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Creating new states of matter in complex materials

January 21, 2019

Terahertz-driven phonon upconversion in SrTiO3

Direct manipulation of the atomic lattice using intense long-wavelength laser pulses has become a viable approach to create new states of matter in complex materials. Conventionally, a high-frequency vibrational mode is driven resonantly by a mid-infrared laser pulse and the lattice structure is modified through indirect coupling of this infrared-active phonon to other, lower-frequency lattice modulations. Here, we drive the lowest-frequency optical phonon in the prototypical transition metal oxide SrTiO3 well into the anharmonic regime with an intense terahertz field. We show that it is possible to transfer energy to higher-frequency phonon modes through nonlinear coupling. Our observations are carried out by directly mapping the lattice response to the coherent drive field with femtosecond X-ray pulses, enabling direct visualization of the atomic displacements.

Figure: a, Strong terahertz radiation (red) interacts with the STO soft-mode phonon (yellow). The degree of resonant overlap can be tuned by temperature. Energy is exchanged with higher-frequency phonon modes (turquoise, purple) through nonlinear coupling. The STO unit cell and two lowest-frequency zone-centre TO eigenmodes are indicated at the top of the figure. b, Phonon motion is probed in the time domain with ultrafast XRD in reflection geometry.

See also:

Reference: Kozina, M., M. Fechner, P. Marsik, T. van Driel, J. M. Glownia, C. Bernhard, M. Radovic, D. Zhu, S. Bonetti, U. Staub and M. C. Hoffmann (2019). Terahertz-driven phonon upconversion in SrTiO3. Nat. Phys. (10.1038/s41567-018-0408-1) Kozina-2019

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