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Electronic and ionic processes influence on electrical properties of TlBr crystals J. Vaitkus Institute of Materials Science and Applied Research (IMSAR), Vilnius University, Lithuania Co-authors: V. Gostilo, S.Zatoloka Baltic Scientific Instruments, Latvia; A.Mekys, J.Storasta, A.Žindulis IMSAR, Vilnius University, Lithuania J.Banys, Faculty of Physics, Vilnius University, Lithuania; J.Vaitkus IWORID6, Glasgow, 2004.06.25-29 Basic: The interest in TlBr crystal is due to its high average atomic number (Tl: 81, Br: 35), high density (7.5 g/cm3) and wide bandgap (2.7 eV). The photon stopping power of TlBr crystal is greater than any of the semiconductors discussed. Therefore this material is promising for Xand γ- ray detector applications. K.S.Shah et al. IEEE Trans.Nucl.Sci. (1989) v.39(1). Problem: The stability of TlBr radiation detector is not good, the investigation of degradation phenomena and improving the properties are important for the future of detectors -9 10 0.92 eV 0.50 eV TlBr dark current (dc) multiple heating -11 II 8 A cycle of dark current and mobility vs temperature 2 I, A 10 10 ,cm /Vs -10 10 12 -12 10 -13 10 0.71 eV 6 4 0.94 eV III 2 I 3.2 3.6 J.Vaitkus 4.0 4.4 -1 1000/T, K 3.0 4.8 3.2 3.4 3.6 3.8 -1 1000/T, K 4.0 4.2 5.2 IWORID6, Glasgow, 2004.06.25-29 Outline: 1. Investigation of photoconductivity spectra & electrical conductivity (at different frequencies and temperature) 2. The contacts degradation phenomena. 3. A fractal approach. The schematic view on the samples: the true photos of the crystals but not the contacts A fresh crystal J.Vaitkus A “tired” crystal IWORID6, Glasgow, 2004.06.25-29 Spectral Dependencies of Photoconductivity 1 Shows the edge of intrinsic PC at 2.75 eV and a deep level at 2.63 eV Sample M5 If / If max 0.1 0.01 The spectra shows PC is related with the space charge regions, and they changes with bias voltage and a sign 0 T=60 C U=+20V 0 T=20 C U=+20V 420 430 440 450 460 470 480 , nm Sample M14 1.0 If / If max If / If max 1.0 0.5 Sample P3 (1.2) 0.5 +10V -10V U=+20V U= -20V RT RT 0.0 0.0 420 430 440 450 , nm J.Vaitkus 460 470 480 420 430 440 450 460 , nm IWORID6, Glasgow, 2004.06.25-29 470 The dielectric spectroscopy The complex dielectric permittivity * = ’ - i“ was measured by a capacitance bridge HP4284A in the frequency range 20 Hz - 1 MHz. Temperature dependence of frequencies. the real part and of the imaginary part of dielectric permitivity at different At low frequencies dielectric losses increase with increasing temperature and cause increase of the real part of the dielectric permittivity. If can be caused by the big ionic conductivity as it was already shown previously [Secco, R.A., Secco, E.A. and Chen, Q. Defects and ionic conductivity in TlCl, TlBr and TlI at high pressure and temperature. Journal of solid state chemistry 141 (1998) 462-465p.]. At low frequencies, the conductivity phenomena dominate in the dielectric spectra. With such a high value of conductivity the contacts and barrier regions can play an important role. J.Vaitkus IWORID6, Glasgow, 2004.06.25-29 Electrical conductivity at high temperature The electric conductivity: = 0". = DC + As, where DC is the DC conductivity and As is the AC conductivity. (A.K.Joncher, Dielectric relaxation in solids, London, Celsea Dielectric Press (1983).) = 0exp(EA/kT). EA = 0.8 eV, 0 = 6,7 10-15 S/m. Conductivity are caused by Tl ions, which can move in the crystal lattice. J.Vaitkus IWORID6, Glasgow, 2004.06.25-29 Electric modulus Frequency dependence of the real part and the imaginary part of electrical modulus at different temperatures. The conductivity of mobile ions can be related to the electrical modulus: M*() = 1/*() = M'() + M"(). The low frequency value of M' is zero and represents a lack of the restoring force for the electric field induced mobile Tl ions. As frequency increases, each ion moves a shorter and shorter distance until finally the electric field changes so rapidly that the ions only oscillate within the confinements of their potential energy wells. As a result, M' increases to a maximum asymptotic value M() = 1/(). The spectra of M" show a slightly asymmetric peak centered in the dispersion region of M’. The region where the peak occurs ( = 1) is indicative of the transition from long-range (left) to short-range (right) ion mobility and the peak frequency corresponds to the average electric field (or conductivity) relaxation time, 1/. The broadening in the modulus spectra indicates a cooperative motion of mobile ions, especially in the higher frequency range. J.Vaitkus IWORID6, Glasgow, 2004.06.25-29 Dark current frequency dependence 1E-5 1E-6 E=0,80eV 0,80eV , m -1 1E-7 f, kHz 100 1000 -1 -1 , m -1 1E-5 1E-8 1E-9 f, kHz 1,2 3,7 7,8 35 241 667 11,4 2,6 5,4 17 100 480 1000 1E-6 1E-7 2.4 1E-10 2.7 3.0 3.3 3.6 3.9 4.2 4.5 4.8 5.1 5.4 -1 2.6 2.8 3.0 3.2 3.4 3.6 3.8 4.0 4.2 4.4 4.6 4.8 5.0 1000/T, K 1000/T, K -1 Dark current vs temperature and vs frequency. Peculiarities related to the percolation character of ion drift and, probably, the specific features related to ion oscillations and space charge effects. J.Vaitkus IWORID6, Glasgow, 2004.06.25-29 Tl-TlBr-Au -11 6x10 -11 4x10 dI/dt, A/h 330 I, nA 325 2.0 320 1.6 -11 T, K 310 0 -2x10 315 1.2 -11 2x10 -11 -4x10 0 100 305 0.8 200 300 derivative of Furje spectrum without a noise 0 100 200 300 400 500 phase, deg 0.0 0.4 500 time, h 300 295 400 0.2 500 0 -500 -1000 0,042 time, h -11 Electric current time dependence in TlBr in system Al-Tl-TlBr-Al and applied 30V DC voltage. Total charge 2,33mC (1,45·1016 particles). A deposited Tl contact disappears due to ionic conductivity and characteristic instabilities (spikes) are observed. J.Vaitkus Amplitude 1x10 -12 5x10 0,055 0 0.00 0.05 0.10 0.15 0.20 0.25 frequency, 1/h IWORID6, Glasgow, 2004.06.25-29 0.30 A new result was found by direct Tl+ ions transport: diffusion – limited aggregation is responsible for a dendritic structures which could be grown by Tl+ or electrode ion electrodiffusion. -9 2.4x10 Proposed: spikes appear during a growth of a dendrit or creation of cluster -9 I, A 2.1x10 -9 1.8x10 A fractal analysis approach seems very promising. -9 1.5x10 200 225 250 275 300 time, h A part from the current time dependence Typical fractal system: Cu electrode and mineral water The current vs time dependence J.Vaitkus IWORID6, Glasgow, 2004.06.25-29 Conclusions: 1. Photoconductivity spectra demonstrates the electric field redistribution in the sample and an existence of the deep centres. 2. Frequence dependence of conductivity allows to measure the ionic conductivity and demonstrates the regions of ionic instabilities. T < 250 K is promising for improve a stability of detectors. 3. Tl+ ion current time dependence shows the fractal behaviour of ion migration. J.Vaitkus IWORID6, Glasgow, 2004.06.25-29 Fractal in the natural colours Thank you for your attention ! J.Vaitkus IWORID6, Glasgow, 2004.06.25-29