Publications Nano-Optics Division

Nanotechnology, with its broad impact on societally relevant applications, relies heavily on the availability of accessible nanofabrication methods. Even though a host of such techniques exists, the flexible, inexpensive, on-demand and scalable fabrication of functional nanostructures remains largely elusive. Here we present a method involving nanoscale electrohydrodynamic ink-jet printing that may significantly contribute in this direction. A combination of nanoscopic placement precision, soft-landing fluid dynamics, rapid solvent vapourization, and subsequent self-assembly of the ink colloidal content leads to the formation of scaffolds with base diameters equal to that of a single ejected nanodroplet. The virtually material-independent growth of nanostructures into the third dimension is then governed by an autofocussing phenomenon caused by local electrostatic field enhancement, resulting in large aspect ratio. We demonstrate the capabilities of our electrohydrodynamic printing technique with several examples, including the fabrication of plasmonic nanoantennas with features sizes down to 50 nm.

We have investigated the behaviour of inverted poly(3-hexylthiophene) : [6,6]-phenyl-C-61-butyric acid methyl ester (P3HT : PCBM) solar cells with different active layer thickness upon changing light intensity. Using white-light bias external quantum efficiency (EQE) measurements and photocurrent transient measurements we explain the different thickness dependence of device performance of inverted (ITO/ZnO/P3HT : PCBM/WO3/Ag) and standard (ITO/PEDOT : PSS/P3HT : PCBM/Ca/Al) cells. Whereas for inverted devices where high EQEs of up to 68% are measured under low light intensities (similar to 3.5 mW cm(-2)), a dramatic reduction in EQE is observed with increasing white-light bias (up to similar to 141.5 mW cm(-2)) accompanied by a severe distortion of the EQE spectrum. For the inverted device this spectral distortion is characterized by a dip in the EQE spectrum for wavelengths corresponding to maximum light absorption and becomes more prominent with increasing active layer thickness. For regular P3HT : PCBM devices, in contrast, a less dramatic reduction in EQE with increasing light intensity and only a mild change in EQE spectral shape are observed. The change in EQE spectral shape is also different for standard devices with a relative reduction in EQE for spectral regions where light is absorbed less strongly. This asymmetry in device behaviour is attributed to unbalanced charge transport with the lower mobility carrier having to travel further on average in the inverted device structure. Thus at high light intensities charge recombination is more pronounced at the front half of the device (close to the transparent electrode) for inverted cells where most of the light is absorbed, and more pronounced at the back half of the device for standard cells. Our results therefore indicate that bulk charge transport mobilities rather than vertical composition gradients are the dominant factor in determining the performance of standard and inverted P3HT : PCBM cells.

We report on two orders of magnitude reduction in the fluorescence lifetime when a single molecule placed in a thin film is surrounded by two gold nanospheres across the film interface. By attaching one of the gold particles to the end of a glass fiber tip, we could control the modification of the molecular fluorescence at will. We find a good agreement between our experimental data and the outcome of numerical calculations. (C) 2012 Optical Society of America

We devise new optical antennas that reduce the excited-state radiative lifetimes of emitters to the order of 100 fs while maintaining quantum efficiencies of about 80% at a broadband operation. Here, we combine metallic nanoparticles with planar dielectric structures and exploit design strategies from plasmonic nanoantennas and concepts from cavity quantum electrodynamics to maximize the local density of states and minimize the nonradiative losses incurred by the metallic constituents. The proposed metallodielectric hybrid antennas promise an important impact on various fundamental and applied research fields, including photophysics, ultrafast plasmonics, bright single-photon sources, and Raman spectroscopy.

Efficient interaction of light and matter at the ultimate limit of single photons and single emitters is of great interest from a fundamental point of view and for emerging applications in quantum engineering. However, the difficulty of generating single-photon streams with specific wavelengths, bandwidths, and power as well as the weak interaction probability of a single photon with an optical emitter pose a formidable challenge toward this goal. Here, we demonstrate a general approach based on the creation of single photons from a single emitter and their use for performing spectroscopy on a second emitter situated at a distance. While this first proof of principle realization uses organic molecules as emitters, the scheme is readily extendable to quantum dots and color centers. Our work ushers in a new line of experiments that provide access to the coherent and nonlinear couplings of few emitters and few propagating photons.