L. Kipp

Sharper images by focusing soft X-rays with photon sieves.

Fresnel zone plates consisting of alternating transmissive and opaque circular rings can be used to focus X-rays. The spatial resolution that can be achieved with these devices is of the order of the width of the outermost zone and is therefore limited by the smallest structure (20–40 nm) that can be fabricated by lithography today. Here we show that a large number of pinholes distributed appropriately over the Fresnel zones make it possible to focus soft X-rays to spot sizes smaller than the diameter of the smallest pinhole. In addition, higher orders of diffraction and secondary maxima can be suppressed by several orders of magnitude. In combination with the next generation of synchrotron light sources (free-electron lasers) these ‘photon sieves’ offer new opportunities for high-resolution X-ray microscopy and spectroscopy in physical and life sciences.

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.

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.

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-assembled nanowire formation during Cu deposition on atomically flat Vse2 surfaces studied by microscopic methods

Abstract Self-assembled metallic nanostructures gain increasing interest in nanotechnologies and might find application in future electronic device fabrication. Upon UHV deposition of copper onto cleaved layered crystals of VSe 2 , self-assembled networks of nanowires and nanoclusters are observed to form and found to be remarkably stable even during storage under ambient conditions and at moderately increased temperatures. Transmission and scanning electron microscopy combined with scanning tunneling and atomic force microscopy have been used to characterize the arrangements, structure and dimensions of the nanostructures and the substrate before metal deposition. On the flat parts of the substrate, self-similar nanowire networks form with wire diameters ranging from 8 to 250 nm and mesh dimensions ranging from 0.35 to 10 μm. The nanowires are preferentially aligned along low-index crystal directions and possess polycrystalline structure. Nanoclusters are formed within the meshes of the nanowire network. A model for the self-assembled growth of nanostructures during metal deposition, which takes into account the electronic charge exchange of adsorbed atoms with the substrate, will be discussed.

Focusing light with a reflection photon sieve.

An advanced type of diffractive optical element is presented that combines the concept of the photon sieve with an off-axis, off-normal incidence reflection geometry. Compared to transmission optical elements, the signal-to-background ratio is significantly increased by separating the first from other diffraction orders without drastically reducing the size of the smallest diffractive element. The reflection photon sieve produces sharp foci at maximum contrast and offers the advantages of effective heat dissipation and a large working space above the focal plane. Experimental results for a device working at a photon energy of 100 eV are presented and compared to theory.

Photoswitching of azobenzene multilayers on a layered semiconductor

In situ photoelectron spectroscopy is used to study the adsorption and photoisomerization of azobenzene multilayers on the layered semiconductor HfS 2 at liquid nitrogen temperatures. The measured valence band spectra indicate weak molecule–substrate coupling and provide evidence for reversible switching of azobenzene multilayers by light with different wavelengths. The photoswitching manifests itself in spectral shifts due to changes in the electrical surface conductance and in modifications of the electronic structure consistent with the results of outer valence Green’s function calculations. The photoemission results appear to establish azobenzene as an optoelectrical molecular switch.