RESUMO
A strong increase of spontaneous radiative emission from colloidally synthesized CdSe/CdS/PMMA hybrid particles is achieved when manipulated into plasmonic bullseye resonators with the tip of an atomic force microscope (AFM). This type of antenna provides a broadband resonance, which may be precisely matched to the exciton ground state energy in the inorganic cores. Statistically analyzing the spectral photoluminescence (PL) of a large number of individual coupled and uncoupled CdSe/CdS/PMMA quantum dots, we find an order of magnitude of intensity enhancement due to the Purcell effect. Time-resolved PL shows a commensurate increase of the spontaneous emission rate with radiative lifetimes below 230 ps for the bright exciton transition. The combination of AFM and PL imaging allows for sub-200 nm localization of the particle position inside the plasmonic antenna. This capability unveils a different coupling behavior of dark excitonic states: even stronger PL enhancement occurs at positions with maximum spatial gradient of the nearfield, effectively adding a dipolar component to original quadrupole transitions. The broadband maximization of light-matter interaction provided by our nanoengineered compound systems enables an attractive class of future experiments in ultrafast quantum optics.
RESUMO
We use an arbitrary waveform generator to generate a clean sinusoidal modulation from the otherwise nonlinear acousto-optic modulator (AOM). A closed loop optimization script is applied to reduce high order harmonic distortion to less than 0.05% in a high AOM diffraction efficiency regime. This low level of distortion allows us to measure the nonlinear response to photoexcitation of many materials. We demonstrate this technique in a pump-probe experiment to measure the Nonlinear Photo-Modulated Reflectivity (NPMR) of surfaces. NPMR served us as the basis for developing super-resolution microscopy for non-fluorescence samples (label-free) as well as a tool in studying the ultrafast nonlinear response of photo-excited plasmonic nano-structures. Our methodology could be applied to other imaging systems in which measuring nonlinearity is desirable, such as fluorescence and photoacoustic microscopy.
RESUMO
The recent advances in far-field super-resolution (SR) microscopy rely on, and therefore are limited by the ability to control the fluorescence of label molecules. We demonstrated a far field label-free SR methodology that relies on the nonlinear response of the reflectance to photo-modulation by a pump laser. Here we extend our approach in two directions. We show that the method can be further simplified and improved by using a single beam rather than a pump and probe or by adding spatial probe modulation to improve resolution. Additionally, we demonstrate SR in sectioning and further investigate the dynamics of non-linearity in photo-modulated reflectance. These new modalities of nonlinear photo-modulated reflectivity (NPMR) enhance its applicability using lower orders of nonlinear response.
