• 专利附录
  • 专利说明
  • 权利要求
  • 类似技术
  • 同族专利
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    • 专利摘要:
    Solid white noble gases for nuclear reactions. An object of the present invention is a solid target of noble gases for nuclear reactions comprising a porous film of a material selected from silicon, copper, cobalt, titanium, aluminum or tungsten, which contains in its pores a gas that is selects between helium and neon, pure or combinations thereof with each other and with argon. Other objects of the invention are the method of preparation of the solid target, as well as its use in experiments of elastic dispersion and inverse kinematics. (Machine-translation by Google Translate, not legally binding)
    公开号:ES2582052A1
    申请号:ES201630711
    申请日:2016-05-31
    公开日:2018-01-04
    发明作者:Vanda Cristina Fortio Godinho；Jaime CABALLERO-HERNANDEZ；Asunción FERNANDEZ CAMACHO；Francisco Javier FERRER FERNANDEZ；Joaquin GOMEZ CAMACHO；Begoña FERNANDEZ MARTÍNEZ
    申请人:Consejo Superior de Investigaciones Cientificas CSIC；Universidad de Sevilla；
    IPC主号:
    专利说明:

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    DESCRIPTION
    SECTOR OF THE INVENTION
    Nuclear physics and particularly the study of the properties of nuclei far from the stability line
    STATE OF THE TECHNIQUE
    One of the most powerful experimental tools for investigating the properties of nuclei away from the stability line ("exotic" nuclei) is the study of nuclear reactions with either protons [elastic dispersion (p, p), transfer of a neutron (p, d), transfer of two neutrons (p, t)], either with ions of He [elastic dispersion (4He, 4He), transfer of two neutrons (4He, 6He) and even transfer of four neutrons (4He , 8He)].
    Note that exotic nuclei cannot be used as targets in these nuclear reactions, due to their short life and therefore these experiments are carried out using as an ion beam the exotic nuclei and as a target the light ion (p, d, He). Since the object of study is the projectile, and not the target, these experiments are called "reverse kinematics."
    For proton reactions, since hydrogen is gas, polyethylene (CH2) n sheets are often used to have a solid hydrogen blank that is introduced into the reaction chamber. The study of nuclear reactions of exotic nuclei with solid targets of He, would be very useful to obtain information of these nuclei complementary to that obtained with hydrogen targets.
    The use of He targets is difficult since He is a gas, and does not form solid molecules as in the case of H. Despite this, experiments with gas targets have been made, in which the gradual loss of energy from the beam, as well as the difficulty of obtaining an acceptable angular resolution, since the point where the reaction occurs is not known a priori. White ones have also been used
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    of metallic solids implanted with He in which the amount of He is limited by the ionic creep used for implantation.
    The use of H and He targets is reflected in the state of the art since 1939:
    - N. P. Heydenburg; R. B. Roberts "Deuteron-Deuteron, Proton-Helium, and Deuteron-Helium Scattering” Physical Review vol. 56 (1939) 1092-1095
    - N. P. Heydenburg; L. R. Hafstad and M. A. I had "The Scattering of Protons by Protons. III" Physical Review vol. 56 (1939) 1078-1091.
    Other relevant publications that can be mentioned between 1940 and 2000 are:
    - G. Freier; E. Lampi; W. Sleator and J.H. Williams "Angular Distribution of 1- to 3.5-MeV Protons Scattered by He” Physical Review vol. 75 (9) (1949) 1345-1347 in which the angular distribution of protons dispersed by 4He is measured in the laboratory system in the range of 1 to 3.5 MeV and at a range of angles between 10 ° and 164 ° The dispersion chamber was filled with purified gaseous helium by pre-storage in an activated carbon trap, before passing it into the vacuum chamber.
    - A.C.L. Barnard; C. M; Jones and J.L. Weil "Elastic Scattering of 2-11 MeV protons by He4" Nuclear Physics 50 (1964) 604-620 in which the effective sections for elastic dispersion of protons by 4He were measured in a range of proton energies between 2 <Ep < 11 MeV using a tandem accelerator.
    - W. Bradfield-Smith; T. Davinson; A. DiPietro; A.M. Laird; A.N. Ostrowski;
    A.C. Shotter; P.J. Woods; S. Cherubini; W. Galster; J.S. Graulich; P. Leleux;
    L. Michel; A. Ninane; J. Vervier; J. Gorres; M. Wiescher; J. Rahighi and J. Hinnefeld. “Investigation of (a, p) reactions using a radioactive beam”; Nuclear Instruments and Methods in Physics Research A 425 (1999). In this publication, the target chamber consists of two parts: a first blank connected to the beam and the second, separated from the first by a metal window, which could be filled with helium gas at a pressure of 66 mbar, having a chamber filled with gas instead of a cell allowed sweeping wider ranges of energy.
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    - M.S. Smith and K.E. Rehm "Nuclear Astrophysics Measurements with Radioactive Beams”, Ann, Rev. Nucl. Part. Sci. (2001), 51: 91-130, article in which experiments relevant to astrophysics are described, in which hydrogen and helium appear as important targets .
    Already more recently, liquid He white targets have been described which is presented by filling a compact aluminum cell, which is maintained at a temperature below the boiling point of the gas, which may be hydrogen, deuterium or helium. [H. Ryuto; M. Kunibu; T. Minemura; T. Motobayashi; K. Sagara; S. Shimoura; M. Tamaki; Y. Yanagisawa and Y. Yano. "Liquid hydrogen and helium targets for radioisotope beams at RIKEN”; Nuclear Instruments and Methods in Physics Research A, 555 (2005), 1-5].
    In 2014, J. Walshe; M. Freer; C. Wheldon; L. N. Achouri; , N. I. Ashwood;
    W. N. Catford; I. C. Celik; N. Curtis; F. Delaunay; B. Fernández-Domínguez; L. Grassi; Tz. Kokalova; M. Marquis; N. A. Orr; L. Prepolec; V. Scuderi; N. Soic and V. Tokic. "The thick target inverse kinematics technique with a large acceptance silicon detector array"; Journal of Physics: Conference Series 569 (2014) 012052, describe an experimental technique for the study of elastic dispersion using a gaseous blank. The target is I gaseous refills a chamber, adjusting the pressure so that the incident beam is stopped in the gas volume.
    -R. Raabe; A. Andreyev; M. Huyse; A. Piechaczek; P. Van Duppen; L. Weissman; A. Wohr; C. Angle; S. Cherubini; A. Musumarra; D. Baye; P. Descouvemont; T. Davinson, A. Di Pietro; A. M. Laird; A. Ostrowski; A. Shotter; L. I. Galanina; and N. S. Zelenskaya. "2n-transfer contribution in the 4He (6He, 6He) 4He cross section at Ecm. = 11.6 MeV”, Phys. Rev. C 67, 044602 (2003). In this publication the target consists of a sheet of Ta (0, 7 pm thick) implanted with He at different energies The total mass thickness of He in the layer is 2.7 x1017 particles / cm2, although the atomic content of impurities of H, 12C and 16O in this sample is found in quantities comparable to the amount of He.
    -P. Ujic; A. Lagoyannis; T. J. Mertzimekis; F. de Oliveira Santos; S. Harissopulos; P. Demetriou; L. Perrot; Ch. Stodel; M.-G. Saint-Laurent; O. Kamalou; A. Lefebvre-Schuhl; A. Spyrou; M. A. Amthor; S. Grevy; L. Caceres; H. Koivisto; M. Laitinen; J. Uusitalo and R. Julin. "Alpha-particle capture reactions in inverse kinematics relevant to p-
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    process nucleosynthesis ” AIP Conference Proceedings 1377, (2011) 321 where the 4He reaction (78Kr, Y) 82Sr is studied using a 50 pg / cm2 sheet of Al (0.2 pm) implanted with 1.3 x1017 particles / cm2 of He.
    The development of solid helium targets, with a high number of He particles and a low amount of impurities (H, C, O) through their incorporation into silicon, would be very useful, since it would allow nuclear dispersion experiments, using the same detection systems that are used for solid hydrogen (polyethylene) targets, with robustness and withstanding a high number of irradiations without significant loss of He as already demonstrated in Si targets: I have already undergone a high number of irradiation (creep equal to 6x1017 particles / cm-2) without significant loss of He.
    The preparation of these materials is reflected in R. Schierholz; B. Lacroix; V. Godinho; J. Caballero-Hernández; M. Duchamp and A. Fernández. "STEM-EELS analysis reveals stable high-density He in nanopores of amorphous silicon coatings deposited by magnetron sputtering." Nanotechnology, Volume 26, Number 7 (2015) 075703, in which details of the deposition by sputtering ("magnetron sputtering") in terms of materials (specifically, Si), high vacuum conditioning, angle, distance, power, He pressure, etc. The results of the experiment are provided in terms of the product obtained, of which it is mentioned that it has an atomic 21% of He and of which a porosity of 22% is calculated. It is also mentioned that the density of He inside the pores is 25 to 54 at / nm-3 and the values of the calculation of the pressure of He inside the pores are collected.
    It would also be desirable to have self-supported solid targets for nuclear reactions that improve the performance obtained with the devices and materials referred to in the prior art.
    BRIEF DESCRIPTION OF THE INVENTION
    Different terms used throughout the description of the present invention are defined below.
    In nuclear reactions, the atomic nucleus is defined as a target which, when bombarded by neutrons or charged particles (projectile), reacts by emitting a
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    or more particles. Solid white is defined as a solid material that contains the atomic nucleus of interest.
    Substrate is defined as the physical support on which the porous coating is deposited.
    Mass gas thickness is defined as the thickness of the material used as white in units of mass per unit area. The unit used will be atoms of material per square centimeter. The reason for this is that in the interaction of charged particles with matter, there is a functional relationship with the density of the medium.
    Atomic percentage (% at) is defined as the percentage of atoms of a given element with respect to the total number of atoms.
    The ratio between the gas and the material of the porous film is defined as the ratio between the number of atoms in the gas and the number of atoms in the material of the porous film.
    Self-supporting coating is defined as the coating without substrate that can be handled.
    In a first aspect, the object of the present invention constitutes a solid target of noble gases for nuclear reactions comprising a porous film of a material selected from silicon, copper, cobalt, titanium, aluminum or tungsten, which contains in its pores a gas that is selected from helium and neon, cigars or combinations thereof with each other and with argon.
    In order to obtain the best performance as a target for nuclear reactions, the porous film has a mass thickness of gas between 50 x 1015 at / cm2 and 10000 x 1015 at / cm2 with a ratio between the gas and the material of the porous film included between 0.05 and 0.50 and the presence of impurities remains the same or below 5% at for O of 1% at for C.
    In a preferred embodiment, the porous film is made of silicon or cobalt and has a mass thickness related to these elements between 1000 and 20,000 x 1015 at / cm2. In an even more preferred embodiment, the gas contained in the pores of the film is helium. A second aspect of the object of the present invention is the process of preparing the solid blank on substrate or self-supporting defined above. This procedure includes the following stages:
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    The deposition of these porous layers has been performed by sputtering ("magnetron sputtering") using a blank of a material selected from Silicon, Copper, Cobalt, Titanium, Aluminum, Tungsten in an atmosphere of He, Ne, pure or combinations of them with each other or with Ar. Before the deposition, a vacuum is made in the chamber with heating of the walls to reach residual voids in the range of 5x10-5 to 10-4 Pa. For the production of coatings with different mass gas thickness, mixtures with different fractions have been used of X / (X + Ar), from 0.2 to 1 X, where X is the gas: He, Ne or mixture of both keeping the total pressure constant at 4.9 Pa and a substrate-white distance between 5 and 10 cm . A radio frequency source or a dc source is used, preferably at a power of 50 to 300 W. The thickness of the coating is controlled by adjusting the deposition time and the applied power. In a preferred embodiment, the deposition stage has a duration between 30 minutes and 5 hours.
    Finally, the use of solid targets in elastic dispersion experiments and in reverse kinematics experiments is a third object of the invention.
    The coatings used as solid targets in elastic dispersion experiments are deposited on monocrystalline silicon substrates or glazed carbon substrates. The self-supported coatings used as targets in inverse kinematics experiments were previously deposited on sodium chloride substrates. The transfer of the coating of this substrate to the frame, in which it remains self-supporting, is done by immersing the sodium chloride with the coating in distilled water. The coating that detaches from the substrate, floats, and recovers with the frame.
    BRIEF DESCRIPTION OF THE FIGURES
    Figure 1: a) Detail of the porous microstructure of the silicon layer; b) electron diffraction of the coating showing its amorphous character.
    Figure 2: Proton backscatter spectrum of the coating
    Figure 3: Scanning micrograph of self-supporting coating
    Figure 4: Image of the coating on the frame
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    Figure 5: Proton backscatter spectrum of the self-supporting coating
    Figure 6: a) Si solid white scheme: I have coated by Au; b) proton backscatter spectrum on the solid target and c) effective section leaves 4He (H, H) 4He elastic dispersion between 0.6 and 3.0 MeV at 165 °.
    Figure 7: a) 6Li ++ ion forward dispersion device of 6 MeV energy and 30 ° dispersion angle in samples Si: He and b) 6Li ++ ion forward dispersion spectrum of 6 MeV energy and angle of 30 ° dispersion in sample Yes: I have self-supported
    MODE OF EMBODIMENT OF THE INVENTION
    A series of examples are described below by way of illustration of the invention.
    Example 1. Manufacture of the solid white of He with mass metal thickness between 1000 x1015 at / cm2 and 3000 x1015 at / cm2 and mass thickness of gas between 50 x1015 at / cm2 and 1500 x1015 at / cm2
    The solid blank that is subsequently used in nuclear reactions of elastic dispersion is prepared using the magnetron sputtering technique in a vacuum chamber, using an initial blank for sputtering pure silicon (Kurt J. Lesker 99.999%) of 5 cm in diameter , in an atmosphere of He. Prior to deposition, a vacuum is made in the chamber with heating of the walls to achieve residual voids in the range of 1 * 10 "4 Pa. The coating is deposited at a pressure of 4.9 Pa, in dynamic flow, measured in a Capacitance pressure gauge and using a radio frequency source at a power of 50 W. The distance between the initial target for sputtering and the sample holder is 5 cm and the coating is deposited for 4 hours on monocrystalline silicon substrates with orientation (100 ).
    The microstructure of the coating has been studied by transmission electron microscopy (TEM). Figure 1 shows a micrograph of the coating where you can see the porous structure of ellipsoidal pores with diameters between 2 and 30 nm. Electron diffraction (ED) shows that the porous coating is amorphous.
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    The composition and mass thickness of the sample were analyzed by proton backscatter spectrometry (Figure 2). The coating has a total mass thickness of 4250 x1015 at / cm2 and consists of 2750 x1015 at / cm2 of Si and 1400 x1015 at / cm2 of He with an O incorporation of 100 x1015 at / cm2.
    Example 2. Manufacture of the self-supporting solid white I with a mass metal thickness between 3000 x1015 at / cm2 and 20000 x1015 at / cm2 and a mass gas thickness between 1500 x1015 at / cm2 and 10000 x1015 at / cm2
    The self-supporting solid white that is subsequently used in nuclear reactions of reverse kinematics, is prepared using the magnetron sputtering technique in a vacuum chamber, using an initial blank for sputtering pure silicon (Kurt J. Lesker 99.999%) of 5 cm diameter, in an atmosphere of He. Prior to deposition, a vacuum is made in the chamber with heating of the walls to achieve residual voids in the range of 4 * 10 "4 Pa. The coating is deposited at a pressure of 4.9 Pa, in dynamic flow, measured in a Capacitance pressure gauge and using a radio frequency source at a power of 150 W. The distance between the initial target for sputtering and the sample holder is 10 cm and the coating is deposited for 5 hours on sodium chloride and silicon substrates.
    The microstructure of the coating has been studied by scanning electron microscopy in the sample deposited on monocrystalline silicon presented in Figure 3.
    The coating deposited on sodium colide was transferred to the frame by immersing the sodium chloride with the coating in distilled water. The coating detaches from the sodium chloride substrate, floats and recovers with the frame. It is then allowed to air dry.
    The composition and mass thickness of the sample were analyzed by proton backscatter spectrometry (Figure 5). The coating has a
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    total mass thickness of 14000 x1015 at / cm2 and consists of 9100 x1015 at / cm2 of Si and 4200 x1015 at / cm2 of He with an incorporation of O of 700 x1015 at / cm2.
    Example 3. Study of the effective section of the elastic dispersion 4He (H, H) 4He between 0.6 and 3.0 MeV at 165 ° using a solid white of He
    This example describes the study of the effective section of the elastic dispersion 4He (H, H) 4He using as a solid white of He a porous silicon coating containing He.
    The coating is prepared using the magnetron sputtering technique in a vacuum chamber, using an initial blank for sputtering pure silicon (Kurt J. Lesker 99, 999%) of 5 cm in diameter, in an atmosphere of He. Prior to deposition, a vacuum is made in the chamber with heating of the walls to achieve residual voids in the range of 4 * 10 "4 Pa. The coating is deposited at a pressure of 4.9 Pa, in dynamic flow, measured in a Capacitance pressure gauge and using a radio frequency source at a power of 150 W. The distance between the initial target for sputtering and the sample holder is 5 cm and the coating is deposited for 30 minutes on monocrystalline silicon substrates.
    The proton backscatter spectrometry analysis of the coating (Figure 6b) has a total mass thickness of 2200 x1015 at / cm2 and consists of 1500 x1015 at / cm2 of Si and 700 x1015 at / cm2 of He.
    On the solid white, prepared as defined in the preceding paragraphs, a thin layer of gold was deposited, used as an internal standard for dose measurement. In the deposition of this layer an Emitech K550 metallizer was used in an Ar atmosphere with a 10mA discharge for 90s. Au has been chosen as a surface material since the effective section of the Au (H, H) Au process is known (Rutherford) in the entire range of energies studied. The concentrations of Au, Si and He indicated are chosen to have layers thin enough to avoid significant losses or dispersion in energy of the proton beam and thick enough to obtain visible signals from the elements.
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    The solid blank used is schematized in Figure 6 (a). It consists of a system of two layers stacked on a substrate. The outermost layer is a thin Au film of 1.1 x 1015 at / cm2. The next layer consists of a porous layer of Si with He.
    The solid white is placed in a vacuum chamber at 5 x 10-4 Pa pressure. A beam of protons (H +) is affected with energies in the range of 0.6 to 3.0 MeV in steps of 0.1 MeV. The protons dispersed by the Au, the Si and the He of the sample have different energies. The energy of these protons is measured using a "Passivated Implanted Planar Silicon" (PIPS) type detector placed at a certain dispersion angle. From the measurement of the intensities of the Au and He signals the section can be calculated Effective dispersion 4He (H, H) 4He for a given angle and energy of the incident H +, by comparison with the effective section of the Au (H, H) Au process using the formula
    0He (E) = ^ Au, Ruth (E) "(AHe / AAu)" ((Nt) Au / (Nt) He)
    where oAu, Ruth (E) is the Rutherford effective section of the protons on Au at a given energy E, (AHe / AAu) is the quotient of the areas of the signals of He and Au respectively and ((Nt) Au / ( Nt) He) are the mass thickness of Au and He respectively.
    By changing the energy of the incident H + beam it is possible to obtain effective section curves for a given angle (Figure 6c)
    Example 4. Elastic dispersion 4He (6Li, 6Li) 4He as the basis for inverse kinematic experiments 4He (11Li, 11Li) 4He
    In this example, a self-supporting solid solid white He is used, comprising a porous layer of Si with He, to study by reverse kinematics the effective section of the 6Li (4He, 4He) 6Li process. This example is presented to illustrate that it would be possible to use the solid target of He described below in inverse kinematics experiments for studies of nuclear reactions with radioactive isotopes such as 11Li.
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    The self-supporting solid blank that is used to study nuclear reactions by reverse kinematics is prepared using the magnetron sputtering technique in a vacuum chamber, using an initial blank for sputtering pure silicon (Kurt J. Lesker 99.999%) of 5 cm. diameter, in an atmosphere of He. Prior to deposition, a vacuum is made in the chamber with heating of the walls to reach residual voids in the range of 4 * 10-4 Pa. The coating is deposited at a pressure of 4.9 Pa, in dynamic flow, measured in a capacitance pressure gauge and using a radio frequency source at a power of 150W. The distance between the initial target for sputtering and the sample holder is 10 cm and the coating is deposited for 5 hours on sodium chloride substrates. The coating deposited on sodium colide was transferred to the frame by immersing the sodium chloride with the coating in distilled water. The coating detaches from the sodium chloride substrate, floats and recovers with the frame. Let it air dry.
    The self-supporting solid white used is schematized in Figure 7 (a). It consists of a self-supporting layer of Si: I have placed it on a rack. The mass thickness of the elements in the layer is 9100 x 1015 at / cm2 of Si and 4200 x 1015 at / cm2 of He (measured by p-EBS).
    The self-supporting solid white is placed in a vacuum chamber at 5 x 10-4 Pa pressure. A beam of 6Li ions with an energy of 6.0 MeV is affected. The different elements of the sample disperse the Li ion beam with different energies because these elements have different masses. In addition, the 6Li ions when interacting with the self-supporting solid white are capable of removing atoms from the sample. The energy of the dispersed and plucked ions in the self-supporting solid white is measured with a PIPS type Si detector at 30 ° dispersion angle as shown in Figure 7 (a). The spectrum of the dispersion experiment is shown in Figure 7 (b). In it you can see, (from higher to lower energy) the signals corresponding to the Li ions dispersed in the Si of the sample (5110 keV), He ions receding (torn) of the sample by Li ions (4045 keV), Li ions dispersed in the He of the sample (3225 keV) and Si ions receded (removed) from the sample by Li ions (2365 keV). The ratio of heights between the Li peaks dispersed by the He of the sample and the Si of the sample (0.03) conforms to the prediction of the theoretical models in force for a sample with a
    He / Si ratio = 0.45. These models take effective sections already known and accepted. These data demonstrate the possibility of using the self-supporting solid white He described in heavy ion dispersion experiments. Although 6Li ions have been used in this example, the self-supporting solid white could be 5 in the same way used in inverse kinematics experiments with exotic ion beams such as 6He, 8He, 11Li, 7Be, 11Be, 10C and 11C.
    权利要求:
    Claims (11)
    [1]
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    1. Solid solid of noble gases for nuclear reactions comprising a porous film of a material that is selected from Si, Cu, Co, Ti, Al and W, which contains in its pores a gas that is selected between He and Ne pure or combinations thereof with each other and with Ar, characterized in that the porous film has a mass of gas between 50 x 1015at / cm2 and 10000 x 1015 at / cm2 with a ratio between the gas and the material of the porous film between 0.05 and 0.50 and also characterized in that the impurity content of O is equal to or less than 5% and the impurity content of C is equal to or less than 1%.
    [2]
    2. Solid white according to claim 1, characterized in that the porous film is silicon or cobalt and has a mass thickness referred to those elements between 1000 and 20000 x 1015 at / cm2.
    [3]
    3. Solid white according to claims 1 or 2, characterized in that the gas contained in the pores of the film is He.
    [4]
    4. Process for preparing a solid blank as defined in claims 1 to 3 comprising:
    - setting vacuum conditions between 5 x 10 "5 and 10" 4 Pa in a chamber with heating on the walls
    - deposition by sputtering in the chamber of the previous stage of the porous film of a material selected from Si, Cu, Co, Ti, Al and W in an atmosphere of pure He and Ne or combinations thereof with each other and with Ar at a pressure of 4.9 Pa and at a distance between substrate and initial blank for sputtering of 5 to 10 cm, using a source that is selected between radio frequency or direct current.
    [5]
    5. Method according to claim 4, wherein the power of the source is between 50 and 300 W.
    [6]
    6. Method according to claims 4 and 5, wherein the deposition stage has a duration between 30 minutes and 5 hours.
    [7]
    7. Use of a solid blank as defined in claims 1 to 3 in elastic dispersion experiments.
    10. Use according to claim 7 wherein the solid targets are deposited on
    monocrystalline silicon substrates.
    [9]
    9. Use according to claim 7, wherein the solid targets are deposited on glazed carbon substrates.
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    [10]
    10. Use of a solid blank as defined in claims 1 to 3 in inverse kinematics experiments.
    [11]
    11. Use according to claim 10 wherein self-supporting coatings 20 are used as solid targets.
    [12]
    12. Use according to claim 11 wherein the self-supporting coatings are previously deposited on NaCl substrates.
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    同族专利:
    公开号 | 公开日
    ES2582052B1|2018-10-18|
    WO2017207848A1|2017-12-07|
    WO2017207848A9|2018-11-22|
    引用文献:
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