T. Rohwer

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.

Time-domain classification of charge-density-wave insulators

Distinguishing insulators by the dominant type of interaction is a central problem in condensed matter physics. Basic models include the Bloch-Wilson and the Peierls insulator due to electron-lattice interactions, the Mott and the excitonic insulator caused by electron-electron interactions, and the Anderson insulator arising from electron-impurity interactions. In real materials, however, all the interactions are simultaneously present so that classification is often not straightforward. Here, we show that time- and angle-resolved photoemission spectroscopy can directly measure the melting times of electronic order parameters and thus identify-via systematic temporal discrimination of elementary electronic and structural processes-the dominant interaction. Specifically, we resolve the debates about the nature of two peculiar charge-density-wave states in the family of transition-metal dichalcogenides, and show that Rb intercalated 1T-TaS(2) is a Peierls insulator and that the ultrafast response of 1T-TiSe(2) is highly suggestive of an excitonic insulator.

Time-resolved x-ray photoelectron spectroscopy at FLASH

The technique of time-resolved pump-probe x-ray photoelectron spectroscopy using the free-electron laser in Hamburg (FLASH) is described in detail. Particular foci lie on the macrobunch resolving detection scheme, the role of vacuum space-charge effects and the synchronization of pump and probe lasers. In an exemplary case study, the complete Ta 4f core-level dynamics in the layered charge-density-wave (CDW) compound 1T-TaS2 in response to impulsive optical excitation is measured on the sub-picosecond to nanosecond timescale. The observed multi-component dynamics is related to the intrinsic melting and reformation of the CDW as well as to extrinsic pump-laser-induced vacuum space-charge effects.

Ultrafast Modulation of the Chemical Potential in BaFe2As2 by Coherent Phonons

Author(s): Yang, LX; Rohde, G; Rohwer, T; Stange, A; Hanff, K; Sohrt, C; Rettig, L; Cortes, R; Chen, F; Feng, DL; Wolf, T; Kamble, B; Eremin, I; Popmintchev, T; Murnane, MM; Kapteyn, HC; Kipp, L; Fink, J; Bauer, M; Bovensiepen, U; Rossnagel, K | Abstract: Time- and angle-resolved extreme ultraviolet photoemission spectroscopy is used to study the electronic structure dynamics in BaFe2As2 around the high-symmetry points Γ and M. A global oscillation of the Fermi level at the frequency of the A1g(As) phonon mode is observed. It is argued that this behavior reflects a modulation of the effective chemical potential in the photoexcited surface region that arises from the high sensitivity of the band structure near the Fermi level to the A1g(As) phonon mode combined with a low electron diffusivity perpendicular to the layers. The results establish a novel way to tune the electronic properties of iron pnictides: coherent control of the effective chemical potential. The results further suggest that the equilibration time for the effective chemical potential needs to be considered in the ultrafast electronic structure dynamics of materials with weak interlayer coupling.

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.

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.

Probing the switching state of a surface-mounted azobenzene derivative using femtosecond XUV photoemission

Photoemission spectroscopy using femtosecond XUV light pulses is applied to probe the isomerization state of the molecular switch 3-(4-(4-hexyl-phenylazo)-phenoxy)-propane-1-thiol deposited by liquid phase self-assembly on Au(111). Spectral shifts of valence-electronic signatures that we associate with the carbon C2s orbital enable us to distinguish the trans and the cis isomerization state of the adsorbed molecules. These preliminary results envision the potential to probe reversible switching processes of surface-mounted molecules in real time by tracking the temporal evolution of the electronic and nuclear degrees of freedom in a femtosecond XUV photoemission experiment.