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Arne Morlok

Publications and source records attributed to Arne Morlok.

3 recordsLinked to original sources

Size characterization of neutral rare-gas clusters based on time-resolved polarization anisotropy measurements

The size determination of neutral clusters is experimentally challenging. In particular, weakly-bound rare-gas clusters tend to fragment upon ionization, resulting in systematic errors in cluster size studies. In contrast, characterization of the temporal polarization anisotropy dephasing provides a soft detection scheme for cluster size estimation, which avoids fragmentation of the clusters. Here, we present a systematic experimental study of argon and neon clusters in the size range of 50 to 10.000 atoms using this technique. In order to extract the mean cluster sizes from the data, we present an efficient analytical model of the polarization anisotropy dephasing of an ensemble of doped clusters. The approach shows remarkable sensitivity to small changes in the mean cluster size of just a few tens of atoms and allows us to refine the widely used Hagena scaling law for the estimation of rare-gas cluster sizes.

physics.atm-clus

Ultrafast configuration changes and anomalous diffusion of an aromatic adsorbate on rare-gas nanoparticles

Nanoparticles (NPs) exhibit tunable catalytic properties and serve as nanoreactors for controlled multimolecular chemistry. The kinetics and reactivity of such systems are critically governed by the surface binding configurations of adsorbates, their stochastic fluctuations, and the adsorbate mobility across the nanosurface. However, resolving these properties with sufficient structural, spatial, and temporal resolution remains a major experimental challenge. Here, we study phthalocyanine adsorbates on rare-gas clusters as a test case. By combining high-resolution two-dimensional electronic spectroscopy and molecular dynamics simulations, we reveal the configurational dynamics of the adsorbates and establish a direct relation between these dynamics and the nanoscale properties of the clusters. Our findings indicate sub-diffusive surface motion and trapping of the adsorbate within single surface facets. Such dynamical behavior seems unexpected considering the weak adsorbate-surface interaction and cluster temperatures close to the sublimation point. These results provide direct insight into the ultrafast binding dynamics of molecular adsorbates on nanoscale objects, which is critical for our understanding of the chemistry of such systems.

physics.chem-ph

Strong-field quantum control in the extreme ultraviolet using pulse shaping

Tailored light-matter interactions in the strong coupling regime enable the manipulation and control of quantum systems with up to unit efficiency, with applications ranging from quantum information to photochemistry. While strong light-matter interactions are readily induced at the valence electron level using long-wavelength radiation, comparable phenomena have been only recently observed with short wavelengths, accessing highly-excited multi-electron and inner-shell electron states. However, the quantum control of strong-field processes at short wavelengths has not been possible, so far, due to the lack of pulse shaping technologies in the extreme ultraviolet (XUV) and X-ray domain. Here, exploiting pulse shaping of the seeded free-electron laser (FEL) FERMI, we demonstrate the strong-field quantum control of ultrafast Rabi dynamics in helium atoms with high fidelity. Our approach unravels a strong dressing of the ionization continuum, otherwise elusive to experimental observables. The latter is exploited to achieve control of the total ionization rate, with prospective applications in many XUV and soft X-ray experiments. Leveraging recent advances in intense few-femtosecond to attosecond XUV to soft X-ray light sources, our results open an avenue to the efficient manipulation and selective control of core electron processes and electron correlation phenomena in real time.

physics.atom-ph