Andrea Cavalleri

Abstract:

We report femtosecond resonant soft x-ray diffraction measurements of the dynamics of the charge order and of the crystal lattice in nonsuperconducting, stripe-ordered La1.875Ba0.125CuO4. Excitation of the in-plane Cu-O stretching phonon with a midinfrared pulse has been previously shown to induce a transient superconducting state in the closely related compound La1.675Eu0.2Sr0.125CuO4. In La1.875Ba0.125CuO4, we find that the charge stripe order melts promptly on a subpicosecond time scale. Surprisingly, the low temperature tetragonal (LTT) distortion is only weakly reduced, reacting on significantly longer time scales that do not correlate with light-induced superconductivity. This experiment suggests that charge modulations alone, and not the LTT distortion, prevent superconductivity in equilibrium.

Abstract:

We measure the ultrafast recombination of photoexcited quasiparticles (holon-doublon pairs) in the one dimensional Mott insulator ET-F(2)TCNQ as a function of external pressure, which is used to tune the electronic structure. At each pressure value, we first fit the static optical properties and extract the electronic bandwidth t and the intersite correlation energy V. We then measure the recombination times as a function of pressure, and we correlate them with the corresponding microscopic parameters. We find that the recombination times scale differently than for metals and semiconductors. A fit to our data based on the time-dependent extended Hubbard Hamiltonian suggests that the competition between local recombination and delocalization of the Mott-Hubbard exciton dictates the efficiency of the recombination.

Abstract:

We present a pulse-shaping scheme operating in the mid-infrared (MIR) wavelength range up to 20 μm. The spectral phase is controlled by a specially designed large stroke 32-actuator deformable mirror in a grating-based 4f configuration. We demonstrate the shaper capability of compressing the MIR pulses, imparting parabolic and third-order spectral phases and splitting the spectral content to create two independent pulses.

Abstract:

Optical pulses at THz and mid-infrared frequencies tuned to specific vibrational resonances modulate the lattice along chosen normal mode coordinates. In this way, solids can be switched between competing electronic phases and new states are created. Here, we use vibrational modulation to make electronic interactions (Hubbard-U) in Mott-insulator time dependent. Mid-infrared optical pulses excite localized molecular vibrations in ET-F2TCNQ, a prototypical one-dimensional Mott-insulator. A broadband ultrafast probe interrogates the resulting optical spectrum between THz and visible frequencies. A red-shifted charge-transfer resonance is observed, consistent with a time-averaged reduction of the electronic correlation strength U. Secondly, a sideband manifold inside of the Mott-gap appears, resulting from a periodically modulated U. The response is compared to computations based on a quantum-modulated dynamic Hubbard model. Heuristic fitting suggests asymmetric holon-doublon coupling to the molecules and that electron double-occupancies strongly squeeze the vibrational mode.