a flowing granular solid
    • 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
    • G01N23/02—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 transmitting the radiation through the material
    • G01N23/06—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 transmitting the radiation through the material and measuring the absorption
    • G01N23/083—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 transmitting the radiation through the material and measuring the absorption the radiation being X-rays
    • G—PHYSICS
    • G01—MEASURING; TESTING
    • G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
    • G01N9/00—Investigating density or specific gravity of materials; Analysing materials by determining density or specific gravity
    • G01N9/24—Investigating density or specific gravity of materials; Analysing materials by determining density or specific gravity by observing the transmission of wave or particle radiation through the material

Definitions

  • the invention provides a method and apparatus for remote measurement of density of gas, fluids, solids or mixtures of the above.
  • the disclosed method of MP-densitometry allows for a densitometer which is transportable, low cost and uses only low activity sources, i.e. , license exempt activity.
  • the invention relates to improvements in gamma densitometry using sources emitting several high energy photons simultaneously, and detecting the signals of these photons in coincidence to reduce the background hundreds of times and provide precision in density measurements better than that of the standard gamma densitometer but with a source with 10, 000-fold lower activity than the one used in a standard gamma densitometry (license exempt activity).
  • Such devices are referred to here as Multiphoton densitometers (MP- densitometers) or enhanced gamma densitometers (EGD).
  • Gamma densitometers are used to measure the parameters of bulk fluids. Especially important is the use of densitometers in characterization of petroleum and petroleum products, e.g., measurement of relative fractions of petroleum, water and gas.
  • the main problem is large variability of fluid composition and inhomogeneities. Statistical sampling of the properties is made very difficult by the presence of large bubbles of gas, thick layers of water and a combination of all types of small bubbles.
  • Gamma densitometers are also used for measurement of density of granulated material.
  • density is an important parameter when handling grains, hops and other agricultural products.
  • it is easier to measure the density of grains in flow than to measure their weight, grains size distribution, and then calculate the density.
  • the direct measurement of density permits estimation of the fraction of water in the sample.
  • Densitometers are often used to measure properties of mixture(s) of fluids/gases/solids.
  • the typical example is in the petroleum industry where crude oil is a mixture of petroleum, water and gas.
  • the densitometers are used not only to measure the density of mixture, but are a part of more complex system that determines the composition of the crude oil.
  • the dependence of absorption of high energy photons on the chemical composition can be used.
  • a plurality of radiation sources with very different energies are used.
  • densitometers use the absorption of radiation (electromagnetic or sound waves) by matter.
  • the ideal densitometer should have
  • the invention relates to a method for determining the density of a gas, liquid, solid or mixed sample comprising measuring the attenuation and preferably the scatter of at least one of a plurality of photons concurrently emitted by a radioisotope, wherein at least two of the photons are detected in coincidence in at least two detectors.
  • the method may involve: (a) placing a radioactive source capable of concurrently emitting at least two photons so that emitted photons pass through the sample,
  • the invention may employ long life positron-gamma radioemitters listed in Table 1 , long life nuclear cascade radioemitters listed in Table 1, and long life electron capture radioemitters listed in Table 2.
  • the total source activity may be below 10 microCi and background may be rejected in the photon detectors by (i) selecting low natural radioactive background elements; (ii) analyzing pulse height and pulse shape; or (iii) using coincidence signature, individually or in combination.
  • the method may further comprise shaping the signals from the detectors to have width of less than 2.0 microseconds, and using a fast coincidence circuit to diminish pile-up artifacts.
  • the width is shaped to less than 0.5 microseconds and a very fast coincidence circuit is used to diminish the pile-up artifacts.
  • the signals from the detectors may be on-line or off-line analyzed by DSO to establish the fraction of pile-ups, and appropriate software correction is used to estimate the true count rate.
  • the method may involve placing the scintillator in an appropriate Dewar and stabilizing its temperature electronically with a precision of a few degrees Celsius, preferably with precision of at least 1° C. This may involve use of both an appropriate heater (preferably ohmic heater) and cooler (preferably Peltier element) and means to homogenize temperature by forced air flow.
  • an appropriate heater preferably ohmic heater
  • cooler preferably Peltier element
  • Temperatures of both scintillator and HVS/amplifier module may be sensed with precision of at least 0.2 ° C, and preferably with precision of about 0.1° C, by temperature to voltage converter (electronic thermometer) and the equivalent voltage is then measured by appropriate voltage sensor (ADC/DSO) in a central processing unit.
  • temperature to voltage converter electronic thermometer
  • ADC/DSO appropriate voltage sensor
  • an analog voltage signal equivalent to a temperature is sent to appropriate voltage sensor (ADC/DSO) in the central processing unit by means of shielded coaxial cable.
  • the analog voltage signal equivalent to a temperature is preferably transformed in an optocoupler, sent by fiber optics, decoded by light to voltage converter and then measured by an appropriate voltage sensor (ADC/DSO) in the central processing unit.
  • the analog voltage signal equivalent to a temperature is alternatively transformed in voltage to frequency converter, sent by shielded cable, preferably coaxial cable, and is measured by appropriate frequenciometer in the central processing unit.
  • measurement of temperature of scintillator and HVS/amplifier module is performed at least 10 times per second. The method may involve implementation of a statistical rejection procedure.
  • a preset number of temperature measurements (typically a few hundred) is acquired, and temperature values that deviate from running average of temperature by more than 95% (more than two sigma) are rejected and replaced by weighted average over closest four measurements of temperature.
  • the measurement of temperature of scintillator and HVS/amplifier module is used to calculate the true count rate, i.e., the count rate drifts due to temperature changes are accounted for by software.
  • Temperature compensation may be performed by means of calibration curve which is a product of three polynomial curves taking in to account temperature sensitivity of scintillator, PMT and HVS/divider and amplifier, respectively .
  • Temperature compensation may use 3D look-out tables established in a precedent calibration procedure, or the temperature dependence of DSO is periodically measured with a system containing means for signal multiplexing and means to generate pulses of well known and temperature independent shape.
  • the temperature gain calibration for each detector is obtained by a series of measurements in both OR and AND mode acquisition.
  • a plurality of methods may be used to eliminate the long term drifts of count rate, e.g., due to element aging, including the use of external sources of X-ray and gamma-ray photons with known energies with at least two different lines, including mechanical means for removal or shielding the sources; and the use of two separate modes operation, namely measurement mode and calibration mode.
  • At least three counters may be used in measurement mode and at least two channels of DSO in calibration mode.
  • a calibration mode comprises the steps of measuring pulse shapes, calculating the energy spectrum, estimating pile-up and dead-time corrections, and measuring external electromagnetic interference.
  • the results of a calibration run can be compared with previous calibration runs, and the look-up calibration tables are upgraded for subsequent use for adjustment of raw data.
  • a plurality of methods can be implemented to compare the data in OR and AND data acquisition mode, including acquisition of at least 100,000 events with both pulse-height and pulse shape rejection enabled followed by the establishment of detection efficiencies in which the count rate rates in the detectors A and B are compared without the use of the above said rejections.
  • steps may be taken to account for the influence of container walls, e.g. pipeline walls, including calibrations performed when the container is empty or filled with liquid of known density.
  • the liquids are either water or hydrocarbons with well known density.
  • the calibration source has activity lower than 0.5 microCi the energy spectrum is preferably obtained with DSO and all rejections enabled for three test configurations, i.e. with empty pipeline, pipeline filled with hydrocarbon with known density and pipeline filled with water.
  • the calibration source has activity lower than 5 microCi the count rates in the selected energy window are preferably obtained with coincidence enabled for three test configurations, i.e. with empty pipeline, pipeline filled with hydrocarbon with known density and pipeline filled with water.
  • the source has activity lower than 10 microCi the count rates in the selected energy window are preferably obtained with coincidence enabled.
  • a statistical rejection procedure may be implemented, wherein a preset number of coincidence counts (N) (typically a few hundred counts) is acquired, and the count rates that deviates more than two sq ⁇ t(N) from the average value N are rejected and replaced by weighted average over closest four measurements of count rate.
  • N preset number of coincidence counts
  • a holder for placing a radioactive source near a sample so that photons from the source pass through the sample at least two detectors capable of detecting at least two photons concurrently emitted by a radioisotope and generating a corresponding signal, at least one of the detectors being placed across the sample from the source and capable of measuring the attenuation and preferably the scatter of at least one of the photons concurrently emitted by the source, and (c) a data processor for converting the signals to density measurements.
  • the detectors may be operated in coincidence mode in a symmetric sandwich configuration as in drawing 2; in a modified symmetric sandwich configuration as in drawing 3; in a compensated sandwich configuration as in drawing 4; or in a triangular configuration as in drawing 8; and for thin foil or plate samples, in a compensated flat symmetric sandwich configuration as in drawing 9, in an asymmetric sandwich with separator configuration as in drawing 10, or in a modified triangular configuration as in drawing 11.
  • the detectors may be operated in coincidence mode in an asymmetric sandwich configuration as in drawing 5; in a shifted asymmetric sandwich configuration as in drawing 6; or in a modified asymmetric sandwich configuration as in drawing 7.
  • the source may be placed inside a spool made of material with appropriate mechanical characteristics (e.g. strength and weight) but low atomic number such as beryllium, plastic reinforced with appropriate fiber, aluminum, vanadium or titanium.
  • the spool has essentially elliptic cross-section, with total cross-section surface close to the cross- sectional surface of two pipes it is joining.
  • the source may be placed inside a bypass made of material with appropriate mechanical characteristics but low atomic number such as beryllium, plastic reinforced with appropriate fiber, aluminum, vanadium or titanium.
  • the bypass has essentially elliptical cross-section, with total cross-section surface much smaller than the cross-section of the main pipe.
  • the apparatus may further comprise a third, anticoincidence detector to diminish background as in drawing 12.
  • the detectors are scintillators, and at least one of the detectors is Na ⁇ (Tl) with a thickness of at least 2" coupled to PMTs.
  • the detectors are of substantially the same size and consist of the Na ⁇ (Tl) scintillators with a thickness of at least
  • At least one of the detectors may be a BGO scintillator with a thickness of at least 1 " coupled to PMT. At least one of the detectors may be a BaF 2 scintillator with a thickness of at least 2" coupled to UV light sensitive PMTs. Or at least one of the detectors may be either GSO(Ce), CsF or CeF 3 scintillator with a thickness of at least 2" coupled to PMT. Where a radioisotope from Family 2 is used, at least one the said detectors is preferably a Na ⁇ (Tl), CaF 2 (Eu) or YAP scintillator with thickness of less than 0.5" coupled to PMTs.
  • An apparatus optimized for radioisotopes from Family 2 uses hardware and software means to reject events due to interaction of CR in PMTs, and may have background due to electrons emitted from PMT diminished by application of appropriate thick optical windows made of quartz or other ultrapure, optically transparent materials.
  • radioactive background is diminished by the use of an essentially cylindrical shield including at least one heavy metal component and placed around at least one of the detectors, and appropriate thick optical windows made of quartz or other ultrapure, optically transparent materials.
  • the shield preferably comprises a few millimeter of Pb/Sn/Cu, the Cu being placed closest to the scintillator and further comprising a shield between the PMT and PMT base.
  • One detector may be smaller than the other with the shield placed only around the smaller detector.
  • the separator is preferably placed around the source and close to one of the detectors, and PMTs are selected to have radioactive background of less than 0.1 cps.
  • MP-densitometry includes coincident detection and pulse shape analysis to achieve an excellent signal to background ratio (S/B) for low activity sources, and optimal use of photons with different energies.
  • S/B signal to background ratio
  • the following working definitions are used: low energy photons: 10 keV ⁇ E ⁇ 100 keV, and high energy photons: E > 100 keV.
  • photons emitted in the atomic shell rearrangements are called X-rays and photons emitted by the nuclear transitions and/or positron annihilations are called gamma-rays.
  • the low energy photons (LEP) of importance in this invention are either X-rays or gamma-rays, but high energy photons (HEP) are always gamma-rays.
  • LEP low energy photons
  • HEP high energy photons
  • Family 1 Positrons emitted by the source annihilate with a nearby electron into two gamma rays, each with an energy of 511 keV. These gamma rays are emitted back-to-back because of momentum conservation and their coincident detection is strongly angle- correlated.
  • positron-nuclear gamma In positron-nuclear gamma (PG) emitters an emitted positron is followed by a nuclear gamma transition. The positron annihilates, as described above and there is also an additional nuclear gamma ray.
  • PG positron-nuclear gamma
  • NC nuclear cascade gamma
  • Electron capture (EC) isotopes In this case an atomic X-ray and a nuclear gamma ray are emitted (see Table 2).
  • Tables 1 and 2 show the lifetimes of the radioisotopes in years and days. The energies of the photons are listed in Handbook of Chemistry and Physics, Edition CRC, New York, relevant portion of which are hereby incorporated by reference.
  • Isotope Family 1 Long life positron-gamma (PG) and nuclear cascade (NC) isotopes.
  • Isotope Family 2 Long Life EC isotopes.
  • MP-densitometer compatible sources In some applications not only density but also composition need to be determined, e.g., multiphase measurements in petroleum industry. This can be accomplished using numerous potential sources with emission energies properly selected to enable differentiation of the materials and to facilitate elimination of various backgrounds. Furthermore, sources with lifetime longer than a month are preferred.
  • the use of low activity sources is highly advantageous. The power and practicability of the disclosed procedures are connected with the use of new, very low background and highly sensitive detection techniques applicable to some radioisotopes. Specifically, the use of
  • MPD Photon Detectors
  • VLBD Very low radioactive background detectors
  • PG positron-gamma
  • NC nuclear cascade
  • EC electron capture
  • PG emitters there are additional advantages due to the presence of back-to back annihilation photons, i.e. , the geometry is better defined for this case.
  • additional third high energy photons permit redundant measurement, and allow estimation of the average atomic number of the object under study.
  • EC emitters there are typically only two coincident photons, and one of those is always a rather low energy X-ray (emitted due to atomic shell rearrangement).
  • use of EC emitters leads to an asymmetric geometry, where two very different detectors are used.
  • the NC emitters appropriate for MP-densitometry emit spatially non-correlated photons.
  • NC emitters When they emit two photons of very different energies, the instrumentation is similar to the case of EC emitters.
  • NC emitters are important because some of them produce two very high energy photons, like ⁇ Co with energies of 1,173 and 1,332 keV, respectively.
  • the geometrical configuration may be different from the case of PG emitters and both detectors can be located at the same side of the sample.
  • PG emitters where high energy photons, e.g., annihilation photons are used in a coincidence scheme to reject background. Because very fast scintillators can be used to detect photons, important advantages of maximal count rate may be realized.
  • Scintillators are the most popular detectors for quantitation of hard X-rays and gamma- rays. Good energy resolution is a major advantage in the design of low radioactive background detectors. Among the scintillators Na ⁇ (Tl) and CsI(Tl) produce the best light yield, while photomultiplier tubes (PMTs) permit counting of single photoelectrons.
  • PMTs photomultiplier tubes
  • NaI(Tl)/PMT combination is very popular, but other scintillator-PMT combinations are also of importance, including CsI(Tl), CsF, BF 2 , CaF 2 (Eu), YAP(Ce), BGO, and GSO(Ce).
  • CsI(Tl)/PMT combination is very popular, but other scintillator-PMT combinations are also of importance, including CsI(Tl), CsF, BF 2 , CaF 2 (Eu), YAP(Ce), BGO, and GSO(Ce).
  • Li ⁇ (Tl) Na ⁇ (Tl), CaF 2 (Eu)
  • high energy photons Na ⁇ (Tl), CsI(Tl), BGO, BaF 2 , YAP(Ce), CeF 3 , and GSO(Ce)
  • the MP-densitometer system should be portable, robust and user-friendly. Many of the operations are in remote locations, i.e., system should be self-contained. Thus, low cost
  • the general principle underlying the present invention comprises a method according to which sources emitting concurrently a plurality of energetic photons (E > 10 keV) are detected in setups with an optimized configuration.
  • the apparatus implementing the optimal detection schemes are disclosed.
  • Standard gamma densitometer and MP-densitometer Existing gamma densitometers use the simplest possible configuration: the sample is placed between the radiation source and the detector (see Figure 1). In this configuration only a few elements can be optimized; energy /activity of the source and the detector itself. In the following, we disclose a MP- densitometer that eliminates the limitations of prior-art gamma densitometers.
  • the background due to Cosmic Rays (CR) is an important component of the total background in a single detector configuration.
  • the energy deposited in one detector is often very different from the energy deposited in the second detector, which permits rejection of background due to CR primary particles.
  • secondary particles shower initiated by CR in atmosphere have a characteristic density which considerably limits the sensitivity because of the background due to secondaries.
  • use of coincidence scheme is very efficient in eliminating radioactive background in scintillators, PMTs and shields.
  • a preferred implementation of a detector according to the invention uses two essentially identical crystals. This is a good choice when annihilation photons are detected, and for some nuclear cascade isotopes, e.g., ⁇ Co.
  • many other important sources emit photons of quite different energies; often one photon is a soft X-ray (E ⁇ 50 keV) while the second photon is a nuclear gamma-ray, say E > 500 keV.
  • E ⁇ 50 keV soft X-ray
  • E > 500 keV nuclear gamma-ray
  • MP-densitometers can operate in very different configurations as “symmetric” and “asymmetric” sandwiches, respectively.
  • sandwich geometry is counter-intuitive but enables the tradeoff between a lot of requirements because it:
  • the simplest "symmetric sandwich” geometry is the one in which the MPD source is placed inside of the object whose properties are measured. This is the preferred implementation when properties of gas/fluid mixtures in flow are measured.
  • the "symmetric sandwich” geometry is shown in Figure 2. More specifically, for measurement of gas/fluid mixture density, a “spool” can be placed between two fragments of a normal pipeline.
  • the “spool” has diameter equal to the main pipe but is made of material with low attenuation coefficient, e.g., beryllium, plastic enforced with kevlar/carbon fiber, aluminum, vanadium or titanium.
  • the "spool” is made according to stringent mechanical tolerances, i.e., both the geometric dimensions and wall thickness are made with better than 0.1 % precision.
  • This "spool” contains in the center a small, hydrodynamically shaped container in which the source is placed. This geometry is especially efficient and easy to calibrate in the case of PG emitters, wherein the two annihilation photons are emitted back-to-back. Thus, the count rates in both detectors should be very close to each other. This facilitates self-diagnostics and self-calibration.
  • the "symmetric sandwich” geometry was optimized for a particular situation of liquid flow. It allows measurement of laminar flow of gas/fluid mixtures, wherein the fluid moves close to the vertical pipeline walls and the flow of gas is mostly in the center of the vertical pipe. Note, that in this situation the velocity of gas and fluid are quite different leading to additional "dynamic pressure" compression of gas and modifying the efficient density. However, it can also be implemented in some other applications, such as in the measurement of properties of granulated material, e.g., grain, seeds or cement.
  • the "symmetric sandwich" geometry also permits determining if flow is turbulent (no difference between top and bottom detectors) or laminar
  • the "compensated sandwich” geometry is shown in Figure 4.
  • the source is placed between two objects; a measured sample whose properties are unknown, and a "standard sample” with similar and perfectly known properties.
  • a pair of matched detectors is preferred, with almost identical detection efficiency, energy resolution and temperature dependence.
  • the concept of "relative” measurements is implemented, i.e., difference in count rate is proportional to difference of densities between the "unknown” and “standard”.
  • This method is very efficient, when measurements of relatively small objects are required, especially when better than 0.1 % precision in density /physical dimensions is needed.
  • This configuration is “robust” and permits high reliability self-calibration. It is especially important, when the artifacts due to pileup and due to multiple scattering are important.
  • Another innovative application is wherein the "relative density /dimensions" of an object are to be measured. By using the known standard, the majority of calibration artifacts, e.g., temperature dependence can be eliminated.
  • FIG. 5 is the most useful.
  • the PG source e.g., ⁇ Na
  • a very large detector say 6" in diameter
  • a big detector consisting of a plurality of smaller detectors operated in parallel may be used.
  • the large detector does not need to be placed exactly opposite the source at the other side of the object. This leads to a configuration called "shifted asymmetric sandwich" (see Figure 6).
  • the second detector is placed under an angle, higher absorption length is achieved, permitting better relation between density precision and statistical uncertainty in the count rate.
  • the change of angle leads to some increase of absorption in pipe walls and increases considerably the absorption in petroleum.
  • the efficient signal decreases and appropriate calibrations should be used.
  • only part of the flow is sampled in density estimation. Actually, in this case absorption in petroleum is higher than absorption in the walls of pipe, and thedecrease in count rate should be comensated by the increase of measurement time.
  • this configuration cannot be used in prior-art gamma densitometers which are essentially limited by their signal/background ratio. It is, however, useful in MP-densitometers wherein the sensitivity is limited by statistics rather than a signal/background ratio.
  • the "modified asymmetric sandwich" shown in Figure 7 is especially useful, when objects of very large diameter are studied using PG isotopes, including objects so large, that even annihilation photons are substantially absorbed. For example, for 10 inch pipelines with 0.375" steel walls about 95% of annihilation photons are absorbed. In this case, the two detectors have very different functions. The detector close to the source detects unscattered photons and serves as trigger.
  • the second detector measures the number and spectrum of scattered photons. It should be relatively large with size comparable to the thickness of the object to be studied.
  • the large detector consists of two slabs of relatively slow Csl scintillator, each about 2" thick and 16" long. Each Csl scintillator is coupled to a separate PMT and chain of electronics. Using this configuration, the signal/background ratio better than 100 was achieved using only 1 microCi source for 10 "-diameter pipes filled with water.
  • An important, "triangular" configuration is disclosed in Figure 8.
  • This configuration is not applicable to PG isotopes but is appropriate for NC isotopes, wherein two high energy and directionally uncorrelated photons are emitted, e.g., such is a case of ⁇ o.
  • This geometry is appropriate for density measurement in the largest pipes, wherein the highest possible energy of photons is an advantage because it limits the attenuation and permits reasonable statistics. Note, however, that only a fraction of the object volume is efficiently measured, which in the case of inhomogeneous objects including mrbulent flow of liquids in pipes may lead to some artifacts. Data analysis minimizes these artifacts.
  • a special "spool” can be produced from aluminum or titanium rather than stainless steel.
  • the stopping power is smaller for a thickness with the same mechanical properties.
  • a few times lower attenuation in metal is achieved, and a lower activity source can be used.
  • the oval shape can be used instead of a "spool” with essentially circular cross-section. With appropriate dimensions, the change on the flow speed will be minimal but the attenuation will be a few-fold diminished.
  • the "spool" can consist of two parallel channels, i.e., the liquid flow can be bypassed.
  • the 24" pipe with 1 " walls. Assuming an 8" bypass the walls needs to be only 0.25" thick. Thus, the attenuation diminishes about fourfold. Taking in account the coincident method of readout used in the MP-densitometry; the activity of a source may be about 16-fold lower.
  • MP-densitometer configurations optimized for EC sources We disclosed above the MP-densitometers optimized for measuring densities of large ( > 2" thickness) objects. However, there are important applications for MP-densitometry for smaller objects, such as measurement of thickness of thin foils, flats and plates of plastic, paper and metal. In this case, the attenuation of gamma rays is small and sources with lower energy should be used.
  • the MP-densitometers work best, when the sample absorbs from about 50 to 80% of emitted radiation. For the X-ray, however, the attenuation coefficient is very dependent on the atomic number of the absorbing media because the photoelectric effect dominates. Thus, the applicable energy range is from about 20 keV for paper/plastic/aluminum foils to about 100 keV for steel or cooper foils.
  • MP-densitometer based on use of low energy EC emitters.
  • this device the X-ray densitometer.
  • An appropriate EC source is 125 I, which emits photons with 27, 31 and 35 keV.
  • this source we achieved the radioactive background of less than 1 cpd.
  • background improvement of about 50,000 when compared with prior-art devices has been achieved.
  • MP-densitometers optimized for the thin films application are of three different types, namely:
  • Figure 9 provides a schematic view of a "compensated flat symmetric sandwich" configuration of a MP-densitometer.
  • a single EC source is placed between two samples, one of unknown density /dimensions and another being a standard sample.
  • Two matched detectors are used each with diameter much larger than the thickness of the objects. This is a geometry which facilitates the relative measurement and compensation of the artifacts providing the properties of two detectors are well matched.
  • the EC isotope with very different energies of X-ray and gamma ray are used.
  • FIG. 10 A schematic view of an "asymmetric sandwich with separator" configuration of MP- densitometer is shown in Figure 10.
  • a single EC source is placed on one side of the object whose density and/or dimensions are to be studied.
  • Small X-ray detector is placed close to a source and larger gamma ray detector on the other side of the sample. The two detectors work in coincident mode.
  • the advantage of this configuration is its versatility. Using it, objects of diverse shape, not only flats can be evaluated.
  • the instrument can be relatively easily rescaled for samples with different dimensions.
  • the attenuation properties of material from which the sample is fabricated has to be known rather well and a reliable calibration procedure is required.
  • the second detector should have the best energy resolution possible. Typically it will be a Ge detector or Na ⁇ (Tl) scintillator. Note the placement of the "separator" around the EC source.
  • the use of separator permits substantial diminishment of cross-talk between the two detectors leading to low radioactive background.
  • the use of a separator diminishes the requirements on speed of pulse-shape analysis and permits to overcome the pileup problem.
  • This configuration may employ digital signal processor (DSP) cards.
  • DSP digital signal processor
  • one of the photons is an X-ray with relatively low energy and second photon is a gamma ray, whose energy can be selected to be quite high.
  • the soft X-ray cannot penetrate a large object but it can be used as a trigger to diminish the background.
  • This configuration leads to the lowest background, because a X-ray detector can be very small and thin. Using this configuration, a background lower than 0.1 cpm was achieved. Furthermore, such detectors are much more portable because the X-ray detector can be miniaturized. From a large class of EC radioisotopes (see Table 2), the energy of a gamma ray can be selected to optimize the resolution of a MP-densitometer for a diverse object.
  • Figure 11 provides a schematic view of a "modified triangular" configuration of a MP- densitometer.
  • a single EC source is placed on one side of the object whose density /dimensions are to be studied.
  • Two gamma ray detectors are placed on the other side of the object. The size of detectors and the distance between them is much larger than the thickness of the object. The two detectors work in coincident mode and are separated by a passive shield.
  • the main advantage of this geometry is that both detectors are placed on the same side of a studied object. Actually, in many applications, the density of fast moving flats/plates is studied. The mechanical limitations of the transport system means that the volume under the flats is at premium.
  • the triangular geometry is advantageous because the EC source can be of very small dimensions, down to mm 3 .
  • the source can be a thin ( ⁇ 1 mm in diameter), capillary or plastic rod.
  • Another advantage of this geometry is that two detectors placed in parallel have much lower background that two detectors placed face-to-face. A factor of ten improvement in S/B is possible.
  • a sophisticated graded passive shield can be placed between the detectors. It can be further enhanced by the use of active anticoincidence detector as an anti-CR shield (see Figure 12).
  • the disadvantage of triangular geometry is the lower geometric detection efficiency than other configurations.
  • a new element is the use of a "separator", a thin sheet of high atomic number metal with a hole in which the source is placed.
  • the use of the separator permits further background rejection. Note, that for high energy photons, the separator has to be so thick that it considerably limits the geometrical detection efficiency. For soft X-rays, the millimeter thick separator made of heavy metals (tungsten, gold, lead) absorbs almost all of the photons. It limits a crosstalk without significant change of geometrical detection efficiency. In X-ray densitometer it is appropriate to physically isolate the scintillators as much as possible to reduce induced X-ray crosstalk between them.
  • the thickness of the samples is relatively small (a few millimeters) this can be achieved by incorporating a few mm thick sheet of lead or copper into the sample holder.
  • Isolation of the detectors very effectively reduces the background in the single-photon 125 I region of interest (ROI).
  • Na ⁇ (Tl) or CsI(Tl) based detectors show considerable sensitivity to the geometry and diameter of the opening in the separator. Detector isolation has less effect on the background in CaF 2 (Eu)-based systems because these detectors do not produce secondary X-rays in the 125 I ROI.
  • the PG source e.g., 22 Na
  • the PG source emits not only two annihilation photons, but also 1275 keV photon. Comparison of the attenuation of these photons with and without fluid, permits to factor out the influence of pipe on the count rates. Furthermore, we observed that the mechanical precision of the placement of the pipe within the densitometer may lead to a systematic error of about 2-3 % in the case of prior-art gamma densitometers. These kinds of errors are easy to detect and eliminate when using the MP- densitometer.
  • Multiphoton Detector MPD
  • VLBD very low radioactive background detector
  • Sources of background A1-A4 and B1-B3 are dependent on detector size; typically they grow linearly with the mass of the detector.
  • Sources C1-C2 are dependent on the size of
  • the background sources D1-D2 tend to be independent of the size or type of the detector. Furthermore, they are much more important for photons with energy lower than 50 keV.
  • the first group of backgrounds (A1-A4) leads to backgrounds of the order of a few cps.
  • the second group of backgrounds (B1-B3) is an important source of background in prior-art gamma densitometers. Actually, the background due to CR induced dark currents in PMTs (C2) are proportional to background due to a direct hit by CR (B3), which is much easier to count.
  • the background due to direct hits by CRs is periodically measured and used to evaluate the other sources of background (BI, B2 and C3). If the sum of these background is above a preset threshold (periods of high CR activity) they can be accounted for in the density measurement.
  • the background sources from the third group (C1-C2) are the most difficult to reject by hardware means.
  • MP-densitometers use a synergistic combination of coincidence, hardware means and sophisticated pulse shape analysis. Coincidence permits about a 100-fold decrease in background, and additionally our pulse shape analysis software permits rejection of about 90% of the background. This requires use of on-line pulse shape analysis, including appropriate software. Software for background rejection limits the maximal count rate, and is very difficult to implement when the actual detector count-rate is much larger than 10 kHz.
  • the electronic and vibrational pickup noise is very much system and site dependent. In petroleum industry applications it tends to be large, because the detectors are placed close to pipeline, whereas the data acquisition system, i.e., the computer, is often placed in a trailer. For example, during experimental tests of MP-densitometer in CONOCO Test Facility, Lafayette, Louisiana, this distance was about 90 feet. Even when using well- grounded coax cables, the observed electromagnetic noise without coincidence is about 100 cpm. In prior-art gamma densitometers, this source of noise is considerably lower than the radioactive background. However, in MP-densitometers wherein the radioactive background was diminished a thousandfold, the electromagnetic interference is an important source of uncertainty. We disclose the use of:
  • All sources of background can be classified into two categories. First, there are sources which are essentially constant, e.g., A1-A3 and Cl. These sources of background can be accounted for by appropriate calibration, and their influence can be attenuated (but not eliminated). However, there are many sources of background which are highly variable, both geographically and as a function of time. For example, environmental radioactive background is often dominated by radon and is strongly weather dependent. Also, the background due to CR is not only geographic position dependent, but is also modulated by solar flares activity leading to changes of geomagnetic cutoffs. Thus, the radioactive background in prior-art gamma densitometers cannot be calibrated, leading to spurious residuals in density measurements. On the other hand, the background in MP-detectors is suppressed about a thousandfold and the background variations are negligible.
  • MP-densitometers In MP-densitometers according to the invention, the coincidence between two photons emitted by an appropriate source is used to diminish the radioactive background. For example, when using a suitable long life PG source ( 22 Na), scattering of the annihilation photons leads to change of both total number of detected photons and to substantial change of the spectrum. Algorithms for estimating the density of the studied object depend on this change of the spectrum. Thus, the use of scintillators with the highest energy resolution, namely Na ⁇ (Tl) is disclosed. However, for larger objects, this leads to either reduction of detection efficiency when 3" thick crystals are used or increase of background when 4" or 5" -diameter crystals are used.
  • the optimal Na ⁇ (Tl) crystal diameter is a function of pipeline diameter.
  • the 3" crystals are optimal.
  • the optimal crystal diameter is 4" and 5", respectively.
  • the rise-time of scintillation light in Na ⁇ (Tl) is about 200 ns, and typically about 500 ns pulse shaping is used. For sources in excess of 5 microCi this leads to the pileup artifacts. We observed the uncertainty of about 0.5% in count rate for 3" pipelines filled with petroleum. This leads to 1.5% precision in density measurement.
  • MP-densitometers may be improved by the use of scintillators different from Na ⁇ (Tl).
  • CsI(Tl) has only marginally lower energy resolution but about twice higher stopping power. Alas, it is a slower scintillator than Na ⁇ (Tl) and thus leads to higher pileup artifacts; CsI(Tl) should not be used when the source activity is above 1 microCi.
  • Use of BGO is suggested, even if this crystal has about four times lower energy resolution.
  • the advantages of BGO crystals are about three times higher stopping power and faster scintillation. Thus, for the same stopping power the pileup is about a factor ten smaller and also background is somewhat lower.
  • the X-ray detector may be built of CaF 2 (Eu) rather than Na ⁇ (Tl). Using CaF 2 (Eu) some sources of background (especially the dark currents) can be rejected better than when using Na ⁇ (Tl). Alas, CaF 2 (Eu) is also a much slower scintillator, and typically the shaping time of a few microseconds is used. Thus, it should be used only when the radioactive source is below 0.5 microCi, i.e., only in the case of rather small objects.
  • YAP(Ce) yttrium-aluminum-phosphate scintillator
  • Temperature stabilization/compensation schemes in MP-densitometers Accurate measurement of density requires a high stability detector system. The observed drifts are predominantly due to changes in ambient temperature, which cause drifts in the yield of the scintillators as well as changes in gains of the PMT's and amplifiers. In prior-art gamma densitometers, the temperature drifts are the dominating sources of measurement errors. For example, many oil wells and pipelines are located in deserts, where the diurnal temperature variations can be as large as 50°C. Similarly, the temperature gradients are very large and site dependent in the metallurgic industry where, the gamma densitometers are often placed very close to moving slabs of very hot metal.
  • the light yield from Na ⁇ (Tl) scintillator is changed by up to 3% when temperature varies by 10°C.
  • the typical dependence of a coincident count rate in Na ⁇ (Tl) based MP-densitometer on temperature is shown in Figure 13.
  • the temperature dependence of scintillator may be more complicated in particular cases.
  • BaF 2 there are two components, one very fast emitting an UV light and another much slower emitting in visible. The first component is almost temperature independent, wherein the second component is strongly temperature dependent and becomes negligible at above 65 °C.
  • the crystal temperature is kept above 40 °C to diminish artifacts.
  • the main method of correcting for temperature artifacts is to stabilize the temperature of the crystals.
  • Each detector may be independently stabilized in temperature.
  • the schematic drawings of the temperature stabilization system are provided in Figure 14.
  • each detector is placed in a massive, explosion proof box typically made of aluminum.
  • the appropriate Dewar with internal dimensions of about 3.5" is mounted inside this box.
  • PMTs are very bad heat conductors due to a high vacuum inside and only a very thin wall of glass.
  • the Dewar covers essentially only a scintillator and PMT assembly and is additionally insulated around the PMT neck with porous plastic material.
  • the fast reacting ohmic heaters e.g., high power transistors are placed on the good conductor metal plates, typically aluminum or copper attached to the crystal.
  • the temperature is homogenized inside the Dewar by the use of miniaturized fans.
  • the temperature stabilization is obtained by the direct feed back using a fast electronically readable thermometer.
  • a feedback loop is established between the output of scintillators (position of photoabsorption peak) and the parameters of the temperature stabilization system. Practically, it is preferable to use only heating rather than both heating and cooling. In this case, the temperature is established higher than the expected maximum temperature of the environment.
  • the additional temperature compensation system is used in MP-densitometer (see Figure 15).
  • three temperature sensors are placed in each detector; two on the crystal and one on the integral high voltage supply (HVS)/amplifier module.
  • the thermometers output is amplified by a DC-DC amplifier to a signal of about 5V.
  • the information from these sensors is sent several times a second to a digital oscilloscope card and is on-line analyzed by the computer.
  • the voltages from electronic thermometers are electronically modified in a voltage-to-frequency converter, and are sent by the cables that are used for transmission of pulses from detectors to data acquisition computer.
  • the electronic thermometer has a digital RS320 interface and is directly coupled to the input ports of the data acquisition computer. After reception the data are software filtered to remove spikes due to electromagnetic interference and averaged. In all these implementations the reliable temperature measurements with precision of about 0.2% were achieved. Note, that the temperature of crystals is often a few degree Celsius different from temperature of PMT base. This is accounted in software in which three temperature compensation curves are calculated independently, for scintillation crystals, high voltage supply/dividers and signal amplifiers, respectively.
  • Both heating and cooling by means of the Peltier effect may be used so that the crystals temperature is stabilized below the ambient temperature. This permits use of the operational temperature, in which the temperature coefficient of the scintillator is minimal.
  • the temperature dependent drifts of the high voltage supplies, preamplifiers and ADC's are important, and it is preferable to use stable electronics and high voltage power supply for the PMTs.
  • the high voltage power supplies for the PMTs have been stabilized by introducing a high gain negative feedback and using as a reference Max 580 chips with low temperature coefficient (1-2 ppm/°C). We also use 1 % metal film resistors with a low temperature coefficient.
  • the voltage divider for the PMT is based on the same type of resistors.
  • the temperature sensitivity and long term stability of DSO's are especially important in coincident systems.
  • the relative drifts of two channels as a function of ambient temperamre change is often larger than the intrinsic resolution of DSO.
  • the calibration procedure is initiated, wherein the pulse from the well-stabilized pulse generator is applied in parallel to both channels of a data acquisition system and counted in both OR and AND modes.
  • the applications of MP-densitometers can be divided into two classes. In the first class, density measurement with precision of a few percent is required and long term stability of the count rate should be about 0.3 to 0.5 % .
  • temperamre stabilization and compensation are fully sufficient. Furthermore, a periodical calibration of detectors is recommended. In the second class of applications, e.g., in two phase measurements of oil/ water mixmres, better than 1 % density precision is required. Thus, the count rate uncertainty should be 0.1 - 0.3 % which is really difficult to achieve. To enable this count-stability a few innovative techniques are used in MP-densitometers to further diminish the remaining temperamre induced drifts in the PMTs and scintillators. These drifts can be compensated by adjusting the gains of the amplifiers, so that the acquired spectra will be unchanged. Electronics permits control of these gains.
  • An optional element of the long term stabilization of the detectors is the use of calibrated low energy photon sources consisting of at least two low energy lines. These calibration energies are sufficiently different so that these two lines can be distinguished by a detector.
  • this is a few hundred nCi source, that is mechanically shielded and the obscurator is computer activated.
  • the MP-densitometers use two modes of data acquisition: measurement mode and calibration mode.
  • measurement mode the main effort is to diminish the pileup and dead-time effects.
  • the fast electronics and system of fast counters are used.
  • calibration mode the main effort is to evaluate the influence of different background sources (natural radioactivity, CRs, electronic interference). Also, the efficiency of temperamre stabilization compensation system is checked.
  • DSO digital storage oscilloscope
  • the look-up calibration tables are upgraded which are used to adjust the raw data.
  • the data are obtained for both detectors in OR as well as in AND modes. Thus any differences between the detectors showing a malfunction can be analyzed.
  • the MPD normally operates in OR and the AND mode, with considerable background reduction through pulse shape analysis.
  • the typical background without shape analysis is about 100 counts per second.
  • the background in the OR mode is 50 counts per minute.
  • AND mode the MPD instruments permit about thousandfold lower background.
  • the AND data serve to establish the material density and the OR data are also analyzed (either on-line or periodically) to permit the reliable calibration of the system, e.g., to monitor the temperamre drifts and pile up problems.
  • the software estimates the pileup corrections to the counting rate. These corrections are very different at OR and AND mode of operation. It is important that the pileup corrections are estimated at the level of raw data, i. e. , before background rejection. Self-diagnostics and self-calibration programs permit concordance of the OR and AND counting rate data with accuracy of about 0.2%.
  • the calibration procedure depends on the MP-densitometer configuration, and in the following the case of "modified symmetric sandwich" using 22 Na source, is described as an example.
  • the user can request the software to perform this procedure at any time but typically the calibration runs are performed each hour. No calibrated source is needed, because the reasonably high activity (1- 5 microCi) 22 Na source is already present.
  • the program acquires 100,000 events with all pulse-height and pulse-shape rejections enabled. Once the acquisition is finished, the spectrum is analyzed to determine the ROI for a photoelectric absorbtion peak of annihilation photons. The count rate (cpm) within this ROI is determined.
  • the detection efficiency may be established from the ratio of cpm/dpm.
  • the program starts a second round of data acquisition with pulse-shape rejection disabled (as the calibration source activity is high at the 511 keV line, there is no need to reject the background, and no real events are discarded).
  • Spectra for both detectors (A and B) are built until 200,000 events are acquired. Subsequently the spectrum of each detector is analyzed to estimate the count rates in the 1 -photon and 2-photon peaks and efficiencies of the detectors are calculated. The data are checked for consistency by comparing the estimates from detectors A and detector
  • the pileup pulses are detected and their frequency estimated. With the pulse shape analysis available, the pileup pulses are easily detected due to a characteristic, two peak structure. With statistics of about 200,000 pulses analyzed the sub-set of about 2,000 pileup pulses are typically analyzed, for which the distance between two peaks is measured. This permits statistical analysis of the pileup artifacts.
  • the system is ready to count samples of the same geometry as the last calibration sample used. Acquisition is performed either for a preset time or until a preset number of counts (determining the statistical uncertainty of counting) have been acquired in the ROI. The program then estimates the actual decay rate in the source using the previously computed DE. The sample counting data are then stored to disk in an ASCII data file which can be transferred to any database or spreadsheet program for analysis.
  • the calibration is performed with pipelines empty or filled with water so as to permit comparison with previous calibration runs.
  • the calibration can be performed with any fluid in the pipeline because it is mainly based on pulse shape analysis of non-attenuated annihilation photons in OR mode.
  • the two detectors with 3" Nal (Tl) crystals were coupled to 3" PMT and bases
  • the signals were processed by amplifier/shaper electronics and then transferred to a PC 486/66 equipped with proprietary data acquisition cards.
  • the computer was installed in the control room about 90 feet away from the detectors.
  • the coincident trigger selected the coincident signal from two detectors within the energy interval 100 - 600 keV, which correspond to both scattered and not scattered annihilation photons.
  • the MP-densitometer is working in three modes: in two calibration modes and in the data acquisition mode.
  • the signal from a low activity (0.3 microCi 22 Na) source is processed by a proprietary coincident card and is subsequently analyzed with the DSO.
  • the coincident trigger is tuned for a selected region of interest (ROI) in energy.
  • ROI depends on a geometrical configuration of the system and may be different for two detectors in an asymmetric configuration.
  • the MP-densitometer is calibrated using the 2 microCi source in two density points: with an empty and water filled pipe. In this mode the smoothed count rate and temperatures (see below) are stored and temperamre compensation look-up tables are calculated.
  • the signal from a coincident trigger is accumulated for a given number of times (100 times per minute).
  • the use of a statistical rejection procedure is disclosed, wherein the count rates that are more than two sqrt(N) off from the average value N are rejected and replaced by a weighted average over the closest four points. Then all the counts are summed over and this number is accepted as a real number of counts during a given time interval (1 min).
  • the same procedure is applied to the signals from two temperamre sensors installed on the two detectors. Every minute the signals from the temperamre sensors, coincident (AND) count-rate and non-coincident (OR) count rates are written in the file.
  • the density of the mixture inside the pipeline is calculated and stored using the coincident count rate corrected for the current detector temperamre, and the reference points obtained during the calibration run.
  • the time dependence of the temperatures of both detectors, coincident count rate and density are presented on the monitor in the real time.
  • the digital output density signal is converted into analog DC voltage in the range 1 - 5 V.
  • MP-densitometer optimized for EC sources There are important applications of MP- densitometry for smaller objects ( ⁇ 3"). guch as the measurement of thickness of thin foils and slabs of metal, plastic and paper. ⁇ this case, the attenuation of gamma rays is small and sources with lower energy should be used.
  • the MP-densitometers works best of all, when the sample absorbs from about 50 to 80% of emitted radiation. For the X-ray, however, the attenuation coefficient is very dependent on the atomic number of the absorbing media because the photoelectric effect dominates. Thus, the practicable energy range is from about 20 keV for paper/plastic/aluminum foils to about 100 keV for steel or cooper foils.
  • the third, anticoincidence detector is used to eliminate the cross-talk between the two signal detectors.
  • Na ⁇ (Tl) scintillator crystals are believed to be optimal for detection of X-rays.
  • the background rejection is inversely proportional to the square of the energy resolution, which for Na ⁇ (Tl) is about 50% better than for other scintillators.
  • an MPD system can achieve a background of about 0.5 counts per week (0.5 cpw).
  • Na ⁇ (Tl) is mechanically fragile, e.g., it often cracks when submitted to temperamre gradients and/or during transportation;
  • CaF 2 (Eu) has a surprisingly low background for 125 I detection because in AND mode the background is dominated by soft X-ray emitted and absorbed in one crystal coincident with some source of energy detected in the second crystal.
  • any absorbtion of an external photon with E > 35 keV in the crystal leads to remission of 26 keV or 32 keV photons from rearrangement of atomic shells.
  • the characteristic iodine X-rays are emitted when the Na ⁇ (Tl) crystal is used. These cannot be distinguished from the 25 and 31 keV photons emitted by 125 I.
  • CaF 2 (Eu) consists of only low atomic number elements.
  • the characteristic X-rays have less than 15 keV energy and can be differentiated from radio-iodine X-rays.
  • Na ⁇ (Tl) or Csl should be used for EC radioisotopes with atomic number of either less than 40 or larger than 70.
  • CaF 2 (Eu) is a preferred scintillator.
  • the crystals themselves are preferably very thin and the surface of the PMT cathodes is about fifteen times larger than the surface of the crystals.
  • the scintillators used in X-ray detectors should be shielded from radioactivity in the photomultipliers to which they are coupled, such as from beta particles and low energy photons.
  • a 5-mm thick quartz window is placed between the PMT and the scintillator. Quartz is preferred both for its excellent optical properties and its high purity; quartz matches the optical density of CaF 2 (Eu) very well and is acceptable for NaI(Tl). We did not observe any increase in background due to radioactive contamination in quartz. Further improvement can be achieved by using materials with higher stopping power than quartz. We disclose the use of high-purity GeO 2 and germanium- based glasses for this purpose. They have very low intrinsic radioactive background and their higher atomic number and density is an advantage over quartz windows.
  • Such windows with a few millimeters thickness will efficiently stop low energy photons as well as beta particles without degrading the optical qualities of the scintillator/PMT systems.
  • the optical properties of gelica and germanium glass match Na ⁇ (Tl) better than quartz does.
  • Even higher density glasses based on lead may be used as well as high density transparent crystals such as PbF 2 and bismuth germanite (BGO).
  • BGO bismuth germanite
  • undoped crystals should be used so as not to generate artifacts due to scintillation within the BGO.
  • the optical density of these materials is higher than for CaF 2 (Eu) or Na ⁇ (Tl).
  • the use of a thin layer of special optical greases, e.g., powdered PbF 2 in silicon grease can match the optical properties of the scintillator and window and the window and PMT.
  • Both background and detection efficiency in the modified asymmetric sandwich geometry depends on the dimensions of the small crystal.
  • the source can be small, often about 1 mm in diameter.
  • An optimal configuration is one with two crystals of both different material and different diameters.
  • the detector close to the source should be small and thin, typically 0.75" or 1 " in diameter.
  • the detector on the other side of the measured object should be much larger, typically 3" or 4" in diameter.
  • the two detectors are differentiated not only by their dimensions but also use different scintillators; depending of the type of source used it should be either Na ⁇ (Tl), YAP(Ce), CsF or BGO.
  • a preferred implementation of the MP-densitometer optimized for detection of EC isotopes, e.g., 125 I, is an "asymmetric sandwich", consisting of two modules, the smaller of them preferably placed in a low radioactive background shield consisting of heavy metals, typically a sandwich consisting of a few millimeters of Pb /Sn/Cu.
  • the shield is essentially cylindrical, with the thin window close to where the scintillator is placed.
  • there is a thinner shield between the PMT and the PMT base containing high voltage supply, high voltage divider, and preamplifier. Additionally, the somewhat thicker shield is placed after the said PMT base.
  • Each of the detector modules consists of the following elements:
  • PMT base assembly consisting of HV supply, high voltage divider and preamplifier.
  • 125 I is an appropriate source for a plurality of MP-densitometry applications, preferably using flat detectors (1 mm thick Na ⁇ (Tl) or 1.5 mm thick CaF 2 (Eu)).
  • Thinner scintillators decrease the DE of the system while for larger crystals the signal to background ratio effectively diminishes.
  • the scintillators are coupled through quartz windows 3-5 mm thick to a high resolution PMTs which are selected for low background.
  • the PMT signals are amplified and shaped using proprietary electronics built into the PMT bases. To reduce the flux of background photons from the bases to the scintillators the bases are isolated from the PMTs with 5 mm of lead and 1 mm of copper plating with holes for the PMT pins.
  • At least one of the detectors is placed in graded lead + tin + copper shields (typically, 0.25" lead, 2 mm tin, 1 mm copper).
  • the detectors are placed face-to-face a few millimeters from one another and a crosstalk eliminator is placed between one of the detectors and the sample.
  • this is a 1 mm thick copper sheet mounted in a lead frame. Openings are left in the copper sheet for the source.
  • a plastic, e.g. delrin, guide ensures that foil is centered in the detector system.
  • An important element of the preferred implementation is the use of selected PMTs made of glass with low contamination by ⁇ K. More specifically, we disclose use of the Electron Tubes Inc. 2" or 3" PMTs preferably selected to present less than 0.1 cps background.
  • An element of the design is decoupling the PMT base from the PMT by means of a graded shield consisting of three layers of metal with very different atomic numbers. Typically, such a graded shield consists of about 0.5" of Pb, 0.15" of Sn and about 0.1 " of Cu.
  • PMT base fabricated from selected materials with low radioactive background is preferred, e.g., using pure Al for the supporting frame, resistors and capacitors selected for low radioactive background, and in-free solder, e.g., made of pure Sn or Sn Pb alloy. All passive and active elements of PMT base are selected to have a very low temperamre drift, and active compensation techniques to eliminate temperamre dependent gain drift are disclosed.
  • Data acquisition in MP-densitometry is based on amplifying and shaping the signals from the PMTs coupled to each detector and building a combined energy spectrum for subsequent analysis.
  • the counts in an appropriate energy region of interest (ROI) for the desired isotope are then integrated to determine the count rate.
  • ROI energy region of interest
  • An important part of the preferred implementation is the use of both OR and AND modes for data acquisition and analysis.
  • the use of a multichannel DSO for on line background rejection is disclosed.
  • the use of triangular shaping and software rejection of fast pulses due to signals induced by Cosmic Rays in PMT is disclosed.
  • the particular optimization, when using CaF 2 (Eu) scintillators is to have a pulse rise time of ⁇ 0.75 microseconds and a fall time of about 3 microseconds.
  • Self-diagnostic and self-calibration for reliably matching the count rates in OR and AND modes are important, including on-line baseline restoration and pileup rejection techniques.
  • coincident mode the use of DSO to match the shape and temporal coincidence of pulses from two detector modules are preferred.
  • On-line software- based pulse fitting procedures overcome these conflicting requirements.
  • the DE detection efficiency
  • the DE can be determined from the spectrum itself using the Eldridge formula.
  • the data acquisition hardware is mounted inside the dedicated PC controlling the MP- densitometer.
  • the data acquisition electronics consists of a triggering circuit, amplification/attenuation modules for each detector, 3 digital timer/counters, and a dual channel 20 MHz digital storage oscilloscope (DSO) which is used both as a 2-input pulse shape/height analyzer. Furthermore, additional DSO or two ADC are used to monitor detector temperamre.
  • DSO digital storage oscilloscope
  • the triggering circuit produces a rectangular trigger pulse whenever a pulse exceeding a preset threshold amplitude is registered in either detector. If pulses are registered simultaneously in both detectors, a higher amplimde trigger pulse is produced. It is thus possible to count separately coincident and non-coincident events.
  • the trigger pulse is sent to the external trigger input of the DSO or DSP.
  • the triggering circuit is proprietary and disclosed in the following.
  • the amplification/attenuation modules adjust the amplimdes of the pulses so that the region of interest is within the 0-1 Volt window of the DSO or DSP and that particles of the same energy produce pulses of the same amplimde in both channels.
  • the first of the 3 timer/counters is used as a precise acquisition time timer (counting the 2.5 kHz reference pulses).
  • the second timer/counter counts all trigger pulses produced by the triggering circuit, while the third counts only triggers associated with coincident events.
  • the data acquired from these counters are used to directly evaluate losses due to acquisition system dead time and thus enable the system to correctly count high activity sources.
  • the DSO (for example a CSLite manufactured by Gage Inc.) is capable of simultaneous sampling of two input channels with 8-bit accuracy and up to 20 MHz sampling rate and has an additional external trigger input.
  • the data are stored in onboard memory and can be transferred to the host PC RAM by standard memory-to-memory transfer via the DSO's 8- bit access to the PC bus.
  • the dead time is strictly non-extendable and by means of the counters described above we always correct for dead time losses.
  • the DSO is rearmed and initialized after each acquired and processed event.
  • the pulse traces are transferred from the DSO to the host PC memory and are analyzed for amplimde and shape by software.
  • the DSO is set up to continuously chart the input voltages in the two channels and wait for a triggering pulse in the trigger input.
  • a trigger pulse is registered, the DSO is allowed to capture a predetermined number of post-trigger points and is then stopped.
  • the relevant portion of the traces (typically 20 pre -trigger and 108 post-trigger points at 20 MHz sampling) is transferred to the host PC memory for analysis. The transfer procedure takes less than 200 microseconds per trace for a 486-DX66 computer.
  • the analysis begins with computation of the baseline and the pulse amplimdes in each detector. This shows whether the event occurred in detector A, detector B or both.
  • the pulse amplimdes are adjusted for the current baselines, and if the latter are unacceptably distorted the event is rejected. Then, a number of pulse shape parameters are evaluated and compared with the ranges of acceptable values established by the software at a system setup.
  • a not rejected event is added to the appropriate spectrum (spectrum of a detector A, spectrum of a detector B, or 2D spectrum of coincident events).
  • the DSO is reset for acquisition of the next event. Any events occurring during the processing time are lost (dead time).
  • the spectral data are processed, they are adjusted for this dead time.
  • the acquisition can be preset to collect data either for a given interval of time or until given statistics is acquired. The acquisition can also be terminated by the user at any time.
  • the software program contains a simple data file browser which allows viewing and analysis of data from single and series of measurements.
  • the user can select a data file to be viewed through a system of menus, see the estimated density and measurement uncertainty, plot the count rates vs. time from beginning of measurement series and print out the data with statistical uncertainties. Both the temperamre compensated and raw data can be accessed.
  • a more intensive analysis and merging of data can be performed using a commercial spreadsheet program.
  • the MP-densitometer software may be coded in Borland Pascal and Assembly language (to speed up the pulse processing) and can operate under DOS using a Windows-like GUI shell, or under MS-Windows using the DelphiTM software development system (Borland International), which uses the extended Borland Pascal language.
  • the software sets the acquisition rejection parameters for each newly assembled detector system.
  • This program determines the optimal trigger levels and pulse shape rejection parameters for the system and creates internal data files to store these parameters. These parameters generally do not have to be redetermined during the lifetime of the system unless a major component (e.g. , a PMT/base or DSO card) is replaced.
  • a major component e.g. , a PMT/base or DSO card

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Abstract

Un densitomètre multiphotons (densitomètre-MP) destiné à une télémesure de densité utilise des sources multiphotons spéciales présentant une très faible activité ne nécessitant pas d'autorisation, pour la mesure de la densité d'échantillons. Pour un mélange de gaz/huile/eau à l'intérieur de tubes en acier de 3 pouces, la précision de mesure, utilisant une source de 2 microCi, est sensiblement équivalente à celle obtenue avec un densitomètre gamma de la technique actuelle utilisant une source de 300 milliCi. Le densitomètre MP utilisant une source de 1 microCi mesure la dentisité, avec une imprécision inférieure à 1 %, de fluides se trouvant à l'intérieur de tubes d'une plage de diamètres allant jusqu'à 10 pouces. L'invention permet d'obtenir un fond très faible (ordres de grandeur inférieurs à ceux de densitomètres gamma de la technique actuelle) par la sélection d'éléments, de géométrie, d'électronique et de logiciels de densitomètres. La réduction des imprécisions du système, un plan de compensation de température, la régulation active de température, une analyse statistique en temps réel et un lissage du signal de sortie ont permis l'élimination des effets dûs à la température et de l'accumulation d'artefacts. Avec une source de très faible activité, le densitomètre MP présente une précision de mesures de densité de l'ordre de 1 % pour un flux laminaire d'huile/eau. L'imprécision est égale à 0,5 % pour des temps de mesure plus longs de l'ordre de quelques minutes.
PCT/US1997/002224 1996-02-07 1997-02-07 Procede et appareil de telemesure de densite WO1997029356A1 (fr)

Priority Applications (3)

Application Number Priority Date Filing Date Title
EP97906575A EP0879410A1 (fr) 1996-02-07 1997-02-07 Procede et appareil de telemesure de densite
AU21230/97A AU2123097A (en) 1996-02-07 1997-02-07 Method and apparatus for remote density measurement
NO983601A NO983601D0 (no) 1996-02-07 1998-08-05 Fremgangsmåte og anordning for fjernmåling av tetthet

Applications Claiming Priority (4)

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US1125796P 1996-02-07 1996-02-07
US60/011,257 1996-02-07
US66809996A 1996-06-20 1996-06-20
US08/668,099 1996-06-20

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WO (1) WO1997029356A1 (fr)

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WO2003021234A1 (fr) * 2001-09-06 2003-03-13 Commonwealth Scientific And Industrial Research Organisation Indicateurs de densite et de niveau possedant une source de rayons gamma a ultrafaible activite
WO2003042666A2 (fr) * 2001-11-10 2003-05-22 Schlumberger Technology B.V. Mesure de densite fluidique
GB2396907A (en) * 2002-12-31 2004-07-07 Schlumberger Holdings Monitoring solids in pipes
WO2008026936A1 (fr) * 2006-08-29 2008-03-06 Roxar Flow Measurement As Gammamètre oblique
CN101017126B (zh) * 2007-03-01 2010-05-19 丹东东方测控技术有限公司 双探测器在线密度测量方法和在线密度计
DE102009001641A1 (de) * 2009-03-18 2010-09-23 Endress + Hauser Gmbh + Co. Kg Radiometrische Messanordnung
RU2442889C1 (ru) * 2010-10-01 2012-02-20 Анатолий Георгиевич Малюга Способ градуировки радиоизотопных плотномеров
CN102879410A (zh) * 2012-08-22 2013-01-16 北京乾达源科技有限公司 一种在线测量油水气多相流含率的方法及装置
WO2013043074A1 (fr) * 2011-09-20 2013-03-28 Siemens Aktiengesellschaft Appareil de mesure de la composition d'un flux de mélange multiphasé
WO2014074004A1 (fr) * 2012-11-08 2014-05-15 Siemens Aktiengesellschaft Procédé de détermination de débit de constituants de mélange multiphasé
WO2016014411A1 (fr) * 2014-07-22 2016-01-28 Shell Oil Company Procédés de détection de dépôts de ligne d'écoulement par densitométrie à rayons gamma
DE102017130534A1 (de) * 2017-12-19 2019-06-19 Endress+Hauser SE+Co. KG Verfahren zum Kalibrieren einer radiometrischen Dichte-Messvorrichtung
EP4067863A3 (fr) * 2021-04-01 2022-10-12 Endress+Hauser SE+Co. KG Procédé d'étalonnage d'un dispositif de mesure radiométrique de densité
WO2023122186A1 (fr) * 2021-12-21 2023-06-29 Schlumberger Technology Corporation Procédé et appareil pour mesurer la concentration en sulfure d'hydrogène d'un mélange gazeux avec absorption de rayons gamma
CN117890257A (zh) * 2024-03-14 2024-04-16 南京愚工智能技术有限公司 一种放射性密度计安装结构及密度监测装置
CN117890257B (zh) * 2024-03-14 2024-05-24 南京愚工智能技术有限公司 一种放射性密度计安装结构及密度监测装置

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CN107331430B (zh) * 2017-08-10 2023-04-28 海默科技（集团）股份有限公司 一种多相流相分率测定装置双源双能级射线源仓

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US4145917A (en) * 1977-04-14 1979-03-27 Vsesojuzny Nauchno-Issledovatelsky I Konstruktorsky Institut "Tsvetmetavtomatika" Method of measuring properties of a fluid in a container and device for realizing same
US4284895A (en) * 1978-02-21 1981-08-18 Ira Lon Morgan Method and apparatus for tomographic examination of an object by penetrating radiation
US5331163A (en) * 1991-02-25 1994-07-19 Washington University Radioactive areal density detector with scintillating receiver
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Cited By (28)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2003021234A1 (fr) * 2001-09-06 2003-03-13 Commonwealth Scientific And Industrial Research Organisation Indicateurs de densite et de niveau possedant une source de rayons gamma a ultrafaible activite
AU2002337348B2 (en) * 2001-11-10 2008-03-13 Schlumberger Technology B.V. Fluid Density Measurement
WO2003042666A2 (fr) * 2001-11-10 2003-05-22 Schlumberger Technology B.V. Mesure de densite fluidique
WO2003042666A3 (fr) * 2001-11-10 2004-02-05 Schlumberger Technology Bv Mesure de densite fluidique
GB2405694A (en) * 2001-11-10 2005-03-09 Schlumberger Holdings Fluid density measurement
GB2405694B (en) * 2001-11-10 2006-05-10 Schlumberger Holdings Fluid density measurement
US7206376B2 (en) 2001-11-10 2007-04-17 Schlumberger Technology Corporation Fluid density measurement
GB2396907A (en) * 2002-12-31 2004-07-07 Schlumberger Holdings Monitoring solids in pipes
GB2396907B (en) * 2002-12-31 2005-03-16 Schlumberger Holdings Method and apparatus for monitoring solids in pipes
US7402796B2 (en) 2002-12-31 2008-07-22 Schlumberger Technology Corporation Method and apparatus for monitoring deposition of solids in pipelines using a plurality of radiation sources pointing to a unique detector
US7978815B2 (en) 2006-08-29 2011-07-12 Roxar Flow Measurement As Compact gammameter
WO2008026936A1 (fr) * 2006-08-29 2008-03-06 Roxar Flow Measurement As Gammamètre oblique
WO2008026935A1 (fr) * 2006-08-29 2008-03-06 Roxar Flow Measurement As Gammamètre compact
CN101017126B (zh) * 2007-03-01 2010-05-19 丹东东方测控技术有限公司 双探测器在线密度测量方法和在线密度计
DE102009001641B4 (de) 2009-03-18 2023-10-19 Endress+Hauser SE+Co. KG Radiometrische Messanordnung
DE102009001641A1 (de) * 2009-03-18 2010-09-23 Endress + Hauser Gmbh + Co. Kg Radiometrische Messanordnung
RU2442889C1 (ru) * 2010-10-01 2012-02-20 Анатолий Георгиевич Малюга Способ градуировки радиоизотопных плотномеров
WO2013043074A1 (fr) * 2011-09-20 2013-03-28 Siemens Aktiengesellschaft Appareil de mesure de la composition d'un flux de mélange multiphasé
CN102879410A (zh) * 2012-08-22 2013-01-16 北京乾达源科技有限公司 一种在线测量油水气多相流含率的方法及装置
WO2014074004A1 (fr) * 2012-11-08 2014-05-15 Siemens Aktiengesellschaft Procédé de détermination de débit de constituants de mélange multiphasé
WO2016014411A1 (fr) * 2014-07-22 2016-01-28 Shell Oil Company Procédés de détection de dépôts de ligne d'écoulement par densitométrie à rayons gamma
CN111542743A (zh) * 2017-12-19 2020-08-14 恩德莱斯和豪瑟尔欧洲两合公司 用于校准辐射式密度测量装置的方法
DE102017130534B4 (de) * 2017-12-19 2020-12-03 Endress+Hauser SE+Co. KG Verfahren zum Kalibrieren einer radiometrischen Dichte-Messvorrichtung
DE102017130534A1 (de) * 2017-12-19 2019-06-19 Endress+Hauser SE+Co. KG Verfahren zum Kalibrieren einer radiometrischen Dichte-Messvorrichtung
EP4067863A3 (fr) * 2021-04-01 2022-10-12 Endress+Hauser SE+Co. KG Procédé d'étalonnage d'un dispositif de mesure radiométrique de densité
WO2023122186A1 (fr) * 2021-12-21 2023-06-29 Schlumberger Technology Corporation Procédé et appareil pour mesurer la concentration en sulfure d'hydrogène d'un mélange gazeux avec absorption de rayons gamma
CN117890257A (zh) * 2024-03-14 2024-04-16 南京愚工智能技术有限公司 一种放射性密度计安装结构及密度监测装置
CN117890257B (zh) * 2024-03-14 2024-05-24 南京愚工智能技术有限公司 一种放射性密度计安装结构及密度监测装置

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CA2245813A1 (fr) 1997-08-14
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NO983601D0 (no) 1998-08-05

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