Ultrafast control of material optical properties via the infrared resonant Raman effect

Abstract

The Raman effect -- inelastic scattering of light by lattice vibrations (phonons) -- produces an optical response closely tied to a material's crystal structure. Here we show that resonant optical excitation of IR and Raman phonons gives rise to a Raman scattering effect that can induce giant shifts to the refractive index and induce new optical constants that are forbidden in the equilibrium crystal structure. We complete the description of light-matter interactions mediated by coupled IR and Raman phonons in crystalline insulators -- currently the focus of numerous experiments aiming to dynamically control material properties -- by including a forgotten pathway through the nonlinear lattice polarizability. Our work expands the toolset for control and development of new optical technologies by revealing that the absorption of light within the terahertz gap can enable control of optical properties of materials over a broad frequency range.

15 pages, 6 figures

References in corpus (3)

• Nonlinear lattice dynamics as a basis for enhanced superconductivity in YBa2Cu3O6.5
• Metastable ferroelectricity in optically strained $SrTi{O}_3$
• Nonlinear light-matter interaction at terahertz frequencies

Cited by in corpus (12)

• Terahertz-Light Driven Coupling of Antiferromagnetic Spins to Lattice
• Multi-gap topology and non-Abelian braiding of phonons from first principles
• Two-dimensional THz spectroscopy of nonlinear phononics in the topological insulator ${\mathrm{MnBi}}_2{\mathrm{Te}}_4$
• Discovery of enhanced lattice dynamics in a single-layered hybrid perovskite
• Coherent control of the translational and point group symmetries of crystals with light
• Many-Body Floquet Theory for Radiative Heat Transfer in Time-Modulated Systems
• Phonon state tomography of electron correlation dynamics in optically excited solids
• Excitation protocols for non-linear phononics in bismuth and antimony
• Terahertz-driven parametric excitation of Raman-active phonons in LaAlO${}_3$
• Terahertz light driven coherent excitation of a zone-folded Raman-active phonon mode in the Spin-Ladder System ${\alpha }^{\prime }$-NaV${}_2$O${}_5$
• Quantized Acoustoelectric Floquet Effect in Quantum Nanowires
• Interference-Controlled Radiative Heat Transport in Time-Modulated Networks