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Register a new userNonlocal nonlinear phononics
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Added by
Meredith Henstridge
Publication date
2021
fields
Physics
and research's language is
English
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Nonlinear phononics relies on the resonant optical excitation of infrared-active lattice vibrations to coherently induce targeted structural deformations in solids. This form of dynamical crystal-structure design has been applied to control the functional properties of many interesting systems, including magneto-resistive manganites, magnetic materials, superconductors, and ferroelectrics. However, phononics has so far been restricted to protocols in which structural deformations occur locally within the optically excited volume, sometimes resulting in unwanted heating. Here, we extend nonlinear phononics to propagating polaritons, effectively separating in space the optical drive from the functional response. Mid-infrared optical pulses are used to resonantly drive an 18 THz phonon at the surface of ferroelectric LiNbO3. A time-resolved stimulated Raman scattering probe reveals that the ferroelectric polarization is reduced over the entire 50 micron depth of the sample, far beyond the ~ micron depth of the evanescent phonon field. We attribute the bulk response of the ferroelectric polarization to the excitation of a propagating 2.5 THz soft-mode phonon-polariton. For the highest excitation amplitudes, we reach a regime in which the polarization is reversed. In this this non-perturbative regime, we expect that the polariton model evolves into that of a solitonic domain wall that propagates from the surface into the materials at near the speed of light.
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Nonlinear interactions between phonon modes govern the behavior of vibrationally highly excited solids and molecules. Here, we demonstrate theoretically that optical cavities can be used to control the redistribution of energy from a highly excited coherent infrared-active phonon state into the other vibrational degrees of freedom of the system. The hybridization of the infrared-active phonon mode with the fundamental mode of the cavity induces a polaritonic splitting that we use to tune the nonlinear interactions with other vibrational modes in and out of resonance. We show that not only can the efficiency of the redistribution of energy be enhanced or decreased, but also the underlying scattering mechanisms may be changed. This work introduces the concept of cavity control to the field of nonlinear phononics, enabling nonequilibrium quantum optical engineering of new states of matter.
Optical nonlinearities in solids reveal information about both the in-plane rotational and out-of-plane inversion symmetries of a crystal. In the van der Waals material hexagonal boron nitride (hBN) both these symmetries and the linear vibrational properties have led to the rich physics of mid-infrared phonon-polaritons. However, the role of strong electron-phonon nonlinearities requires further study. In this work, we investigate both theoretically and experimentally the rich interplay of phonon anharmonicity and symmetry in phonon-polariton mediated nonlinear optics. We show that large enhancements (>30x) of third-harmonic generation occur for incident femtosecond pulses that are resonant with the hBN transverse optical phonons. In addition, we predict and observe large transient sub-picosecond duration second-harmonic signals during resonant excitation, which in equilibrium is forbidden by symmetry. This surprising result indicates that instantaneous crystal inversion symmetry breaking can be optically induced and controlled via phonon interactions by both the power and polarization of the pump laser.
We grow accustomed to the notion that optical susceptibilities can be treated as a local property of a medium. In the context of nonlinear optics, both Kerr and Raman processes are considered local, meaning that optical fields at one location do not produce a nonlinear response at distinct locations in space. This is because the electronic and phononic disturbances produced within the material are confined to a region that is smaller than an optical wavelength. By comparison, Brillouin interactions can result in a highly nonlocal nonlinear response, as the elastic waves generated through the Brillouin process can occupy a region in space much larger than an optical wavelength. The nonlocality of these interactions can be exploited to engineer new types of processes, where highly delocalized phonon modes serve as an engineerable channel that mediates scattering processes between light waves propagating in distinct optical waveguides. These types of nonlocal optomechanical responses have been recently demonstrated as the basis for information transduction, however the nontrivial dynamics of such systems has yet to be explored. In this work, we show that the third-order nonlinear process resulting from spatially extended Brillouin-active phonon modes involves mixing products from spatially separated, optically decoupled waveguides, yielding a nonlocal joint-susceptibility. We further explore the coupling of multiple acoustic modes and show that multi-mode acoustic interference enables a tailorable nonlocal-nonlinear susceptibility, exhibiting a multi-pole frequency response.
Recent years witnessed much broader use of Brillouin inelastic light scattering spectroscopy for the investigation of phonons and magnons in novel materials, nanostructures, and devices. Driven by developments in instrumentation and the strong need for accurate knowledge of energies of elemental excitations, the Brillouin - Mandelstam spectroscopy is rapidly becoming an essential technique, complementary to the Raman inelastic light scattering spectroscopy. We provide an overview of recent progress in the Brillouin light scattering technique, focusing on the use of this photonic method for the investigation of confined acoustic phonons, phononic metamaterials, magnon propagation and scattering. The Review emphasizes emerging applications of the Brillouin - Mandelstam spectroscopy for phonon engineered structures and spintronic devices and concludes with a perspective for future directions.
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