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@PHDTHESIS{Chen:723103,
      author       = {Chen, Chao},
      othercontributors = {Wuttig, Matthias and Lobo, Ricardo P. S. M.},
      title        = {{D}ielectric properties of amorphous phase-change
                      materials},
      school       = {RWTH Aachen University},
      type         = {Dissertation},
      address      = {Aachen},
      reportid     = {RWTH-2018-223963},
      pages        = {1 Online-Ressource (x, 174 Seiten) : Illustrationen},
      year         = {2018},
      note         = {Veröffentlicht auf dem Publikationsserver der RWTH Aachen
                      University; Dissertation, RWTH Aachen University, 2018},
      abstract     = {The AC conductivities and dielectric properties of five
                      amorphous phase-change materials (PCMs) and three ordinary
                      chalcogenides have been determined by employing a
                      combination of the AC electrical measurement (0.5 Hz –
                      186.2 Hz), the impedance spectroscopy (9 kHz – 3 GHz) and
                      the optical spectroscopy (20 cm-1 – 12000 cm-1, i.e., 0.6
                      THz – 360 THz). Those measurements almost range from the
                      DC limit to the first interband transition. In addition, the
                      temperature dependence of the low-frequency dielectric
                      permittivity and the AC conductivities of amorphous PCMs
                      were also investigated by the AC electrical measurement in
                      the range of 4 K – 170 K and by the impedance spectroscopy
                      in the range of 220 K – 350 K. Moreover, the aging effect
                      on these properties of amorphous GeTe thin films annealed
                      for one hour at successively higher temperatures, i.e. 333
                      K, 353 K, 373 K, 393 K, 403 K was studied by the AC
                      electrical measurement. This work mainly focuses on
                      amorphous PCMs. Firstly, measurements of AC conductivities
                      of amorphous PCMs have been extensively used to understand
                      the conduction process in these materials. No frequency
                      dependence of AC conductivities is discernible in the
                      impedance spectroscopy measurements, which is in line with
                      charge transport via extended states. Secondly, the
                      permittivities of amorphous PCMs are frequency independent
                      among the impedance measurement frequency range.
                      Consequently, there are no dielectric relaxations in this
                      range. Thirdly, the static dielectric constants of amorphous
                      PCMs significantly exceed their optical dielectric
                      constants. This observation is corroborated by transmittance
                      measurements in the far-infrared, which show optical
                      phonons. Particular attention is also paid to the
                      correlation between the dielectric constant and Born
                      effective charge of the amorphous phase-change materials.
                      From the intensity of these phonon modes, a large Born
                      effective charge is derived. Nevertheless, it is known that
                      crystalline PCMs such as GeTe possess even significantly
                      larger Born effective charges. Crystallization is hence
                      accompanied by a huge increase in the Born effective charge,
                      which reveals a significant change of bonding upon
                      crystallization. Interestingly, a clear stoichiometry trend
                      in the static dielectric constant along the pseudo-binary
                      line between GeTe and Sb2Te3 has been identified. On the
                      other hand, there is a comparison of dielectric properties
                      between the PCMs and non-PCMs. The optical dielectric
                      constants of amorphous PCMs increase a lot after
                      crystallization, while there is no difference between the
                      optical dielectric constants of the amorphous and
                      crystalline chalcogenide AgInTe2. This illustrates that the
                      PCMs undergo a change from covalent bonding to resonant
                      bonding on crystallization, but the amorphous and
                      crystalline phases of ordinary chalcogenides are both
                      governed by virtually the same covalent bonds. In addition,
                      the static dielectric constants obtained for PCMs on the
                      pseudo-binary line between GeTe and Sb2Te3 are compared with
                      those obtained for ordinary covalently-bonded chalcogenide
                      semiconductors. The static dielectric constants of both PCMs
                      and non-PCMs significantly enhance from amorphous to
                      crystalline, which hints that the contribution of infrared
                      active phonons is remarkably strengthened in the crystalline
                      states of both PCMs and non-phase-change materials.
                      Moreover, the temperature dependence of dielectric constants
                      of amorphous chalcogenides shows the contribution
                      enhancement of infrared active phonons with temperature.
                      Lastly, the aging effect on the dielectric property of
                      amorphous GeTe thin films derived from the experimental
                      results is in good agreement with the results of density
                      functional theory (DFT) calculations, which at the same time
                      reveal the bonding mechanisms and atomic structures in the
                      representative amorphous phase.},
      cin          = {131110 / 130000},
      ddc          = {530},
      cid          = {$I:(DE-82)131110_20140620$ / $I:(DE-82)130000_20140620$},
      typ          = {PUB:(DE-HGF)11},
      doi          = {10.18154/RWTH-2018-223963},
      url          = {https://publications.rwth-aachen.de/record/723103},
}