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

Nature
A von HoegenAndrea Cavalleri

Abstract

Nonlinear optical techniques at visible frequencies have long been applied to condensed matter spectroscopy. 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 frequencies. For example, the nonlinear excitation of lattice vibrations has enabled the dynamic control of material functions. So far it has only been possible to exploit second-order phonon nonlinearities 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 transit...Continue Reading

References

Dec 17, 2004·Nature·J ItataniD M Villeneuve
Jan 15, 2011·Science·D FaustiA Cavalleri
Sep 30, 2009·Journal of Physics. Condensed Matter : an Institute of Physics Journal·Paolo GiannozziRenata M Wentzcovitch
Mar 31, 2012·Nature·B ZaksM S Sherwin
Jun 26, 2015·Nature·G VampaP B Corkum
May 27, 2017·Physical Review Letters·R MankowskyA Cavalleri

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Citations

Jul 3, 2020·Nature·H LakhotiaE Goulielmakis
Mar 9, 2019·Physical Review Letters·Courtney L JohnsonJeremy A Johnson
May 2, 2020·Physical Review Letters·Liang LiPeixiang Lu
Apr 2, 2019·Physical Review Letters·Michael WoernerIgal Brener
Jul 3, 2020·Nature·Michael A Sentef
Mar 14, 2019·Materials·Wencan LiJingjun Xu
Jan 9, 2021·Physical Review Letters·Denis GoležAndrew J Millis
Apr 16, 2021·Nature·Qian LiHaidan Wen
Jun 9, 2021·Nano Letters·Dominik M Juraschek, Prineha Narang
Jun 12, 2019·The Journal of Physical Chemistry Letters·Chao LianBryan M Wong
Aug 21, 2019·Accounts of Chemical Research·Julian GargiuloEmiliano Cortés

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