Polarization-sensitive pulse reconstruction by momentum-resolved photoelectron streaking.

The precise knowledge of the electric field in close proximity to metallic and dielectric surfaces is a prerequisite for pump-probe experiments aiming at the control of dynamic surface processes. We describe a model to reconstruct this electric field in immediate surface proximity from data taken in photoelectron THz-streaking experiments with an angle-resolved electron analyzer. Using Monte-Carlo simulations we are able to simulate streaking experiments on arbitrary surfaces with a variety of initial electron momentum distributions and to reconstruct the effective electric field at the surface. Our results validate the approach and suggest energy regimes for optimal pulse reconstruction.

Perspective: Opportunities for ultrafast science at SwissFEL.

We present the main specifications of the newly constructed Swiss Free Electron Laser, SwissFEL, and explore its potential impact on ultrafast science. In light of recent achievements at current X-ray free electron lasers, we discuss the potential territory for new scientific breakthroughs offered by SwissFEL in Chemistry, Biology, and Materials Science, as well as nonlinear X-ray science.

Detecting and utilizing minority phases in heterogeneous catalysis.

Highly active phases in carbon monoxide oxidation are known, however they are transient in nature. Here, we determined for the first time the structure of such a highly active phase on platinum nanoparticles in an actual reactor. Unlike generally assumed, the surface of this phase is virtually free of adsorbates and co-exists with carbon-monoxide covered and surface oxidized platinum. Understanding the relation between gas composition and catalyst structure at all times and locations within a reactor enabled the rational design of a reactor concept, which maximizes the amount of the highly active phase and minimizes the amount of platinum needed.

Coupling of Excitons and Discrete Acoustic Phonons in Vibrationally Isolated Quantum Emitters.

The photoluminescence emission by mesoscopic condensed matter is ultimately dictated by the fine-structure splitting of the fundamental exciton into optically allowed and dipole-forbidden states. In epitaxially grown semiconductor quantum dots, nonradiative equilibration between the fine-structure levels is mediated by bulk acoustic phonons, resulting in asymmetric spectral broadening of the excitonic luminescence. In isolated colloidal quantum dots, spatial confinement of the vibrational motion is expected to give rise to an interplay between the quantized electronic and phononic degrees of freedom. In most cases, however, zero-dimensional colloidal nanocrystals are strongly coupled to the substrate such that the charge relaxation processes are still effectively governed by the bulk properties. Here we show that encapsulation of single colloidal CdSe/CdS nanocrystals into individual organic polymer shells allows for systematic vibrational decoupling of the semiconductor nanospheres from the surroundings. In contrast to epitaxially grown quantum dots, simultaneous quantization of both electronic and vibrational degrees of freedom results in a series of strong and narrow acoustic phonon sidebands observed in the photoluminescence. Furthermore, an individual analysis of more than 200 compound particles reveals that enhancement or suppression of the radiative properties of the fundamental exciton is controlled by the interaction between fine-structure states via the discrete vibrational modes. For the first time, pronounced resonances in the scattering rate between the fine-structure states are directly observed, in good agreement with a quantum mechanical model. The unambiguous assignment of mediating acoustic modes to the observed scattering resonances complements the experimental findings. Thus, our results form an attractive basis for future studies on subterahertz quantum opto-mechanics and efficient laser cooling at the nanoscale.

Stable single-photon emission by quantum dot/polymer hybrid particles.

Colloidal quantum dots are well-established probes for quantum optical experiments. However, they possess a limited stability toward their environment. Herein, the generation of hybrid particles composed of a high optical quality quantum dot centered in a polymer particle by means of a miniemulsion polymerization procedure is reported. This embedding strongly enhances emission intensity and photochemical stability of these single-photon emitters. At the same time, their colloidal mobile nature is not compromised.

Polyfluorene Nanoparticles and Quantum Dot Hybrids via Miniemulsion Polymerization.

Suzuki-Miyaura polycondensation of 2-(4,4,5,5-tetramethyl-1,3,2-dioxaborolan-2-yl)-7-bromo-9,9-dioctylfluorene in aqueous miniemulsion with only two equivalents of NaOH as a base yields colloidally stable nanoparticles of polyfluorene with Mn ca. 2 × 104 g mol-1 and particle sizes of 40-85 nm, depending on the surfactant concentration. Polymerization in the presence of CdSe/CdS core/shell quantum dots affords hybrid nanoparticles of nonaggregated quantum dots, in particular nanoparticles composed of a single quantum dot embedded in a polyfluorene shell. Microphotoluminescence spectroscopy on single hybrid particles reveals an enhanced photostability of the quantum dots and indicates an efficient Förster energy transfer from the polyfluorene shell to the quantum dot.