Haiyun Liu

Clocking the Melting Transition of Charge and Lattice Order in 1T−TaS2 with Ultrafast Extreme-Ultraviolet Angle-Resolved Photoemission Spectroscopy

Charge density waves (CDWs) underpin the electronic properties of many complex materials. Near-equilibrium CDW order is linearly coupled to a periodic, atomic-structural distortion, and the dynamics is understood in terms of amplitude and phase modes. However, at the shortest timescales lattice and charge order may become de-coupled, highlighting the electronic nature of this many-body broken symmetry ground state. Using time and angle resolved photoemission spectroscopy with sub-30-fs XUV pulses, we have mapped the time- and momentum-dependent electronic structure in photo-stimulated 1T-TaS2, a prototypical two-dimensional charge density wave compound. We find that CDW order, observed as a splitting of the uppermost electronic bands at the Brillouin zone boundary, melts well before relaxation of the underlying structural distortion. Decoupled charge and lattice modulations challenge the view of Fermi Surface nesting as a driving force for charge density wave formation in 1T-TaS2.

Femtosecond all-optical synchronization of an X-ray free-electron laser

Many advanced applications of X-ray free-electron lasers require pulse durations and time resolutions of only a few femtoseconds. To generate these pulses and to apply them in time-resolved experiments, synchronization techniques that can simultaneously lock all independent components, including all accelerator modules and all external optical lasers, to better than the delivered free-electron laser pulse duration, are needed. Here we achieve all-optical synchronization at the soft X-ray free-electron laser FLASH and demonstrate facility-wide timing to better than 30 fs r.m.s. for 90 fs X-ray photon pulses. Crucially, our analysis indicates that the performance of this optical synchronization is limited primarily by the free-electron laser pulse duration, and should naturally scale to the sub-10 femtosecond level with shorter X-ray pulses.

Optically induced coherent transport far above Tc in underdoped YBa2Cu3O6+δ

We report on a photo-induced transient state of YBa2Cu2O6+x in which transport perpendicular to the Cu-O planes becomes highly coherent. This effect is achieved by excitation with mid-infrared optical pulses, tuned to the resonant frequency of apical oxygen vibrations, which modulate both lattice and electronic properties. Below the superconducting transition temperature Tc, the equilibrium signatures of superconducting interlayer coupling are enhanced. Most strikingly, the optical excitation induces a new reflectivity edge at higher frequency than the equilibrium Josephson plasma resonance, with a concomitant enhancement of the low frequency imaginary conductivity. Above Tc, the incoherent equilibrium conductivity becomes highly coherent, with the appearance of a reflectivity edge and a positive imaginary conductivity that increases with decreasing frequency. These features are observed up to room temperature in YBa2Cu2O6.45 and YBa2Cu2O6.5. The data above Tc can be fitted by hypothesizing that the light re-establishes a transient superconducting state over only a fraction of the solid, with a lifetime of a few picoseconds. Non-superconducting transport could also explain these observations, although one would have to assume transient carrier mobilities near 10^4 cm^2/(V.sec) at 100 K, with a density of charge carriers similar to the below Tc superfluid density. Our results are indicative of highly unconventional non-equilibrium physics and open new prospects for optical control of complex solids.

THz-Frequency Modulation of the Hubbard U in an Organic Mott Insulator.

We use midinfrared pulses with stable carrier-envelope phase offset to drive molecular vibrations in the charge transfer salt ET-F_{2}TCNQ, a prototypical one-dimensional Mott insulator. We find that the Mott gap, which is probed resonantly with 10 fs laser pulses, oscillates with the pump field. This observation reveals that molecular excitations can coherently perturb the electronic on-site interactions (Hubbard U) by changing the local orbital wave function. The gap oscillates at twice the frequency of the vibrational mode, indicating that the molecular distortions couple quadratically to the local charge density.

Possible observation of parametrically amplified coherent phasons in K0.3MoO3 using time-resolved extreme-ultraviolet angle-resolved photoemission spectroscopy

. Prompt depletion of the charge-densitywavecondensatelaunchescoherentoscillationsoftheamplitudemode,observedasa1.7-THz-frequencymodulationofthebondingbandposition.Incontrast,theantibondingbandoscillatesatabouthalfthisfrequency.Weattributetheseoscillationstocoherentexcitationofphasonsviaparametricamplificationofphasefluctuations.DOI: 10.1103/PhysRevB.88.045104 PACS number(s): 78

A dynamical stability limit for the charge density wave in K0.3MoO3

We study the response of the one-dimensional charge density wave in K_{0.3}MoO_{3} to different types of excitation with femtosecond optical pulses. We compare direct excitation of the lattice at midinfrared frequencies with injection of quasiparticles across the low energy charge density wave gap and with charge transfer excitation in the near infrared. For all three cases, we observe a fluence threshold above which the amplitude-mode oscillation frequency is softened and the mode becomes increasingly damped. We show that all the data can be collapsed onto a universal curve in which the melting of the charge density wave occurs abruptly at a critical lattice excursion. These data highlight the existence of a universal stability limit for a charge density wave, reminiscent of the Lindemann criterion for the melting of a crystal lattice.

Angle-resolved photoemission spectroscopy with 9-eV photon-energy pulses generated in a gas-filled hollow-core photonic crystal fiber

A recently developed source of ultraviolet radiation, based on optical soliton propagation in a gas-filled hollow-core photonic crystal fiber, is applied here to angle-resolved photoemission spectroscopy (ARPES). Near-infrared femtosecond pulses of only few μJ energy generate vacuum ultraviolet radiation between 5.5 and 9 eV inside the gas-filled fiber. These pulses are used to measure the band structure of the topological insulator Bi2Se3 with a signal to noise ratio comparable to that obtained with high order harmonics from a gas jet. The two-order-of-magnitude gain in efficiency promises time-resolved ARPES measurements at repetition rates of hundreds of kHz or even MHz, with photon energies that cover the first Brillouin zone of most materials.

Ultrafast Tr-ARPES with Artemis XUV Beamline

A new HHG XUV beamline at Artemis, user open-access facility at CLF, offers unique capabilities optimised for Tr-ARPES. Current result on ultrafast melting of Mott and charge order in TaS2 will be presented.

Time-and-Angle-Resolved Photoemission Spectroscopy with Mid-IR Pump and 30 fs EUV Probe

Time- and angle-resolved photoemission spectroscopy directly enables observation of electron dynamics in condensed matter. Using EUV high harmonic probe extends the observation window in energy and momentum. Tuneable mid-infrared pumping allows control of excitation mechanisms.

Monochromatised XUV Pulses for Ultrafast Science at the Artemis Facility

XUV pulses produced through high harmonic generation can probe electron dynamics in complex solid materials and in gas-phase atoms and molecules. This is demonstrated in gas-phase and condensed matter experiments at the Artemis facility.