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Nonlocal nonlinear phononics

Abstract:
Nonlinear phononics relies on the resonant optical excitation of infrared-active lattice vibrations to induce targeted structural deformations in solids. This form of dynamical crystal structure design has been applied to control the functional properties of many complex solids, including magnetic materials, superconductors and ferroelectrics. However, phononics has so far been restricted to protocols in which structural deformations occur within the optically excited volume, sometimes resulting in unwanted heating. Here, we extend nonlinear phononics to propagating polaritons, spatially separating the functional response from the optical drive. We use mid-infrared optical pulses to resonantly drive a phonon at the surface of ferroelectric LiNbO3. Time-resolved stimulated Raman scattering reveals that the ferroelectric polarization is reduced over the entire 50 µm depth of the sample, far beyond the micrometre depth of the evanescent phonon field. We attribute this effect to the anharmonic coupling between the driven mode and a polariton that propagates into the material. For high excitation amplitudes, we reach a regime in which the ferroelectric polarization is reversed, as revealed by a sign change in the Raman tensor coefficients of all the polar modes.
Publication status:
Published
Peer review status:
Peer reviewed

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Publisher copy:
10.1038/s41567-022-01512-3

Authors


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Institution:
University of Oxford
Division:
MPLS
Department:
Physics
Sub department:
Atomic & Laser Physics
Oxford college:
Merton College
Role:
Author
ORCID:
0000-0002-3143-0850


Publisher:
Springer Nature
Journal:
Nature Physics More from this journal
Volume:
18
Pages:
457-461
Publication date:
2022-03-07
Acceptance date:
2022-01-14
DOI:
EISSN:
1745-2481
ISSN:
1745-2473


Language:
English
Keywords:
Pubs id:
1246438
Local pid:
pubs:1246438
Deposit date:
2023-04-21

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