Andrea Cavalleri

Abstract:

The nature of the incipient ferroelectric transition in SrTiO3 has been a long-standing puzzle in condensed matter physics. One explanation involves the competition between ferroelectricity and an instability characterized by the mesoscopic modulation of the polarization. These polarization density waves, which should intensify near the quantum critical point, break local inversion symmetry and are difficult to characterize with conventional X-ray scattering methods. Here we probe inversion symmetry breaking at finite momenta and visualize the instability of the polarization at the nanometre scale in SrTiO3 by combining a femtosecond X-ray free-electron laser with terahertz coherent control methods. We found polar-acoustic collective modes that are soft, particularly at the tens of nanometre scale. These precursor collective excitations provide evidence for the conjectured mesoscopic-modulated phase in SrTiO3.

Abstract:

Inhomogeneities crucially influence the properties of quantum materials, yet methods that can measure them remain limited and can access only a fraction of relevant observables. For example, local probes such as scanning tunnelling microscopy have documented that the electronic properties of cuprate superconductors are inhomogeneous over nanometre length scales. However, complementary techniques that can resolve higher-order correlations are needed to elucidate the nature of these inhomogeneities. Furthermore, local tunnelling probes are often effective only far below the critical temperature. Here we develop a two-dimensional terahertz spectroscopy method to measure Josephson plasmon echoes from an interlayer superconducting tunnelling resonance in a near-optimally doped cuprate. The technique allows us to study the multidimensional optical response of the interlayer Josephson coupling in the material and disentangle intrinsic lifetime broadening from extrinsic inhomogeneous broadening for interlayer superconducting tunnelling. We find that inhomogeneous broadening persists up to a substantial fraction of the critical temperature, above which this is overcome by the thermally increased lifetime broadening.

Abstract:

Coherent optical driving in quantum solids is emerging as a research frontier, with many reports of interesting non-equilibrium quantum phases1–4 and transient photo-induced functional phenomena such as ferroelectricity5, 6, magnetism7–10 and superconductivity11–14. In high-temperature cuprate superconductors, coherent driving of certain phonon modes has resulted in a transient state with superconducting-like optical properties, observed far above their transition temperature Tc and throughout the pseudogap phase15–18. However, questions remain on the microscopic nature of this transient state and how to distinguish it from a non-superconducting state with enhanced carrier mobility. For example, it is not known whether cuprates driven in this fashion exhibit Meissner diamagnetism. Here we examine the time-dependent magnetic field surrounding an optically driven YBa2Cu3O6.48 crystal by measuring Faraday rotation in a magneto-optic material placed in the vicinity of the sample. For a constant applied magnetic field and under the same driving conditions that result in superconducting-like optical properties15–18, a transient diamagnetic response was observed. This response is comparable in size with that expected in an equilibrium type II superconductor of similar shape and size with a volume susceptibility χv of order −0.3. This value is incompatible with a photo-induced increase in mobility without superconductivity. Rather, it underscores the notion of a pseudogap phase in which incipient superconducting correlations are enhanced or synchronized by the drive.