Introduction into Positron Annihilation

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Introduction into Positron Annihilation Introduction (How to get positrons? What is special about positron annihilation?) The methods of positron annihilation (positron lifetime, Doppler broadening, ACAR...) Interaction of positrons with solids (thermalization, diffusion, trapping) The trapping model (Which defects are detectable? Determination of absolute defect concentrations. The sensitivity limit of defect detection.) Defect investigation - Examples (vacancies in thermal equilibrium; defects after electron irradiation and plastic deformation; grown-in vacancies in semiconductors) Future developments (Positron Microscopy in Munich, Livermore and Bonn) Literature: R. Krause-Rehberg, H.S. Leipner Positron Annihilation in Semiconductors Springer-Verlag, 1998 ISBN 3-540-64371-0

Introduction Positrons are obtained either by: - β + decay: 22 Na 22 Ne + β + + ν e + γ (1.27MeV) (half life: 2.6 years, up to 10 6 e + /s) - pair production using a beam of MeV-electrons onto a target (Bremsstrahlung creates positrons; 10 9 e + /s; discontinuous positron beam) - nuclear reaction: 113 Cd(n,γ) 114 Cd three γ rays and pair production; continuous positron beam; 10 10 e + /s (Forschungsreaktor München) Positrons hit the sample: - Sandwich geometry ( 22 Na source between two identical samples) - positron beam (source and sample separated)

Effect of Positron Trapping in Crystal Lattice Defects - Positron wavefunction is localized at vacancy site until annihilation - Positron annihilation parameters change when annihilating in a defect - Defects can by detected (identification and quantification)

Positron Trapping Potential - Attractive potential mainly due to missing ion (repelling core is absent) - in semiconductors: additional Coulomb tails ( 1/r rather extended) - no positron trapping by positive vacancies

The Methods of Positron Annihilation

The Positron Lifetime Measurement - Positron lifetime is measured as time difference between 1.27 MeV quantum (β + decay) and 0.511 MeV quanta (annihilation process) - PM=photomultiplier; SCA=single channel analyzer (constant-fraction type); TAC=time to amplitude converter; MCA= multi channel analyzer

Positron Lifetime Spectra Counts 10 6 10 5 10 4 10 3 t b = 218 ps As grown Cz Si Plastically deformed Si t 2 = 320 ps t 3 = 520 ps 0 1 2 3 4 5 Time [ns] - lifetime spectra consist of exponential decay components - positron trapping in open-volume defects leads to long-lived lifetime components - spectra analysis is performed by non-linear fitting routines after source and background subtraction - result: lifetimes τ i and intensities I i k + 1 Ii t Nt () = å exp- t t i = 1 i F HG i I KJ

The Methods of Positron Annihilation

Angular Correlation of Annihilation Radiation - ACAR Coincidence counting rate N z c : s 0 0 - N ( Q, Q ) = A ( Q mc, Q mc, p ) p c x y c x y z d z

2D-ACAR of defect-free GaAs (Tanigawa et al., 1995) 3D-Fermi surface can be reconstructed from measurements in several directions of a single crystal

2D-ACAR of Copper Theory Experiment p z along [100] Fermi surface of copper (Berko, 1979) p y along [010]

Three Methods of Positron Annihilation

Measurement of Doppler Broadening - electron momentum in propagation direction of 511 kev γ-ray leads to Doppler broadening of annihilation line - can be detected by conventional energy-dispersive Ge detectors and standard electronics

Line Shape Parameters S parameter: S = A S /A 0 W parameter: W = A W /A 0 W parameter mainly determined by annihilations of core electrons (chemical information)

Doppler Coincidence Spectroscopy - coincident detection of second annihilation γ reduces background - use of a second Ge detector improves energy resolution of system

Doppler Coincidence Spectra 10 0 10-1 GaAs:Zn Relative intensity 10-2 10-3 10-4 10-5 500 505 510 515 520 525 g-ray energy [kev] E 1 +E 2 = 2 m 0 c 2 =1022 kev

Thermalization in Solids - broad positron emission spectrum - deep implantation into solids - no use for study of defects in thin layers - moderation necessary Mean (maximum) implantation depth of unmoderated positrons (1/e 0.999): Si: 50µm (770µm) GaAs: 22µm (330µm) PbS: 15µm (220µm)

Moderation of Positrons moderation efficiency: 10-4

Implantation Profiles of monoenergetic Positrons - depth resolution is function of implantation depth - exact implantation profiles are obtained by Monte-Carlo simulations L mz F m z PzE (, ) = exp - H G I - 1 m z z K J NM 0 0 m O QP z = f (E,ρ) z 0 = const. m = 2 (Makhov, 1961)

The Positron Beam System at Halle University spot diameter: 5mm time per single Doppler measurement: 20 min time per depth scan: 8 hours

The positron beam system at Halle University differential pumping beam valve 22 Na Source sample chamber magnetic beam guidance system Doppler coincidence measurement

The Diffusion of Positrons Diffusion can be described by the time-dependent diffusion equation: l t n t D 2 + ( r, ) = + Ñ n + ( r, t )-Ñ v n + ( r, t ) - n + ( r, t d eff ). n + (r,t)... positron density ν d... drift velocity (electric field) λ eff =1/τ b + κ(r)... effective annihilation rate κ = µc µ... trapping coefficient C... defect density Mean free path l and positron diffusion length L + in semiconductors is mainly determined by acoustic phonon scattering Þ D µ T -0.5 at 300 K: l [nm] L [nm] Si 7 220 GaAs 5.3 200

Positron Trapping in a Single Defect Type dnb() t dt dnd () t dt b =- l + k n b d b () t =- l n () t + k n () t g d d d b solution: decay spectrum abbreviations: 1 1 =, t =, + t 1 2 lb kd ld I 1 I, I = - = l - l + k 1 2 2 k d b d d F HG t Dt () = Iexp - I exp 1 I F HG KJ + 2 t - 1 t 2 The t i and I i are measured Þ k is obtained: k d F I = m d = HG 2 C - I1 t b 1 1 t d I KJ t I KJ

Positron Trapping in a Dislocation the dislocation line (shallow trap) acts as a funnel for the trapping in deep traps b... bulk v... vacancy t... deep trap st... shallow trap λ i... annihilation rates κ i, J... trapping rates δ... detrapping (escape) rate

Determination of absolute Defect Densities Trapping rate [s -1 ] Average positron lifetime 10 11 10 10 10 9 10 8 10-8 10-7 10-6 10-5 10-4 10-3 10-2 t d V - t b V - Sensitivity range V 2- V 0 V + V 2- V 0 V + the trapping coefficient µ k = µc must be determined by an independent method positron trapping may be strongly temperature-dependent Þ µ= f (T) defect in Si 300K µ (10 15 s -1 ) V - 1 V 2-2 V 0 0.5 V + < 0.1 dislocation 1 cm 2 s -1 10-8 10-7 10-6 10-5 10-4 10-3 10-2 Vacancy concentration vacancy cluster n µ 1V

Vacancies in thermal Equilibrium Vacancy concentration in thermal equilibrium: in metals H F» 1...4 ev Þ at T m [1v]» 10-4...-3 fits well to the sensitivity range of positron annihilation C 1v F I KJ F S ( T) = exp H G 1v exp k Tungsten E F = (4.0 ± 0.3) ev F HG F 1v H kt I KJ W parameter fit to trapping model (Ziegler, 1979) temperature (K)

Defects in Ge after Electron Irradiation electron irradiation generates Frenkel pairs vacancy annealing and defect reactions may be studied by positrons Ge e - irr. at 4K (Polity et al., 1997)

Defects in Si induced by Ion Implantation ion implantation is most important doping technique in planar technology main problem: generation of defects Þ positron beam measurements (Eichler et al., 1997)

Defect density as function of deposited ion energy RBS results Defect generation follows Chadderton s model of homogenous nucleation: (L.T. Chadderton, Rad. Eff. 8 (1971) 1) [defect] ~ dose 0.5 valid for RBS- and positron data only exception: Si self-implantation positron results can be explained: extra Si atoms are interstitials and kill vacancies that are seen by positrons but not by RBS (Eichler et al., 1997)

(Petters et al., 1998) Plastic Deformation and Electron Irradiation in Pb

The nature of the EL2 defect in GaAs one of mostly investigated defects exhibiting metastability at low T under light illumination stable metastable (Dabrowski 1988, Chadi 1988) there were several structural models of EL2 the above shown model was proven by positron annihilation (Krause et al., 1990)

Other Positron Techniques Low-Energy Positron Diffraction (LEPD): more simple theoretical calculation of diffraction pattern (no electron-electron interaction) Positron-Annihilation-induced Auger Electron Spectroscopy (PAES): no background due to secondary electrons & very surface-sensitive Positron Microprobe/Microscope Forschungsreaktor München: very strong continuous positron source and remoderation Þ three-dimensional imaging of defect distributions Univ. Bonn: combination of Scanning Electron Microscopy and a focussed (1 µm) positron beam of variable energy Þ defect imaging

The Positron Microscope at Bonn University