Hostname: page-component-586b7cd67f-r5fsc Total loading time: 0 Render date: 2024-11-24T12:07:21.724Z Has data issue: false hasContentIssue false
  • English
  • Français

Structural Properties of Chalcopyrite-related 1:3:5 Copper-poor Compounds and their Influence on Thin-film Devices

Published online by Cambridge University Press:  31 January 2011

Sebastian Lehmann ,
David Fuertes Marrón ,
José Manuel Merino Álvarez ,
Maximo Léon ,
Michael Tovar ,
Yvonne Tomm ,
Christian Wolf ,
Susan Schorr ,
Thomas Schedel-Niedrig  and
Martha Ch Lux-Steiner
Sebastian Lehmann
Affiliation:
[email protected], Helmholtz-Centre Berlin for materials and energy, Glienicker Street 100, Berlin, 14109, Germany, +49-30-8062-2299, +49-30-8062-3199
David Fuertes Marrón
Affiliation:
[email protected], Universidad Politécnica de Madrid, Instituto de Energía Solar-ETSIT, Madrid, Spain
José Manuel Merino Álvarez
Affiliation:
[email protected], Universidad Autónoma de Madrid, Departamento de Física Aplicada, C-XII, Madrid, Spain
Maximo Léon
Affiliation:
[email protected], Universidad Autónoma de Madrid, Departamento de Física Aplicada, C-XII, Madrid, Spain
Michael Tovar
Affiliation:
[email protected], Helmholtz-Centre Berlin for Materials and Energy, Institute Complex Magnetic Materials, Berlin, Germany
Yvonne Tomm
Affiliation:
[email protected], Helmholtz-Centre Berlin for Materials and Energy, Institute for Solar Fuels and Energy Storage, Berlin, Germany
Christian Wolf
Affiliation:
[email protected], Helmholtz-Centre Berlin for Materials and Energy, Departement: Trace Elements, Berlin, Germany
Susan Schorr
Affiliation:
[email protected], Free University Berlin, Geosciences, Berlin, Germany
Thomas Schedel-Niedrig
Affiliation:
[email protected], Helmholtz-Centre Berlin for Materials and Energy, Institut for heterogeneous Materials (E-I2), Berlin, Germany
Martha Ch Lux-Steiner
Affiliation:
[email protected], Helmholtz-Centre Berlin for Materials and Energy, Institut for heterogeneous Materials (E-I2), Berlin, Germany
Get access

Abstract

Chalcopyrite-based devices show highest conversion efficiencies among present thin film architectures with values of 20% at laboratory scale. This outstanding performance has been achieved for quaternary Cu(Inx,Ga1-x)Se2 (x˜0.7) compound material. However, a strong correlation between the performance and the gallium content or, in other words, low versus high bandgap materials has been recognized. One critical issue in this discussion is the formation of a copper-depleted near-surface phase with 1:3:5 and 1:5:8 stoichiometries. In earlier reports, surface phases with corresponding compositions have been found on CuInSe2, CuGaSe2 and Cu(Inx,Ga1-x)Se2 thin films. These near-surface phases show a positive influence on the performance of cells based on low bandgap Cu(Inx,Ga1-x)Se2 material due to n-type inversion and band gap widening compared to bulk properties. A tendency towards a neutral or even a negative impact of the near-surface phase on wide band gap material (high gallium content) has recently been reported [1]. Nevertheless, the structural models of copper-poor chalcopyrite-related compounds have been controversially discussed in literature but a stannite-type structural model is most suitable as will be presented. In any case, the relation of the structural properties between chalcopyrite and 1:3:5 phases is crucial for the performance of related devices.

In this contribution we will report about the structural analysis of the Cu(Inx,Ga1-x)3Se5 solid solution series by means of anomalous x-ray scattering using synchrotron radiation, powder and single crystal neutron diffraction. Contributions of the isoelectronic species Cu+ and Ga3+ could be separated by these experiments. Bulk samples synthesized from the elements and heat treated at 650°C after the main reaction step - the latter in order to allow equilibrium structure formation - were investigated. Structural data like lattice parameters, tetragonal distortion and cation distribution were obtained for the complete Cu(Inx,Ga1-x)3Se5 solid solution series. The stannite-type structural model was assigned to all members of the investigated 1:3:5s which will be strengthened by simulations. We observed that the tetragonal distortion vanishes for compositions close to a gallium content as used for highest efficiency Cu(Inx,Ga1-x)Se2 devices. However, the tetragonal distortion depends critically on the cation distribution which is in turn controlled by the thermal history of the sample, as we have recently reported for pure CuGaSe2 [1]. This means that we can plot a direct correlation for the misfit between chalcopyrite and 1:3:5 phases depending on the gallium content and the thermal treatment of the considered thin films. These results will widen the understanding of the chalcopyrite-based thin film photovoltaic devices.

[1] S. Lehmann et al., Phys. Stat. Sol. A (in press)

Keywords

crystallographic structureneutron scatteringphotovoltaic
Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 1165: Symposium M – Thin-Film Compound Semiconductor Photovoltaics–2009 , 2009 , 1165-M03-09
Copyright
Copyright © Materials Research Society 2009

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

References

1. Green, M. A. Emery, K. Hishikawa, Y. and Warta, W., Prog. Phot.: Res. Appl., 17, 85 (2009)Google Scholar
2. Schmid, D. Ruckh, M. and Schock, H.W. Appl. Surf. Science, 103, 409–426, (1992)Google Scholar
3. Meeder, A. Weinhardt, L. Stresing, R. Marrón, D. Fuertes, Würz, R., Babu, S.M. Schedel-Niedrig, T., Lux-Steiner, M.C., Heske, C. and Umbach, E. Jour. of Phys. and Chem. of Solids, 64, 1553–1557, (2003)Google Scholar
4. Lehmann, S. Bär, M., Marrón, D. Fuertes, Pistor, P. Wiesner, S. Rusu, M. Kötschau, I., Lauermann, I. Grimm, A. Sokoll, S. Fischer, C.H. Schedel-Niedrig, T., Lux-Steiner, M.C. and Jung, Ch., Thin Solid Films, 511-512, 623–627, (2006)Google Scholar
5. Bär, M., Rusu, M. Lehmann, S. Schedel-Niedrig, Th., Lauermann, I. and Lux-Steiner, M.Ch., Appl. Phys. Lett., 93, 232104, (2008)Google Scholar
6. Lehmann, S. Marrón, D. Fuertes, Tovar, M. Tomm, Y. Wolf, C. Schorr, S. Schedel-Niedrig, T., Arushanov, E. and Lux-Steiner, M. Ch., Phys. Stat. Sol. A DOI 10.1002/pssa.200881221 (2009)Google Scholar
7. Dianoux, A.J. and Lander, G. Neutron Data Booklet (ILL), (2001)Google Scholar
8. Rietveld, H.M. Jour. Appl. Cryst., 2, 65–71, (1969)Google Scholar
9. Többens, D.M., Stüβer, N., Knorr, K. Mayer, H.M. and Lampert, H. Mat. Science Forum, 378-381, 288–293, (2001)Google Scholar
10.http://ts.nist.gov/MeasurementServices/ReferenceMaterials/Google Scholar
11.http://www.ill.eu/sites/fullprof/Google Scholar
12. Mikkelsen, J.C. J. Electr. Mater., 10(3), 541, (1981)Google Scholar
13. Palatnik, L.S. and Belova, E.K. Soviet Physics Crystallography, 10(4), 395, (1967)Google Scholar
14. Gödecke, T., Haalboom, T. and Ernst, F. Zeitschrift f. Metallkunde 91(8), 622, (2000)Google Scholar
15. Boehnke, U.C. and Kuehn, G. J. Mat. Science, 22, 1635, (1987)Google Scholar
16. Schorr, S. Geandier, G. and Korzun, B.V. Phys. Stat. Sol. (c), 3(8), 2610,(2006)Google Scholar
17. Lehmann, S. PhD thesis, Freie Universität Berlin, 2007 Google Scholar
18.Merino/Lehmann to be submittedGoogle Scholar
19. Wang, H.P. Lam, L.L. and Shih, I. J. Crys. Growth, (200), 137, (1999)Google Scholar
20. Marín, G., Tauleigne, S. Wasim, S.M. Guevara, R. Delgado, J.M. Rincón, C., Mora, A.E. and Pérez, G.S., Mat. Res. Bull., 33(7), 1057–1068, (1998)Google Scholar
21. Paskowicz, W. Lewandowska, R. and Bacewicz, R. Jour. of All. Comp., 362, 241, (2004)Google Scholar
22. Hönle, W., Kühn, G., and Boehnke, U.C. Cryst. Res. Technol., 23(10/11), 1347, (1988)Google Scholar
23. Hanada, T. Yamana, A. Nakamura, Y. Nittono, O. and Wada, T. Jpn, J. Appl. Phys., 36 (Part2, No. 11B), L1494, (1997)Google Scholar
24. Manolikas, C. Landuyt, J. van, Ridder, R. de, and Amelinckx, S. Phys. Stat. Sol. (a), 55, 709, (1979)Google Scholar
25. Zhang, S.B. Wei, S.H. and Zunger, A. Phys. Rev. Lett., 78 (21), 4059, (1997)Google Scholar
26.International Tables for Crystallography: Volume A, Kluwer Academic Publishers, (1999)Google Scholar
27. Young, R. A.: “The Rietveld Method”, Oxford University Press, (1995)Google Scholar
28. Suri, D.K. Nagpal, K.C. and Chadha, G.K. J. Appl. Cryst., 22, 578, (1989)Google Scholar
29. Shafarman, W. Klenk, R. and Mccandless, B.E. J. Appl. Phys., 79, 7324, (1996)Google Scholar