Spectroscopy of 3, 4, 9, 10-perylenetetracarboxylic dianhydride (PTCDA) attached to rare gas samples: clusters vs. bulk matrices. I. Absorption spectroscopy.

The interaction between 3, 4, 9, 10-perylenetetracarboxylic dianhydride (PTCDA) and rare gas or para-hydrogen samples is studied by means of laser-induced fluorescence excitation spectroscopy. The comparison between spectra of PTCDA embedded in a neon matrix and spectra attached to large neon clusters shows that these large organic molecules reside on the surface of the clusters when doped by the pick-up technique. PTCDA molecules can adopt different conformations when attached to argon, neon, and para-hydrogen clusters which implies that the surface of such clusters has a well-defined structure without liquid or fluxional properties. Moreover, a precise analysis of the doping process of these clusters reveals that the mobility of large molecules on the cluster surface is quenched, preventing agglomeration and complex formation.

Spectroscopy of 3, 4, 9, 10-perylenetetracarboxylic dianhydride (PTCDA) attached to rare gas samples: clusters vs. bulk matrices. II. Fluorescence emission spectroscopy.

The interaction between 3, 4, 9, 10-perylenetetracarboxylic dianhydride (PTCDA) molecules and solid rare gas samples is studied by means of fluorescence emission spectroscopy. Laser-excited PTCDA-doped large argon, neon, and para-hydrogen clusters along with PTCDA embedded in helium nanodroplets are spectroscopically characterized with respect to line broadening and shifting. A fast non-radiative relaxation is observed before a radiative decay in the electronic ground state takes place. In comparison, fluorescence emission studies of PTCDA embedded in bulk neon and argon matrices result in much more complex spectral signatures characterized by a splitting of the different emission lines. These can be assigned to the appearance of site isomers of the surrounding matrix lattice structure.

Exciton-Exciton Interaction and Optical Gain in Colloidal CdSe/CdS Dot/Rod Nanocrystals.

Exciton-exciton interaction in dot/rod CdSe/CdS nanocrystals has proved to be very sensitive to the shape of nanocrystals, due to the unique band alignment between CdSe and CdS. Repulsive exciton-exciton interaction is demonstrated, which makes CdSe/CdS dot/rods promising gain media for solution-processable lasers, with projected pump threshold densities below 1 kW cm(-2) for continuous wave lasing.

Silicon microcavity arrays with open access and a finesse of half a million.

Optical resonators are essential for fundamental science, applications in sensing and metrology, particle cooling, and quantum information processing. Cavities can significantly enhance interactions between light and matter. For many applications they perform this task best if the mode confinement is tight and the photon lifetime is long. Free access to the mode center is important in the design to admit atoms, molecules, nanoparticles, or solids into the light field. Here, we demonstrate how to machine microcavity arrays of extremely high quality in pristine silicon. Etched to an almost perfect parabolic shape with a surface roughness on the level of 2 Å and coated to a finesse exceeding F = 500,000, these new devices can have lengths below 17 µm, confining the photons to 5 µm waists in a mode volume of 88λ3. Extending the cavity length to 150 µm, on the order of the radius of curvature, in a symmetric mirror configuration yields a waist smaller than 7 µm, with photon lifetimes exceeding 64 ns. Parallelized cleanroom fabrication delivers an entire microcavity array in a single process. Photolithographic precision furthermore yields alignment structures that result in mechanically robust, pre-aligned, symmetric microcavity arrays, representing a light-matter interface with unprecedented performance.