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A5: Nanoscale and low dimensional effects

M. Winkler1, A.L. Hansen2, T. Dankwort3, J. D. Koenig1, H. Böttner1, K. Bartholomé1, W. Bensch2, L. Kienle3
1) Fraunhofer IPM, Freiburg 2) Institute of Inorganic Chemistry,  University Kiel 3) Institute for Materials Science, Synthesis and Real Structure, University Kiel

In 2001, outstanding properties were reported  for Bi2Te3/Sb2Te3 thin film superlattice (SL) structures grown by metal-organic chemical vapor deposition (MOCVD) [[1]]. In order to gain more insight into the path-breaking ZT value of 2.4 and the underlying mechanisms, investigations aiming at reproducing, re-examining and possibly improving this kind of nanolayered structures were carried out.

Two synthesis methods were used: 1.) Nanoalloying, i.e. the deposition of element films and subsequent annealing to induce compound formation by sputtering / MBE setup and 2.) Epitaxial deposition by MBE. We present a comprehensive study on transport properties, structural properties and thermal stability of the SLs by (HR)XRD, SIMS, SEM and (S)TEM. Supplementary theoretical calculations concerning the electrical anisotropy of Bi2Te3 / Sb2Te3 SLs will also be shown.

The nanoalloyed SLs are easy to fabricate on many substrate materials, display a high structural quality and very pronounced c-axis texture, high PFs of up to 40-50 µW/cmK² and thermal conductivities down to 0.40 W/mK. However, the thermal stability of the nanostructuring is inferior to epitaxial material.

The epitaxially deposited Bi2Te3/Sb2Te3 SL films display very sharply defined interfaces down to period lengths as small as 6 nm. This is the first reported reproduction of Bi2Te3/Sb2Te3 SLs with such small period lengths. Low lattice thermal conductivities down to ~ 0.3 W/mK were determined. Remarkably, due to charge carrier compensation effects only low Seebeck coefficients and carrier mobilities were observed, preventing high ZT values. In-situ XRD and TEM heating experiments showed a decay of the nanostructure above temperatures of ~ 350 °C. Annealing the films led to a huge improvement of the power factor to values of 46 µW/cmK².




[1] R. Venkatasubramanian, E. Siivola, T. Colpitts & B. O'Quinn., Nature 413, 597 (2001)