Nuclear techniques in solid state research. Manfred Forker
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1 Nuclear techniques in solid state research Manfred Forker 1
2 Nuclear techniques in solid state research Radioactive probe techniques Ion-beam analysis Radioactive probe nuclei, muons (µ), positrons ( ß + ) Scattering of α, p, d, n, He,... γ, ß,... Radiation properties mainly modified by hyperfine interactions Analysis of modified energy, angular distribution, etc. 2
3 Applications of radioactive isotopes and ion beams to Electronic properties of impurities in metals and semiconductor Exchange interactions in magnetically ordered solids Studies of radiation damage Diffusion processes Determination of the lattice sites of dopants Site-selective doping of semiconductors Donor acceptor interaction in semiconductors Hydrogen passivation and diffusion in semiconductors Optical studies of impurities and defects in semiconductors 3
4 Nuclear techniques in solid state research Literature: G. Schatz and A.Weidinger, Nuclear Condensed Matter Physics: Nuclear Methods and Applications, (Pfeiffer-Wiley,1996) Doris Forkel-Wirth Exploring solid state physics properties with radioactive isotopes Rep. Prog. Phys. 62 (1999) W.R. Leo, Techniques for Nuclear and Particle Physics Experiments, Springer G.F. Knoll: Radiation Detection and Measurement, Wiley R. Röhlsberger, Nuclear Condensed Matter Physics with Synchrotron Radiation, Basic Principles, Methodology and Applications; Series: Springer Tracts in Modern Physics, Vol. 208, 2004 ; ISBN:
5 Ion-beam analysis Scattering of α, p, d, n, He,... RBS Ion beam Target nucleus STIM PIXE SE PIGE Analysis of modified energy, angular distribution, etc. Ion Beam Techniques RBS: Rutherford back scattering ERD: Elastic recoil detection PIXE: Particle induced x-ray emission PIGE: Particle induced gamma emission NRA: Nuclear reaction analysis STIM: Scanning Transmission Ion Microscopy SE: Secondary emission Channeling 5
6 Radioactive probe techniques Hyperfine Interaction Methods γ, ß,... properties modified mainly by hyperfine interactions (HFI) Mössbauer Effect Perturbed angular correlations Myon spinrotation Nuclear orientation E γ = E 0 ± E E 0 = 10 kev 1 MeV E = 10-6 ev Hyperfine interactions: E/E Non-HFI methods Positron annihilation, PET Radioactive tracer, diffusion Transmutation doping Emission channeling 6
7 Scale and Components of Nuclei Quarks Atom 10-9 m Nucleus m Number of nuclei Nucleon m Z protons charge +1 N neutrons charge 0 A = Z + N A Symbol: ZX Isotope: N± n ZX Stable nuclei approx. 275 Nuclei occuring in nature: approx. 300 Total number of nuclei: approx Main interactions: Strong attractive nuclear forces between nucleons Repulsive Coulomb interaction between protons 7
8 The valley of stability N = Z Too many protons ß + decay p n + + e + ν Too many neutrons ß - decay n p + e + ν 8
9 9
10 Modes of nuclear decay α decay A Z X A 4 2 Y + Z 2 2 He α particle β - decay 0 1e electron n p + e + ν γ decay A Z X * A X + γ Z photon β + decay 0 +1 e 0 +1e positron p n + + e + ν e - capture p + e n + ν 10
11 Example of a ß - decay ( ) N = Z ß - spectrum E max kinetic ß energy 11
12 Example of a ß + /EC decay ( ) I + e 52Te neutrino N = Z ß+ energy spectrum 12
13 Radioactive atoms as probes in solid state research Production by nuclear reactions Nuclear reactors : e.g. 180 Hf (n,γ) 181 Hf, 116 Cd(n, γ) 117 Cd Particle accelerators (cyclotrons): e.g. 111 Cd(p,n) 111 In, 75 As(α,2n) 77 Br Half-lifes T 1/2 : Days: laboratory experiments: allows systematic studies as a function of temperature, pressure, annealing, etc 57 Co (T 1/2 = 270 d) 57 Fe (ME source), 181 Hf (T 1/2 = 43d) 181 Ta (PAC source) Isotopes commercially available Hours: requires nearby reactor, cyclotron, on-line mass separator One measurement per sample, limited possibilities of sample treatment PAC experiments: 111m Cd, T 1/2 = 48 min, Emission channeling (EC) 24 Na, T 1/2 = 15 h Minutes: On-line experiments: ME, PAC, EC equipment directly connected to accelerators or mass separators CERN) ME: 119 In ( T 1/2 = 48 min) 119 Sn, PAC: 79 Rb ( T 1/2 = 23min) 79 Kr 13
14 Doping procedures Nuclear reactions: In some cases, samples can be doped via nuclear reactions inside the material. Examples: doping of cadmium compounds with 111 In via the reaction 111 Cd (p,n) 111 In and with 117 Cd via 116 Cd (n,γ) 117 Cd or the production of 77 Br in arsenic compounds via the 75 As (α, 2n) 77 Br reaction Deposition Heating Diffusion Sample e.g. Cu Recoil and ion implantation 14
15 Doping by ion implantation sample Separation magnet Mass separator as off-line implanter Acceleration voltage Radioactive ion source Recoil implantation at heavy ion accelerators (e.g. VICKSI, Berlin; Pelletron, USP) Recoil energy ~ MeV Implantation range ~ μm 15
16 Online implantation at radioactive ion beam accelerators ISOLDE: First On-Line Isotope Mass Separator starting in 1967 Isotope production by spallation, fission, or fragmentation reactions 60 KeV mass separated radioactive ion beams 16
17 Elements for which radioactive beams are available at ISOLDE Radioactive isotopes used for solid state studies 17
18 Radioactive beam facilities ISOL (ISOLDE, ISAC, Oak Ridge, Louvain-la-Neuve, ): Accelerator p-beam Target Ion source Spallation/fragmentation of target nuclei Separator Post Accelerator Low energy radioactive beam (<12 MeV/A) Fragmentation (NSCL, GSI, RIKEN, GANIL, ): Heavy ion beam Gas stopper Separator Post Accelerator Low energy radioactive beam (<12 MeV/A) Accelerator Target Fragmentation of beam nuclei Separator High energy radioactive beam ( MeV/A)
19 Basic concepts of radiation detection Detector categories Gas-filled detectors Scintillation detectors Semiconductor detectors Other solid state detectors Ionisation-chamber (α, β) Proportional Counter ( α,β,γ) Geiger-Müller- Counter (β, γ) Solid Scintillation- Detectors e.g. NaJ:Tl (γ, β) M. Forker, Nucl. Methods in Solid State Research, CBPF 2012 M. Forker, Nuclear Detectors techniques in solid state Germanium research, CBPF Single 2012 (α, β, γ) H3, C14 Silizium-Diodes and Single Crystals (α, β, γ) Crystal (β), γ ) CsI(Tl) and LaBr 3 crystals coupled to PIN/APD photodiodes Liquid-Szintillations- Photoluminescence glasses (β, γ) Thermoluminescence crystals (β, γ) Filmemulsions (β, γ) 19
20 Interaction processes of charged particles in matter Inelastic collision: excitation Inelastic collision: ionisation Elastic collision Bremsstrahlung 20
21 Alpha particles in matter Interaction pattern Alpha range in water Range (mm) Cloud chamber photograph Energy (MeV) Alpha range in air Range (cm) Energy (MeV) 21
22 Interaction pattern Electrons (ß-) in matter ß - range in water Range (cm) Energy (MeV) Cloud chamber photograph ß- range in air Range (cm) Energy (MeV) 22
23 Interaction of photons (γ-rays) in matter Processes : Photo effect, Compton effect, Pair production, Raleigh scattering Photo effect Compton effect hν hν* hν hν θ E kin = hν -E B E kin Photons posses momentum!!! Confirmation of the particle-like character of photons predicted by Einstein 23
24 Interaction of photons ( γ-rays ) with matter Pair production Raleigh (elastic) scattering 511 kev hν hν hν hν E ɣ 1022 kev 511 kev annihilation 24
25 Absorption of photons in matter I 0 I(x) I(x) = I 0 exp (-µx) M edge L edge K edge Absorption coefficient Raleigh Total Compton Photo Pair production in nucl. field K,L,M edge: The absorption increases abruptly when the photon energy exceeds the binding energy of the K-, L-, M-electron 25
26 Neutron interactions with matter Inelastic scattering of neutrons Nuclear reaction n n n * Elastic scattering of neutrons 10 B+n 7 Li+α Fission n n n 26
27 Gas-filled detectors Principle: Incident radiation ionises the gas, producing electron-ion pairs. These charges are collected by applying a voltage U between anode and cathode U E 2 E 1 < E 2 E ion (Ar) = 15 ev With increasing U: Ionisation chamber Proportional counter Geiger Müller counter 27
28 Scintillation detector: Scintillation crystal + photomultiplier Ionisation Scintillator crystal Secondary photons Dynodes Amplification: 10 8 ɣ-photon Scintillator Photo electron Signal out Secondary secundary electrons electrons signal Protection cap + Reflector Photo cathode cathode High voltage: 1-2 kv Scintillators: NaI(Tl), CsI(Tl), BaF 2, BGO,..; Plastic: Anthracene, Photo cathodes: Ag-O-Cs, GaAs:Cs, Sb-Cs, Bialkali (Sb-K-Cs, Sb-Rb-Cs),.. 28
29 The principle of semiconductor detectors particles, photons, X- or γ-rays Conduction band + - Photon E gap Electron semiconductor Valence band Hole The incident radiation produces electron-holes pairs in a semiconductor band structure. As in a ionisation chamber, these mobile charge carriers are collected by applying a voltage to the electrodes Charge losses by recombination must be avoided. This requires Intrinsic Semiconductors of very high purity Principal advantage compared to gas-filled and scintillation detectors is the much higher number of charge carriers/kev. This results in a much better energy resolution Material Ge 0.67 Si 1.0 GaAs 1.42 C (Diamant) E gap (ev) 5.5 Energy resolution E/E N -1/2, N = number of particles/ɣ 29
30 Energy resolution of scintillation and semiconducting detectors scintillation detector NaJ(Tl) + photo mult. E/E~10 % Energy resolution E/E N -1/2, N = number of particles/ɣ semiconducting detector HP Ge E/E~1.5 % 30
31 Lifetime measurements Important parameter: the time resolution of coincidence spectrometers Decay I = 0 I= 1 I = 0 γ 1 γ 2 τ Det.1 stop γ 2 clock γ 1 photomultiplier scintillator Det.1 start Consider : γ 1 and γ 2 with delay t Experiment N coi (t) Coincidence spectrum N coi (t) ideal real τ R t time 31
32 K.S. Shaha,*, J. Glodoa, M. Klugermana, L. Cirignanoa, W.W. Mosesb, S.E. Derenzob, and M.J. Weberb Radiation Monitoring Devices, Watertown, MA 02472, USA Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA γ, α, β 32 Scintillators for lifetime measurements e - Short decay time = Fast time response electrons time HgI 2, PdI 2,CuI LaCl 3 (Ce)
33 Important inorganic scintillator materials used in nuclear physics and nuclear medicine Energy resolution E/E N -1/2, N = number of particles/ɣ Detection efficiency Time resolution Energy resolution 33
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