ORGANIC SCINTILLATORS
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1 RGANIC SCINTILLATRS Igor Nemchenok
2 Contents 1. Scintillation method of the radiation and particles detection. 2. rganic scintillators Brief characteristic The nature of the molecular excited states Advantages. 3. rganic scintillators in the JINR Laboratory of Nuclear Problems Scintillators of usual composition (C, H based) Polystyrene-based plastic scintillators Linear alkylbenzene-based liquid scintillators Element-loaded scintillators B-loaded polystyrene-based plastic scintillators Rare-earth elements-loaded polymethylmethacrylate-based plastic scintillators Gd-loaded liquid scintillators Gd-loaded liquid scintillator for DAYA BAY neutrino experiment.
3 1. Scintillation method of the radiation and particles detection Definitions Scintillation short-time event of the radioluminescence with the duration no more than few microseconds. Scintillating compound compound which produces scintillations under the radiation. Scintillator the definite amount of the scintillating compound contained in the scintillation detector as an element sensitive to radiation. Stages of the radiation detection process by the help of the scintillation detector: Scintillator conversion of the radiation energy to the light energy by means of the luminescence; light photons collection to the PMT s photocathode; light photons adsorption by the photocathode and photoelectrons emission; electrons multiplying in the PMT; electronics and software processing of the current s impulses arising at the PMT s outlet. Light reflector PMT High voltage source Electronics and software
4 1. Scintillation method of the radiation and particles detection Mechanism of the radioluminescence event: Energy transfer from radiation (or particle) to excitation and ionization of atoms and molecules and formation of secondary particles; Energy transfer from excited and ionized particles directly to emitting centers (atoms, molecules etc.); Light emission by emitting centers Definition Relative light output ratio of amplitude of pulses of scintillation detector to the same parameter of standard detector in the same experimental conditions. Counts Energy
5 1. Scintillation method of the radiation and particles detection Scintillation materials Inorganic rganic Main differences Inorganic scintillators rganic scintillators Monocrystalline and polycrystalline Liquefied noble gases: Ar, Kr, Xe Single crystals High light output Low light output Alkali halides: NaI(Tl), CsI(Tl), CsI, CsI(Na), CsI(C 3 ), LiF(W), LiF(Eu) Plastic Slow Fast thers: ZnSe, CW, BG, GS Liquid
6 2. rganic scintillators 2.1. Brief characteristic CH CH C C rganic single crystals anthracene trans-stilbene tolan p-terphenyl CH 3 CH 3 CH 3 CH 3 CH 3 Liquid scintillators (LS) solutions of organic luminescent compounds and some special additives in organic liquid solvents CH 3 CH 3 toluene p-xylene pseudocumene α-methylnaphthalene CH 2 CH n CH 2 CH n CCH 3 H 3 C CH 3 CH 2 CH n CH 2 C n Plastic scintillators (PS) solutions of organic luminescent compounds and some special additives in organic polymeric solvents CH 3 CH 3 polystyrene polyvinyltoluene polyvinylxylene polymethylmethacrylate
7 2. rganic scintillators 2.1. Brief characteristic Characteristic Polystyrene Polyvinyltoluene CH 2 CH n CH 2 CH n Density, g/cm CH 3 Index of refraction Hygroscopicity no no Wavelength of the maximum of emission spectrum, nm ( ) * ( )* Light output, relatively to anthracene syngle crystal, % (55 57) * (60 68)* H:C relation Response function, ns (2 3) * (2 3)* * For most wide spread scintillators
8 2. rganic scintillators 2.1. Brief characteristic Definitions Basic (main) scintillator s compound : 1. transparent for scintillation photons; 2. its content predominates in scintillator. hν 1 Primary additive admixture to the basic scintillator s compound which is able to emit optical photons under excitation received of the basic scintillator s compound molecules. hν 2 (ν 2 < ν 1 ) Waveshifter (secondary additive) compound, incorporating to organic scintillator and converting primary additive emission to the emission with the longer wavelength. hν 3 (ν 3 < ν 2 )
9 2. rganic scintillators 2.1. Brief characteristic 1,2 Base compound Primary additive Waveshifter 1,2 Demands to scintillation additives Adsorption PMT's relative spectral sensitivity 1,0 0,8 0,6 0,4 0,2 0,0 1,0 0,8 0,6 0,4 0,2 0, Wavelength, nm PS PMT 0,0 0, Wavelength, nm 1,0 0,8 0,6 0,4 0,2 1,0 0,8 0,6 0,4 0,2 Luminescence Relative intensity of luminescence Intensive adsorption; High quantum yield ; verlapping of the emission spectrum of the base compound with the adsorption spectrum of the primary additive; verlapping of the emission spectrum of the primary additive with the adsorption spectrum of the waveshifter; Emission spectrum of the waveshifter must be in the region of high spectral sensitivity of widespread PMTs or other devices. Emission spectrum of the polystyrene-based PS (primary additive p- terphenyl; waveshifter PPP) and typical curve of the PMT s spectral sensitivity (entrance window - borosilicate glass, bialkaline photocathode.
10 2. rganic scintillators 2.1. Brief characteristic Primary additives p-terphenyl(ppp) N 2,5-diphenyloxazole (PP) N 2-(4-biphenylyl)-5-phenyloxazole (BP) N N N Waveshifters 2-phenyl-5-(4-biphenylyl)- 1,3,4-oxadiazole (PBD) 2-(1-napthyl)-5-phenyloxazole (α-np) CH 3 N N CH 3 CH CH CH N H 3 C N CH 1,4-di-(5-phenyl-2-oxazolyl)- benzene (PPP) 1,4-di-(4-methyl-5-phenyl-2-oxazolyl)- benzene (dimethyl-ppp) CH 3 1,4-bis-(2-methylstyryl)benzene (bis-msb)
11 2. rganic scintillators 2.1. Brief characteristic Aromatic compounds (arenes) large group of the compounds of the carbocyclic series with molecules containing stable cyclic atomic bunching of six carbon atoms (benzene ring) possessing special chemical characteristics. benzene H H H H H H H S NH H H H H furan thiophene pyrrole H Hukkel rule: compounds which molecules form plane cycle and contain 4n + 2 (where n nonnegative integer) π-electrons are aromatic.
12 2. rganic scintillators 2.1. Brief characteristic Nonane C 9 H 20 Hexadecane C 16 H 34 Kerosene (light fraction white spirit) CCH 3 CH 2 C CH 3 n Polymethylmethacrylate Secondary solvent naphthalene
13 2. rganic scintillators 2.2. The nature of the molecular excited states Energy transfer Photochemical reaction The main photophysical processes Adsorption S0 S1 Fluorescence S1 S0 Nonradiative desactivation Intercombinational conversion е Adsorption T0 S1 Phosphorescence T1 S0 The diagram of electronic-vibrational states of polyatomic molecule and paths of radiative (solid arrows) and nonradiative (dashed arrows) transitions. Photophysical process Duration, seconds Adsorption Fluorescence (singlet-singlet light emission) Phosphorescence (triplet-singlet light emission) Internal conversion (nonradiative transition to lower state of the same multiplicity) Intercombination conversion (nonradiative transition from excited singlet state to excited triplet state) Vibrational-rotational relaxation
14 2. rganic scintillators 2.3. Advantages Fast response; High stability to different actions (radiation resistance, photo resistance, thermo resistanse, moisture resistance, ); Relative simplicity of construction of detectors of any shape and configuration; Possibility of large-scale detectors construction; Relatively low cost; Possibility of using simple methods of decreasing of radioactive impurity concentrations; Possibility of directional changing of properties due to molecular nature of luminescence.
15 2. rganic scintillators 2.3. Advantages Elements or isotopes Applications 6 Li, 10 B, 113 Cd, 155 Gd, 157 Gd, 235 U Neutron detectors, searching for neutrinos oscillations 176 Yb, 160 Gd, 115 In, 100 Mo, 37 Cl Detection of Sun neutrinos Pb Detection of astrophysics neutrinos 19 F, 73 Ge Searching for Dark Matter 150 Nd, 160 Gd, 100 Mo, 130 Te, 82 Se Searching for double β-decay Pb, Sn, W, Hg, Bi High energy physics
16 3. rganic scintillators in the JINR Laboratory of Nuclear Problems Scintillators Unloaded (C, H based) Element-loaded Plastic (polystyrene) B-loaded Rare-earth loaded Liquid (LAB) Plastic Gd-loaded Nd-loaded Polystyrene Plastic Liquid Plastic Polymethyl methacrylate α-methylnaphtalene Phenylcyclohexane LAB PMMA
17 3.1. Scintillators of usual composition (C, H based) Polystyrene-based PSs CH CH 2 n Basic compound: polystyrene N N Primary additive: 1,4-diphenylbenzene (p-terphenyl) Waveshifter: 1,4-di-(5-phenyl-2-oxazolyl)benzene (PPP)
18 3.1. Scintillators of usual composition (C, H based) Polystyrene-based PSs Basic compound Polystyrene Fire safety Yes Toxicity No Hygroscopicity No Density, g/cm 3 1,05 Index of refraction 1,58 Light output, relatively to anthracene single crystal, % 52 λ max of luminescence, nm 421 Transparency, cm 170 Response function, ns 2,5 Number of hydrogen atoms, cm -3, ,85 Number of carbon atoms, cm -3, ,85
19 3.1. Scintillators of usual composition (C, H based) Polystyrene-based PSs Methods of plastic scintillators production: Radical bulk polymerization; Suspension polymerization; Methods of plastics processing: pressure molding, extrusion. Advantages of radical bulk polymerization: Best counting and spectrometric properties; High transparency; Possibility of production of large size and different shape scintillators. Main stages of PS production by radical bulk polymerization: Dehydration of raw styrene; Styrene rectification under the reduced pressure; Luminescent additives dissolution in styrene; Filtration and loading styrene solution to the polymerization mold; Polymerization: HC CH 2 CH CH 2 n n heating styrene polystyrene
20 3.1. Scintillators of usual composition (C, H based) Polystyrene-based PSs Temperature, 0 C Time, hours Temperature conditions of the polymerization stage
21 3.1. Scintillators of usual composition (C, H based) Polystyrene-based PSs
22 3.1. Scintillators of usual composition (C, H based) Polystyrene-based PSs
23 3.1. Scintillators of usual composition (C, H based) Polystyrene-based PSs
24 3.1. Scintillators of usual composition (C, H based) Polystyrene-based PSs
25 3.1. Scintillators of usual composition (C, H based) Linear alkybenzene-based LS Requirements to LS for large-scale detectors: High scintillation efficiency; High transparency; High flash point; High stability; Low toxicity; Low solvent action to acrylic plastics; Availability.
26 3.1. Scintillators of usual composition (C, H based) Linear alkybenzene-based LS LAB is the large-capacity product of the petrochemical industry. The main LAB application is the production of the biodegradable synthetic detergents. LAB is a mixture of the monoalkyl benzene derivatives with the number of the carbon atoms in the side chain from 9 to 14. The main LAB components contain from 10 to 13 carbon atoms in the side chain. There are about 80% 85 % of the 1-phenylalkanes CH 2 C n H 2n-1, where n = 8 13 and about 15% 20% of the 2-phenylalkanes in the LAB. CH CH 3 C n H 2n-1, where n = 7 12
27 3.1. Scintillators of usual composition (C, H based) Linear alkybenzene-based LS Specific gravity, g/cm Boiling point, o C Flash point, o C 147 Mean value of the molecular mass, g/mole No of H atoms per 1 cm
28 3.1. Scintillators of usual composition (C, H based) Linear alkybenzene-based LS Primary additive Waveshifter N 2,5-diphenyloxazole (PP) N N 1,4-bis-(5-phenyl-2-oxazolyl)benzene (PPP) N 2,5-diphenyloxazole (PP) H 3 C N N CH 3 1,4-bis(4-methyl-5-phenyl-2-oxazolyl)benzene (dimethyl-ppp) N CH 3 2,5-diphenyloxazole (PP) CH CH CH CH 1,4-bis(2-methylstyryl)benzene (bis-msb) CH 3
29 3.1. Scintillators of usual composition (C, H based) Linear alkybenzene-based LS 1,0 1,00 Light output, relative units 0,8 0,6 0,4 0,2 Light output, relative units 0,95 0,90 0,85 0,80 0,75 Source 137 Cs Light output, relative units 0,0 0,0 0,1 0,2 0,3 0,4 0,5 0,6 0,7 1,00 0,95 0,90 0,85 PP mass fraction, % Light output, relative units 0,70 0,000 0,005 0,010 0,015 1,05 1,00 0,95 0,90 0,85 PPP mass fraction, % Standard sample: solvent pseudocumene; primary additive PP (5 g/l); waveshifter bis-msb (10 mg/l). 0,80 0,000 0,002 0,004 0,006 0,008 0,010 Dimethyl-PPP mass fraction, % 0,80 0,000 0,002 0,004 0,006 0,008 0,010 Bis-MSB mass fraction, %
30 3.1. Scintillators of usual composition (C, H based) Linear alkybenzene-based LS 450 Intensity, rel. units Wavelength, nm 0.5% PP % PPP 0.5% PP LAB Exitation nm
31 3.1. Scintillators of usual composition (C, H based) Linear alkybenzene-based LS Source 207 Bi ē K : 482 kev and 976 kev γ: 569,7 kev and 1064 kev 207 Bi Al-mylar film teflon 5 mm Al filter 20 ml violet glass
32 3.1. Scintillators of usual composition (C, H based) Linear alkybenzene-based LS Counts/channel V = 20 ml H = 1.17 cm ē K + γ spectrum Channel Counts/channel Counts/channel ē K spectrum Channel γ spectrum Channel FWHM
33 3.1. Scintillators of usual composition (C, H based) Linear alkybenzene-based LS Scintillator Light output* FWHM, % Transparency (430 nm), m 0.5% PP, % PPP % PP, % dimethyl-ppp % PP, % bis-msb *Relatively to the standard sample: liquid solvent pseudocumene; primary additive PP (5 g/l); Waveshifter bis-msb (10 mg/l)
34 3.2. Element-loaded scintillators Requirements to element-containing additives: Good solubility in organic media; ptical transparency ( nm); Thermal stability; Stability to atmospheric 2 ; Stability to hydrolysis; Photostability; Stability to other actions.
35 3.2. Element-loaded scintillators B-loaded polystyrene-based PS Experimental samples: diameter 3 cm, height 0.9 cm. Mass fraction of B: 0.38%, 0.75%, 2% and 5% CH CH 2 n Polymeric base: polystyrene H H H H H - carbon atoms - boron atoms H H H H o-carborane (C 10 B 2 H 12 ) N N Activator: 1,4-diphenylbenzene (p-terphenyl) Waveshifter: 1,4-di-(5-phenyl-2-oxazolyl)benzene (PPP)
36 3.2. Element-loaded scintillators B-loaded polystyrene-based PS Diameter 7 cm, Height 5,7 cm
37 3.2. Element-loaded scintillators B-loaded polystyrene-based PS Mass fraction of B, % Characteristics Density, g/cm Index of refraction Number of B atoms per cm 3, Number of H atoms per cm 3, Number of C atoms per cm 3, λ max of luminescence, nm Transparency* ( λmax ), % Relative light output, % Thermal neutrons (E 0.5 ev) detection efficiency, % *Relatively to air
38 3.2. Element-loaded scintillators Rare-earth elements-loaded PMMA-based PSs
39 3.2. Element-loaded scintillators Rare-earth elements-loaded PMMA-based PSs Rare earth containing additive LnX 3 6H 2 Salt (X = Cl -, N 3 - ) H 3 C CH 3 N P N H 3 C CH 3 N H 3 C CH 3 phosphoric acid hexamethyltriamide (HMPA) C 18 H 54 X 3 GdN 9 3 P 3 = Gd[HMPA] 3 X 3
40 3.2. Element-loaded scintillators Rare-earth elements-loaded PMMA-based PSs CH 2 C C CH 3 n Experimental samples: diameter 3 cm, height 1 cm. Mass fraction of gadolinium: 1%, 2% and 3% CH 3 Polymethylmethacrylate Naphthalene N N N 2,5-Diphenyloxazole (PP) 1,4-Di-(5-phenyl-2-oxazolyl)benzene (PPP)
41 3.2. Element-loaded scintillators Rare-earth elements-loaded PMMA-based PSs Characteristics Mass fraction of gadolinium, % Density, g/cm Index of refraction Number of Gd atoms per cm 3, Number of H atoms per cm 3, Number of C atoms per cm 3, λ max of luminescence, nm λ max Transparency* ( ), % Light output, % Thermal neutrons (E 0.5 ev) detection efficiency, %
42 3.2. Element-loaded scintillators Rare-earth elements-loaded PMMA-based PSs Relative light output, % Gd-loaded PS Nd-loaded PS 20 0,0 0,5 1,0 1,5 2,0 2,5 3,0 Mass fraction, %
43 3.2. Element-loaded scintillators Rare-earth elements-loaded PMMA-based PSs Transmittance, % Nd-loaded PS 0 Gd-loaded PS Wavelength, nm
44 3.2. Element-loaded scintillators Gd-loaded LSs Phenylcyclohexane (PCH) Tributyl phosphate (TBP) C 4 H 9 P C 4 H 9 C 4 H 9 Composition C 12 H 16 Boiling point, o C Flash point, o C 98 Melting point, o C 5 Specific gravity, g/cm 3 0,95 Index of refraction 1,525 1,527 Scintillation efficiency, relative to toluene* 1,02 Composition C 12 H 27 4 P Boiling point, o C 289 Flash point, o C 120 Melting point, o C - 80 Specific gravity, g/cm 3 0,97 Index of refraction 1,422 1,423 Scintillation efficiency, relative to toluene *P. Fodor-Csanyi, Gy. Inzelt. The International Journal of Applied Radiation and Isotopes, 1971, V. 22, pp
45 3.2. Element-loaded scintillators Gd-loaded LSs mixed solvent: PCH (60%vol.) + TBP (40%vol.); primary additive PP (0,5%); light shifter PPP (0,01%); Gd-containing additive Gd[HMPA] 3 Cl 3 (0,1% Gd) Scintillator Light output, relative to anthracene Unloaded 50% 0,1% Gd-loaded 46% (52%*) *After 2 removing.
46 3.2. Element-loaded scintillators Gd-loaded LSs CH 3 H 9 C 4 P C 4 H 9 C 4 H 9 α-methylnaphthalene (alpha-mn) Flash point - 82 o C Tributylphosphate Flash point o C N Gd(N 3 ) 3 x 6H 2 2-(-biphenylyl)-5-phenyloxazole (BP) Gadolinium nitrate
47 3.2. Element-loaded scintillators Gd-loaded LSs Concentration of gadolinium, mg/ml Characteristics Boiling point, o C Flash point, o C > 82 > 82 > 82 > 82 > 82 Density, g/cm Index of refraction Number of Gd atoms per cm 3, λ max of luminescence, nm λ max Transparency* ( ), % Light output, % * Quartz cell, length 5 cm, relative to air
48 3.2. Element-loaded scintillators Gd-loaded LS for DAYA BAY neutrino experiment ν e + p e + + n
49 3.2. Element-loaded scintillators Gd-loaded LS for DAYA BAY neutrino experiment
50 3.2. Element-loaded scintillators Gd-loaded LS for DAYA BAY neutrino experiment Far site 1600 m from Lingao 2000 m from Daya verburden: 350 m Mid site ~1000 m from Daya verburden: 208 m Daya Bay Near 360 m from Daya Bay verburden: 97 m Ling Ao Near 500 m from Lingao verburden: 98 m Ling Ao NPP Ling Ao-ll NPP (under const.) Daya Bay NPP
51 3.2. Element-loaded scintillators Gd-loaded LS for DAYA BAY neutrino experiment
52 3.2. Element-loaded scintillators Gd-loaded LS for DAYA BAY neutrino experiment
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55 3.2. Element-loaded scintillators Gd-loaded LS for DAYA BAY neutrino experiment Composition: Solvent LAB; Primary additive PP (3g/L); N 2,5-diphenyloxazole (PP) Wave shifter bis-msb (15 mg/ml); CH 3 CH CH CH CH Gd-containing additive Gd(TMHA) 3 (0.1% Gd) CH 3 1,4-bis-(2-methylstyryl)benzene (bis-msb) CH 3 CH 3 TMHA: 3,3,5-trimethylhexanoic acid CH 3 CH CH 2 C CH 2 C CH 3 H
56 3.2. Element-loaded scintillators Gd-loaded LS for DAYA BAY neutrino experiment GdCl 3 6H NH 4 TMHA Gd(TMHA) 3 3H 2 + 3NH 4 Cl + 3H 2 Two methods IHEP (Beijing) technology: the synthesis of the solid Gd-additive in water medium BNL technology: water-organic extraction
57 3.2. Element-loaded scintillators Gd-loaded LS for DAYA BAY neutrino experiment Water solution of GdCl 3 6H 2 0 Water solution of NH 4 TMHA Reduced pressure IHEP technology: the synthesis of the solid Gd-additive in water medium
58 3.2. Element-loaded scintillators Gd-loaded LS for DAYA BAY neutrino experiment Water solution of GdCl 3 6H 2 0 Water solution of NH 4 TMHA LAB phase BNL technology: water-organic extraction Water phase LAB phase Water phase
59 3.2. Element-loaded scintillators Gd-loaded LS for DAYA BAY neutrino experiment Height of the sample, cm Total registration efficiency, %, for E n < 0.4 ev Gd-LS 1 12 ± 2 LS 2 19 ± ± ± 5 17 ± 3 Total registration efficiency, % Height of the sample, cm
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