arXiv subjects

Marcel Reutzel

Publications and source records attributed to Marcel Reutzel.

25 records · Page 2Linked to original sources

arXiv2021

Plasmonically assisted channels of photoemission from metals

We analyse recently measured nonlinear photoemission spectra from Ag surfaces that reveal resonances whose energies do not scale with the applied photon energy but stay pinned to multiples of bulk plasmon energy $\hbarω_p$ above the Fermi level. To elucidate these unexpected and peculiar features we investigate the spectra of plasmons generated in a solid by the optically pumped electronic polarization and their effect on photoemission. By combining quadratic response formalism for calculations of photoemission yield, a nonperturbative approach to inelastic electron scattering, and first-principles calculations for the electronic structure, we demonstrate the dependence of probability amplitude for single- and multiplasmon excitations on the basic parameters characterizing the photon pulse and the system. The resulting multiexcitation spectrum evolves towards a truncated plasmonic coherent state. Analogous concept is extrapolated to interpret plasmon generation by multiphoton excited electronic polarization. Based on this we elaborate a scenario that the thus created real plasmons act as supplementary frequency-locked pump field for non-Einsteinian plasmonically assisted channels of photoemission from metals. The established paradigm enables assignment and assessment of the observed linear $\hbarω_p$- and nonlinear $2\hbarω_p$-electron yields from Ag. Such effects may be exploited for selective filtering of optical energy conversion in electronic systems.

cond-mat.mtrl-sci↗

arXiv2020

Direct Access to Auger recombination in Graphene

Auger scattering channels are of fundamental importance to describe and understand the non-equilibrium charge carrier dynamics in graphene. While impact excitation increases the number of carriers in the conduction band and has been observed experimentally, direct access to its inverse process, Auger recombination, has so far been elusive. Here, we tackle this problem by applying our novel setup for ultrafast time-resolved photoelectron momentum microscopy. Our approach gives simultaneous access to charge carrier dynamics at all energies and in-plane momenta within the linearly dispersive Dirac cones. We thus provide direct evidence for Auger recombination on a sub-10~fs timescale by identifying transient energy- and momentum-dependent populations far above the excitation energy. We compare our results with model calculations of scattering processes in the Dirac cone to support our experimental findings.

cond-mat.other↗

arXiv2020

Electromagnetic dressing of the electron energy spectrum of Au(111) at high momenta

Light-engineering of quantum materials via electromagnetic dressing is considered an on-demand approach for tailoring electronic band dispersions and even inducing topological phase transitions. For probing such dressed bands, photoemission spectroscopy is an ideal tool, and we employ here a novel experiment based on ultrafast photoemission momentum microscopy. Using this setup, we measure the in-plane momentum-dependent intensity fingerprints of the electromagnetically-dressed sidebands from a Au(111) surface for s- and p-polarized infrared driving. We find that at metal surfaces, due to screening of the driving laser, the contribution from Floquet-Bloch bands is negligible, and the dressed bands are dominated by the laser-assisted photoelectric effect. Also, we find that in contrast to general expectations, s-polarized light can dress free-electron states at large photoelectron momenta. Our results show that the dielectric response of the material must carefully be taken into account when using photoemission for the identification of light-engineered electronic band structures.

cond-mat.mes-hall↗

arXiv2020

Towards full surface Brillouin zone mapping by coherent multi-photon photoemission

We report a novel approach for coherent multi-photon photoemission band mapping of the entire Brillouin zone with infrared light that is readily implemented in a laboratory setting. We excite a solid state material, Ag(110), with intense femtosecond laser pulses to excite higher-order multi-photon photoemission; angle-resolved electron spectroscopic acquisition records photoemission at large in-plane momenta involving optical transitions from the occupied to unoccupied bands of the sample that otherwise might remain hidden by the photoemission horizon. We propose this as a complementary ultrafast method to time- and angle-resolved two-color, e.g. infrared pump and extreme ultraviolet probe, photoemission spectroscopy, with the advantage of being able to measure and control the coherent electron dynamics.

cond-mat.other↗

arXiv2018

Excitation of two-photon photoemission where epsilon is near zero on Ag(111)

Because silver has epsilon-near-zero (ENZ) in the near-UV spectral region, its optical response is expected to be dominantly plasmonic and nonperturbatively nonlinear. The ENZ properties of Ag have made it the material of choice for investigation of plasmonic optical effects in physics, chemistry, optics, and nanotechnology. We investigate the nonlinear angle-resolved two-photon photoemission (2PP) spectroscopy of Ag(111) surface in the ENZ region. In addition to the well-understood and documented spectroscopic features of Einsteinian photoemission involving dipole excitations of the single-particle occupied and unoccupied surface states, 2PP spectra possess other distinct features where the optical fields excite or are modified by the collective virtual and real plasmon excitations.

cond-mat.mes-hall↗

arXiv2018

Coherent two-dimensional multiphoton photoelectron spectroscopy of metal surfaces

Light interacting with metals elicits an ultrafast coherent many-body screening response on sub- to few-femtosecond time-scales, which makes its experimental observation challenging. Here, we describe the coherent two-dimensional (2D) multi-photon photoemission study of the Shockley surface state (SS) of Ag(111) as a benchmark for spectroscopy of the coherent nonlinear response of metals to an optical field in the perturbative regime. Employing interferometrically time-resolved multi-photon photoemission spectroscopy (ITR-mPP), we correlate the coherent polarizations and populations excited in the sample with final photoelectron distributions where the interaction terminates. By measuring the non-resonant 3- and 4-photon photoemission of the SS state, as well as its replica structures in the above-threshold photoemission (ATP), we record the coherent response of the Ag(111) surface by 2D photoemission spectroscopy and relate it to its band structure. We interpret the mPP process by an optical Bloch equation (OBE) model, which reproduces the main features of the surface state coherent polarization dynamics recorded in ITR-mPP experiments: The spectroscopic components of the 2D photoelectron spectra are shown to depend on the nonlinear orders of the coherent photoemission process m as well as on the induced coherence n.

physics.optics↗

arXiv2016

Chemoselective Reactivity of Bifunctional Cyclooctynes on Si(001)

Controlled organic functionalization of silicon surfaces as integral part of semiconductor technology offers new perspectives for a wide range of applications. The high reactivity of the silicon dangling bonds, however, presents a major hindrance for the first basic reaction step of such a functionalization, i.e., the chemoselective attachment of bifunctional organic molecules on the pristine silicon surface. We overcome this problem by employing cyclooctyne as the major building block of our strategy. Functionalized cyclooctynes are shown to react on Si(001) selectively via the strained cyclooctyne triple bond while leaving the side groups intact. The achieved selectivity originates from the distinctly different adsorption dynamics of the separate functionalities: A direct adsorption pathway is demonstrated for cyclooctyne as opposed to the vast majority of other organic functional groups. The latter ones react on Si(001) via a metastable intermediate which makes them effectively unreactive in competition with the direct pathway of cyclooctyne's strained triple bond.

physics.chem-ph↗