Letter | Published:

Probing the interatomic potential of solids with strong-field nonlinear phononics

Nature volume 555, pages 7982 (01 March 2018) | Download Citation

Abstract

Nonlinear optical techniques at visible frequencies have long been applied to condensed matter spectroscopy1. However, because many important excitations of solids are found at low energies, much can be gained from the extension of nonlinear optics to mid-infrared and terahertz frequencies2,3. For example, the nonlinear excitation of lattice vibrations has enabled the dynamic control of material functions4,5,6,7,8. So far it has only been possible to exploit second-order phonon nonlinearities9 at terahertz field strengths near one million volts per centimetre. Here we achieve an order-of-magnitude increase in field strength and explore higher-order phonon nonlinearities. We excite up to five harmonics of the A1 (transverse optical) phonon mode in the ferroelectric material lithium niobate. By using ultrashort mid-infrared laser pulses to drive the atoms far from their equilibrium positions, and measuring the large-amplitude atomic trajectories, we can sample the interatomic potential of lithium niobate, providing a benchmark for ab initio calculations for the material. Tomography of the energy surface by high-order nonlinear phononics could benefit many aspects of materials research, including the study of classical and quantum phase transitions.

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Acknowledgements

We thank R. Merlin and M. Altarelli for discussions. The research leading to these results received funding from the European Research Council under the European Union’s Seventh Framework Programme (FP7/2007–2013)/ERC Grant Agreement No. 319286 (QMAC). We acknowledge support from the Deutsche Forschungsgemeinschaft via the excellence cluster ‘The Hamburg Centre for Ultrafast Imaging—Structure, Dynamics and Control of Matter at the Atomic Scale’ and the Priority Program SFB925 ‘Light induced Dynamics and Control of Correlated Quantum Systems’.

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Affiliations

  1. Max Planck Institute for the Structure and Dynamics of Matter, 22761 Hamburg, Germany

    • A. von Hoegen
    • , R. Mankowsky
    • , M. Fechner
    • , M. Först
    •  & A. Cavalleri
  2. Department of Physics, University of Oxford, Clarendon Laboratory, Oxford OX1 3PU, UK

    • A. Cavalleri

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Contributions

A.C., together with A.v.H. and R.M., conceived this project. R.M., A.v.H. and M. Först built the experimental set-up. A.v.H. and R.M. conducted the experiment and analysed the data. M. Fechner performed the DFT calculations. A.v.H. conducted the FDTD simulation. All authors interpreted the data and contributed to the manuscript.

Competing interests

The authors declare no competing financial interests.

Corresponding authors

Correspondence to A. von Hoegen or A. Cavalleri.

Reviewer Information Nature thanks M. Kira and the other anonymous reviewer(s) for their contribution to the peer review of this work.

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https://doi.org/10.1038/nature25484

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