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Phys Rev Lett. 2018 Aug 03;121(5):055701. doi: 10.1103/PhysRevLett.121.055701.

Ultrafast Relaxation Dynamics of the Antiferrodistortive Phase in Ca Doped SrTiO_{3}.

Physical review letters

M Porer, M Fechner, E M Bothschafter, L Rettig, M Savoini, V Esposito, J Rittmann, M Kubli, M J Neugebauer, E Abreu, T Kubacka, T Huber, G Lantz, S Parchenko, S Grübel, A Paarmann, J Noack, P Beaud, G Ingold, U Aschauer, S L Johnson, U Staub

Affiliations

  1. Swiss Light Source, Paul Scherrer Institute, 5232 Villigen-PSI, Switzerland.
  2. Max Planck Institute for the Structure and Dynamics of Matter, CFEL, 22761 Hamburg, Germany.
  3. Materials Theory, ETH Zürich, 8093 Zürich, Switzerland.
  4. Department of Physical Chemistry, Fritz Haber Institute of the Max Planck Society, 14195 Berlin, Germany.
  5. Institute for Quantum Electronics, ETH Zürich, 8093 Zürich, Switzerland.
  6. Department of Inorganic Chemistry, Fritz Haber Institute of the Max Planck Society, 14195 Berlin, Germany.
  7. Department of Chemistry and Biochemistry, University of Bern, 3012 Bern, Switzerland.

PMID: 30118273 DOI: 10.1103/PhysRevLett.121.055701

Abstract

The ultrafast dynamics of the octahedral rotation in Ca:SrTiO_{3} is studied by time-resolved x-ray diffraction after photoexcitation over the band gap. By monitoring the diffraction intensity of a superlattice reflection that is directly related to the structural order parameter of the soft-mode driven antiferrodistortive phase in Ca:SrTiO_{3}, we observe an ultrafast relaxation on a 0.2 ps timescale of the rotation of the oxygen octahedron, which is found to be independent of the initial temperature despite large changes in the corresponding soft-mode frequency. A further, much smaller reduction on a slower picosecond timescale is attributed to thermal effects. Time-dependent density-functional-theory calculations show that the fast response can be ascribed to an ultrafast displacive modification of the soft-mode potential towards the normal state induced by holes created in the oxygen 2p states.

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