CN1322173C - Process for preparing high temperature cerium blended lutetium pyrosilicate scintillation monocrystal - Google Patents

Process for preparing high temperature cerium blended lutetium pyrosilicate scintillation monocrystal Download PDF

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CN1322173C
CN1322173C CNB2004100534382A CN200410053438A CN1322173C CN 1322173 C CN1322173 C CN 1322173C CN B2004100534382 A CNB2004100534382 A CN B2004100534382A CN 200410053438 A CN200410053438 A CN 200410053438A CN 1322173 C CN1322173 C CN 1322173C
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crystal
temperature
scintillation
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cerium
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CN1587447A (en
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赵广军
严成锋
徐军
夏长泰
介明印
何晓明
张连翰
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Shanghai Institute of Optics and Fine Mechanics of CAS
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Abstract

The present invention relates to a method for preparing high-temperature cerium-doped lutetium pyrosilicate scintillation crystals Lu2(1-x-y-z)Re2xCe2yM2zSi2O7. The method has the key point that equivalent Si3N4 raw materials with strong reducibility, such as CeO2, etc. and trace elements of Zr, Ta or Mg, etc. are introduced in the preparation of raw materials, CeO2 is reduced into Ce2O3 in the melting of materials by heating and crystal growth, and lutetium pyrosilicate scintillation monocrystals containing Ce<3+> ions are synthesized through the reaction of the Ce2O3 and oxide, such as SiO2, Re2O3, etc. Cerium-doped lutetium pyrosilicate scintillation high-temperature scintillation crystals prepared by the method of the present invention contain scintillation crystal minimal Ce<4+> ions, and have good crystal lattice perfection and irradiation resistance.

Description

Mix the preparation method of cerium disilicic acid lutetium high temperature scintillating monocrystal
Technical field:
The present invention relates to field of crystal growth, particularly doping trivalent cerium ion (Ce 3+) disilicic acid lutetium high temperature scintillating monocrystal: Lu 2 (1-x-y-z)Re 2xCe 2yM 2zSi 2O 7(wherein Re represents other rare earth element except that Lu, as: one of Y, Gd, Sc, Yb etc. or multiple mixing, M represents metal ions such as Zr, Mg, Ta; 0≤x≤0.3,0.001≤y≤.05,0.00001≤z≤0.0005), and growth method.Be specifically related at initial oxidation raw material (Lu 2O 3, Re 2O 3, CeO 2, SiO 2) the middle adding and CeO 2Si Deng molar equivalent 3N 4Raw material adopts crystal pulling method, falling crucible method and other melt growth method to be prepared and mixes trivalent cerium ion disilicic acid lutetium high temperature scintillation crystal.
Background technology:
Inorganic scintillation crystal can be widely used in research Application Areass such as high energy physics nuclear physics detecting, image nuclear medicine (PET, CT), industrial online detection, safety inspection, geology archaeology, celestial observation.The BGO scintillation crystal is traditional inorganic scintillation crystal, and its biggest advantage is to have bigger density and effective atomic number (ρ=7.13g/em 3, Z Eff=74), therefore has broad application background in high energy physics nuclear physics and nuclear medicine diagnostic fields such as (PET).But there is light output little (light output is about 7-10%Nal (Tl) relatively) in the BGO crystal, grows shortcomings such as (300ns) fall time, and this has just limited BGO crystalline range of application greatly.
The high-temperature oxide scintillation crystal of Ce ion doping as: Ce:GSO, Ce:LSO, Ce:YAP, Ce:LuAP etc. are the novel scintillator crystal materials of a class that comes across the end of the eighties in last century-nineties.With traditional NaI:T1, BGO, BaF2, low melting points such as PWO (being no more than 1500 ℃) inorganic scintillation crystal is compared, the high-temperature oxide scintillation crystal of Ce ion doping is exported (being about BGO crystalline 2-10 doubly) and fast decay (being about BGO crystalline 1/5-1/20) with high light, and therefore, this scintillation crystals enjoys people's attention, referring to: 2002 " artificial lens journal " the 31st the 3rd phase of volume, 291-297 page or leaf.Wherein, the Ce:LSO scintillation crystal is the scintillation crystal that paid close attention to by people at present, compare with the BGO crystal, the Ce:LSO scintillation crystal has higher light output (being about 7 times of BGO crystalline), optical attenuation constant (being about BGO crystalline 1/7) reaches density and the effective atomic number (ρ=7.4g/cm suitable with the BGO crystal faster 3, Z Eff=66), referring to U.S.Pat.No:4,958,080.But the Ce:LSO scintillation crystal has and contains a large amount of Lu elements in high melt point (being about 2200 ℃), the crystal and have shortcomings such as natural radioactivity, so this scintillation crystal is difficult to preparation and the detector made has higher background noise.
Recently, people have found cerium ion-doped disilicic acid lutetium crystal (Ce:Lu again 2-xM xSi 2O 7, be called for short Ce:LPS) and be a kind of inorganic scintillation crystal preferably, this crystal belongs to oblique system, and lattice parameter is respectively: a=6.765 , b=8.839 , c=4.715 , β=101.96 °, density and effective atomic number are respectively 6.23g/cm 3And Z Eff=64.The Ce:LPS scintillation crystal has higher light output and is about 13000-22000Ph/MeV, optical attenuation (being about 30ns) faster, more attractive attention be that this crystalline fusing point has only 1900 ℃, reduced about 200-300 ℃ than the LSO crystal, therefore more or less freely preparation, referring to: U.S.Pat.No:6,437,336.
Cerium ion-doped high temperature scintillation crystal belongs to extrinsic scintillation crystal, and trivalent cerium ion is the luminescence center in the crystal.Its luminescence mechanism is commonly considered as being finished by following 3 steps, and (a) at first scintillation crystal absorbs energetic ray or particle, thereby produces a large amount of electron-hole pairs in lattice; (b) a large amount of high-octane electron-hole pairs carry out relaxation by the interaction between electronics one electronics, electronics one phonon, and it is right to become the thermalized electron hole with energy gap energy at last, and the thermalized electron hole is to transferring energy to Ce again 3+The ionoluminescence center; (c) Ce 3+Ion is sent out twinkling light by the transition of 5d-4f.Studies show that, contain Ce in the crystal 4+During ion, will quencher Ce 3+Thereby the ionoluminescence center reduces the light output of scintillation crystal.Referring to: Journal ofLuminescience 87-89 phase,, 266-268 page or leaf in 2000; Journal of Luminescience 60-611994 P963-966; Nuclear Instruments and Methods in Physics Research A the 320th volume 1992, the 263-272 page or leaf.
Formerly in the technology, cerium ion-doped rare earth disilicic acid lutetium series scintillation crystal (Ce:Lu 2-xM xSi 2O 7, be called for short Ce:LPS), in crystal growing process, the general Ce:Lu that directly adopts 2-xM xSi 2O 7Oxide compound (the Re of correspondence in the chemical formula 2O 3, SiO 2And Ce 2O 3) raw material prepares in molar ratio that the synthetic polycrystal grows, referring to U.S.Pat.No:6,437,336.
Formerly the cerium ion-doped Ce:LPS scintillation crystal of technology growth has following shortcoming: because Ce 2O 3Raw material is easy to become stable tetravalence attitude ion when carrying out sintering in air atmosphere or weak oxide atmosphere, and adopt melt growth methods such as crystal pulling method, float-zone method to be weak oxide atmosphere, the crystal of Huo Deing will contain a certain amount of quadrivalent cerium ion at last, thereby has reduced the output of crystalline light.
In addition, formerly there is more lattice imperfection in the Ce:LPS scintillation crystal of technology growth, thereby reduced the crystalline scintillation properties.
Summary of the invention:
The objective of the invention is to overcome the shortcoming of technology formerly, provide a kind of preparation method who mixes cerium disilicic acid lutetium high temperature scintillation crystal, this single crystal Lu 2 (1-x-y-z)Re 2xCe 2yM 2zSi 2O 7Contain Ce 4+Ion is minimum, has perfection of lattice and anti-radiation performance preferably.
Technical solution of the present invention is as follows:
Key of the present invention is in the process of preparation raw material, introduces and CeO 2The Si of equivalent strong reducing property 3N 4Raw material, and introduce elements such as Zr, the Ta of trace or Mg, and in temperature increasing for melting materials and crystal growing process with CeO 2Be reduced into Ce 2O 3, again with SiO 2And Re 2O 3Deng the synthetic Ce that contains of oxide compound reaction 3+Ionic disilicic acid lutetium high temperature scintillating monocrystal.
Technical solution of the present invention is as follows:
A kind of preparation method who mixes cerium disilicic acid lutetium high temperature scintillating monocrystal, this method comprises the following steps::
1. press the chemical formula Lu of doping trivalent cerium ion disilicic acid lutetium 2 (1-x-y-z)Re 2xCe 2yM 2zSi 2O 7Prepare burden, wherein Re represents other rare earth element except that Lu, and M represents Zr, Mg, Ta metal ion; 0≤x≤0.3,0.001≤y≤0.05,0.00001≤z≤0.0005 is behind selected x, y, the z, by the mol ratio of each component oxide correspondence, i.e. Lu 2O 3: Re 2O 3: CeO 2: MO 2: SiO 2=(1-x-y-z): x: 2y: 2z: 2 weighing initial feed, the purity of each initial feed are all greater than 99.99%, and then take by weighing and CeO 2The Si of equivalent mole 3N 4Raw material, the i.e. Si of y/6 mole 3N 4Raw material;
2. each component raw material thorough mixing is become uniform mixed powder;
3. under the pressure of 1-5Gpa, the blended powder is pressed into columned material cake, carried out low-temperature sintering 10-24 hour being lower than under 500 ℃ the temperature;
4. with in the packaged Iridium Crucible of advancing in the burner hearth of burned material, with the burner hearth sealing and vacuumize, vacuum tightness is about 10 -3-10 -4Pa is in order to guarantee CeO 2Fully reduced, under this vacuum tightness, adopt the Frequency Induction Heating mode to carry out temperature increasing for melting materials with 300-500 ℃/hr heat-up rate;
5. locate when the interior material piece of crucible is warmed up to 1000-1200 ℃, carried out constant temperature 2-3 hour in this temperature range;
6. continue to be warming up to 1900-2000 ℃ with the heat-up rate of 300-500 ℃ of ./hr, wait to expect all fusings after, in this temperature range constant temperature 1-2 hour again;
7. in burner hearth, slowly charge into N 2Gas or Ar gas make the air pressure of burner hearth remain on 1-1.25atm, then, under the Tc of single crystal of the present invention, generally in 1850-1950 ℃ of scope, adopt the cerium ion-doped disilicic acid lutetium high temperature scintillation crystal of technology growth of crystal pulling method, in crystal growing process, adopt pure Lu 2Si 2O 7Seed crystal, the speed of growth are 1-5mm/hr, and the crystal rotating speed is 10-80RPM, crystal through sowing, behind undergauge, shouldering, isometrical, ending and the cooling process, crystal growth is finished.
Described temperature increasing for melting materials adopts plumbago crucible, perhaps tungsten crucible.
Described Lu 2Si 2O 7The seed crystal direction is axial or other crystallization direction of a, b, c.
The present invention compares with technology formerly since in initial feed by adding strong reducing property Si 3N 4Raw material, in vacuum atmosphere with stable CeO 2The raw material reduction is incorporated in the disilicic acid lutetium high temperature scintillation crystal for tervalent cerium ion.Since in disilicic acid lutetium crystal, added the Zr of trace, Mg, and elements such as Ta can suitably be corrected the distortion of lattice, have increased the anti-irradiation ability of crystalline greatly.In addition, owing in the preparation raw material process, added the Si of equivalent 3N 4Raw material, the Si element is excessive relatively, can remedy SiO in crystal growing process 2The scarce Si element problem that volatilization brings.
Embodiment:
Introducing Si of the present invention 3N 4Behind the raw material, in the temperature increasing for melting materials process, make full use of Si 3N 4Strong reducing property, impel and contain a large amount of Ce in melt and the crystal 3+Ion.Simultaneously, since trace Zr, Ta, and the adding of different valence state element such as Mg can also be eliminated the colour center that causes owing to variation of valence, thereby increase the anti-irradiation ability of crystalline greatly, has also increased the LPS perfection of lattice simultaneously.
In the temperature increasing for melting materials process in the raw material following chemical reaction will take place:
Si 3N 4+12CeO 2→6Ce 2O 3+3SiO 2+2N 2?↑ (1)
Doping trivalent cerium ion (Ce of the present invention 3+) disilicic acid lutetium high temperature scintillating monocrystal: Lu 2 (1-x-y-z)Re 2xCe 2yM 2zSi 2O 7(wherein Re represents other rare earth element except that Lu, as: one of Y, Gd, Sc, Yb etc. or multiple mixing, M represents metal ions such as Zr, Mg, Ta; 0≤x≤0.3,0.001≤y≤0.05,0.00001≤z≤0.0005) concrete fabricating technology scheme is as follows:
<1〉by doping trivalent cerium ion disilicic acid lutetium chemical formula Lu 2 (1-x-y-z)Re 2xCe 2yM 2zSi 2O 7In the mol ratio of each component oxide correspondence carry out the weighing initial feed, the purity of each initial feed is all greater than 99.99%.Each component raw material that is promptly taken by weighing and mole proportioning thereof are as follows: Lu 2O 3: Re 2O 3: CeO 2: MO 2: SiO 2=(1-x-y-z): x: 2y: 2z: 2.And then take by weighing and CeO 2The Si of equivalent mole 3N 4Raw material, the i.e. Si of y/6 mole 3N 4Raw material adds in the above-mentioned oxide raw material.
<2〉above-mentioned each component raw material thorough mixing that takes by weighing is become uniform mixed powder;
<3〉will mix raw material, under the pressure of 1-5Gpa, the blended powder is pressed into columned material cake (material cake diameter is slightly less than the vessels crucible diameter), under being lower than 500 ℃ temperature, carries out low-temperature sintering 10-24 hour to remove organism, water and the low melting point impurity in the raw material;
<4〉with in the packaged Ir gold crucible that advances in the burner hearth of burned material, with the burner hearth sealing and vacuumize, vacuum tightness is about 10 -3-10 -4Pa.In order to guarantee CeO 2Fully reduced, under this vacuum tightness, adopt the Frequency Induction Heating mode to carry out temperature increasing for melting materials with 300-500 ℃/hr heat-up rate;
<5〉the material piece in crucible is warmed up to 1000-1200 ℃ and locates, and in order to make aforesaid equation (1) sufficient reacting, carries out constant temperature 2-3 hour in this temperature range;
<6〉continue to be warming up to 1900-2000 ℃ with the heat-up rate of 300-500 ℃ of ./hr, wait to expect all fusings after, for the abundant reaction that guarantees raw material and mix, in this temperature range constant temperature 1-2 hour again;
<7〉in burner hearth, slowly charge into N 2Gas or Ar gas shiled gas make the air pressure of burner hearth remain on 1-1.25atm.Then, at doping trivalent cerium ion (Ce 3+) disilicic acid lutetium high temperature scintillating monocrystal: Lu 2 (1-x-y-z)Re 2xCe 2yM 2zSi 2O 7(wherein Re represents other rare earth element except that Lu, as: one of Y, Gd, Sc, Yb etc. or multiple mixing, M represents metal ions such as Zr, Mg, Ta; 0≤x≤0.3,0.001 under the Tc≤y≤0.05,0.00001≤z≤0.0005) (generally in 1850-1950 ℃ of scope), adopt the cerium ion-doped disilicic acid lutetium high temperature scintillation crystal of technology growth of crystal pulling method, in crystal growing process, adopt pure Lu 2Si 2O 7Seed crystal, the speed of growth are 1-5mm/hr, and the crystal rotating speed is about 10-80RPM.Crystal through sowing, undergauge, shouldering, isometrical, ending, behind the cooling supervisor, crystal growth is finished.
The above-mentioned processing step of the present invention<4〉described in temperature increasing for melting materials can also adopt graphite heating, perhaps mode such as W heating is carried out temperature increasing for melting materials;
The above-mentioned processing step of the present invention<7〉described in the crystallization range of cerium ion-doped disilicic acid lutetium scintillation crystal at 1800 ℃-2000 ℃, Tc depends primarily on cerium ion-doped disilicic acid lutetium high temperature scintillation crystal Lu 2 (1-x-y-z)Re 2xCe 2yM 2zSi 2O 7In what of the element of Re representative and content thereof and different, generally the fusing point along with the increase disilicic acid lutetium high temperature crystal of Re constituent content will be reduced to 1850 ℃ from 1950 ℃.
The above-mentioned processing step of the present invention<7〉described in Lu 2Si 2O 7Seed crystal generally adopts a, b, c is axial or other special crystallization direction carries out crystalline growth.
Below by embodiment preparation process of the present invention is explained, but should not limit its protection domain with this.
Example 1: preparation Lu 1.99798Ce 0.002Zr 0.00002Si 2O 7Disilicic acid lutetium scintillation crystal
According to above-mentioned processing step<1〉to take by weighing purity respectively by above-mentioned chemical formula be 99.999% exsiccant 0.99899mol Lu 2O 3, 2mol SiO 2, 0.002mol CeO 2, 0.00002mol ZrO 2With 0.00016mol Si 3N 4Raw material, 1500g altogether; By above-mentioned processing step<2〉the above-mentioned component thorough mixing that takes by weighing is become uniform powder; By above-mentioned processing step<3〉will mix raw material, under the pressure of 1Gpa, the blended powder is pressed into φ 78 * 10mm 3The material cake, 500 ℃ sintering temperatures 15 hours to remove organism, water and the low melting point impurity in the raw material; By above-mentioned processing step<4〉go into φ 80 * 60mm with burned material is packaged 3Ir gold crucible in, and in the lifting furnace of packing into, the sealing burner hearth also is evacuated to 5 * 10 -3Pa.Under this vacuum tightness, adopt the Frequency Induction Heating mode to carry out temperature increasing for melting materials with 400 ℃/hr heat-up rate; By above-mentioned processing step<5〉when the material piece in the crucible is warmed up to 1000 ℃, constant temperature 2.5 hours; By above-mentioned processing step<6〉continue to be warming up to 2000 ℃ with the heat-up rate of 400 ℃ of ./hr, wait to expect all fusings after, for the abundant reaction that guarantees raw material and mix, constant temperature 1.5 hours in this temperature range again; By above-mentioned processing step<7〉in burner hearth, slowly charge into N 2Gas makes the air pressure of burner hearth remain on 1.25atm.Under 1950 ℃ of Tcs, adopt the axial Lu of b then 2Si 2O 7Seed crystal adopts Czochralski grown crystal.In crystal growing process, the speed of growth is 2mm/hr, and the crystal rotating speed is about 30RPM.Crystal through sowing, undergauge, shouldering, isometrical, ending, behind the cooling supervisor, crystal growth is finished, and can obtain the indehiscent Lu of φ 35 * 50mm perfect crystalline 1.99798Ce 0.002Zr 0.00002Si 2O 7Water white crystal can be widely used in the fields such as high energy physics nuclear physics and image nuclear medicine.
Example 2: preparation Lu 1.389Ce 0.010Gd 0.6Mg 0.001Si 2O 7Disilicic acid lutetium scintillation crystal
According to processing step<1 in the foregoing description 1〉by above-mentioned chemical formula Lu 1.389Ce 0.005Gd 0.6Si 2O 7Take by weighing purity respectively and be 99.999% exsiccant 0.6945mol Lu 2O 3, 2mol SiO 2, 0.01mol CeO 2, 0.001mol MgO and 0.00083mol Si 3N 4Raw material, 1500g altogether; Repeat processing step<2 in the foregoing description 1〉<3<4 and<5; By processing step<6 in the foregoing description 1〉continue to be warming up to 1980 ℃ with the heat-up rate of 400 ℃ of ./hr, after waiting to expect all to melt, constant temperature is 1.5 hours in this temperature range; By processing step<7 in the foregoing description 1〉in burner hearth, slowly charge into N 2Gas makes the air pressure of burner hearth remain on 1.25atm.Under 1870 ℃ of Tcs, adopt the axial Lu of b then 2Si 2O 7Seed crystal adopts Czochralski grown crystal.In crystal growing process, the speed of growth is 2.5mm/hr, and the crystal rotating speed is about 40RPM.Crystal through sowing, undergauge, shouldering, isometrical, ending, behind the cooling supervisor, crystal growth is finished.Can obtain the indehiscent colourless transparent crystal of φ 35 * 50mm perfect crystalline at last, can be widely used in the fields such as high energy physics nuclear physics and image nuclear medicine.
Example 3: preparation Lu 1.789Ce 0.010(Y0.5Gd 0.5) 0.2Zr 0.001Si 2O 7Disilicic acid lutetium scintillation crystal
According to processing step<1 in the foregoing description 2〉by above-mentioned chemical formula Lu 1.789Ce 0.010(Y 0.5Gd 0.5) 0.2Zr 0.001Si 2O 7Take by weighing purity respectively and be 99.999% exsiccant 0.8945mol Lu 2O 3, 2mol SiO 2, 0.01molCeO 2, 0.001mol ZrO 2With 0.00083mol Si 3N 4Raw material, 1500g altogether; Repeat processing step<2 in the foregoing description 1〉〉<3<4 and<5; By processing step<6 in the foregoing description 2〉continue to be warming up to 1950 ℃ with the heat-up rate of 400 ℃ of ./hr, after waiting to expect all to melt, constant temperature is 2 hours in this temperature range; By processing step<7 in the foregoing description 2〉in burner hearth, slowly charge into Ar gas, make the air pressure of burner hearth remain on 1atm.Under 1900 ℃ of Tcs, adopt the axial Lu of b then 2Si 2O 7Seed crystal adopts Czochralski grown crystal.In crystal growing process, the speed of growth is 1mm/hr, and the crystal rotating speed is about 25RPM.Crystal through sowing, undergauge, shouldering, isometrical, ending, behind the cooling supervisor, crystal growth is finished.Can obtain φ 35 * 50mm perfect crystalline disilicic acid lutetium crystal at last, the crystal water white transparency can be widely used in the fields such as high energy physics nuclear physics and image nuclear medicine.

Claims (2)

1, a kind of preparation method who mixes cerium disilicic acid lutetium high temperature scintillating monocrystal is characterized in that this method comprises the following steps:
1. press the chemical formula Lu of doping trivalent cerium ion disilicic acid lutetium 2 (1-x-y-z)Re 2xCe 2yM 2zSi 2O 7Prepare burden, wherein Re represents other rare earth element except that Lu, and M represents Zr, Mg, Ta metal ion; 0≤x≤0.3,0.001≤y≤0.05,0.00001≤z≤0.0005 is behind selected x, y, the z, by the mol ratio of each component oxide correspondence, i.e. Lu 2O 3: Re 2O 3: CeO 2: MO 2: SiO 2=(1-x-y-z): x: 2y: 2z: 2 weighing initial feed, the purity of each initial feed are all greater than 99.99%, and then take by weighing and CeO 2The Si of equivalent mole 3N 4Raw material, the i.e. Si of y/6 mole 3N 4Raw material;
2. each component raw material thorough mixing is become uniform mixed powder;
3. under the pressure of 1-5Gpa, the blended powder is pressed into columned material cake, carried out low-temperature sintering 10-24 hour being lower than under 500 ℃ the temperature;
4. with the packaged Iridium Crucible of advancing in the burner hearth of burned material, or plumbago crucible, or in the tungsten crucible, with the burner hearth sealing and vacuumize, vacuum tightness is about 10 -3-10 -4Pa is in order to guarantee CeO 2Fully reduced, under this vacuum tightness, adopt the Frequency Induction Heating mode to carry out temperature increasing for melting materials with 300-500 ℃/hr heat-up rate;
5. work as Iridium Crucible, or plumbago crucible, or the material piece in the tungsten crucible is warmed up to 1000-1200 ℃ and locates, carried out constant temperature 2-3 hour in this temperature range;
6. continue to be warming up to 1900-2000 ℃ with the heat-up rate of 300-500 ℃ of ./hr, wait to expect all fusings after, in this temperature range constant temperature 1-2 hour again;
7. in burner hearth, slowly charge into N 2Gas or Ar gas make the air pressure of burner hearth remain on 1-1.25atm, then, under the Tc of single crystal of the present invention, generally in 1850-1950 ℃ of scope, adopt the cerium ion-doped disilicic acid lutetium high temperature scintillation crystal of technology growth of crystal pulling method, in crystal growing process, adopt pure Lu 2Si 2O 7Seed crystal, the speed of growth are 1-5mm/hr, and the crystal rotating speed is 10-80RPM, crystal through sowing, undergauge, shouldering, isometrical, ending, behind the cooling supervisor, crystal growth is finished.
2, the preparation method who mixes cerium disilicic acid lutetium high temperature scintillating monocrystal according to claim 1 is characterized in that described Lu 2Si 2O 7The seed crystal direction is axial or other crystallization direction of a, b, c.
CNB2004100534382A 2004-08-04 2004-08-04 Process for preparing high temperature cerium blended lutetium pyrosilicate scintillation monocrystal Expired - Fee Related CN1322173C (en)

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