K. Rossnagel

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.

On the origin of charge-density waves in select layered transition-metal dichalcogenides

The occurrence of charge-density waves in three selected layered transition-metal dichalcogenides-1T-TaS(2), 2H-TaSe(2) and 1T-TiSe(2)-is discussed from an experimentalists point of view with a particular focus on the implications of recent angle-resolved photoelectron spectroscopy results. The basic models behind charge-density-wave formation in low-dimensional solids are recapitulated, the experimental and theoretical results for the three selected compounds are reviewed, and their band structures and spectral weight distributions in the commensurate charge-density-wave phases are calculated using an empirical tight-binding model. It is explored whether the origin of charge-density waves in the layered transition-metal dichalcogenides can be understood in a unified way on the basis of a few measured and calculated parameters characterizing the interacting electron-lattice system. It is found that the predictions of the standard mean-field model agree only semi-quantitatively with the experimental data and that there is not one generally dominant factor driving charge-density-wave formation in this family of layer compounds. The need for further experimental and theoretical scrutiny is emphasized.

Fermi Surface and Quasiparticle Dynamics of Na0:7CoO2 Investigated by Angle-Resolved Photoemission Spectroscopy

We present the first angle-resolved photoemission study of Na0.7CoO2, the host material of the superconducting NaxCoO2.nH(2)O series. Our results show a hole-type Fermi surface, a strongly renormalized quasiparticle band, a small Fermi velocity, and a large Hubbard U. The quasiparticle band crosses the Fermi level from M toward Gamma suggesting a negative sign of effective single-particle hopping t(eff) (about 10 meV) which is on the order of magnetic exchange coupling J in this system. Quasiparticles are well defined only in the T-linear resistivity (non-Fermi-liquid) regime. Unusually small single-particle hopping and unconventional quasiparticle dynamics may have implications for understanding the phase of matter realized in this new class of a strongly interacting quantum system.

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.

Non-thermal separation of electronic and structural orders in a persisting charge density wave

The simultaneous ordering of different degrees of freedom in complex materials undergoing spontaneous symmetry-breaking transitions often involves intricate couplings that have remained elusive in phenomena as wide ranging as stripe formation, unconventional superconductivity or colossal magnetoresistance. Ultrafast optical, X-ray and electron pulses can elucidate the microscopic interplay between these orders by probing the electronic and lattice dynamics separately, but a simultaneous direct observation of multiple orders on the femtosecond scale has been challenging. Here we show that ultrabroadband terahertz pulses can simultaneously trace the ultrafast evolution of coexisting lattice and electronic orders. For the example of a charge density wave (CDW) in 1T-TiSe2, we demonstrate that two components of the CDW order parameter--excitonic correlations and a periodic lattice distortion (PLD)--respond very differently to 12-fs optical excitation. Even when the excitonic order of the CDW is quenched, the PLD can persist in a coherently excited state. This observation proves that excitonic correlations are not the sole driving force of the CDW transition in 1T-TiSe2, and exemplifies the sort of profound insight that disentangling strongly coupled components of order parameters in the time domain may provide for the understanding of a broad class of phase transitions.

Quantum phase transition from triangular to stripe charge order in NbSe2

The competition between proximate electronic phases produces a complex phenomenology in strongly correlated systems. In particular, fluctuations associated with periodic charge or spin modulations, known as density waves, may lead to exotic superconductivity in several correlated materials. However, density waves have been difficult to isolate in the presence of chemical disorder, and the suspected causal link between competing density wave orders and high-temperature superconductivity is not understood. Here we used scanning tunneling microscopy to image a previously unknown unidirectional (stripe) charge-density wave (CDW) smoothly interfacing with the familiar tridirectional (triangular) CDW on the surface of the stoichiometric superconductor NbSe2. Our low-temperature measurements rule out thermal fluctuations and point to local strain as the tuning parameter for this quantum phase transition. We use this quantum interface to resolve two longstanding debates about the anomalous spectroscopic gap and the role of Fermi surface nesting in the CDW phase of NbSe2. Our results highlight the importance of local strain in governing phase transitions and competing phenomena, and suggest a promising direction of inquiry for resolving similarly longstanding debates in cuprate superconductors and other strongly correlated materials.

Direct comparison between potential landscape and local density of states in a disordered two-dimensional electron system.

The local density of states (LDOS) of the adsorbate-induced two-dimensional electron system (2DES) on n-InAs(110) is studied by scanning tunneling spectroscopy. In contrast to a similar 3DES, the 2DES LDOS exhibits 20 times stronger corrugations and rather irregular structures. Both results are interpreted as consequences of weak localization. Fourier transforms of the LDOS reveal that the k values of the unperturbed 2DES still dominate the 2DES, but additional lower k values contribute. To clarify the origin of the LDOS patterns, we measure the potential landscape of the 2DES area. We use it to calculate the expected LDOS and find reasonable agreement between calculation and experiment.

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.

Vacuum space charge effect in laser-based solid-state photoemission spectroscopy

We report a systematic measurement of the space charge effect observed in the few-ps laser pulse regime in laser-based solid-state photoemission spectroscopy experiments. The broadening and the shift of a gold Fermi edge as a function of spot size, laser power, and emission angle are characterized for pulse lengths of 6 ps and 6 eV photon energy. The results are used as a benchmark for an N-body numerical simulation and are compared to different regimes used in photoemission spectroscopy. These results provide an important reference for the design of time and angle-resolved photoemission spectroscopy setups and next-generation light sources.

Iron(II) Spin‐Crossover Complexes in Ultrathin Films: Electronic Structure and Spin‐State Switching by Visible and Vacuum‐UV Light

The electronic structure of the iron(II) spin crossover complex [Fe(H2bpz)2(phen)] deposited as an ultrathin film on Au(111) is determined by means of UV-photoelectron spectroscopy (UPS) in the high-spin and in the low-spin state. This also allows monitoring the thermal as well as photoinduced spin transition in this system. Moreover, the complex is excited to the metastable high-spin state by irradiation with vacuum-UV light. Relaxation rates after photoexcitation are determined as a function of temperature. They exhibit a transition from thermally activated to tunneling behavior and are two orders of magnitude higher than in the bulk material.