Fyzikální ústav Akademie věd ČR

Exploiting dimensionality and defect mitigation in Srn+1TinO3n+1 to create tunable microwave dielectrics

C. H. Lee1,2, N. D. Orloff3,4, T. Birol5, Y. Zhu5, V. Goian6, E. Rocas7, R. Haislmaier2, E. Vlahos2, J. A. Mundy5, L. F. Kourkoutis5,8, Y. Nie1, M. D. Biegalski9, J. Zhang1, M. Bernhagen10, N. A. Benedek11, Y. Kim5, J. D. Brock5, R. Uecker10, X. X. Xi12, V. Gopalan2, D. Nuzhnyy6, S. Kamba6, D. A. Muller5,8, I. Takeuchi13, J. C. Booth3, C. J. Fennie5, D. G. Schlom1,8

The miniaturization and integration of frequency-agile microwave circuits — relevant to electronically tunable filters, antennas, resonators and phase shifters — with microelectronics offers tantalizing device possibilities, yet requires thin films whose dielectric constant at gigahertz frequencies can be tuned by applying a quasi-static electric field. Appropriate systems such as BaxSr1−xTiO3 have a paraelectric–ferroelectric transition just below ambient temperature, providing high tunability. Unfortunately, such films suffer significant losses arising from defects. Recognizing that progress is stymied by dielectric loss, we start with a system with exceptionally low loss — Srn+1TinO3n+1 phases — in which (SrO)2 crystallographic shear planes provide an alternative to the formation of point defects for accommodating non-stoichiometry. Here we report the experimental realization of a highly tunable ground state arising from the emergence of a local ferroelectric instability in biaxially strained Srn+1TinO3n+1 phases with n ≥ 3 at frequencies up to 125 GHz. In contrast to traditional methods of modifying ferroelectrics — doping or strain — in this unique system an increase in the separation between the (SrO)2 planes, which can be achieved by changing n, bolsters the local ferroelectric instability. This new control parameter, n, can be exploited to achieve a figure of merit at room temperature that rivals all known tunable microwave dielectrics.

Layered crystallic structure of Srn+1TinO3n+1 with  n = 1–6 (left) and dielectric permitivity vs. temperature dependency in thin layers of Srn+1TinO3n+1 (right). Temperature in permitivity peaks is matching the temperature of transition to ferroelectric state.

1Department of Materials Science and Engineering, Cornell University, Ithaca, New York 14853, USA
2Department of Materials Science and Engineering, Pennsylvania State University, University Park, Pennsylvania 16802, USA
3National Institute of Standards and Technology, Boulder, Colorado 80305, USA
4Department of Physics, University of Maryland, College Park, Maryland 20742, USA
5School of Applied and Engineering Physics, Cornell University, Ithaca, New York 14853, USA
6Institute of Physics ASCR, Na Slovance 2, 182 21 Prague 8, Czech Republic
7Department of Signal Theory and Communications, Universitat Politècnica de Catalunya, 08034 Barcelona, Spain
8Kavli Institute at Cornell for Nanoscale Science, Ithaca, New York 14853, USA
9Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA
10Leibniz Institute for Crystal Growth, Max-Born-Strasse 2, D-12489 Berlin, Germany
11Materials Science and Engineering Program, The University of Texas at Austin, Austin, Texas 78712, USA
12Department of Physics, Temple University, Philadelphia, Pennsylvania 19122, USA
13Department of Materials Science and Engineering, University of Maryland, College Park, Maryland 20742, USA

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