Coherent two-dimensional fluorescence micro-spectroscopy

We have developed coherent two-dimensional (2D) fluorescence micro-spectroscopy which probes the nonlinear optical response at surfaces via fluorescence detection with sub-micron spatial resolution. This enables the investigation of microscopic variations in heterogeneous systems. An LCD-based pulse shaper in 4 f geometry is used to create collinear trains of 12-fs visible/NIR laser pulses in the focus of an NA = 1.4 immersion-oil microscope objective. We demonstrate the capabilities of the new method by presenting 2D spectra, analyzed via phase cycling, as a function of position of selected sub-micron regions from a laterally nanostructured polycrystalline thin film of fluorinated zinc phthalocyanine (F16ZnPc). (c) 2018 Optical Society of America under the terms of the OSA Open Access Publishing Agreement.