Theory of nonlinear phononics for coherent light-control of solids

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.Comment: updated to reflect the published versio

Cavity-mediated electron-photon superconductivity

We investigate electron paring in a two-dimensional electron system mediated by vacuum fluctuations inside a nanoplasmonic terahertz cavity. We show that the structured cavity vacuum can induce long-range attractive interactions between current fluctuations which lead to pairing in generic materials with critical temperatures in the low-Kelvin regime for realistic parameters. The induced state is a pair density wave superconductor which can show a transition from a fully gapped to a partially gapped phase - akin to the pseudogap phase in high-$T_c$ superconductors. Our findings provide a promising tool for engineering intrinsic electron interactions in two-dimensional materials.Comment: 11 page

Parametric amplification of optical phonons

Amplification of light through stimulated emission or nonlinear optical interactions has had a transformative impact on modern science and technology. The amplification of other bosonic excitations, like phonons in solids, is likely to open up new remarkable physical phenomena. Here, we report on an experimental demonstration of optical phonon amplification. A coherent mid-infrared optical field is used to drive large amplitude oscillations of the Si-C stretching mode in silicon carbide. Upon nonlinear phonon excitation, a second probe pulse experiences parametric optical gain at all wavelengths throughout the reststrahlen band, which reflects the amplification of optical-phonon fluctuations. Starting from first principle calculations, we show that the high-frequency dielectric permittivity and the phonon oscillator strength depend quadratically on the lattice coordinate. In the experimental conditions explored here, these oscillate then at twice the frequency of the optical field and provide a parametric drive for lattice fluctuations. Parametric gain in phononic four wave mixing is a generic mechanism that can be extended to all polar modes of solids, as a new means to control the kinetics of phase transitions, to amplify many body interactions or to control phonon-polariton waves

Metastable ferroelectricity in optically strained SrTiO3SrTiO_3

Fluctuating orders in solids are generally considered high-temperature precursors of broken symmetry phases. However, in some cases these fluctuations persist to zero temperature and prevent the emergence of long-range order, as for example observed in quantum spin and dipolar liquids. $SrTiO_3$ is a quantum paraelectric in which dipolar fluctuations grow when the material is cooled, although a long-range ferroelectric order never sets in. We show that the nonlinear excitation of lattice vibrations with mid-infrared optical pulses can induce polar order in $SrTiO_3$ up to temperatures in excess of 290 K. This metastable phase, which persists for hours after the optical pump is interrupted, is evidenced by the appearance of a large second-order optical nonlinearity that is absent in equilibrium. Hardening of a low-frequency mode indicates that the polar order may be associated with a photo-induced ferroelectric phase transition. The spatial distribution of the optically induced polar domains suggests that a new type of photo-flexoelectric coupling triggers this effect

Transiently enhanced interlayer tunneling in optically driven high-Tc superconductors

Recent pump-probe experiments reported an enhancement of superconducting transport along the c axis of underdoped YBa2Cu3O6+δ (YBCO), induced by a midinfrared optical pump pulse tuned to a specific lattice vibration. To understand this transient nonequilibrium state, we develop a pump-probe formalism for a stack of Josephson junctions, and we consider the tunneling strengths in the presence of modulation with an ultrashort optical pulse. We demonstrate that a transient enhancement of the Josephson coupling can be obtained for pulsed excitation and that this can be even larger than in a continuously driven steady state. Especially interesting is the conclusion that the effect is largest when the material is parametrically driven at a frequency immediately above the plasma frequency, in agreement with what is found experimentally. For bilayer Josephson junctions, an enhancement similar to that experimentally is predicted below the critical temperature Tc. This model reproduces the essential features of the enhancement measured below Tc. To reproduce the experimental results above Tc, we will explore extensions of this model, such as in-plane and amplitude fluctuations, elsewhere.Deutsche Forschungsgemeinschaft; SFB 925; EXC 1074; Joachim Herz StiftungFirst author draf

Nonlinear light-matter interaction at terahertz frequencies

Strong optical pulses at mid-infrared and terahertz frequencies have recently emerged as a powerful tool to manipulate and control the solid state and especially complex condensed matter systems with strongly correlated electrons. The recent developments in high-power sources in the 0.1-30 THz frequency range, both from table-top laser systems and Free-Electron Lasers, has provided access to excitations of molecules and solids, which can be stimulated at their resonance frequencies. Amongst these, we discuss free electrons in metals, superconducting gaps and Josephson plasmons in layered superconductors, vibrational modes of the crystal lattice (phonons), as well as magnetic excitations. This Review provides an overview and illustrative examples of how intense THz transients can be used to resonantly control matter, with particular focus on strongly correlated electron systems and high-temperature superconductors.Comment: 55 pages, 34 figure

Probing the Interatomic Potential of Solids by Strong-Field Nonlinear Phononics

Femtosecond optical pulses at mid-infrared frequencies have opened up the nonlinear control of lattice vibrations in solids. So far, all applications have relied on second order phonon nonlinearities, which are dominant at field strengths near 1 MVcm-1. In this regime, nonlinear phononics can transiently change the average lattice structure, and with it the functionality of a material. Here, we achieve an order-of-magnitude increase in field strength, and explore higher-order lattice nonlinearities. We drive up to five phonon harmonics of the A1 mode in LiNbO3. Phase-sensitive measurements of atomic trajectories in this regime are used to experimentally reconstruct the interatomic potential and to benchmark ab-initio calculations for this material. Tomography of the Free Energy surface by high-order nonlinear phononics will impact many aspects of materials research, including the study of classical and quantum phase transitions

Terahertz field control of interlayer transport modes in cuprate superconductors

We theoretically show that terahertz pulses with controlled amplitude and frequency can be used to switch between stable transport modes in layered superconductors, modelled as stacks of Josephson junctions. We find pulse shapes that deterministically switch the transport mode between superconducting, resistive and solitonic states. We develop a simple model that explains the switching mechanism as a destablization of the centre of mass excitation of the Josephson phase, made possible by the highly non-linear nature of the light-matter coupling

Proposed cavity Josephson plasmonics with complex-oxide heterostructures

We discuss how complex-oxide heterostructures that include high-Tc superconducting cuprates can be used to realize an array of sub-millimeter cavities that support Josephson plasmon polaritons. These cavities have several attractive features for new types of light matter interaction studies and we show that they promote "ultrastrong" coupling between THz frequency radiation and Josephson plasmons. Cavity electrodynamics of Josephson plasmons allows to manipulate the superconducting order-parameter phase coherence. As an example, we discuss how it could be used to cool superconducting phase fluctuations with light