2D and 3D optical nanoscopy of single molecules at cryogenic temperatures

Abstract : In this thesis, we present the development of a cryogenic super-resolution optical nanoscopy thatcan resolve molecules at nanometric distances, called the Excited State Saturation (ESSat)Microscopy.ESSat microscopy is a scanning confocal imaging technique based on the optical saturation of thezero phonon line of a single fluorescent molecule. It uses a patterned illumination beam thatcontains a ‘zero-intensity’ region at the focus of the microscope objective with a large intensitygradient around. We achieved a sub-10 nm resolution in the lateral direction and 22 nm resolutionin the axial direction with extremely low excitation intensities of few tens of kWcm-2. Comparedto other super-resolution imaging techniques, like STED, RESOLFT, etc., our technique offers aunique opportunity to super-resolve single molecules with overlapping optical resonances and thatare much closer than the diffraction limit. In addition, it is possible to determine the orientation ofmolecular dipoles from the fluorescent ESSat images. Since coherent dipole-dipole couplinginteractions between single quantum emitters have a very high coupling efficiency at short distancemuch smaller than the diffraction limit, it is important to resolve them well below it. ESSatmicroscopy thus paves a way to disclose the rich spatial and frequential signatures of the coupledsystem and to manipulate their degree of entanglement.
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Reenu Baby. 2D and 3D optical nanoscopy of single molecules at cryogenic temperatures. Optics [physics.optics]. Université de Bordeaux, 2018. English. ⟨NNT : 2018BORD0119⟩. ⟨tel-01897735⟩

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