EP0189438A1 - Appareil pour inhibition optique d'un echantillon - Google Patents

Appareil pour inhibition optique d'un echantillon

Info

Publication number
EP0189438A1
EP0189438A1 EP19850903094 EP85903094A EP0189438A1 EP 0189438 A1 EP0189438 A1 EP 0189438A1 EP 19850903094 EP19850903094 EP 19850903094 EP 85903094 A EP85903094 A EP 85903094A EP 0189438 A1 EP0189438 A1 EP 0189438A1
Authority
EP
European Patent Office
Prior art keywords
sample
quench
photodetector
pulse height
liquid crystal
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Withdrawn
Application number
EP19850903094
Other languages
German (de)
English (en)
Inventor
Charles A. Keenan
Donald L. Horrocks
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Beckman Coulter Inc
Original Assignee
Beckman Instruments Inc
Beckman Industrial Corp
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Beckman Instruments Inc, Beckman Industrial Corp filed Critical Beckman Instruments Inc
Publication of EP0189438A1 publication Critical patent/EP0189438A1/fr
Withdrawn legal-status Critical Current

Links

Classifications

    • G—PHYSICS
    • G01—MEASURING; TESTING
    • G01T—MEASUREMENT OF NUCLEAR OR X-RADIATION
    • G01T1/00—Measuring X-radiation, gamma radiation, corpuscular radiation, or cosmic radiation
    • G01T1/16—Measuring radiation intensity
    • G01T1/20—Measuring radiation intensity with scintillation detectors
    • G01T1/204—Measuring radiation intensity with scintillation detectors the detector being a liquid
    • G01T1/2042—Composition for liquid scintillation systems
    • G01T1/2045—Liquid scintillation quench systems
    • G—PHYSICS
    • G02—OPTICS
    • G02F—OPTICAL DEVICES OR ARRANGEMENTS FOR THE CONTROL OF LIGHT BY MODIFICATION OF THE OPTICAL PROPERTIES OF THE MEDIA OF THE ELEMENTS INVOLVED THEREIN; NON-LINEAR OPTICS; FREQUENCY-CHANGING OF LIGHT; OPTICAL LOGIC ELEMENTS; OPTICAL ANALOGUE/DIGITAL CONVERTERS
    • G02F1/00—Devices or arrangements for the control of the intensity, colour, phase, polarisation or direction of light arriving from an independent light source, e.g. switching, gating or modulating; Non-linear optics
    • G02F1/01—Devices or arrangements for the control of the intensity, colour, phase, polarisation or direction of light arriving from an independent light source, e.g. switching, gating or modulating; Non-linear optics for the control of the intensity, phase, polarisation or colour 
    • G02F1/13—Devices or arrangements for the control of the intensity, colour, phase, polarisation or direction of light arriving from an independent light source, e.g. switching, gating or modulating; Non-linear optics for the control of the intensity, phase, polarisation or colour  based on liquid crystals, e.g. single liquid crystal display cells
    • G02F1/1313—Devices or arrangements for the control of the intensity, colour, phase, polarisation or direction of light arriving from an independent light source, e.g. switching, gating or modulating; Non-linear optics for the control of the intensity, phase, polarisation or colour  based on liquid crystals, e.g. single liquid crystal display cells specially adapted for a particular application

Definitions

  • the present invention relates generally to liquid scintillation counting and, more particularly, to an appa ⁇ ratus for the optical quench of a sample.
  • Liquid scintillation techniques are well known for measuring the activity of samples containing radionuc- lides.
  • a radioactive sample typically a beta emit ⁇ ter
  • a * liquid scintillation medium is dissolved or suspended in a * liquid scintillation medium.
  • Nuclear disintegrations occurring in the sample produce visible light flashes or scintillations in the scintillation medium with the amount of light emitted from a scintillation being proportional to the energy of the corresponding disintegration.
  • a liquid scintillation counter measures the relative intensities of scintillations occurring ⁇ in the liquid scintillation medium.
  • scintillations occurring within the scintillating medium are detected ' by a suitable photodetector which produces output pulses having pulse heights proportional to the intensity of the detected scintillations.
  • the liquid scintillation counter counts the pulses in a plurality of pulse height channels or "windows" having, upper and lower pulse height limits that together span a predetermined range of pulse heights. The counts accumulated in each window may then be plotted with respect to corresponding pulse heights to provide a pulse
  • counting efficiency The scintillation count rate detected in a quenched sample as compared with the disin- tegration...rate occurring within the sample is commonly referred to as "counting efficiency".
  • Quenching acts equally on all events produced by the same type of excitation particle, for example, electron (beta), alpha, proton, and so on. Thus, if quenching is sufficient to reduce the measured response for one disin ⁇ tegration by a given percentage, it will reduce all res ⁇ ponses by the same percentage. In a liquid scintillation counter, quenching results in a shift of the pulse height spectrum detected by the counter to lower pulse height values, which is commonly referred to as "pulse height shift".
  • a quench curve which plots counting efficiency with respect to the amount or degree of quench.
  • the quench curve may then be used to correct the count rate of a sample for the effects of quench.
  • the quench of one or more samples is varied. For each degree of quench, the sample counts per unit time is measured for some predeter ⁇ mined portion of the pulse height spectrum. By dividing the counts per unit time for such portion of the pulse height spectrum by the disintegrations per unit time occurring in the sample, the efficiency for each degree of quench is determined.
  • a quench curve is then constructed by plotting efficiencies determined as just described versus the measured degree of quench.
  • U.S. Patent 3,688,120 discloses externally varying sample quench by either moving the photodetectors away from the sample or introducing mechanically driven variable aperture iris type lenses, between the sample and the photodetectors.
  • the former technique requires that shielding surrounding the counting chamber be enlarged to accom ⁇ modate the movement of the photodetectors, an important drawback where a compact, light-weight liquid scintilla ⁇ tion counter is desired.
  • the latter technique also suffers from an important disadvantage, namely, the iris lenses mechanically obscure portions of the sample from the photodetectors, thereby optically quenching the sample in a nonuniform fashion.
  • the apparatus of the present invention overcomes the disadvantages and drawbacks of the prior art and provides an apparatus for optical quench which is compact, easily placed between the sample and the photodetectors, which provides uniform attenuation and thus uniform quench, and which provides repeatable quench levels.
  • an apparatus in accordance with the present invention includes a photodetector, means for positioning a sample in an operative relationship with respect to the photodetector, and a liquid crystal light valve disposed between the sample and the photodetector when the sample is in the operative relationship.
  • the liquid crystal light valve in response to an attenuation signal, varies its light transmission characteristic.
  • a power supply provides the attenuation signal to the liquid crystal light valve.
  • the apparatus may further include means responsive to the photodetector for generating a control signal.
  • the power supply is responsive to the control signal to there ⁇ by vary the attenuation signal and thus vary the attenua ⁇ tion of the liquid crystal light valve.
  • Fig. 1 is a block diagram of a liquid scintillation counting system for practicing the method of the present invention.
  • Fig. 2 is a graphical plot of pulse height distribu ⁇ tion spectra of a liquid scintillation sample at three varying levels of quench.
  • Fig. 3 is a graphical plot of log CP versus normal ⁇ ized values (R) of pulse height values PH.
  • Fig. 4 is a graphical plot of a quench curve deter ⁇ mined in accordance with the present invention.
  • Fig. 5 is a graphical plot of a pulse height spectrum for a radionuclide contained in an unknown sample wherein the DP of such sample for various portions of the pulse height spectrum are determined in accordance with the present invention.
  • a liquid scintillation counting system in accordance with the pre ⁇ sent invention.
  • the scintillation counting system is arranged ..to. measure radioactivity issuing from a sample generally indicated at 10 and comprising a vial disposed within a shielded counting chamber and containing a liquid scintillation medium and sample.
  • a pair of photomulti- plier tubes (PMTs) 12 and 14 is arranged to detect and convert the scintillations of the sample 10 to correspond ⁇ ing output voltage pulses, each such pulse haying an amp ⁇ litude proportional to the photon intensity of the corres ⁇ ponding scintillation detected.
  • the PMTs 12 and 14 pro ⁇ prise a pair of coincident output pulses for each detected scintillation.
  • the quenching means 15 includes means for optically varying the apparent quench of the sample 10 as detected by the PMTs 12 and -6-
  • the sample optical quenching means 15 includes two liquid crystal light valves 15a and 15b dis ⁇ posed between the sample 10 and the PMTs 12 and 14, res ⁇ pectively.
  • the light valves 15a and 15b variably attenu ⁇ ate the light from scintillations occuring within the sample 10 in response to an adjustable AC voltage from a controllable voltage source 15c of conventional design.
  • the adjustable voltage may be adjustable over a range of about 3 volts to 30 volts AC (rms), and may have a frequency in the range of about 30 Hz to 1000 Hz.
  • the controllable voltage source 15c is in turn controlled by means of a control signal generated as is described hereinbelow.
  • the liquid crystal light valves may be, for example, of a type CIN available from UCE, Inc., Norwalk, Connecticut.
  • An example of a suitable commercially available power supply usable as the controllable voltage source 15c is a Model 3310A available 'from Hewlett-Packard Company.
  • each of-the- PMTs 12 and 14 is coupled as an input to a combined pulse summation circuit and amplifier 16, the output of which is an analog pulse.
  • a combined pulse summation circuit and amplifier 16 the output of which is an analog pulse.
  • each PMT 12 and 14 is also coupled as an input to a coincidence circuit 18 which produces an output pulse upon receipt of essentially coincident input pulses.
  • the outputs from the pulse summation and ampli ⁇ bomb 16 and the coincidence circuit 18 are both applied to an analog gate 20 which passes the analog output from the - 7- pulse summation and amplifier 16 when the output pulse from the coincidence circuit 18 is also received by the gate 20.
  • the coinci ⁇ dent pulses from such PMTs 12 and 14 are summed by the pulse summation and amplifier 16 and are applied to the gate 20.
  • the coincident pulses from the PMTs 12 and 14 are also detected by the coincidence circuit 18 which applies a pulse to the gate 20.
  • the coincidence circuit 18 In the presence of the output pulse from the coincidence circuit 18, the analog output pulse from the pulse summation and amplifier 16 is passed by the gate 20.
  • the output of the gate 20 is applied to an analog-to- digital (ADC) logarithmic pulse height converter 22 which provides a digital output logarithmically proportional to the height of the analog pulse applied thereto.
  • ADC analog-to- digital
  • the digi ⁇ tal output of the ADC pulse height converter 22 is applied to a microprocessor-based control unit 24.
  • the control unit 24 is of conventional design and includes a micro ⁇ processor--and related memory and input-output interface units, all well known in the art.
  • the control unit 24 compares the value of the digial output from the ADC pulse height converter 24 to a " plurality of predetermined values which define a plurality of energy ranges or windows to ⁇ gether spanning a predetermined energy or pulse height range.
  • the control unit 24 determines which window the digital value falls within and accordingly increments one storage location within a pulse height distribution storage area 26.
  • the pulse height distribution storage area 26 includes a plur ⁇ ality of storage locations corresponding to the windows established by the control unit 24. As the liquid scin ⁇ tillation counting process is performed, the values stored in the various storage locations within the storage area -8-
  • the storage area 26 may comprise, for example, a portion of the memory accessible to and controlled by the micro ⁇ processor within the control unit 24, each storage loca ⁇ tion within such storage area 26 being cleared or reset prior to the start of a liquid scintillation counting procedure.
  • the control unit 24 also directs the positioning of the sample 10 within a counting chamber by a conventional sample positioning means 28.
  • the control unit 24 further actuates conventional external standard positioning means 30 for selectively positioning an external standard source, such as a cesium-137 gamma source, in an operative position for irradiating the sample 10 to generate a Comp- ton pulse height spectrum.
  • the control unit 24 also provides the control signal to the sample quenching means 15 and in the embodiment of Fig. 1 in particular to the controllable voltage source 15c. As described above, the degree of optical quenching of the sample 10 is varied in response -to_ the control signal from the control unit 24.
  • the control signal may be either analog or digital depending upon the particular circuitry within the variable voltage source 15c, all of which may be accomplished using conven ⁇ tional means.
  • the liquid scintillation counting system of Fig. 1 further includes a conventional display unit 32 such as a cathode ray tube (CRT) and a suitable input device such as a keyboard 34.
  • the display unit 32 can display the count rate derived in a particular window or may display a curve graphically showing the pulse height distribution spec ⁇ trum.
  • the display unit 32 also displays a pulse height value PH corresponding to an inflection point I on the Compton edge automatically located and determined as des- -9- cribed hereinbelow and as also described in U.S. Pat. 4,075,480 referenced above.
  • Fig. 1 is essentially a conventional multichannel liquid scintillation counting system or ana ⁇ lyzer modified in accordance with the teachings of the present invention.
  • Such conventional multichannel analyz ⁇ ers are well known in the art such as, for example, the 5800 and 9800 series liquid scintillation counters avail ⁇ able from Beckman Instruments, Inc.
  • the apparatus of Fig. 1 optically varies the quench of the single sample 10.
  • the system measures the CPM of the sample within a window wide enough, to include all detected pulses produced by the sample, the CPM of the sample occurring within a predeter ⁇ mined window, sometimes referred to hereinafter as a "cal ⁇ ibration window", and the pulse height of a unique point on the pulse height spectrum when the sample is exposed to the standard source.
  • the DPM of the single sample is then determined using the method of U.S. Patent 4,060,728 which is assigned to the assignee of the present application and which is incorpoated by reference herein. For each CPM measurement within the calibration window, the efficiency is determined by dividing such CPM by DPM.
  • a quench rela ⁇ tionship may then be generated by relating efficiency of each such CPM measurement to an indication of quench for each such measurement.
  • a single sample in accordance with the method of the present invention uniquely yields a quench relationship or curve from a single sample without destroying the sample or relying upon DPM determined by pipetting a calibration standard into the sample.
  • the DPM for an unknown sample may be determined using the quench relationship uniquely developed as just described. To do so, the CPM within the calibration window and quench are measured for the unknown sample. Having determined the quench, the efficiency for such sample is determined from the quench relationship. The DPM for the sample may then be found by dividing the CPM by the efficiency.
  • the control unit 24 begins by command ⁇ ing the sample positioning means 28 to position the sample 10 within the counting chamber adjacent the PMTs 12 and 14.
  • the control unit 24 also adjusts the sample optical quenching means 15 for a first amount of quench which, in the embodiment disclosed herein, is a minimum amount of quench.
  • the control unit 24 generates the control -signal that is applied to the controllable voltage source 15c to thereby control the output of the voltage source 15c such that the valves 15a and 15b provide a minimum of optical attenuation.
  • the control unit 24 com ⁇ mands the standard source positioning means 30 to position the standard source into an operative position adjacent the sample 10 for irradiating the sample 10. , he system counts the pulses from the PMTs 12 and 14 in a plurality of counting windows to determine the counts developed for both the standard source and the sample.
  • the control unit 24 commands the standard source positioning means 30 to remove the standard source from its operative position to an inoperative position where the standard source does not contribute to the scintillations occurring within the sample 10.
  • the system again counts pulses from the PMTs 12 and 14 in a plurality of counting windows to determine -li ⁇ the counts developed for the sample alone.
  • the net counts developed in response to standard source are then deter ⁇ mined for the various counting windows by subtracting the counts obtained for the sample alone from the counts obtained for both the standard source and the sample. Such net counts are used to plot a standard source pulse height curve 50 as seen in Fig. 2.
  • the control unit 24 determines a unique point on the pulse height curve which in the preferred embodiment is the inflection point I- j _ of the curve 50.
  • a preferred method for locating such inflection point of the Compton edge, that is, where the second derivative of the edge is zero, is described in U.S. Patent 4,075,480 which is in ⁇ corporated herein by reference. Briefly, the inflection point is located by counting in a plurality of windows along the Compton edge and by calculating the second deri ⁇ vative (that is, the slope of the slope of the edge) at spaced points along the edge by subtracting the counts of adjacent counting windows.
  • the inflection point When a group of two spaced derivatives, is obtained, one positive and one negative, the inflection point is thus determined to be between the locations of the two derivatives. Thereafter, conven ⁇ tional interpolation techniques are employed to determine the exact location of the inflection point I ] _ between the derivative values.
  • the corresponding pulse height value PH* j _ is determined by the control unit 24 and may be displayed, for example, on the display unit 32.
  • control unit 24 adjusts the lower and upper window limits corresponding to a selected storage location within the storage area 26 to establish a window W (Fig. 2) wide enough to include all the pulses issuing from the sample -12-
  • the lower limit of the win ⁇ dow W is set at zero plus height while the upper limit of the window W is set a sufficient distance outward on the pulse height axis so that the window W includes all of the pulses issuing from the sample alone.
  • the sample alone may have a pulse height spectrum 52 which is completely included within the window W.
  • the count rate for the sample alone within window W is designated CPM* j _.
  • the control unit 24 may sum the contents of the storage locations within the stor ⁇ age area 26 which together span the window W rather than readjusting the upper and lower window limits for a selec ⁇ ted storage location as just described. In either case, the control unit 24 operates such that the system of Fig. 1 counts all of the pulses issuing from the sample alone, i.e. CPM ] _.
  • the sample is also counted within a predetermined or calibration window to provide a " value CP_MC- ] _.
  • the control unit 24 varies the control signal applied to the sample optical quenching means- 15 so as to vary the optical quench of the sample 10.
  • the control signal is applied to the controllable voltage source 15c, causing the output of the voltage source 15c to vary and correspondingly in ⁇ crease the attenuation of the liquid crystal light valves 15a and 15b, thereby increasing the optical quench of the sample 10.
  • the control unit 24 again positions the stan ⁇ dard source first in an operative relationship and then in an inoperative relationship with the sample 10, determines -13- a second unique point I2 on a second curve 54 (Fig. 2), and counts the sample 10 alone in the window W, all in a manner as previously described.
  • a pulse height curve for the sample 10 above is as shown by curve 53 of Fig. 2.
  • the system of Fig. 1 repeats the steps just described for varying degrees of optical quench, thereby generating a plurality of unique pulse height values PH * j_-PH n and corresponding CPM and CPMC values, CPM-j_ through and in ⁇ cluding CPM n and CPMCJL through and including CPMC n .
  • One such value PH3 may correspond to an inflection point I3 on a third curve 56 as seen in Fig. 2.
  • the sample 10 alone may have a pulse height curve 58 for the degree of quench represented by PH3.
  • the DPM for the sample 10 is determined in accord ⁇ ance with the teachings of U.S. Patent 4,060,728 which is incorporated herein by reference.
  • the pulse heigh_t values are normalized with respect to some selected common pulse height value to provide a plurality of normalized values R* j _ through and including R n for the corresponding pulse height values.
  • the values of R are correla ⁇ ted with corresponding pulse counts CPM* j _ through and in ⁇ cluding CPM n as by graphically plotting log CPM with res ⁇ pect to R as illustrated in Fig. 3.
  • the antilog of such a value determines the sample disin ⁇ tegration rate or DPM. -14-
  • a quench relationship or quench curve in accordance with the present invention may now be determined.
  • the quench relationship or curve is de ⁇ rived from a single optically quenched sample, providing advantages heretofore unattainable in the art.
  • a corresponding efficiency is determined by dividing CPMC by DPM. If efficiency is to be expressed in percentage, the result of the division is multiplied by 100.
  • a corresponding quench representation is also determined.
  • such quench representation is re ⁇ ferred to as an H number.
  • the H number for each CPMC value and corresponding efficiency is found, in a system where pulse height is related to log energy, by subtract ⁇ ing the unique pulse height value corresponding to the CPM value from a reference pulse height value, PH 0 .
  • the ref ⁇ erence pulse height value PH 0 is preferably obtained using a sealed unquenched sample as is known in the art. It is to be noted., however, that any one of the pulse height values could be used as a reference.
  • CP C2 a corresponding efficiency is obtained by dividing CPMC2 by DPM and multiplying by 100.
  • the corresponding quench indication is found by subtracting PH2 from PH *
  • the resulting quench representation is H2.
  • efficiencies and quench indications are determined for the remaining values of CPMC determined above, that is, CPMC 2 through and including CPMC n . Effi ⁇ ciency is then plotted with respect to quench indication (H number) to provide a quench relationship or curve 60 as seen in Fig. 4.
  • quench indication H number
  • the method in accordance with the present invention enables the determination of the quench curve 60 (Fig. 4) from a single sample using optical quen ⁇ ching.
  • the quench curve 60 may be used to determine DPM for an un ⁇ known sample.
  • the unknown sample when counted alone may yield a pulse height curve 62 as shown in Fig. 5.
  • the Compton edge inflection point may correspond, for example, to a pulse height PH U of 700.
  • the H number of 135 corresponds to an efficiency of 40%.
  • the CPMC for the calibration window may be corrected to yield DPM by dividing the CPMC for the calibration window by percent efficiency and multiplying the result by 100.
  • the CPMC within the calibration window for the un ⁇ known sample is 100,000. Consequently, DPM for the unknown sample is 250,000.

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  • Physics & Mathematics (AREA)
  • General Physics & Mathematics (AREA)
  • Nonlinear Science (AREA)
  • Health & Medical Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Molecular Biology (AREA)
  • Spectroscopy & Molecular Physics (AREA)
  • Chemical & Material Sciences (AREA)
  • Crystallography & Structural Chemistry (AREA)
  • Optics & Photonics (AREA)
  • Measurement Of Radiation (AREA)

Abstract

Appareil pour inhiber optiquement un échantillon (10), comprenant un photodétecteur (12, 14), un dispositif pour placer le dispositif en une position opérationnelle par rapport au photodétecteur, et un relais optique à cristaux liquides (15) placé entre l'échantillon et le photodétecteur lorsque l'échantillon est en relation opérationnelle. Les caractéristiques de transmission de lumière du relais optique à cristaux liquides varient en réponse à un signal d'atténuation produit par un dispositif d'alimentation. L'appareil peut en outre inclure des dispositifs sensibles au photodétecteur pour produire un signal de commande, et le dispositif d'alimentation peut en outre être sensible au signal de commande pour faire varier le signal d'atténuation en fonction de celui-ci.
EP19850903094 1984-05-21 1985-05-15 Appareil pour inhibition optique d'un echantillon Withdrawn EP0189438A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
US61217984A 1984-05-21 1984-05-21
US612179 1990-11-13

Publications (1)

Publication Number Publication Date
EP0189438A1 true EP0189438A1 (fr) 1986-08-06

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Family Applications (1)

Application Number Title Priority Date Filing Date
EP19850903094 Withdrawn EP0189438A1 (fr) 1984-05-21 1985-05-15 Appareil pour inhibition optique d'un echantillon

Country Status (4)

Country Link
EP (1) EP0189438A1 (fr)
JP (1) JPS61502217A (fr)
FI (1) FI860290A (fr)
WO (1) WO1985005459A1 (fr)

Families Citing this family (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2013037008A (ja) * 2012-10-01 2013-02-21 National Agriculture & Food Research Organization プラスチックシンチレータを検出器とした放射能探査装置

Family Cites Families (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3688120A (en) * 1967-04-14 1972-08-29 Packard Instrument Co Inc Data processing system employing quench simulation for enabling accurate computation of sample activity levels in liquid scintillation spectrometry
FR2117748A1 (en) * 1970-12-15 1972-07-28 Drouot Lucien Photomultiplier tubes - improved to cut out cross-talk noise
US4019807A (en) * 1976-03-08 1977-04-26 Hughes Aircraft Company Reflective liquid crystal light valve with hybrid field effect mode
US4060728A (en) * 1976-06-14 1977-11-29 Beckman Instruments, Inc. Method of measuring the disintegration rate of beta-emitting radionuclide in a liquid sample
PL109251B1 (en) * 1977-10-12 1980-05-31 Inst Badan Jadrowych Device for damping light stream,specially for additional extinction of scintillation in measurements of activity of radioactive isotopes

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
See references of WO8505459A1 *

Also Published As

Publication number Publication date
FI860290A0 (fi) 1986-01-21
FI860290A (fi) 1986-01-21
JPS61502217A (ja) 1986-10-02
WO1985005459A1 (fr) 1985-12-05

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