Ultrafast spectroscopy of single molecules

We present a single-molecule study on femtosecond dynamics in multichromophoric systems, combining fs pump-probe, emission-spectra and fluorescence-lifetime analysis. At the single molecule level a wide range of exciton delocalisation lengths and energy redistribution times is revealed. Next, two color pump-probe experiments are presented as a step to addressing ultrafast energy transfer in individual complexes

Nanoantenna-enhanced ultrafast nonlinear spectroscopy of a single gold nanoparticle

Optical nanoantennas are a novel tool to investigate previously unattainable dimensions in the nanocosmos. Just like their radio-frequency equivalents, nanoantennas enhance the light-matter interaction in their feed gap. Antenna enhancement of small signals promises to open a new regime in linear and nonlinear spectroscopy on the nanoscale. Without antennas especially the nonlinear spectroscopy of single nanoobjects is very demanding. Here, we present for the first time antenna-enhanced ultrafast nonlinear optical spectroscopy. In particular, we utilize the antenna to determine the nonlinear transient absorption signal of a single gold nanoparticle caused by mechanical breathing oscillations. We increase the signal amplitude by an order of magnitude which is in good agreement with our analytical and numerical models. Our method will find applications in linear and nonlinear spectroscopy of nanoobjects, ranging from single protein binding events via nonlinear tensor elements to the limits of continuum mechanics

molecular recognition at interfaces

In order to investigate molecular recognition on surfaces, an azide- functionalized monolayer was deposited on gold. The monolayer was characterized by X-ray photoelectron spectroscopy (XPS) and angle-resolved near-edge X-ray absorption fine structure (NEXAFS) experiments and the decomposition of the azide upon irradiation with X-ray beams was investigated. Subsequently, various alkyne-functionalized host and guest molecules were attached to the azide by 1,3-dipolar cycloaddition. These modified surfaces and their host–guest chemistry were analysed by XPS and angle-resolved NEXAFS. The reversibility of guest binding was shown for one example as a proof of principle

Full counting statistics of quantum dot resonance fluorescence

The electronic energy levels and optical transitions of a semiconductor quantum dot are subject to dynamics within the solid-state environment. In particular, fluctuating electric fields due to nearby charge traps or other quantum dots shift the transition frequencies via the Stark effect. The environment dynamics are mapped directly onto the fluorescence under resonant excitation and diminish the prospects of quantum dots as sources of indistinguishable photons in optical quantum computing. Here, we present an analysis of resonance fluorescence fluctuations based on photon counting statistics which captures the underlying time-averaged electric field fluctuations of the local environment. The measurement protocol avoids dynamic feedback on the electric environment and the dynamics of the quantum dot's nuclear spin bath by virtue of its resonant nature and by keeping experimental control parameters such as excitation frequency and external fields constant throughout. The method introduced here is experimentally undemanding

Coupling a single solid-state quantum emitter to an array of resonant plasmonic antennas

Plasmon resonant arrays or meta-surfaces shape both the incoming optical field and the local density of states for emission processes. They provide large regions of enhanced emission from emitters and greater design flexibility than single nanoantennas. This makes them of great interest for engineering optical absorption and emission. Here we study the coupling of a single quantum emitter, a self-assembled semiconductor quantum dot, to a plasmonic meta-surface. We investigate the influence of the spectral properties of the nanoantennas and the position of the emitter in the unit cell of the structure. We observe a resonant enhancement due to emitter-array coupling in the far-field regime and find a clear difference from the interaction of an emitter with a single antenna

Ultrafast time-resolved spectroscopy of 1D metal-dielectric photonic crystals

We study the all-optical switching behavior of one-dimensional metal-dielectric photonic crystals due to the nonlinearity of the free metal electrons. A polychromatic pump-probe setup is used to determine the wavelength and pump intensity dependence of the ultrafast transmission suppression as well as the dynamics of the process on a subpicosecond timescale. We find ultrafast (sub-picosecond) as well as a slow (millisecond) behavior. We present a model of the ultrafast dynamics and nonlinear response which can fit the measured data well and allows us to separate the thermal and the electronic response of the system.Comment: 7 pages, 5 figure