Isotopic enrichment of helium-3 through glass

Abstract

Disclosed is a mass selective fluid bandpass filter. This filter provides for selecting gas molecules of a specific mass from a gas sample containing molecules of two or more mass species. This provides for a low power, low cost apparatus for producing .sup.3He from terrestrial sources of helium gas by selective enrichment. This invention further discloses a portable, field deployable means of .sup.3He/.sup.4He ratio determination employing one or more of the effects consisting of: statistical linear regression plots of heat ramps, variable emission currents within a quadruple mass spectrometer, use of a quadrupole mass spectrometer in concert with ultrahigh vacuum maintained by non-evaporable getter pumps, and/or construction of vacuum housing structures from non-steel or non-stainless steel alloys, and or non metallic materials selected from a group consisting of: aluminum, titanium, ceramics, or glass. This provides a compact, sensitive field deployable unit with low power consumption.

Claims

1. A method for determining the .sup.3He/.sup.4He ratio of a gas comprising .sup.3He and .sup.4He comprising the steps of: providing a sample chamber, providing a mass selective supra cooled liquid bandpass filter in communication with the sample chamber, wherein the mass selective supra cooled liquid bandpass filter is made of quartz glass, introducing a sample of the gas comprising .sup.3He and .sup.4He into the sample chamber, heating the mass selective supra cooled liquid bandpass filter made of quartz glass, wherein the heating is performed as a heat ramp including through a temperature window of about 50 to 450 C., and allowing .sup.3He and .sup.4He to selectively pass through the mass selective supra cooled liquid bandpass filter from the sample chamber into an analysis structure during the heat ramp, wherein the analysis structure analyzes the volumes of .sup.3He and .sup.4He passing through the mass selective supra cooled liquid bandpass filter during the heat ramp to determine the .sup.3He/.sup.4He ratio.

2. The method for determining the .sup.3He/.sup.4He ratio of a gas comprising .sup.3He and .sup.4He of claim 1, wherein the analysis structure determines the .sup.3He/.sup.4He ratio by statistical linear regression plots of heat ramps from statistical analysis of mass-2 versus mass-3 trend plot from a heat ramp wherein determination of a positive zero-intercept of the y-axis of the mass-3 plot gives the .sup.3He residual partial pressure.

3. The method for determining the .sup.3He/.sup.4He ratio of a gas comprising .sup.3He and .sup.4He of claim 1, wherein the analysis structure determines the .sup.3He/.sup.4He ratio with a variable emission current within a quadrupole mass spectrometer, wherein a predetermined programmed variation of emission current provides an effective correction to a combined .sup.3He-HD peak when performed in a vacuum with low hydrogen abundance.

4. The method for determining the .sup.3He/.sup.4He ratio of a gas comprising .sup.3He and .sup.4He of claim 1, wherein the analysis structure comprises a quadrupole mass spectrometer in concert with ultrahigh vacuum maintained by non-evaporable getter pumps and ion pumps.

5. The method for determining the .sup.3He/.sup.4He ratio of a gas comprising .sup.3He and .sup.4He of claim 1, wherein the non-evaporable getter pumps and ion pumps eliminate potentially interfering hydrogen isobars of HD and 3H.

6. The method for determining the .sup.3He/.sup.4He ratio of a gas comprising .sup.3He and .sup.4He of claim 1, further comprising the step of providing a vacuum housing between the mass selective supra cooled liquid bandpass filter made of quartz glass and the analysis structure, wherein the vacuum housing is formed from a material selected from a group consisting of aluminum, titanium, stainless steel, ceramics, borosilicate glass, sealing glass and combinations thereof.

7. The method for determining the .sup.3He/.sup.4He ratio of a gas comprising .sup.3He and .sup.4He of claim 1, wherein the quartz glass is of either natural or manmade origin.

8. The method for determining the .sup.3He/.sup.4He ratio of a gas comprising .sup.3He and .sup.4He of claim 1, wherein .sup.3He is separated from .sup.4He when the mass selective supra cooled liquid bandpass filter is within the general given temperature window of about 50 to 450 C.

9. The method for determining the .sup.3He/.sup.4He ratio of a gas comprising .sup.3He and .sup.4He of claim 1, wherein .sup.3He is separated from .sup.4He when the mass selective supra cooled liquid bandpass filter is within the specific given temperature window of about 100 to 450 C.

10. The method for determining the .sup.3He/.sup.4He ratio of a gas comprising .sup.3He and .sup.4He of claim 1, provides for a portable and field deployable instrument, of a weight approximately 150 pounds, is able to be carried by approximately 2 to 4 persons, approximates 2 feet in width, approximates 3 feet in height, approximates 6 feet in length, consumes approximately 3 kilowatt hours per day, operates on electrical potential selected from a group consisting of 24 VDC, 120 VAC, 240 VAC, and combinations thereof, and is enclosed in a weather resistant housing.

11. The method for determining the .sup.3He/.sup.4He ratio of a gas comprising .sup.3He and .sup.4He of claim 1, wherein the specific atomic mass unit at which maximum transmission occurs is influenced by factors including temperature of the supra cooled liquid bandpass filter made of quartz glass, thickness of the supra cooled liquid bandpass filter made of quartz glass, differential pressure across the supra cooled liquid bandpass filter made of quartz glass, and the composition of the supra cooled liquid bandpass filter made of quartz glass.

12. The method for determining the .sup.3He/.sup.4He ratio of a gas comprising .sup.3He and .sup.4He of claim 1, wherein the supra cooled liquid bandpass filter made of quartz glass provides a method for very selective filtering of gases of close atomic mass unit values within the operational range of this filter.

13. The method for determining the .sup.3He/.sup.4He ratio of a gas comprising .sup.3He and .sup.4He of claim 1, wherein the supra cooled liquid bandpass filter made of quartz glass provides a method wherein the atomic mass unit of maximum transmission has a direct relationship with the temperature of the supra cooled liquid bandpass filter made of quartz.

14. The method for determining the .sup.3He/.sup.4He ratio of a gas comprising .sup.3He and .sup.4He of claim 1, wherein the supra cooled liquid bandpass filter made of quartz glass provides a method wherein species of a given atomic mass unit under set conditions are selectively transmitted, whereas species of higher and lower atomic mass unit values are selectively blocked, wherein said mass selective fluid bandpass filter exhibits a high quality, or Q characteristic.

15. The method for determining the .sup.3He/.sup.4He ratio of a gas comprising .sup.3He and .sup.4He of claim 1, wherein the construction of vacuum housing structures from non-steel or non-stainless steel alloys, aluminum, titanium, and or non metallic materials selected from a group consisting of: ceramics, borosilicate glass, or sealing glass provides for vacuum housing structures that are impermeable to the gases to to be filtered by this apparatus.

16. The method for determining the .sup.3He/.sup.4He ratio of a gas comprising .sup.3He and .sup.4He of claim 1, wherein the supra cooled liquid bandpass filter made of quartz glass provides a method that is selectively semipermeable to the gases to to be filtered by this apparatus.

17. The method for determining the .sup.3He/.sup.4He ratio of a gas comprising .sup.3He and .sup.4He of claim 1, wherein the supra cooled liquid bandpass filter made of quartz glass provides a method whereby with constant temperature operation, the filter can selectively pass species of a predetermined atomic mass unit value.

18. The method for determining the .sup.3He/.sup.4He ratio of a gas comprising .sup.3He and .sup.4He of claim 1, wherein the supra cooled liquid bandpass filter made of quartz glass provides a method for very selective filtering of gases of close atomic mass unit values within the operational range of this filter.

19. The method for determining the .sup.3He/.sup.4He ratio of a gas comprising .sup.3He and .sup.4He of claim 1, wherein the construction of vacuum housing structures from non-steel or non-stainless steel alloys, aluminum, titanium, and or non metallic materials selected from a group consisting of: ceramics, borosilicate glass, or sealing glass provides for vacuum housing structures from materials known to produce low to negligible hydrogen outgassing, thereby minimizing the effect of all potentially interfering hydrogen isobars of HD and .sup.3H.

20. The method for determining the .sup.3He/.sup.4He ratio of a gas comprising .sup.3He and .sup.4He of claim 1, wherein the method of calculating .sup.3He/.sup.4He ratio comprising the steps of: sample gas is introduced into a cleared sample chamber at about atmospheric pressure, a heat ramp is started at a predetermined power level, early within the temperature up ramp gates selectively passing .sup.3He open resulting in a .sup.3He temperature curve, with further temperature rise the .sup.3He partial pressure drops below the noise level of the quadrupole mass spectrometer due to the very small amount .sup.3He being masked by the rising levels of .sup.4He, for a predetermined duration the average area under the .sup.3He curve is computed wherein this area becomes the representation of the .sup.3He fraction of the .sup.3He/.sup.4He ratio and is recorded, with further increase in temperature large amounts of .sup.4He enter the ultra high vacuum portion of the instrument, after a predetermined time, the power is cut off to the heater, and the quartz glass undergoes a cool down phase, where during this cool down phase .sup.4He continues to move through the open .sup.4He gates wherein a .sup.4He temperature curve is produced, at points during this cool down curve some .sup.3He again enters but is negligible with relation to the .sup.4He fraction, for a predetermined duration the average area under the .sup.4He curve is computed wherein this area becomes the representation of the .sup.4He fraction of the .sup.3He/.sup.4He ratio and is recorded, the ratio of the .sup.3He area to the .sup.4He area is reported as the .sup.3He/.sup.4He ratio.

21. The method for determining the .sup.3He/.sup.4He ratio of a gas comprising .sup.3He and .sup.4He of claim 1, wherein the method of calculating .sup.3He/.sup.4He ratio comprising the steps of the following operations: a sample is introduced into the sample chamber, the quartz glass filter is heated to a predetermined temperature, the heated quartz glass filter provides for exclusive diffusion of helium and hydrogen, with higher temperatures the heated quartz glass filter more preferentially diffuses helium, the hydrogen gas diffused into the high vacuum chamber is selectively pumped and sequestered by the non-evaporable getter pump, the heating of the quartz glass filter is stopped after a predetermined amount of time, cooling of the quartz glass filter below 45 degrees Celsius effectively closes the quartz glass filter to further hydrogen and helium diffusion, the mass spectrometer measures the helium 3 and helium 4 abundance, electronics calculates and records the helium 3 to helium 4 ratio, the ultra high vacuum valve opens and exposes the vacuum chamber to the noble diode ion pump, the noble diode ion pump pumps and sequesters the helium gas level to below a set threshold as measured by the ultra high vacuum total pressure gauge, the apparatus is now prepared to receive another sample, the process is repeated, in the event that the helium is not pumped by the noble diode ion pump to below the set threshold in a predetermined amount of time such an indication is recorded, if telemetry is available this indication of not reaching a predetermined helium threshold level is telemetered, the unit is then shut down.

Description

DESCRIPTION OF THE DRAWINGS

(1) FIG. 1

(2) A graph of a two-dimensional Cartesian coordinate system of ordered pairs where the ordinate, the y-axis, represents the partial pressure of .sup.3He in Torr, and the abscissa, the x-axis, represent the temperature in degrees Celsius. This plot shows the relative opening and closing of ports allowing conductance of .sup.3He at various temperatures in the upswing of a heat ramp.

(3) FIG. 2

(4) A see through representation of the components of the portable field deployable .sup.3He/.sup.4He ratio detector as seen from the left side.

(5) FIG. 3

(6) An outside view of the portable field deployable .sup.3He/.sup.4He ratio detector as seen from the left side.

(7) FIG. 4

(8) An outside view of the portable field deployable .sup.3He/.sup.4He ratio detector as seen from the top side.

(9) FIG. 5

(10) An outside view of the portable field deployable .sup.3He/.sup.4He ratio detector as seen from the front side.

(11) FIG. 6

(12) An outside view of the portable field deployable .sup.3He/.sup.4He ratio detector as seen from the back side.

REFERENCE NUMERALS IN DRAWINGS

(13) 1. .sup.3He/.sup.4He ratio detector case. 2. .sup.3He/.sup.4He ratio detector sample chamber. 3. Foot. 4. Handle. 5. Fan. 6. Power connector. 7. Communication connector. 8. Heater, thermocouple, and accessories power connector. 9. Quartz glass tube. 10. Graded glass seal. 11. Conflat adapter. 12. Sample chamber tube. 13. Sample chamber endcap. 14. Ultra high vacuum main chamber. 15. Conflat 90 degree elbow. 16. Conflat extension. 17. Flexible conflat extension. 18. Sample inlet pipe. 19. Sample outlet pipe. 20. Quadrupole mass spectrometer. 21. Non evaporable getter housing. 22. Non evaporable getter heater base with electrical connector. 23. Ion pump. 24. Autoresonant ion trap mass spectrometer. 25. In line electric conflat valve. 26. 90 degree electric conflat valve. 27. Cold cathode total pressure gauge. 28. Vacuum purge line with valves. 29. Electronics 30. Graph ordinate, the y-axis, representing .sup.3He partial pressure in Torr. 31. Graph origin. 32. Graph abscissa, the X-axis, representing temperature in degrees Celsius. 33. Estimated noise floor of quadrupole mass spectrometer. 34. .sup.3He gate opening point. 35. .sup.3He gate closing point. 36. .sup.3He high Q gate opening point. 37. .sup.3He high Q gate closing point. 38. Point of .sup.3He signal being swamped by other gases present. 39. Sample chamber enclosed space. 40. Ultra high vacuum enclosed space.

DESCRIPTION OF THE INVENTION

(14) The method for determining the .sup.3He/.sup.4He ratio of a gas comprising .sup.3He and .sup.4He, provides for a portable and field deployable instrument, of a weight approximately 150 pounds, is able to be carried by approximately 2 to 4 persons, approximates 2 feet in width, approximates 3 feet in height, approximates 6 feet in length, consumes approximately 3 kilowatt hours per day, operates on electrical potential selected from a group consisting of 24 VDC, 120 VAC, 240 VAC and combinations thereof, and is enclosed in a weather resistant housing.

(15) The essence of this invention are novel properties of quartz glass discovered by the inventors. It comprises a mass selective fluid bandpass filter. The mass selective fluid bandpass filter is a supercooled fluid. The supercooled fluid is quartz glass. The quartz glass wherein the quartz glass consists of quartz of either natural or manmade origin. The mass selective fluid bandpass filter of this apparatus provides for low-power operation. The mass selective fluid bandpass filter of this apparatus provides for a compact, field deployable unit. The mass selective fluid bandpass filter wherein this apparatus provides for a high sensitivity field deployable instrument for .sup.3He/.sup.4He ratio determination. The mass selective fluid bandpass filter provides a means for very selective filtering of gases of close atomic mass unit values within the operational range of this filter. The mass selective fluid bandpass wherein the specific atomic mass unit at which maximum transmission occurs is influenced by factors including temperature of the glass, differential pressure across the glass, and glass composition. The mass selective fluid bandpass wherein the atomic mass unit of maximum transmission has a direct relationship with the temperature of the glass. The mass selective fluid bandpass filter wherein this filter is a mass bandpass filter in that species of a given atomic mass unit under set conditions are selectively transmitted, whereas species of higher and lower atomic mass unit values are selectively blocked. The mass selective fluid bandpass filter wherein this filter exhibits a high quality, or Q characteristic. The mass selective fluid bandpass filter wherein with constant temperature operation, the filter can selectively pass species of a predetermined atomic mass unit value. The mass selective fluid bandpass filter wherein the sharp cutoff characteristics of this filter's transmission provides means for very selective filtering of gases of close atomic mass unit values within the operational range of this filter. The quartz glass is selectively semipermeable to the gases to to be filtered by this apparatus. The selective semipermeable action on the gases to to be filtered is based on conditions of glass thickness, glass temperature, glass composition, and pressure differential across the glass.

(16) This mass selective filter provides a means of .sup.3He/.sup.4He ratio determination that is portable and field deployable and provides for a high sensitivity field deployable instrument for .sup.3He/.sup.4He ratio determination. The means of .sup.3He/.sup.4He ratio determination consists of a gas inlet and sample structure, a mass selective filter element, and a filtered gas outlet and analysis structure. The means of .sup.3He/.sup.4He ratio determination provides two internally bounded spaces which are separated by structures of stainless steel, borosilicate glass, sealing glass, and quartz glass. The structures of stainless steel, borosilicate glass, and sealing glass are impermeable to the gases to to be filtered by this apparatus. The quartz glass is selectively semipermeable to the gases to to be filtered by this apparatus. The selective semipermeable action on the gases to to be filtered described by the apparatus is based on conditions of glass thickness, glass temperature, glass composition, and pressure differential across the glass. The means of .sup.3He/.sup.4He ratio determination employs one or more of the effects selected from the group consisting of: 1) statistical linear regression plots of heat ramps, 2) variable emission current within a quadruple mass spectrometer, 3) use of a quadrupole mass spectrometer in concert with ultrahigh vacuum maintained by non evaporable getter pumps, 4) construction of vacuum housing structures from non-steel or non-stainless steel alloys, and or non metallic materials selected from a group consisting of: aluminum, titanium, ceramics, or glass, 5) or a mixture thereof. The statistical linear regression plots of heat ramps of provide for .sup.3He/.sup.4He ratio determination from statistical analysis of a mass-2 versus mass-3 trend plot from a heat ramp wherein determination of a positive zero-intercept of the y-axis of the mass-2 trend plot gives the .sup.3He residual partial pressure. The variable emission current within a quadrupole mass spectrometer provide for .sup.3He/.sup.4He ratio determination wherein a predetermined programmed variation of emission current provides an effective correction to a combined .sup.3He-HD peak when performed in a vacuum with low hydrogen abundance. The use of quadrupole mass spectrometer in concert with ultrahigh vacuum maintained by non-evaporable getter pumps provides for .sup.3He/.sup.4He ratio determination wherein the use of high hydrogen pumping speed non-evaporable getter pumps provides for the elimination of all potentially interfering hydrogen isobars of HD and .sup.3H. The construction of vacuum housing structures from non-steel or non-stainless steel alloys, and or non metallic materials selected from a group consisting of: aluminum, titanium, ceramics, or glass provides for the .sup.3He/.sup.4He ratio determination wherein construction of vacuum housing structures is from materials known to produce low to negligible hydrogen outgassing, thereby minimizing the effect of all potentially interfering hydrogen isobars of HD and .sup.3H.

(17) The method for determining the .sup.3He/.sup.4He ratio of a gas comprising .sup.3He and .sup.4He, wherein the construction of vacuum housing structures from non-steel or non-stainless steel alloys, aluminum, titanium, and or non metallic materials selected from a group consisting of: ceramics, borosilicate glass, or sealing glass provides for vacuum housing structures that are impermeable to the gases to to be filtered by this apparatus. This construction of vacuum housing structures from non-steel or non-stainless steel alloys, aluminum, titanium, and or non metallic materials selected from a group consisting of: ceramics, borosilicate glass, or sealing glass provides for vacuum housing structures from materials known to produce low to negligible hydrogen outgassing, thereby minimizing the effect of all potentially interfering hydrogen isobars of HD and .sup.3H.

(18) FIG. 1 shows a portion of the initial up ramp of a heat ramp wherein the gates passing .sup.3He selectively open prior to the gates passing .sup.4He. The graph ordinate (30), the y-axis, represents .sup.3He partial pressure in Torr. The graph origin is at (31). The graph abscissa (32), the X-axis, represents temperature in degrees Celsius. The estimated noise floor of quadrupole mass spectrometer is at (33). The sample points are approximately spaced by 1 minute. (34) shows a point in time wherein .sup.3He gate opening point has been passed and .sup.3He is entering the ultra high vacuum space (UHV). (35) indicates a .sup.3He gate closing point, for though the temperature continues to rise, the .sup.3He partial pressure starts to decline. (37) indicates a .sup.3He high Q gate closing point, for the rate of decline in .sup.3He partial pressure drops much more steeply. This is followed by a .sup.3He high Q gate opening point at (36) wherein the .sup.3He partial pressure increases very steeply. This is sequentially followed by several subsequent .sup.3He high Q gate closing and opening points, ending with a final .sup.3He high Q gate closing point and the .sup.3He signal being swamped by other gases present at point (38). The area under this curve represents the .sup.3He gas accumulation during this heat up ramp phase. After this time other gates open selectively passing 4He.

(19) The high Q bandpass filter whose characteristics are shown in FIG. 1 as described above forms the core of a field deployable instrument capable of the .sup.3He/.sup.4He ratio in sample gases. Helium in general is 5.2 parts per million in regular air. Within this helium fraction, the .sup.3He component normally is about one part per million, with the rest being .sup.4He. That makes the .sup.3He fraction one part per trillion in regular air. This would require a detector with over twelve orders of range to see .sup.3He. The best quadrupole mass spectrometers may have a dynamic range of eight orders of range, but such instruments would not have the resolution see the difference between HD, .sup.3He, and or .sup.3H. Only large, expensive, heavy, lab equipment can make such determinations. Presently, sample gases are collected in copper tubes that are latter sent to labs for analysis. No field equipment exists for such determination. The importance is that .sup.3He is primordial, and the .sup.3He/.sup.4He ratio significantly increases when magma is actively moving underground, as is common before earthquakes.

(20) FIG. 2 shows a see through view of the field deployable instrument capable of the .sup.3He/.sup.4He ratio determination. Basically there are two separated, sealed spaces; the sample chamber enclosed space (39) separated from the ultra high vacuum enclosed space (40). The only communication between the two are microscopic gates which open and close, as controlled by temperature, in the quartz glass tube (9). This tube is connected to a conflat adapter (11) by a graded glass seal (10). Pieces (9), (10), and (11) are fused into one assembly, with the inner portion being continuous with the ultra high vacuum enclosed space (40). The outer portion is continuous with the sample chamber enclosed space (39).

(21) The sample chamber enclosed space is the space bound by the Conflat adapter, the sample chamber tube (12), the sample chamber endcap (13), and the fused assembly of pieces (9), (10), and (11). Also shown are a sample inlet pipe (18), sample outlet pipe (19). For clarity, the electrical connections passing through the sample chamber endcap (13) are not shown.

(22) The ultra high vacuum enclosed space is the internal volumes combined by the fused assembly of pieces (9), (10), and (11); the ultra high vacuum main chamber (14); the Conflat 90 degree elbows (15); the Conflat extension(s) (16); the flexible conflat extension (17); the quadrupole mass spectrometer (20); the autoresonant ion trap mass spectrometer (24); the exposed portion of the closed in line electric conflat valve (25); the exposed portion of the closed 90 degree electric conflat valve (26); the cold cathode total pressure gauge (27); and the vacuum purge line with valves (28) to the exposed portion of it's first closed valve.

(23) The sample chamber enclosed space and the ultra high vacuum enclosed space have been found to be of nearly equal volumes in the units so far tested. In line electric conflat valve is connected to the non-evaporable getter housing (21) which is sealed of by its non-evaporable getter heater base with electrical connector (22).

(24) The 90 degree electric conflat valve (26) is connected to the ion pump (23). When the electric conflat valves are open, the volume of the ultra high vacuum enclosed space is increased in volume by the enclosed spaces of these valves and their respective components. The same is true with the vacuum purge line and it's valves. However, it is the function of these units to rapidly pump out the gases contained within the ultra high vacuum enclosed space in preparation for another sample run.

(25) In sampling and analysis mode, all of these valves are closed. The only entrance of gases into the ultra high vacuum enclosed space would be through open microscopic gates in the active region of the quartz glass tube.

(26) The parts of this assembly are enclosed in the .sup.3He/.sup.4He ratio detector case (1). Within this case is an electronics assembly (29) to control all operation and then calculate and report the results. The sample chamber, sample chamber endcap, quartz glass tube with it's fused graded glass seal which is also fused to the conflat adapter, the sample inlet and outlet pipes, and all enclosed material are collectively referred to as .sup.3He/.sup.4He ratio detector sample chamber (2). Not shown for clarity are the heater windings on the quartz glass tube, the thermocouple above these windings, and the electrical connections. These parts are assembled in accordance with the standard procedures of those experienced with such art.

(27) FIGS. 3, 4, 5, and 6 show external views of the unit. Included are individual foot(s) (3); handle(s) (4); a fan (5); a power connector (6); a communications connector (7); and a heater, thermocouple, and accessories power connector (8).

(28) What is disclosed is a mass selective fluid bandpass filter. This filter provides for selecting gas molecules of a specific mass from a gas sample containing molecules of two or more mass species. This filter provides a means of operation of a portable, field deployable means of .sup.3He/.sup.4He ratio determination.

(29) The mass selective bandpass filter consists of a gas inlet and sample structure, a mass selective filter element, and a filtered gas outlet and analysis structure. The filter element is a supercooled fluid consisting of quartz glass. The quartz glass of the filter element consists of quartz of either natural or manmade origin.

(30) The gas inlet structure consists of a stainless steel tube with a Conflat flange at each end. The inlet end of the cylinder is sealed by a Conflat plate bolted to the flange and sealed with a copper gasket. Centered externally on this inlet plate is machined a smaller Conflat fitting and internal communicating passage to which a smaller Conflat plate is externally bolted and sealed with a copper gasket. Four high vacuum electrical connections pass through this smaller Conflat plate providing for internal electrical connections. Two stainless steel tubes pass through the larger Conflat which are attached at it's internal surface with high vacuum welds according to current practice of those experienced in such art.

(31) The mass selective filter consists of a rounded-end quartz glass cylinder of 2.5-inch outside diameter, 7.5-inches length with 2-mm wall thickness. The open end of this cylinder is attached to a 2.5-inch borosilicate glass cylinder by a graded glass seal of sufficient layers of sealing glass to provide for adequate matching of the thermal expansion characteristics of the quartz cylinder to that of the borosilicate cylinder. This graded glass seal is fabricated according to current practice of those experienced in such art. The other open end of the borosilicate glass cylinder is attached to a 2.5-inch outside stainless steel cylinder according to current practice of those experienced in such art. The other open end of this stainless steel cylinder is vacuum welded to a 4.5-inch Conflat flange according to current practice of those experienced in such art.

(32) The quartz glass section of the glass cylinder is wrapped with commercial heat tape whose electrical connections are attached to corresponding electrical connections passing externally through the smaller Conflat plate. A thermocouple or thermistor temperature sensor is attached to the heated portion of the quartz cylinder according to current practice of those experienced in such art. The electrical connections for the thermocouple or thermistor are attached to remaining two electrical connections passing externally through the smaller Conflat plate. These connections provide for external electrical connections to provide power for the heater and sensor readings for the cylinder temperature.

(33) The 4.5-inch Conflat flange attached to the glass cylinder is bolted and sealed with a copper gasket to a machined Conflat fitting on the filtered gas outlet and collection structure. Peripherally and axially centered on this 4.5 inch machined Conflat fitting is machined a second Conflat fitting which matches the second Conflat flange on the stainless tube of the inlet structure. This second Conflat flange of the inlet structure is bolted and sealed with a copper gasket to the outer, second Conflat fitting machined on the filtered gas outlet and collection structure.

(34) These components and structures are assembled according to current practice of those experienced in such art. This assemblage provides two vacuum tight external connections to an internally contained gas inlet structure space. This space is bounded by the internal surface of the gas inlet structure cylinder, the internal surface of the attached Conflat plate at the inlet end, the surface of the filtered gas outlet and collection structure in communication with said internal space, the external surfaces of the rounded-end quartz glass cylinder, the borosilicate glass cylinder, the graded glass seal, and the portion of the 4.5-inch Conflat flange in communication with this internal space.

(35) This assemblage also provides a second internally contained space in communication with the gas analysis structures. This space is bounded by the internal surfaces of the rounded-end quartz glass cylinder, the borosilicate glass cylinder, the graded glass seal, and the portion of the 4.5-inch Conflat flange in communication with this second internal space.

(36) This assemblage provides two internally bounded spaces which are separated by structures of stainless steel, borosilicate glass, sealing glass, and quartz glass. The stainless steel, borosilicate glass, and sealing glass are impermeable to the gases to to be filtered by this apparatus. The quartz glass is selectively semipermeable to the gases to to be filtered by this apparatus. The selective semipermeable action on the gases to to be filtered is based on conditions of glass thickness, glass temperature, glass composition, and pressure differential across the glass.

(37) Gas comprising species of differing atomic and molecular mass is introduced through one of the stainless steel tubes. This sample gas may be circulated through the sample space by allowing sample gas to bleed out through the second stainless steel tube as determined by ancillary apparatus operated according to current practice of those experienced in such art.

(38) Predetermined mass species from this gas mixture selectively are transmitted across the semipermeable quartz glass section of the mass selective filter. This outlet gas, concentrated to a given mass species exits through the filtered gas outlet to the gas analysis structures.

(39) The semipermeable quartz glass filter behaves analogous to an electrical series resonant circuit comprised of resistance, capacitance, and inductance. Gas transmission is highest at the equivalent of series resonance wherein capacitive and inductive reactances cancel and circuit transmission is limited by the direct current (DC) resistance of the circuit. In this case, resonance represents the species molecular or atomic mass in Atomic Mass Units (AMU).

(40) The specific AMU at which maximum transmission occurs is influenced by factors including temperature of the glass, differential pressure across the glass, and glass composition. It has been observed that AMU of maximum transmission has a direct relationship with the temperature of the glass. We have observed a positive correlation between AMU and glass temperature within the temperature ranges observed with our experiments. With increasing temperature, a higher value of AMU is selectively passed.

(41) This filter is a mass bandpass filter in that species of a given AMU under set conditions are selectively transmitted, whereas species of higher and lower AMU values are selectively blocked. This filter exhibits a high quality, or Q, characteristic. Q is defined as relative transmission at a given AMU value compared with the rejection characteristic of species of slightly higher or lower values of AMU.

(42) For a given set of operating characteristics of glass composition and differential pressure, the AMU value selectively passed is controlled by the temperature of the glass. Ancillary electronic apparatus determine this glass temperature and keep it within a predetermined temperature range by regulating the electric power supplied to the heater.

(43) With constant temperature operation, the filter can selectively pass species of a predetermined AMU. Observed selectivity characteristics indicate that species within 1 AMU of its range can be selectively transmitted or rejected. The given species transmitted at a given time can be changed by adjusting the glass temperature.

(44) The inverse exponential relationship found between the maximum temperature of the applied heat ramp and the calculated R/R.sub.a of the laboratory air indicates greater selective transmission of .sup.3He than that of .sup.4He, for the differential pressure of .sup.3He across the glass is about 5 orders of magnitude lower than that of .sup.4He. This is further suggestive that as the heat ramp temperature further increased, that this selective transmission of .sup.3He then was decreased and at higher temperature selective passage .sup.4He then occurred at these higher temperatures. The exponential drop of this curve was indicative of increasing transmission of .sup.4He which had a partial pressure differential of about 6 orders of magnitude greater across the glass than that of the .sup.3He. This sharp cutoff characteristic of the .sup.3He transmission provides means for very selective filtering of gases of close AMU values within the operational range of this filter.

(45) This invention provides means of .sup.3He/.sup.4He ratio determination which employs one or more of the effects selected from the group consisting of: 1) statistical linear regression plots of heat ramps, 2) variable emission current within a quadrupole mass spectrometer, 3) use of a quadrupole mass spectrometer in concert with ultrahigh vacuum maintained by non evaporable getter pumps, 4) construction of vacuum housing structures from non-steel or non-stainless steel alloys, and or non metallic materials selected from a group consisting of: aluminum, titanium, ceramics, or glass, 5) or a mixture thereof.

(46) The statistical linear regression plots of heat ramps provides for .sup.3He/.sup.4He ratio determination from statistical analysis of a mass-2 versus mass-3 trend plot from a heat ramp wherein determination of a positive zero-intercept of the y-axis of the mass-2 trend plot gives the .sup.3He residual partial pressure.

(47) The variable emission current within a quadrupole mass spectrometer provides for .sup.3He/.sup.4He ratio determination wherein a predetermined programmed variation of emission current provides an effective correction to a combined .sup.3He-HD peak when performed in a vacuum with low hydrogen abundance.

(48) Operation of the Invention

(49) What is disclosed is a method for determining the .sup.3He/.sup.4He ratio of a gas. This provides for selecting gas molecules of a specific mass from a gas sample containing molecules of two or more mass species. This method provides a means of operation of a portable, field deployable means of 3He/4He ratio determination.

(50) A method for determining the .sup.3He/.sup.4He ratio of a gas comprising .sup.3He and .sup.4He comprising the steps of: providing a sample chamber, providing a mass selective supra cooled liquid bandpass filter in communication with the sample chamber, wherein the mass selective supra cooled liquid bandpass filter is made of quartz glass, introducing a sample of the gas comprising .sup.3He and 4He into the sample chamber, heating the mass selective supra cooled liquid bandpass filter made of quartz glass, wherein the heating is performed as a heat ramp including through a temperature window of about 50 to 450 C., and allowing .sup.3He and .sup.4He to selectively pass through the mass selective supra cooled liquid bandpass filter from the sample chamber into an analysis structure during the heat ramp, wherein the analysis structure analyzes the partial pressures of .sup.3He and .sup.4He passing through the mass selective supra cooled liquid bandpass filter during the heat ramp to determine the .sup.3He/.sup.4He ratio.

(51) The analysis structure determines the .sup.3He/.sup.4He ratio by statistical linear regression plots of heat ramps from statistical analysis of mass-2 versus mass-3 trend plot from a heat ramp wherein determination of a positive zero-intercept of the y-axis of the mass-3 plot gives the .sup.3He residual partial pressure. The analysis structure additionally determines the .sup.3He/.sup.4He ratio with a variable emission current within a quadrupole mass spectrometer, wherein a predetermined programmed variation of emission current provides an effective correction to a combined .sup.3He-HD peak when performed in a vacuum with low hydrogen abundance. The analysis structure comprises a quadrupole mass spectrometer in concert with ultrahigh vacuum maintained by non-evaporable getter pumps and ion pumps, wherein the non-evaporable getter pumps and ion pumps eliminate potentially interfering hydrogen isobars of HD and 3H.

(52) The method for determining the .sup.3He/.sup.4He ratio of a gas comprising .sup.3He and .sup.4He of, further comprising the step of providing a vacuum housing between the mass selective supra cooled liquid bandpass filter made of quartz glass, wherein the quartz glass is of either natural or manmade origin, and the analysis structure, wherein the vacuum housing is formed from a material selected from a group consisting of aluminum, titanium, stainless steel, ceramics, borosilicate glass, sealing glass and combinations thereof.

(53) The method for determining the .sup.3He/.sup.4He ratio of a gas comprising .sup.3He and .sup.4He, wherein .sup.3He is separated from .sup.4He when the mass selective supra cooled liquid bandpass filter is within the general given temperature window of about 50 to 450 C., and within the specific given temperature window of about 100 to 450 C.

(54) The method for determining the .sup.3He/.sup.4He ratio of a gas comprising .sup.3He and .sup.4He, wherein the supra cooled liquid bandpass filter made of quartz glass provides a method for very selective filtering of gases of close atomic mass unit values within the operational range of this filter. This supra cooled liquid bandpass filter made of quartz glass provides a method wherein the atomic mass unit of maximum transmission has a direct relationship with the temperature of the supra cooled liquid bandpass filter made of quartz, and the supra cooled liquid bandpass filter made of quartz glass provides a method wherein species of a given atomic mass unit under set conditions are selectively transmitted, whereas species of higher and lower atomic mass unit values are selectively blocked, wherein said mass selective fluid bandpass filter exhibits a high quality, or Q characteristic. The supra cooled liquid bandpass filter made of quartz glass provides a method that is selectively semipermeable to the gases to to be filtered by this apparatus. The supra cooled liquid bandpass filter made of quartz glass provides a method whereby with constant temperature operation, the filter can selectively pass species of a predetermined atomic mass unit value. The supra cooled liquid bandpass filter made of quartz glass provides a method for very selective filtering of gases of close atomic mass unit values within the operational range of this filter.

(55) The method for determining the .sup.3He/.sup.4He ratio of a gas comprising .sup.3He and .sup.4He, wherein the specific atomic mass unit at which maximum transmission occurs is influenced by factors including temperature of the supra cooled liquid bandpass filter made of quartz glass, thickness of the supra cooled liquid bandpass filter made of quartz glass, differential pressure across the supra cooled liquid bandpass filter made of quartz glass, and the composition of the supra cooled liquid bandpass filter made of quartz glass.

(56) The method for determining the .sup.3He/.sup.4He ratio of a gas comprising .sup.3He and .sup.4He of wherein the method of calculating .sup.3He/.sup.4He ratio comprising the steps of: sample gas is introduced into a cleared sample chamber at about atmospheric pressure, a heat ramp is started at a predetermined power level, early within the temperature up ramp gates selectively passing .sup.3He open resulting in a .sup.3He temperature curve, with further temperature rise the .sup.3He partial pressure drops below the noise level of the quadrupole mass spectrometer due to the very small amount .sup.3He being masked by the rising levels of .sup.4He, for a predetermined duration the average area under the .sup.3He curve is computed wherein this area becomes the representation of the .sup.3He fraction of the .sup.3He/.sup.4He ratio and is recorded, with further increase in temperature large amounts of .sup.4He enter the ultra high vacuum portion of the instrument, after a predetermined time, the power is cut off to the heater, and the quartz glass undergoes a cool down phase, where during this cool down phase .sup.4He continues to move through the open .sup.4He gates wherein a .sup.4He temperature curve is produced, at points during this cool down curve some .sup.3He again enters but is negligible with relation to the .sup.4He fraction, for a predetermined duration the average area under the .sup.4He curve is computed wherein this area becomes the representation of the .sup.4He fraction of the .sup.3He/.sup.4He ratio and is recorded, the ratio of the .sup.3He area to the .sup.4He area is reported as the .sup.3He/.sup.4He ratio.

(57) What is disclosed is a method of a sequence of operation for determining the .sup.3He/.sup.4He ratio of a gas. This provides for selecting gas molecules of a specific mass from a gas sample containing molecules of two or more mass species. This method provides a means of operation of a portable, field deployable means of .sup.3He/.sup.4He ratio determination.

(58) The method for determining the .sup.3He/.sup.4He ratio of a gas comprising .sup.3He and .sup.4He wherein the method of calculating .sup.3He/.sup.4He ratio comprising the steps of the following operations: a sample is introduced into the sample chamber, the quartz glass filter is heated to a predetermined temperature, the heated quartz glass filter provides for exclusive diffusion of helium and hydrogen, with higher temperatures the heated quartz glass filter more preferentially diffuses helium, the hydrogen gas diffused into the high vacuum chamber is selectively pumped and sequestered by the non-evaporable getter pump, the heating of the quartz glass filter is stopped after a predetermined amount of time, cooling of the quartz glass filter below 45 degrees Celsius effectively closes the quartz glass filter to further hydrogen and helium diffusion, the mass spectrometer measures the helium 3 and helium 4 abundance, electronics calculates and records the helium 3 to helium 4 ratio, the ultra high vacuum valve opens and exposes the vacuum chamber to the noble diode ion pump, the noble diode ion pump pumps and sequesters the helium gas level to below a set threshold as measured by the ultra high vacuum total pressure gauge, the apparatus is now prepared to receive another sample, the process is repeated, in the event that the helium is not pumped by the noble diode ion pump to below the set threshold in a predetermined amount of time such an indication is recorded, if telemetry is available this indication of not reaching a predetermined helium threshold level is telemetered, the unit is then shut down.

(59) Objects and Advantages

(60) Accordingly, besides the objects and advantages of the selective fluid bandpass filter and means for .sup.3He/.sup.4He ratio determination described in our patent application, several objects and advantages of the present invention are: (a) to provide for a field deployable instrument for .sup.3He/.sup.4He ratio determination. (b) to provide for a compact deployable instrument for .sup.3He/.sup.4He ratio determination. (c) to provide for a low power instrument for .sup.3He/.sup.4He ratio determination. (d) to provide for a high resolution field deployable instrument for .sup.3He/.sup.4He ratio determination. (e) to provide for a commercial means of separation of .sup.3He from available terrestrial helium sources. (f) to provide for a commercial means of fusion reactor fuel production. (g) to provide for a commercial means of target material for neutron detectors used for fusion laboratory experiments. (h) to provide for a commercial means of target material for neutron detectors used for non-fusion laboratory experiments. (i) to provide for a commercial means of target material for neutron detectors used in portable nuclear security monitors.

CONCLUSION, RAMIFICATIONS, AND SCOPE

(61) In the descriptions above, the reader has seen several embodiments of our mass selective fluid bandpass filter and means of portable, field deployable .sup.3He/.sup.4He ratio determination. There are differing applications for these apparatus and means. One example is a portable, field deployable instrument for .sup.3He/.sup.4He ratio determination. Another example is a commercial means of separation of .sup.3He from available terrestrial helium sources. These very different applications make best use of differing embodiments of our mass selective fluid bandpass filter.

(62) The operational embodiment of this invention is applicable to .sup.3He/.sup.4He ratio determination and commercial .sup.3He production. The basic mechanism of the mass selective fluid bandpass filter is to provide for the selective transmission of a gas of specific mass across the filter and provide for the selective blockage of transmission of related gases of nearly identical mass to that of the selected gas. Furthermore, the mass selective fluid bandpass filter and means of this invention has the additional advantages in that: (a) the gas mass selected for transmission is controlled by the temperature of the filter. (b) gases of nearby lower mass are selectively rejected. (c) gases of nearby higher mass are selectively rejected (d) the gas mass selected for transmission is adjustable by changing the temperature of the filter. (e) to provide for a field deployable instrument for .sup.3He/.sup.4He ratio determination. (f) to provide for a compact deployable instrument for .sup.3He/.sup.4He ratio determination. (g) to provide for a low power instrument for .sup.3He/.sup.4He ratio determination. (h) to provide for a high resolution field deployable instrument for .sup.3He/.sup.4He ratio determination. (i) to provide for a high sensitivity field deployable instrument for .sup.3He/.sup.4He ratio determination. (j) to provide for a commercial means of separation of .sup.3He from available terrestrial helium sources. (k) to provide for a commercial means of fusion reactor fuel production. (l) to provide for a commercial means of target material for neutron detectors used for laboratory fusion experiments. (m) to provide for a commercial means of target material for neutron detectors used for laboratory experiments. (n) to provide for a commercial means of target material for neutron detectors used in portable nuclear security monitors.

(63) While our above description contains many specificities, these should not be construed as limitations on the scope of the invention, but rather as an exemplification of one preferred embodiment thereof. Many other variations are possible. For example: (a) thinning the quartz glass membrane from that of our initial experimental conditions. (b) applying pressure to the gas in contact with the glass. (c) increasing the pressure differential across the glass. (d) using a multiplicity of tubes in the filter structure. (e) supporting thin quartz glass windows by either sintered quartz glass or metal in contact with a vacuum. (f) high-temperature heating to fuse the glass covering over the supporting sintered material.

(64) In the descriptions above, we have put forth theories of operation that we believe to be correct. While we believe these theories to be correct, we don't wish to be bound by them. While there have been described above the principals of this invention in connection with specific apparatus, it is to be clearly understood that this description is made only by way of example and is not as a limitation to the scope of the invention. Accordingly, the scope of the invention should be determined not by the embodiment (s) illustrated, but by the appended claims and their legal equivalents.