WO2001055697A1 - Algorithmes prevus pour un appareil spectrophotometrique manuel - Google Patents

Algorithmes prevus pour un appareil spectrophotometrique manuel Download PDF

Info

Publication number
WO2001055697A1
WO2001055697A1 PCT/IB2001/000275 IB0100275W WO0155697A1 WO 2001055697 A1 WO2001055697 A1 WO 2001055697A1 IB 0100275 W IB0100275 W IB 0100275W WO 0155697 A1 WO0155697 A1 WO 0155697A1
Authority
WO
WIPO (PCT)
Prior art keywords
spectmm
sample
collected
stored
spectrum
Prior art date
Application number
PCT/IB2001/000275
Other languages
English (en)
Inventor
Andrew P. Davey
David Gray
Kevin Mellon
Seamus Curran
Nathan COWDEN
Original Assignee
Inspace Limited
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 Inspace Limited filed Critical Inspace Limited
Priority to AU2001234012A priority Critical patent/AU2001234012A1/en
Publication of WO2001055697A1 publication Critical patent/WO2001055697A1/fr

Links

Classifications

    • GPHYSICS
    • G01MEASURING; TESTING
    • G01JMEASUREMENT OF INTENSITY, VELOCITY, SPECTRAL CONTENT, POLARISATION, PHASE OR PULSE CHARACTERISTICS OF INFRARED, VISIBLE OR ULTRAVIOLET LIGHT; COLORIMETRY; RADIATION PYROMETRY
    • G01J3/00Spectrometry; Spectrophotometry; Monochromators; Measuring colours
    • G01J3/28Investigating the spectrum
    • GPHYSICS
    • G01MEASURING; TESTING
    • G01NINVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
    • G01N21/00Investigating or analysing materials by the use of optical means, i.e. using sub-millimetre waves, infrared, visible or ultraviolet light
    • G01N21/17Systems in which incident light is modified in accordance with the properties of the material investigated
    • G01N21/25Colour; Spectral properties, i.e. comparison of effect of material on the light at two or more different wavelengths or wavelength bands
    • G01N21/31Investigating relative effect of material at wavelengths characteristic of specific elements or molecules, e.g. atomic absorption spectrometry

Definitions

  • This invention relates generally to the field of anti-counterfeiting measures and more particularly relates to hand held spectrophotometer based devices, improved algorithms for data interpretation and methods of use.
  • tags often include fluorescent labels or other dye-like substances which, upon proper illumination, provide a specific pattern or spectrum of light emission.
  • Some of these techniques are used, for example, with currency where a previously imprinted dye is detected with an ultraviolet light, a simple procedure.
  • detection methods are relatively simple to counterfeit in that they qualitatively determine the presence or absence of a label which is itself easily detected.
  • the counterfeiter can easily determine that currency under UV illumination has one or more areas labeled with a fluorescent dye which he can then paint onto his counterfeit currency to thereby duplicate the effect of the original bill.
  • Spectrophotometers While more complex dyes are available which require specific wavelengths of illumination and which emit or fluoresce at specific spectral frequencies, such substances typically require the use of a spectrophotometer to identify their presence. Spectrophotometers have traditionally been large bench top instruments and are not portable in nature.
  • Microparts an integrated circuit that can perform some spectrophotometric related detection operations.
  • the Microparts unit relies upon an external PC or other computerized processing unit, as well as external devices for receiving and handling the optically detected output spectrum.
  • the various aspects and principles are addressed with the present invention which provides a hand-held spectrophotometric device capable of providing the necessary illumination to excite one or more light sensitive labels, which upon excitation, emit light at specified frequencies.
  • the hand-held device of the present invention includes a power source, an illumination source, a light emission detector, and a central processing unit capable of interacting with data handling instructions including comparing detected signals against preset conditions to provide a quantitative or qualitative readout with respect to the presence or absence of one or more specific label substances.
  • the apparatus of the present invention may optionally include additional readout ports suitable for communicating real or stored values to other data accumulating or handling devices such as computers, modems, printers and the like.
  • the present invention provides novel algorithms for handling the data provided by the optical detector whereby false readouts occurring from spurious background illumination, varying distances to the object being tested, aging or faulty optical detectors and the like are substantially reduced if not eliminated.
  • Figure 1 provides a block diagram showing the general electronic construction of major compounds of a hand-held spectrophotometric apparatus of the present invention
  • Figure 2 shows a typical three peak sample spectrum
  • Figure 3 shows the three peak spectrum after the 1 st derivative operator
  • Figure 4 shows the basic mechanical construction of the spectrophotometric optical detector
  • Figure 5 shows sample and reference spectra divided into a grid of rectangles for ZPX analysis
  • Figure 6 shows the Algorithm of the entire check routine
  • Figure 7 shows the Algorithm of the ZPX analysis
  • Figure 8 shows the Algorithm of the ZPX program code
  • Figure 9 shows an incremental step in processing
  • Figure 10 shows a portion of the computational step of the preferred algorithm. Detailed Description and Best Mode
  • FIG. 1 there is shown an electronic block diagram of the instant invention.
  • the central processing unit 10 which controls operation of the device in response to switch inputs 16, instructions from external memory 12 as well as data delivered from the analogue to digital ("A-to-D") converter 19 via the amplifier 24.
  • a CPU particularly capable of implementing the algorithms described hereafter is the ATMEGA 603/103 available from Atmel(USA).
  • the ATMEGA103 advantageously has an 8 channel, 10 bit A-to-D converter, 128K of ROM 12 which is useful for storage of algorithms and other data handling routines. 4K of RAM can be advantageously used for calculations and additionally, there is 4K of EEPROM which can be advantageously used to store results.
  • Power supply 17 provides power to the ATMEGA 103 and energizes related peripheral devices including the spectrum processing chip 20, the illumination LED 23, timers 11, external memory 12, and LCD interface 13.
  • Power supply 17 ideally may comprise any of a number of conventional sources of power and while it may rely on externally supplied "wall" power, the preferred embodiment will utilize a battery supply.
  • the battery may be of rechargeable type and the power supply 17 may be configured to provide for recharging of the batter)' given an external power supply or docking station.
  • Drivers 18 control spectrometer chip 20 which may be obtained from Microparts, (Germany), Laubscher or Ocean Optics(US).
  • the spectrometer chip collects the spectrum data mechanically as shown in Figure 4.
  • Fiber optic cable 21 gathers light irradiated from the object being illuminated (not shown) and conveys it to grating 43 which disperses the light into a spectrum of wavelengths, approximately 7nm apart, which are then conducted to pixels 44.
  • the pixels are light sensitive semi-conductor
  • the spectrophotometer chip 20 may be advantageously controlled by periodic timed pulses which first initiate a collection phase during which data accumulates and then terminate the collection phase.
  • the spectrum is spread across 256 pixels with each pixel having a value between 0 and 1,024. These values represent the height of the signal and directly relate to the amount of light impacting the pixel. Each pixel represents a different wavelength.
  • the collecting phase and amplification are set so as to achieve an adequate signal.
  • the spectrophotometer chip 20 is controlled by six separate pulses sent with a specified length and delay relative to each other as stated in the spectrophotometer chip manufacturer specification. All six pulses may be generated by software driven counters in the CPU 10. The pulse lengths may be set using the internal clock while pulse width modulation of the clock provides the relative delays, or alternatively the pulse lengths may be set by the software driven counters in CPU 10.
  • an initial pulse starts the collection of data with a subsequent pulse acting as a stop signal. Once the start pulse has been sent, the A-to-D under software control will sample and store all the amplified data accumulated since the previous start pulse.
  • the stop signal is ideally generated by software so that integration times can be easily adjusted as necessary.
  • one of the counters supplied by the ATMEGA 103 may be polled until it reaches a set value at which time a start pulse is sent synchronizing it with all other signals.
  • all data accumulated since the previous start pulse is sent to the A-to-D converter 19 via amplifier 24.
  • a short initial integration time is used in order to flush any residual signal from the CCD 20 before the actual signal is read at the end of the next start pulse.
  • the A-to-D converter 19 can be controlled by polling one of the counters until a set value is reached and then calling the A-to-D converter 19.
  • the digitized value is stored in external memory 12 and the memory address incremented before the next data value is read. This process may be repeated until all CCD pixel locations have been stored.
  • a sample (not shown) is excited by illumination from a light source such as a light emitting diode (LED) 23 which ideally may be controlled by switch 22 for power saving purposes.
  • LED 23 is preferably a UN emitting diode which has a peak emission at approximately 370 nm. Selection of an LED with emissions in this range more readily permits measurement of the reflectance of the substrate or object to be measured. It has been discovered that the physical orientation of LED 23 and fiber optic collection cable 21 is important and is ideally manipulated, optionally with a UV filter, so that the amount of light from the LED 23 which is reflected into fiber cable 21 is minimized while permitting the fiber collection head to be placed as close to the sample as reasonably possible in order to collect a maximal signal.
  • spectrophotometer chip 20 ideally provides for a calibrated grating from approximately 380 to 790 nanometers, due to reflectance generally from substrates, a substantial portion of the incident UV from LED 23 is returned directly to the fiber head without alternation. Since this data contains no information, it is ideally discarded and this may be accomplished within the software controlling CPU 10. Accordingly, one embodiment of the present invention advantageously provides for analysis between 410 nanomenters and 790 nanometers.
  • Switch inputs 16 may be directly connected to CPU 10 which reads their status as a binary eight bit number. This permits distinguishing whether one or more buttons are being pressed.
  • switch inputs 16 can be expanded to include an alpha numeric key pad interface which would permit greater operator interaction with CPU 10.
  • Switch inputs 16 can be advantageously used to control a menu of operations to be conducted by CPU 10.
  • a library of operations may be stored on the read only memory (ROM) which can be selected and executed.
  • ROM read only memory
  • the pressing of one button sends a "high" signal to CPU 10 which then scrolls through the functions from the library of stored functions.
  • These functions may be displayed via the LCD interface 13 and the button released when the appropriate function has been displayed.
  • the second button can then initiate the process displayed by that particular function such as initiation of the data analysis algorithm.
  • Output may be conveniently represented via a liquid crystal display (LCD) through interface 13 which will ideally display, in addition to menu information concerning operation of the device, results of measurement analysis.
  • LCD liquid crystal display
  • a two line 24 or 16 character LCD may be conveniently used although it is possible for more complex screens to be employed albeit at the expense of size and power consumption. • Additionally, it may be convenient to provide an additional data output method such as, for example, the use of the UART onboard the ATMEL CPU to send/receiveing formation to an RS232 port on any suitable device.
  • the RS232 port offers substantial levels of flexibility and permits a user the option of exporting data to another computing device for further analysis or storage, or to a printer for providing a hard copy.
  • the RS232 port also permits the user to import data to the present invention in order to update the reference data, and/or the library of stored functions.
  • Figure 2 shows a typical spectrum of light intensity versus wavelength that is
  • the first peak centered at 370 nanometers, comprises predominately, a reflection component from the light source which has been unchanged by the sample. Essentially this return of scattered light contains little or no information and accordingly, is preferably eliminated in order to improve the signal-to-noise (S/N) ratio. This discarded region is labeled D in the figure.
  • the second peak 41 comprises an emission of light from the sample which is different than that of the light illuminating the sample.
  • the third peak 42 represents a second order diffraction of the primary peak. The information in this peak is preferably included because the ratio of the signal size to this peak provides an indication of the reflectance from the sample.
  • the determination of the amount of reflectance from the sample is useful in identifying the amount of 'tail" in the 380 nanometer illumination range which leaks into the collected spectrum C.
  • information in this peak can assist in identifying and accommodating the output from "noisy" LED's.
  • this peak is useful in detecting the difference between otherwise identical emissions from labels which have been printed on a plastic surface versus a paper surface. Accordingly, data collected over the wavelength range C is analyzed further.
  • each pixel already provides information regarding the wavelength, recall that each pixel typically represents a 3 nanometer change in wavelength from the adjacent pixel, only intensity components are collected. This provides an array [yi, y 2 ,
  • n is the number of pixels in the spectrum array. While this array may be
  • first derivative ([y ⁇ -y 2 , y 2 -y , y -y 4 , • • ⁇ y n - ⁇ - Yn]) of the signal strength from the sample and subtracting it from the first derivative of a stored reference to provide a new array.
  • Figure 3 demonstrates the results of taking the derivative of light intensity. On this graph, the peaks now occur at the zero crossings and the range of data collected for the sample is shown in the spectrum area labeled C.
  • the sample spectrum representing data that is analysed is labeled S and the spectrum resulting from reflection is labeled R.
  • a rolling median function is used to smooth the data and this is accomplished by taking the median of three points in a series and rolling this median along the curve. This can be represented as median of (dy ⁇ . ⁇ ,
  • match value This single number called a "match value " .
  • the match value then defines a pass/fail situation which may be compared with a stored match value and may be displayed in a variety of formats including the presentation of the actual numbers, a pass/fail effect or other indicia of acceptability.
  • ZPX Zero Point Crossing
  • the ZPX method involves the following steps:
  • Sensitivity - the ZPX method is insensitive to the spectral broadness.
  • the ZPX method in one form allows spectra (or similar analogue information of any description) to be used as an encryption key. This works as follows:
  • the encryption key consists of a series of rectangles through which the reference spectrum passes.
  • Encrypted information may be sent whereby for example, the digits 0-9 correspond to rectangle sides along the wavelength (x) coordinate.
  • the encrypted information takes the form of the equivalent rectangle sides on the signal (y) coordinate, the combination defining a set of rectangles through which the spectrum passes.
  • Decryption may only be achieved with the encryption key i.e. the spectral information; wherein the encrypted positions on the signal (y) coordinate may be mapped back onto equivalent decrypted positions on the wavelength (x) coordinate.
  • the principle benefit of this approach is that it allows the encryption key to be carried in analogue form.
  • This can take the form of for example biometric readings (voice print, retinal scan, fingerprint etc.), or identity cards with coded fluorescent markings.
  • biometric readings voice print, retinal scan, fingerprint etc.
  • identity cards with coded fluorescent markings.
  • the encryption key can be as generally or individually
  • FIGS 6 and 7 illustrate the entire check routine as used in the present invention. This routine includes several preparation steps prior to ZPX analysis.
  • the first is a shortening of the sample and reference spectral arrays in order to remove irrelevant spectral information. This removes for example, features arising from light source reflections.
  • the second step involves normalising the sample and reference arrays to integer values say between 0 and 100.
  • the normalised minimum value in both arrays is set to 0 and the maximum to 100.
  • This step eliminates small differences due to signal size etc.
  • the third step is a prefilter which is a simple comparison of the position of the peak maximum and broadness of the main features(s) in the sample and reference spectra. If the sample and reference are greatly different, the prefilter rejects the sample and automatically returns a match value of 0 without recourse to the ZPX analysis. This step greatly decreases the average computation time required to compare a large number of spectra.
  • the ZPX method calculates the similarity between the former and the reference spectrum, generating the match value as its output.
  • the match value is compared to a cut-off which is statistically predetermined and a "pass” or “fail” is returned depending on the outcome of this comparison.
  • the input comprises the sample and reference arrays, shortened to the appropriate (but equal) size. These two arrays are linearly normalised such that the minimum value is 0 and the maximum is say 100. It should also be noted that the array consists of integers, minimizing the memory storage required and also allowing fast computation.
  • start step is set to 5
  • stop step is set to 95
  • step size 10
  • start step is set to 5
  • stop step is set to 95
  • step size 10
  • the analysis will begin 5% up from the bottom of the spectrum and finish at 95%, incrementing upwards in steps of 10%.
  • the next step involves moving along the sample and reference arrays pairwise looking for points at which the array elements go from positive to negative or vice versa.
  • the points at which the former occur are referred to as "zero point crossings" (ZPX's) and represent the grid rectangles through which the sample and or reference spectra pass.
  • the reference counter is incremented.
  • the agreement counter is also incremented.
  • ZPX is a new computational method, which has proven to be very effective for comparison of emission spectra. Not only is the method flexible and reliable, but it is also computationally efficient due to the limitation of floating point calculations.
  • the ZPX method also has potential application not only for comparison of other types of spectra (such as absorption, reflectance etc.) but might also be applied to other comparison computations such as those used in voice, speech or retinal recognition.
  • the same method could also be adapted to form a unique encryption technique in which the key is effectively analogue information. Again, applications for this might be found in technological areas such as voice print analysis etc.
  • the hand-held spectrophotometer based analysis of emission spectra from fluorescent labels may be used to detect the presence of one or more of such pigment or dye labels placed upon a sample's label or other associated surface.
  • fluorofors such as those readily available from DuPont, Riedel de Haen of Honeywell Speciality Chemicals and others
  • the spectrum resulting from illumination will have increasing degrees of complexity. This complexity will lead to vastly increased difficulty in illegitimate duplication.
  • the luminous spectrum of any material is unique and that while the emission maxima in the luminous spectrum of two materials may be identical, their profiles are not.
  • the luminous spectrum of any material or mixture of materials represents a unique attribute (or analogue code) of the material or mixture.
  • known information can be converted into a mixture of luminous materials and stored covertly in a label and can subsequently be decoded by the present invention by use of known protocol or decoding algorithm.
  • the material mixture when decoded can provide more details than simply presence.
  • the position and/or thickness may also be used to represent additional data by a known formula.
  • the dyes used may be either of organic or inorganic types and will be selected in accordance with the intended object to be labeled, the emissivit spectrum desired and the dye's compatibility with other dyes and labels. While such dyes may be applied directly to labels or other containers associated with the item to be tracked, other applications will require application of the label directly to the item to be tested. In such instances, the labels will need to be selected in order to withstand normal handling during the production, transportation, inventory, and sales cycle. Additionally, the preferred label will be selected to avoid deleterious effects upon the sample item itself.

Landscapes

  • Physics & Mathematics (AREA)
  • Spectroscopy & Molecular Physics (AREA)
  • General Physics & Mathematics (AREA)
  • Health & Medical Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Chemical & Material Sciences (AREA)
  • Analytical Chemistry (AREA)
  • Biochemistry (AREA)
  • General Health & Medical Sciences (AREA)
  • Immunology (AREA)
  • Pathology (AREA)
  • Investigating, Analyzing Materials By Fluorescence Or Luminescence (AREA)

Abstract

L'invention concerne de nouveaux algorithmes particulièrement utiles pour les dispositifs portatifs pilotés par spectrophotomètres. Ces algorithmes permettent d'identifier et de discriminer la présence d'étiquettes qui fournissent un spectre d'émission caractéristique lors de l'éclairage. Ils permettent, en outre, d'analyser ces spectres par rapport aux données préalablement mémorisées pour déterminer les appariements éventuels.
PCT/IB2001/000275 2000-01-26 2001-01-25 Algorithmes prevus pour un appareil spectrophotometrique manuel WO2001055697A1 (fr)

Priority Applications (1)

Application Number Priority Date Filing Date Title
AU2001234012A AU2001234012A1 (en) 2000-01-26 2001-02-22 Algorithms for use in a hand-held spectrophotometric apparatus

Applications Claiming Priority (4)

Application Number Priority Date Filing Date Title
US14955300A 2000-01-26 2000-01-26
US09/491,553 2000-01-26
US19455300A 2000-06-20 2000-06-20
US60/212,863 2000-06-20

Publications (1)

Publication Number Publication Date
WO2001055697A1 true WO2001055697A1 (fr) 2001-08-02

Family

ID=26846836

Family Applications (1)

Application Number Title Priority Date Filing Date
PCT/IB2001/000275 WO2001055697A1 (fr) 2000-01-26 2001-01-25 Algorithmes prevus pour un appareil spectrophotometrique manuel

Country Status (2)

Country Link
AU (1) AU2001234012A1 (fr)
WO (1) WO2001055697A1 (fr)

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US9105848B2 (en) 2006-08-07 2015-08-11 Wake Forest University Composite organic materials and applications thereof

Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4560275A (en) * 1980-04-08 1985-12-24 California Institute Of Technology Portable instant display and analysis reflectance spectrometer
EP0573345A1 (fr) * 1992-06-03 1993-12-08 Commissariat A L'energie Atomique Procédé de comparaison de flots de données et dispositif de mise en oeuvre
US5943437A (en) * 1995-10-09 1999-08-24 Kabushiki Kaisha Kobe Seiko Sho Method and apparatus for classifying a defect on a semiconductor wafer

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4560275A (en) * 1980-04-08 1985-12-24 California Institute Of Technology Portable instant display and analysis reflectance spectrometer
EP0573345A1 (fr) * 1992-06-03 1993-12-08 Commissariat A L'energie Atomique Procédé de comparaison de flots de données et dispositif de mise en oeuvre
US5943437A (en) * 1995-10-09 1999-08-24 Kabushiki Kaisha Kobe Seiko Sho Method and apparatus for classifying a defect on a semiconductor wafer

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US9105848B2 (en) 2006-08-07 2015-08-11 Wake Forest University Composite organic materials and applications thereof

Also Published As

Publication number Publication date
AU2001234012A1 (en) 2001-08-07

Similar Documents

Publication Publication Date Title
US6470093B2 (en) First-order authentication system
EP1490828B1 (fr) Procede de verification du papier-monnaie
CN1073251C (zh) 对伪造品,例如伪钞的检验装置及其检验方法
EP0721717B1 (fr) Procede et systeme d'authentification
KR101333278B1 (ko) 시각적인 반사 스펙트럼 반응을 이용한 향상된 위조 화폐 검출기
KR101297702B1 (ko) 적분된 투과 및 반사 스펙트럼 응답을 이용한 개선된 위조 화폐 검출기
US20100149531A1 (en) Apparatus and method for object authentication using taggant material
EP1066602B1 (fr) Procedes et appareil permettant de surveiller des articles
EP3013595B1 (fr) Système & amp; marqueur de codage de sécurité, dispositif de balayage opto-électronique et procédé de codage d'articles
US6605819B2 (en) Media validation
US20050100204A1 (en) Method and apparatus for detecting fluorescent particles contained in a substrate
EA000733B1 (ru) Устройство для проверки подлинности банкнот
WO2011106522A1 (fr) Sténographie à colorants photosensibles
EP0198819B1 (fr) Appareil pour controler l'authenticite de billets de banque
US6858856B2 (en) Counterfeit detector cash register
US20010052575A1 (en) Hand-held anti-counterfeiting apparatus
WO2001055697A1 (fr) Algorithmes prevus pour un appareil spectrophotometrique manuel
WO2001055975A1 (fr) Appareil anti-contrefacon portable
IE20010366A1 (en) Hand-held anticounterfeiting apparatus vaxed on emission time decay characteristics
AU2021307548A1 (en) Method and system for detecting and authenticating a taggant in a marking via surface-enhanced raman spectroscopy
US10950079B2 (en) Method and apparatus for determining the authenticity of flat objects: banknotes, documents, security labels, and related items
WO2005076742A2 (fr) Dispositif optique portable et procede pour billets de banque
RU2115169C1 (ru) Способ определения подлинности банкноты
EA043851B1 (ru) Способ и система для детекции и проверки подлинности метки в маркировке с помощью поверхностно-усиленной рамановской спектроскопии

Legal Events

Date Code Title Description
AK Designated states

Kind code of ref document: A1

Designated state(s): AE AG AL AM AT AU AZ BA BB BG BR BY BZ CA CH CN CR CU CZ DE DK DM DZ EE ES FI GB GD GE GH GM HR HU ID IL IN IS JP KE KG KP KR KZ LC LK LR LS LT LU LV MA MD MG MK MN MW MX MZ NO NZ PL PT RO RU SD SE SG SI SK SL TJ TM TR TT TZ UA UG US UZ VN YU ZA ZW

AL Designated countries for regional patents

Kind code of ref document: A1

Designated state(s): GH GM KE LS MW MZ SD SL SZ TZ UG ZW AM AZ BY KG KZ MD RU TJ TM AT BE CH CY DE DK ES FI FR GB GR IE IT LU MC NL PT SE TR BF BJ CF CG CI CM GA GN GW ML MR NE SN TD TG

121 Ep: the epo has been informed by wipo that ep was designated in this application
DFPE Request for preliminary examination filed prior to expiration of 19th month from priority date (pct application filed before 20040101)
REG Reference to national code

Ref country code: DE

Ref legal event code: 8642

122 Ep: pct application non-entry in european phase
NENP Non-entry into the national phase

Ref country code: JP