Ultrafast generation and decay of a surface metal.

Band bending at semiconductor surfaces induced by chemical doping or electric fields can create metallic surfaces with properties not found in the bulk, such as high electron mobility, magnetism or superconductivity. Optical generation of such metallic surfaces on ultrafast timescales would be appealing for high-speed electronics. Here, we demonstrate the ultrafast generation of a metal at the (10-10) surface of ZnO upon photoexcitation. Compared to hitherto known ultrafast photoinduced semiconductor-to-metal transitions that occur in the bulk of inorganic semiconductors, the metallization of the ZnO surface is launched by 3-4 orders of magnitude lower photon fluxes. Using time- and angle-resolved photoelectron spectroscopy, we show that the phase transition is caused by photoinduced downward surface band bending due to photodepletion of donor-type deep surface defects. The discovered mechanism is in analogy to chemical doping of semiconductor surfaces and presents a general route for controlling surface-confined metallicity on ultrafast timescales.

Uncovering the (un-)occupied electronic structure of a buried hybrid interface.

The energy level alignment at organic/inorganic (o/i) semiconductor interfaces is crucial for any light-emitting or -harvesting functionality. Essential is the access to both occupied and unoccupied electronic states directly at the interface, which is often deeply buried underneath thick organic films and challenging to characterize. We use several complementary experimental techniques to determine the electronic structure of p -quinquephenyl pyridine (5P-Py) adsorbed on ZnO(1 0 -1 0). The parent anchoring group, pyridine, significantly lowers the work function by up to 2.9 eV and causes an occupied in-gap state (IGS) directly below the Fermi level E F. Adsorption of upright-standing 5P-Py also leads to a strong work function reduction of up to 2.1 eV and to a similar IGS. The latter is then used as an initial state for the transient population of three normally unoccupied molecular levels through optical excitation and, due to its localization right at the o/i interface, provides interfacial sensitivity, even for thick 5P-Py films. We observe two final states above the vacuum level and one bound state at around 2 eV above E F, which we attribute to the 5P-Py LUMO. By the separate study of anchoring group and organic dye combined with the exploitation of the occupied IGS for selective interfacial photoexcitation, this work provides a new pathway for characterizing the electronic structure at buried o/i interfaces.

Laser induced magnetization switching in a TbFeCo ferrimagnetic thin film: discerning the impact of dipolar fields, laser heating and laser helicity by XPEEM.

We investigate laser induced magnetic switching in a ferrimagnetic thin film of Tb22Fe69Co9 by PEEM. Using a small laser beam with a spot size of 3-5 µm in diameter in combination with high resolution magnetic soft X-ray microscopy we are able to discriminate between different effects that govern the microscopic switching process, namely the influence of the laser heating, of the helicity dependent momentum transfer, and of the dipolar coupling. Applying a sequence of femtosecond laser pulses to a previously saturated TbFeCo film leads to the formation of ring shaped magnetic structures in which all three effects can be observed. Laser helicity assisted switching is only observed in a narrow region within the Gaussian profile of the laser spot. Whereas in the center of the laser spot we find clear evidence for thermal demagnetization and in the outermost areas magnetic switching is determined by dipolar coupling with the surrounding film. Our findings demonstrate that by reducing the laser spot size the influence of dipolar coupling on laser induced switching is becoming increasingly important.

A sample holder with integrated laser optics for an ELMITEC photoemission electron microscope.

We present a new sample holder compatible with ELMITEC Photoemission Electron Microscopes (PEEMs) containing an optical lens and a mirror. With the integrated optical elements, a laser beam is focused from the back side of the sample at normal incidence, yielding a minimum spot size of about 1 µm. This opens up new possibilities for local laser excitations in PEEM experiments such as imaging all-optical magnetization switching at a small length scale.