Andrea Cavalleri

Abstract:

Two types of coupling between electromagnetic radiation and a crystal lattice have so far been identified experimentally. The first is the direct coupling of light to infrared-active vibrations carrying an electric dipole. The second is indirect, involving electron-phonon coupling and occurring through excitation of the electronic system; stimulated Raman scattering is one example. A third path, ionic Raman scattering (IRS; refs4,5), was proposed 40 years ago. It was posited that excitation of an infrared-active phonon could serve as the intermediate state for Raman scattering, a process that relies on lattice anharmonicities rather than electron-phonon interactions. Here, we report an experimental demonstration of IRS using femtosecond excitation and coherent detection of the lattice response. We show how this mechanism is relevant to ultrafast optical control in solids: a rectified phonon field can exert a directional force onto the crystal, inducing an abrupt displacement of the atoms from their equilibrium positions. IRS opens up a new direction for the optical control of solids in their electronic ground state, different from carrier excitation. © 2011 Macmillan Publishers Limited. All rights reserved.

Abstract:

We use time- and angle-resolved photoemission spectroscopy with sub-30-fs extreme-ultraviolet pulses to map the time- and momentum-dependent electronic structure of photoexcited 1T-TaS(2). This compound is a two-dimensional Mott insulator with charge-density wave ordering. Charge order, evidenced by splitting between occupied subbands at the Brillouin zone boundary, melts well before the lattice responds. This challenges the view of a charge-density wave caused by electron-phonon coupling and Fermi-surface nesting alone, and suggests that electronic correlations play a key role in driving charge order.

Abstract:

In cuprate superconductors, tunnelling between planes makes three-dimensional superconductive transport possible. However, the interlayer tunnelling amplitude is reduced when an order-parameter-phase gradient between planes is established. As such, interlayer superconductivity along the c-axis can be weakened if a strong electric field is applied along the c-axis. In this Letter, we use high-field single-cycle terahertz pulses to gate interlayer coupling in La1.84Sr0.16CuO4. We induce ultrafast oscillations between superconducting and resistive states and switch the plasmon response on and off, without reducing the density of Cooper pairs. In-plane superconductivity remains unperturbed, revealing a non-equilibrium state in which the dimensionality of the superconductivity is time-dependent. The gating frequency is determined by the electric field strength. Non-dissipative, bi-directional gating of superconductivity is of interest for device applications in ultrafast nanoelectronics and represents an example of how nonlinear terahertz physics can benefit nanoplasmonics and active metamaterials. © 2011 Macmillan Publishers Limited. All rights reserved.

Abstract:

We used ultrafast resonant soft x-ray diffraction to probe the picosecond dynamics of spin and orbital order in La(0.5)Sr(1.5)MnO(4) after photoexcitation with a femtosecond pulse of 1.5 eV radiation. Complete melting of antiferromagnetic spin order is evidenced by the disappearance of a (1/4,1/4,1/2) diffraction peak. On the other hand, the (1/4,1/4,0) diffraction peak, reflecting orbital order, is only partially reduced. We interpret the results as evidence of destabilization in the short-range exchange pattern with no significant relaxation of the long-range Jahn-Teller distortions. Cluster calculations are used to analyze different possible magnetically ordered states in the long-lived metastable phase. Nonthermal coupling between light and magnetism emerges as a primary aspect of photoinduced phase transitions in manganites.

Abstract:

One of the most intriguing features of some high-temperature cuprate superconductors is the interplay between one-dimensional "striped" spin order and charge order, and superconductivity. We used mid-infrared femtosecond pulses to transform one such stripe-ordered compound, nonsuperconducting La1.675Eu0.2Sr0.125CuO 4, into a transient three-dimensional superconductor. The emergence of coherent interlayer transport was evidenced by the prompt appearance of a Josephson plasma resonance in the c-axis optical properties. An upper limit for the time scale needed to form the superconducting phase is estimated to be 1 to 2 picoseconds, which is significantly faster than expected. This places stringent new constraints on our understanding of stripe order and its relation to superconductivity.