Turning at top speed – Publication by B11 (Güdde/Höfer) in Nature

In collaboration with the group of Rupert Huber in Regensburg, Suguru Ito, Jens Güdde and Ulrich Höfer from the new SFB project B11 “Ultrafast dynamics of interface currents” demonstrate efficient high-order harmonic generation at the surface of a topological insulator by driving ballistic electron currents at THz frequencies.

On the surface of a topological insulator (colored surface), electrons (small blue sphere) move with quasi-relativistic speed. When a strong light wave accelerates electrons through the so-called Dirac point (apex of the cone), their velocity abruptly flips. The instantaneous change of velocity leads to the emission of broadband electromagnetic radiation (flash in the middle of the colored surface). Reprinted with permission from Nature (link see below).

In the conducting surface states of topological insulators electrons behave like massless particles, characterized by a linear dispersion (Dirac cone). Under the influence of an electric field, the electrons rapidly switch their direction of motion when their trajectories in momentum come close to the minimum of the cone, the Dirac point. At frequencies in the range of 25 to 35 THz, this is the case for electric field strengths of several MV/cm. It results in the emission of an ultrafast flash of light containing a broadband spectrum up to frequencies of 800 THz that can be analyzed with optical detectors.

This novel mechanism of high-harmonic generation is only possible because the spin-momentum-locking in the Dirac cone prevents efficient electron scattering. The resulting long scattering times of ~1 ps allow to drive strong ballistic electron currents as demonstrated previously with THz-ARPES (Reimann et al. Nature 2018). The emitted high-harmonic radiation has a characteristic polarization dependence related to the Berry curvature of the Dirac cone. Moreover, it can be shifted to arbitrary non-integer multiples of the driving frequency by varying the carrier-envelope phase of the driving field. These specific properties set it apart from HHG processes in bulk semiconductors (Hohenleutner et al. Nature 2015).

In the upcoming third funding period, SFB 1083 will utilize THz high-harmonic radiation generated in this way and exploit its characteristic properties to investigate electron currents at interfaces of topological insulators buried under protecting capping layers. For future device applications, it will be crucial to screen the unusual movement of Dirac electrons from the environment.

Informational Material

Press release of the university of Regensburg (in English and German).

Press release of the university of Marburg (in German).

News of Physics Department, Philipps-Universität Marburg (in German).

– Homepage of the Huber group in Regensburg.

Publication

C.P. Schmid, L. Weigl, P. Grössing, V. Junk, C. Gorini, S. Schlauderer, S. Ito, M. Meierhofer, N. Hofmann, D. Afanasiev, J. Crewse, K.A. Kokh, O.E. Tereshchenko, J. Güdde, F. Evers, J. Wilhelm, K. Richter, U. Höfer, R. Huber
Tuneable non-integer high-harmonic generation in a topological insulator
Nature (2021) DOI:10.1038/s41586-021-03466-7

Contact

Prof. Dr. Ulrich Höfer
Philipps-Universität Marburg
SFB 1083 project B6, B11
Tel.: 06421 28 24215
EMAIL

Quantitative Characterization of Nanometer-Scale Electric Fields via Momentum-Resolved STEM– Publication by A5 (Volz)

Andreas Beyer and coworkers achieved the determination and spatial resolution of electric fields at interfaces with the transmission electron microscope.

Adapted from Beyer et al. (full citation see below) licensed by CC BY-NC-ND 4.0.

Nanometer-scale built-in electric field are the basis of many modern (opto)electronic devices, such as solar cells, lasers or batteries. Optimization of these devices requires precise characterization of such fields at small length scales. With a fast pixelated-detector, A. Beyer and coworkers in SFB project A5 (Volz) acquire a 2D diffraction pattern for every real-space position of the impinging electron beam. In doing so, the momentum transfer of an electric field (or a charge) on the electron beam can be measured, and the electric field, which is invisible in “normal high angle annular dark field images”, can be calculated from the 4D data-set.

In this work, key characteristics, like doping concentration or polarity, of GaAs-based p-n junctions were quantitatively obtained by 4D scanning transmission electron microscopy (4DSTEM). The values are in excellent quantitative agreement with results from other techniques, which – of course – lack lateral resolution.

Publication

A. Beyer, M.S. Munde, S. Firoozabadi, D. Heimes, T. Grieb, A. Rosenauer, K. Müller-Caspary, K. Volz
Quantitative Characterization of Nanometer-Scale Electric Fields via Momentum-Resolved STEM
Nano Lett. (2021) DOI:10.1021/acs.nanolett.0c04544

Contact

Prof. Dr. Kerstin Volz
Philipps-Universität Marburg
SFB 1083 project A5
Tel.: 06421 28 22297
EMAIL

Tracing orbital images on ultrafast time scales – Publication by B6 (Höfer/Wallauer) and A12 (Tautz/Bocquet/Kumpf) in Science

Robert Wallauer and coworkers combined a high harmonic laser source with an electron momentum microscope to record orbital images of the charge transfer at an organic/metal interface with femtosecond time resolution.

 

Excitation scheme for time-resolved photoemission orbital tomography. (b) Measured LUMO momentum maps for three selected delay times between pump and probe pulse. (c) Scheme of intramolecular and substrate-to-molecule excitation pathways. The LUMO pattern of the 0° molecule in (b) is seen to light up faster due to resonant HOMO-LUMO excitation than that of the 90° populated across the CuO Interface. From Wallauer et al, Science 371 (2021) 1056. Reprinted with permission from AAAS.

The microscopic charge-transfer dynamics across molecular interfaces is reflected in the population of electronic orbitals. These were, for the first time, directly monitored with ultrafast time resolution in a joint experimental effort of B6 (Höfer/Wallauer) in Marburg and A12 (Tautz/Bocquet/Kumpf) in Jülich. The experiment records the full two-dimensional intensity distribution of photoemitted electrons in momentum space in a femtosecond pump-probe scheme. Real-space electron distributions and photoemission momentum maps, called orbital tomographs, are related by a Fourier transform.

The model interface PTCDA/CuO/Cu(100) exhibits two distinct excitation pathways for the PTCDA molecule. The parallel component of the electric field of the pump pulse makes a direct HOMO-LUMO transition, while the perpendicular component transfers an electron from the metal across the atomically thin CuO spacer into the molecular LUMO. Once excited, the LUMO decays with a lifetime of 250 fs, independent of the excitation pathway. Real-space electron distributions and photoemission momentum maps, called orbital tomographs, are related by a Fourier transform (Photoemission Orbital Tomography, Wikipedia). 

In the future, the new experimental capability is expected to facilitate the microscopic understanding of charge-transfer and exciton-formation processes at several other classes of organic heterointerfaces with unprecedented detail, including interfaces between 2D semiconductors and layered organic molecular structures.

 

 

Informational Material

Joint press release of the universities of Marburg and Graz and the FZ Jülich (available in English and German).
News, Philipps-Universität Marburg (in German).
News, Universität Graz, Österreich (in German).

 

Publication

R. Wallauer, M. Raths, K. Stallberg, L. Münster, D. Brandstetter, X. Yang, J. Güdde, P. Puschnig, S. Soubatch, C. Kumpf, F.C. Bocquet, F.S. Tautz, U. Höfer
Tracing orbital images on ultrafast time scales
Science 371 (2021) 1056 DOI:10.1126/science.abf3286

 

Contact

Prof. Dr. Ulrich Höfer

Philipps-Universität Marburg

SFB 1083, project B6

Tel.: +49 6421 28-24215

ulrich.hoefer@physik.uni-marburg.de

                

Prof. Dr. Stefan Tautz

FZ Jülich

PGI, Experimental Physics, project A12

Tel.: +49 (0)2461 61-4561

s.tautz@fz-juelich.de