Theory of nonlinear phononics for coherent light control of solids

By A. Subedi, A. Cavalleri, A. Georges. 2013

221 citations recorded by the source corpus.

We present a microscopic theory for ultrafast control of solids with high-intensity terahertz frequency optical pulses. When resonant with selected infrared-active vibrations, these pulses transiently modify the crystal structure and lead to new collective electronic properties. The theory predicts the dynamical path taken by the crystal lattice using first-principles calculations of the energy surface and classical equations of motion, as well as symmetry considerations. Two classes of dynamics are identified. In the perturbative regime, displacements along the normal mode coordinate of symmetry-preserving Raman active modes can be achieved by cubic anharmonicities. This explains the light-induced insulator-to-metal transition reported experimentally in manganites. We predict a regime in which ultrafast instabilities that break crystal symmetry can be induced. This nonperturbative effect involves a quartic anharmonic coupling and occurs above a critical threshold, below which the nonlinear dynamics of the driven mode displays softening and dynamical stabilization.

Subfields: Atomic and Molecular Physics, and Optics, Electrical and Electronic Engineering

View Paper: https://www.semanticscholar.org/paper/b5fc94a6432d06ada871253a738ee22657fece9b

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In Atomic and Molecular Physics, and Optics

In Electrical and Electronic Engineering

Citations in the corpus

Nonlinear light–matter interaction at terahertz frequencies (2016, background): “To lowest order, the lattice Hamiltonian describing the nonlinear interaction reads , where aij are anharmonic coupling constants.”
Ultrafast optical spectroscopy of strongly correlated materials and high-temperature superconductors: a non-equilibrium approach (2016, background): “This is rationalized at a qualitative level by the presence of a non-linear coupling between the ac-driven CuO phonon mode and the inter- and intra-bilayer distances [76, 507](Fig.”
Light-driven ultrafast phonomagnetism (2019, background): “Recently, selective excitation of elementary vibrations of the crystal lattice (phonons) by ultrashort pulses of light has emerged as a novel, low-energy route to control material properties, extending strain engineering to the ultrafast timescales [6–12].”
Dynamical Cooper pairing in nonequilibrium electron-phonon systems (2015, methodology): “APPENDIX A: TYPE I NONLINEARITY—UNIFORM LATTICE DISPLACEMENT A nonlinear phonon coupling of form I, (QIR 0 ) (2)Q0 (see Table I in the main text), acts as a classical force on Q0 proportional to (QIR 0 ) 2 [18,22,30,31].”
Colloquium: Nonthermal pathways to ultrafast control in quantum materials (2021, methodology): “The notion of modeselective control of the crystal lattice in quantummaterials was named “nonlinear phononics” and relies on the symmetries of the crystal and the phonon modes (Först, Manzoni et al., 2011; Subedi, Cavalleri, and Georges, 2014).”
Physics of Ultrathin Films and Heterostructures of Rare-Earth Nickelates (2016, background): “Very recently, a DMFT theoretical framework has appeared to predict the couplings to design materials for far more efficient dynamic control [170].”