M. Wiesenmayer

Collapse of long-range charge order tracked by time-resolved photoemission at high momenta

Intense femtosecond (10−15 s) light pulses can be used to transform electronic, magnetic and structural order in condensed-matter systems on timescales of electronic and atomic motion. This technique is particularly useful in the study and in the control of materials whose physical properties are governed by the interactions between multiple degrees of freedom. Time- and angle-resolved photoemission spectroscopy is in this context a direct and comprehensive, energy- and momentum-selective probe of the ultrafast processes that couple to the electronic degrees of freedom. Previously, the capability of such studies to access electron momentum space away from zero momentum was, however, restricted owing to limitations of the available probing photon energy. Here, using femtosecond extreme-ultraviolet pulses delivered by a high-harmonic-generation source, we use time- and angle-resolved photoemission spectroscopy to measure the photoinduced vaporization of a charge-ordered state in the potential excitonic insulator 1T-TiSe2 (refs 12, 13). By way of stroboscopic imaging of electronic band dispersions at large momentum, in the vicinity of the edge of the first Brillouin zone, we reveal that the collapse of atomic-scale periodic long-range order happens on a timescale as short as 20 femtoseconds. The surprisingly fast response of the system is assigned to screening by the transient generation of free charge carriers. Similar screening scenarios are likely to be relevant in other photoinduced solid-state transitions and may generally determine the response times. Moreover, as electron states with large momenta govern fundamental electronic properties in condensed matter systems, we anticipate that the experimental advance represented by the present study will be useful to study the ultrafast dynamics and microscopic mechanisms of electronic phenomena in a wide range of materials.

Quantum-Well Wave-Function Localization and the Electron-Phonon Interaction in Thin Ag Nanofilms

The electron-phonon interaction in thin Ag nanofilms epitaxially grown on Cu(111) is investigated by temperature-dependent and angle-resolved photoemission from silver quantum-well states. Clear oscillations in the electron-phonon coupling parameter as a function of the silver film thickness are observed. Different from other thin film systems where quantum oscillations are related to the Fermi-level crossing of quantum-well states, we can identify a new mechanism behind these oscillations, based on the wave-function localization of the quantum-well states in the film.

Self-amplified photo-induced gap quenching in a correlated electron material

Capturing the dynamic electronic band structure of a correlated material presents a powerful capability for uncovering the complex couplings between the electronic and structural degrees of freedom. When combined with ultrafast laser excitation, new phases of matter can result, since far-from-equilibrium excited states are instantaneously populated. Here, we elucidate a general relation between ultrafast non-equilibrium electron dynamics and the size of the characteristic energy gap in a correlated electron material. We show that carrier multiplication via impact ionization can be one of the most important processes in a gapped material, and that the speed of carrier multiplication critically depends on the size of the energy gap. In the case of the charge-density wave material 1T-TiSe2, our data indicate that carrier multiplication and gap dynamics mutually amplify each other, which explains—on a microscopic level—the extremely fast response of this material to ultrafast optical excitation.

Time and angle resolved photoemission spectroscopy using femtosecond visible and high-harmonic light

The angle resolved photoelectron spectroscopy (ARPES) has emerged as a leading technique in identifying static key properties of complex systems such as the electronic band structure of adsorbed molecules, ultrathin quantum-well films or high temperature superconductors. We efficiently combined ARPES by using a two-dimensional analyzer for parallel energy (E) and momentum (k||) detection with femtosecond time-resolved spectroscopies. Using time and angle resolved two photon photoemission (2PPE) with visible light pulses, the hot electron dynamics in complex electronic structures are directly accessible by means of angle resolved hot electron lifetime mapping. Furthermore, femtosecond ARPES spectra recorded with high harmonic generation (HHG) light pulses are presented, showing the potential of this technique for future investigations of surface dynamics and photo-induced phase transition processes.

CDW-Superlattice Suppression Probed in Time-Resolved XUV Photoemission at the Border of the Brillouin Zone

Time- and angle-resolved XUV-photoemission at the border of the first Brillouin zone is employed to monitor the ultrafast suppression of a (2×2×2) reconstruction characteristic for the charge density wave (CDW) phase in 1T-TiSe2. The correlation of lattice dynamics and transient electronic response, which is probed in this experiment in parallel, provides new insights into the puzzling nature of the CDW mechanism in 1T-TiSe2.

The nature of a nonlinear excitation pathway from the Shockley surface state as probed by chirped pulse two photon photoemission

Phase-modulated femtosecond laser pulses are used to study the spectral response of a non-resonant two photon excitation from the Cu(111) Shockley surface state (SS). Controlled variations in the spectral phase of the laser pulse were introduced using a tuneable Fork prism phase modulator and resulted in a shift in the peak-position (of up to 110meV), variations in the spectral width (up to 88meV) and changes in the asymmetry of the SS peak as detected by two-photon photoemission. A satisfactory quantitative model of the experimental results can only be achieved if the complete spectral phase up to the third-order dispersion terms is taken into account. Of particular note, we find that a consistent description of this two photon absorption process does not require coupling of the excitation to an intermediate copper bulk state, which contradicts the previous results of Petek et al (1997 Phys. Rev. Lett. 79 4649).

Probing adsorbate dynamics with chirped laser pulses in a single-pulse scheme

Femtosecond dynamics of the model-like adsorption system Cs/Cu111 is probed by two-photon photoelectron spectroscopy 2PPE using phase-modulated chirped laser pulses. The experimental data are quantitatively modeled within a wavepacket propagation approach under explicit consideration of the adsorbate motion. The results enable us to assign characteristic chirped-pulse 2PPE features to the ultrafast adsorbate dynamics associated with the excited state lifetime and the adsorbate motion, and to improve on the qualitative interpretation of experimental data as published in Petek et al. J. Phys. Chem. A 104, 10234 2000 .O ur results show that nonlinear photoemission with a chirped pulse in a single-pulse scheme can complement real-time studies based on pump-probe schemes to gain quantitative insights into the femtosecond dynamics of ultrafast surface processes.