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Microscopy & Magnetism Group

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5 September 2018

Moving Atoms by Photodoping

Figure 1 (a) Transient relative x-ray intensity of the (1.5 0.5 0.5) superlattice reflection of Sr0.97Ca0.03TiO3 upon above bandgap excitation with 40 fs pulses Inset: STO crystal structure as seen along the c-axis. phi measures the antiferrodistortive rotation of the oxygen octahedra (exaggerated) and represents the order parameter. (b) Calculated energy change per STO cubic unit cell as a function of oxygen displacement u/u0 along the in-plane cubic crystal axes resulting from the octahedral rotation at …
Figure 1 (a) Transient relative x-ray intensity of the (1.5 0.5 0.5) superlattice reflection of Sr0.97Ca0.03TiO3 upon above bandgap excitation with 40 fs pulses Inset: STO crystal structure as seen along the c-axis. phi measures the antiferrodistortive rotation of the oxygen octahedra (exaggerated) and represents the order parameter. (b) Calculated energy change per STO cubic unit cell as a function of oxygen displacement u/u0 along the in-plane cubic crystal axes resulting from the octahedral rotation at select hole dopings rho.

Understanding how and how fast we can drive atoms to create a structural phase transition is of fundamental interest as it directly relates to many processes in nature. Here we show that a photoexcitation can drive a purely structural phase transition before the energy is relaxed in the material that corresponds to a “warmer” equilibrated state. By above band gap photoexciting Ca:SrTiO3 and using ultrashort x-ray pulses from the FEMTO slicing source we find a ultrafast reduction of the reflections (Fig. 1a) sensitive to the octahedral rotation transition (inset). This process can be understood by the change of the corresponding potential as a function of hole doping (Fig. 1b), which shows that the distortion amplitude moves to zero with hole doping which is in contrast to electron doping. These results show that even for a transition that is governed by a softening of a particular phonon mode, the ultrafast transition is driven by the electronic change (hole doping) in the chemical potential induced by a fs laser pulse. This points out new possibilities in the ultrafast manipulation of the crystal structure.

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Urs Staub
Laboratory for Synchrotron Radiation — Condensed Matter Physics
Swiss Light Source, Paul Scherrer Institute
5232 Villigen PSI, Switzerland
Telephone: +41 56 310 4494
E-mail: urs.staub@psi.ch


Michael Porer
Laboratory for Synchrotron Radiation — Condensed Matter Physics
Swiss Light Source, Paul Scherrer Institute
5232 Villigen PSI, Switzerland
Telephone: +41 56 310 3469
E-mail: michael.porer@psi.ch
Original Publication
*Ultrafast Relaxation Dynamics of the Antiferrodistortive Phase in Ca doped SrTiO3 *
M. Porer, M. Fechner, E. 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, Noack, P. Beaud, G. Ingold, U. Aschauer, S. L. Johnson, and U. Staub
Physical Review Letters, 3 August 2018
DOI: 10.1103/PhysRevLett.121.055701

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Microscopy and Magnetism Group

Dr. Urs Staub
Swiss Light Source
Paul Scherrer Institut
WSLA/124
5232 Villigen - PSI
Switzerland

Telephone: +41 56 310 4494
E-mail: urs.staub@psi.ch

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