This invention relates to neutron detectors and in particular to solid state neutron detectors.
Neutron detectors are used for monitoring of cargo containers and vehicles for nuclear weapons because neutrons are emitted by radiological materials of interest such as plutonium and they are difficult to shield. Neutron detectors are also used in other applications such as medical diagnostics, oil and gas exploration; and scientific research. The prior art includes several different types of neutron detectors, as described here.
Helium-3 (3He) tube detectors are the dominant technology used for neutron detection due to their superior sensitivity to neutrons. These detectors are also relatively insensitive to high energy electromagnetic (gamma) radiation thus enabling very low false positive detection capability for neutrons. 3He detectors consist of a stainless steel or aluminum tube cathode filled with a gas mixture that contains 3He. An anode wire is located at the center of the tube and a voltage, typically 1000 V, is applied from the cathode to the anode. An incident neutron interacts with an 3He atom, producing a proton and tritium atom that move in opposite directions with 764 KeV kinetic energy, ionizing the surrounding gas. The liberated electrons are collected at the anode producing a detectable pulse. 3He proportional tubes typically vary in diameter up to 50 mm and in length up to 2 meters. The gas is usually pressurized in the tube to increase the 3He density with pressures ranging from 2 to 20 atmospheres. Hand held detectors have more typical dimensions of 25 mm diameter and 10 to 20 cm active length and pressures up to 4 atmospheres.
Boron tri-fluoride (BF3) proportional counters consist of a stainless steel or aluminum tube cathode filled with a gas mixture that contains BF3. The boron is commonly enriched to >90% boron-10 (10B). An anode wire is located in the center of the tube and a voltage, typically 3000V, is applied from the cathode to the anode. An incident neutron interacts with a 10BF3 molecule, producing an alpha and ionized 7Li particle that move in opposite directions, ionizing the surrounding gas. The liberated electrons are collected at the anode producing a detectable pulse. 10BF3 proportional tubes come in similar sizes as the 3He tubes, but typically have ⅕ the sensitivity of the 3He tubes and relatively poor gamma insensitivity. The 10BF3 gas is toxic and each neutron reaction produces three fluorine atoms that are highly corrosive; this poses manufacturing and operational risks for this technology.
Boron-lined proportional counters incorporate the enriched 10B as a solid film coating on the interior tube surface area. Otherwise, the geometry is the same as for the gas filled proportional counters. The tube is filled with two to three atmospheres of buffer gas (e.g. argon gas). An incident neutron interacts with a 10B, producing an alpha and ionized 7Li particle that move in opposite directions, ionizing the surrounding gas. The liberated electrons are collected at the anode producing a detectable pulse. 10B line tubes typically have 1/7 the sensitivity of the 3He tubes and relatively poor gamma insensitivity.
Solid state neutron detectors using crystalline semiconductor materials have been demonstrated; specifically, a 10B layer coated on a GaAs p-n photodiode to provide 4% intrinsic efficiency for neutron detection. However, crystalline semiconductor neutron detectors cannot be stacked to provide higher neutron detection efficiency. Fabrication techniques involving the etching of trenches in the semiconductor photodiode and backfilling with 10B material are under development to increase the neutron detection efficiency of the single 10B layer devices.
Other methods of neutron detection include neutron sensitive scintillating fiber detectors based on 6Li-loaded glass, 10B-loaded plastic; and 6Li-coated or 10B-coated optical fibers. The interaction of the neutron either a 6Li or 10B atom produces particles and gamma radiation that produce visible light. The visible light travels down the optical fiber to a detector, typically a photo-multiplier tube (PMT). The relatively high cost of these technologies has resulted in limited deployment.
What is needed in a low-cost neutron detector that can justify substantially greater deployment.
This invention provides a low-cost device for the detection of thermal neutrons. Thin layers of a material chosen for high absorption of neutrons with a corresponding release of ionizing particles are stacked in a multi-layer structure interleaved with thin layers of hydrogenated amorphous silicon PIN diodes. Some of the neutrons passing into the stack are absorbed in the neutron absorbing material producing neutron reactions with the release of high energy ionizing particles. These high-energy ionizing particles pass out of the neutron absorbing layers into the PIN diode layers creating electron-hole pairs in the intrinsic (I) layers of the diode layers; the electrons and holes are detected by the PIN diodes. These stacks can be mass-produced at very low cost utilizing integrated circuit fabrication processes. A preferred neutron absorbing material is boron 10 (10B) which has a high neutron capture cross section and splits into a high-energy alpha particle and a high-energy lithium 7 isotope each of which can produce ionization in the hydrogenated amorphous silicon PIN diodes.
Preferred embodiments utilize boron enriched in the boron-10 (10B) isotope. When a neutron passes through the detector, the interaction of the neutrons with the 10B isotopes generates ionizing alpha particles and lithium 7 particles to produce electron hole pairs in the intrinsic layers of the PIN diodes. Preferred embodiments include 5, 10, 15 and 22 layer stacks. The stacked structure can provide very high intrinsic efficiency (greater than 80% for a twenty-two 10B layer stack) for thermal neutron detection.
The multiple diodes are electrically combined in parallel to provide the total neutron-induced signal current thus enabling a low overall bias voltage (≈10 V) for the detector. The a-Si:H diodes have a very low cross section for gamma radiation and discrimination circuitry is used to further reduce detection of incident gamma rays. Fast neutrons (with energies greater than 1 eV) can be detected by enclosing the thermal neutron detector in a neutron moderator material (polyethylene, for example) that slows the fast neutrons to thermal velocities.
A key element of invention is the use of hydrogenated amorphous silicon (a-Si:H) for the interleaved diodes. The disordered structure of a-Si:H provides an elastic property to the semiconductor material, relative to crystalline semiconductor materials. This elastic property enables the stacking of a plurality of 10B layers interleaved with the a-Si:H diodes by reducing the interfacial stress between layers. In addition, the a-Si:H diodes can be deposited directly onto metal electrode substrate material. Several other isotopes are available that produce high-energy ionizing particles with the absorption of neutrons and can be used in the place of the boron-10 isotope.
Amorphous silicon cannot detect neutrons directly. Therefore, a neutron absorbing layer is used to capture the neutron and emit one or more ionizing particles that may then be detected in adjacent a-Si:H diodes. Several candidates for this layer with large neutron capture cross-sections include Lithium (7Li), Boron (10B), and Gadolinium (Gd). The preferred embodiment is a 10B layer because it offers a large capture cross-section for thermal neutrons (3840 barns) and rapid emission of moderate energy ionizing alpha particles at 1-2 MeV. 10B occurs with a natural abundance of 19.9%, but this may be increased to nearly 100% by enrichment. In addition, 10B has a relatively low atomic number (Z=5) thus enabling relatively high insensitivity to high energy electromagnetic (gamma) radiation. Another key advantage to using a 10B containing layer is that thin film layers may be grown by conventional semiconductor processes. Neutrons interact with 10B via the 10B(n,α)7Li reaction:
The 7Li produced in the first reaction path begins in the first excited state, but rapidly drops to the ground state via the emission of a 480 KeV gamma ray. The two products (7Li and a) of each reaction are emitted in opposite directions.
The thicknesses of the diode layers are determined based on the range of the ionizing particles in a-Si:H. Higher energy particles have a longer range within the a-Si:H material, so the characteristic range is calculated using the 1.470 MeV alpha particle of the most common reaction. The range of an alpha particle in a-Si:H is given by
where λ=0.2154 MeV−1, S0=497 MeV-cm, and A0=5.47 [Ho Kyung et. al., Journal of the Korean Nuclear Society, Vol. 28, No. 4, pp 397-405, August 1996]. For a 1.47 MeV alpha particle, this yields a range of 5.23 μm. Therefore, the a-Si:H diodes must be at least 5 microns thick for maximum charge pair generation. The average ionizing energy required to generate an electron-hole pair in a-Si:H is 5 eV. The alpha and/or ionized lithium particle will, on average, still retain between 300 KeV-1 MeV of kinetic energy when it leaves the 10B layer and reaches the a-Si:H diode, therefore the particle will generate 60,000-200,000 electrons as it is stopped by the a-Si:H diode.
P
ABS(N)=1−exp└−NPABS,SINGLELAYER┘
where PABS,SINGLELAYER=0.08 is the intrinsic efficiency for neutron detection in a single 10B layer device.
The electrical capacitance scales linearly with the area of the detector; and also scales linearly with the number of stacked a-Si:H diodes, since the capacitance of each diode in the stacked detector adds when connected in parallel. Therefore, the characteristic time constant T=RC grows linearly with the area and number of stacked diodes.
The preferred embodiment for the neutron detector, displayed in
The fabrication the preferred embodiment of the neutron detector shown in
The a-Si:H diode structures are fabricated using plasma enhanced chemical vapor deposition (PECVD). In this process, feedstock gases are delivered to a vacuum chamber and dissociated by means of a radio frequency (RF) plasma. When the gases are broken down, the resulting radicals react at all exposed surfaces, resulting in film growth. The preferred diode is deposited on a substrate, typically 1 mm thick, that has low absorption cross-section for neutrons, including high purity silicon wafer material, or high purity glass material. The first deposited layer for an a-Si:H P-I-N diode is a metal electrode layer such as titanium nitride (TiN), titanium tungsten (TiW), or indium tin oxide (ITO) layer, approximately 300 angstroms thick. The second deposited layer is a p-type doped layer that is produced using silane (SiH4) gas with a small amount of diborane (B2H6) gas; this p-layer is typically 200 angstroms thick. The third deposited layer is the intrinsic amorphous silicon i-layer that is produced using silane gas; this layer is typically 5 microns thick. The fourth deposited layer is an n-type impurity doped layer that combines silane gas with a small amount of phosphine (PH3) gas; this layer is typically 200 angstroms thick. The fifth deposited layer is a top electrode layer such as TiN, TiW, or ITO, approximately 300 angstroms thick.
Amorphous silicon diode structures of the types shown in
A PIN diode structure fabricated from hydrogenated amorphous silicon (a-Si:H) has similar electrical charge generation and collection properties as a crystalline silicon diode. The amorphous P, I, and N layers feature a disordered, but somewhat periodic, spacing of the silicon atoms; these atoms are surrounded by a plurality of hydrogen atoms and held together essentially by a large network of hydrogen bonds. The bulk semiconductor properties arise from averaging the microscopic features of the diode structure. The periodicity of the silicon atoms in the amorphous diode has enough definition so that amorphous semiconductor material has a forbidden energy bandgap separating the conduction and valence bands, and a spatial depletion region primarily in the I-layer. The forbidden energy bandgap in an amorphous material tends to feature a much larger density of energy states than in a crystalline semiconductor material due to the amorphous nature of the material. This leads to increased dark current and lower mobility of charges in an amorphous diode material. However, these material properties can be controlled in an a-Si:H diode to the level required for a high performance neutron detector.
The major practical advantage of a-Si:H diode structures involves the elastic nature of the material. The a-Si:H coating can gracefully incur much larger stresses because the silicon atoms are imbedded in a sea of hydrogen atoms; the hydrogen bonds provide material elasticity that enables the a-Si:H layers to be deposited directly onto non-crystalline materials, such as metal electrode materials, for example. In comparison, crystalline materials, fabricated using molecular beam epitaxy (MBE), require precise lattice matching to a flat underlying crystalline substrate, in order to control the interface stress. This elastic feature of a-Si:H diodes enables both the single 10B layer and the multiple 10B layer neutron detectors to be fabricated.
The 10B layers are deposited in one of three methods; 1) evaporation of enriched 10B powder, 2) plasma enhanced chemical vapor deposition (PECVD) of enriched boron carbide (10BC4) from enriched diborane (10B2H6) and methane (CH4) precursors, which are already used for a-Si:H diode deposition, and 3) sputtering of enriched boron or boron carbide (BH4) targets. 10B powder is commercially available and presently appears to be the most cost effective method for fabrication of the 10B layers. Semiconductor-grade 10B enriched diborane is commercially available for PECVD processing. 10B enriched boron and boron carbide sputter targets are also commercially available.
Neutron detectors require relatively high insensitivity to gamma radiation in order to reduce false positive neutron detections. The Applicant's neutron detector will be relatively insensitive to gamma radiation for three reasons:
Gamma radiation interacts with a-Si:H by different processes depending on the energy of the gamma photon. At low energies up to about 100 KeV, the photoelectric effect is the dominant mode of interaction, where the gamma photon imparts its full energy to a single electron. At energies from about 100 KeV to several MeV, interactions are dominated by Compton scattering, where the gamma ray loses a fraction of its energy to an electron through an inelastic collision. At high energies above several MeV, the interaction is dominated by electron-positron pair production.
The product of the gamma photon interaction with a-Si:H is an energetic electron that will then ionize surrounding atoms as it moves through the a-Si:H material. The range R of an energetic electron in matter is dependent on the energy of the electron and the density of the material it is moving through. This range may be approximated using the following equation
where E is the energy of the energetic electron and ρ is the density of the material [E. M. Hussein, Handbook on Radiation Probing, Gauging, Imaging and Analysis: Volume I Basics and Techniques (Non-Destructive Evaluation Series), Springer; 1 edition (May 31, 2003)].
The upper limit of the gamma energy absorbed in our preferred neutron detector (five 10B layers with adjacent a-Si:H diodes) can be calculated, assuming that the absorbed gamma photon imparts all of its energy in a single event, thereby liberating an energetic electron (beta particle) in the diode stack.
A second preferred embodiment of the thermal neutron detector, displayed in
The neutron detectors can be fabricated using thin-film deposition techniques developed for solar cell and/or thin-film transistor (TFT) fabrication. The primary detector component, the stacked 10B-layer/a-Si:H diode stack, can be manufactured at a dedicated amorphous silicon solar cell foundry or TFT foundry. The neutron detector can be fabricated as a single monolithic semiconductor stack in sizes up to the present limit of solar cell manufacturing technology (˜1 m2). These foundries also possess techniques and equipment for electrically dividing the large areas into the smaller areas required for specified neutron counting rates, as well as inter-connect technology to electrically connect the smaller area detectors to external counting/discrimination circuitry. This will enable large area, high performance neutron detectors to be manufactured at relatively low cost.
Fast neutrons (>1 eV) present a much smaller capture cross section than thermal neutrons (<1 eV) and thus capture efficiency drops dramatically with energy. Thus fast neutrons are nearly invisible to the preferred embodiment of the neutron detector. The energy of fast neutrons can be reduced to that of thermal neutrons by passing the neutrons through a neutron moderator material such as graphite or high density polyethylene (HDPE). A moderator consists of a material with light nuclei that reduce the neutron energy through elastic collisions while presenting a small capture cross section so that the neutron is not absorbed.
Although the present invention has been described above in terms of preferred embodiments, persons skilled in this art will recognize there are many changes and variations that are possible within the basic concepts of the invention. For example, neutrons interact with several other isotopes to produce neutron-alpha reactions. To the extent these isotopes can be incorporated into a solid material they could replace the boron-10 described in the preferred embodiments. Also neutrons interact with other isotopes to produce neutron-proton reactions. Replacing boron 10 with these isotopes would permit the high energy protons to be detected in the a-Si:H diodes. The boron 10 isotope could be replaced by fissionable material such as U-235 in which case fission products would be detected in the aSi:H diodes.
The thickness of the layers can be varied based on considerations such as cost, efficiency, energy of the ionizing particles and other considerations. The a-Si:H layers, for boron-10 alpha particles, will typically have thicknesses of less than 10 microns, preferably between 2 and 10 microns. The neutron absorbing layers for boron may be adjusted based on the degree of enrichment in boron 10, but typically will be less than 10 microns and preferably will range between 1 and 3 microns. When utilizing materials other than boron as the neutron absorber, the thickness will probably need to be adjusted accordingly based on the issues discussed with respect to the specific preferred embodiments.
Therefore the reader should determine the scope of the present invention by the appended claims and not by the specific examples described above.
This application claims the benefit of Provisional Patent Application Ser. No. 61/343,488 filed Apr. 28, 2010.
Number | Date | Country | |
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61343488 | Apr 2010 | US |