Multifunctional far-field luminescence nanoscope for studying single molecules and quantum dots: (50th anniversary of the Institute of Spectroscopy, Russian Academy of Sciences)

Abstract

Far-field fluorescence spectromicroscopy of single quantum emitters (SQEs) (single molecules, quantum dots, color centers in crystals) is an actively developing field of modern photonics, which is in widespread demand in various applications in physics, chemistry, material sciences, life sciences, and quantum technologies. In this paper, we present a description of a multifunctional experimental setup which was developed in recent years at the Institute for Spectroscopy of the Russian Academy of Sciences. It allows measuring optical spectra and fluorescence images of SQEs, as well as their temporal behavior and luminescence kinetics, in a broad range of temperatures (from cryogenic to ambient). It is shown that the spatial coordinates of SQEs can be reconstructed with subdiffractional accuracy (up to a few angstroms). Some examples of the developed methods for multiparameter superresolution microscopy (nanoscopy) of materials and nanostructures are presented.

Microscopic Insight into the Inhomogeneous Broadening of Zero-Phonon Lines of GeV– Color Centers in Chemical Vapor Deposition Diamond Films Synthesized from Gaseous Germane

“…In the first setup, 67 photoluminescence excitation (PLE) spectra were measured in the range 598 to 604 nm (excitation of the ZPLs) with ∼10 GHz spectral resolution and ∼0.5 μm spatial resolution in a broad range of temperatures (4.5−77 K). It was equipped with a continuously tunable dye laser Coherent CR599 (560−630 nm), a temperature-regulated He-4 cryostat (RTI), a microscope objective Melles Griot (40x, 0.65 NA), and an EMCCD camera Andor Ixon Ultra.…”

A quantitative model of multi-scale single quantum dot blinking

“…We performed a set of time-correlated photon counting experiments following the Hanbury Brown and Twiss scheme with single CdSeS/ZnS core/shell QDs at room temperature. 49 Each experiment had a duration of around 780 seconds. The accumulated single photon counting data were used to find the binned intensity trace, photon distribution function (PDF), fluorescence lifetime–intensity distribution (FLID) and PL intensity auto-correlation function (ACF) estimator.…”

Cryogenic Correlative Single‐Particle Photoluminescence Spectroscopy and Electron Tomography for Investigation of Nanomaterials

“…Quite to the contrary, the numerous brightness levels, excitation dipoles, and emission bands observed in the PL would naively indicate a complex cluster of QDs rather than an isolated dot. Often to determine if emission comes from a single emitter, photon antibunching or the g (2) function is measured . However, this requires photon arrival time information that is not easily collected in a wide field imaging setup.…”

“…Often to determine if emission comes from as ingle emitter, photon antibunching or the g (2) function is measured. [46] However,t his requires photon arrival time information that is not easily collected in awide field imaging setup.Here,itis only with the correlative tomography data that we are able to definitively assign these dynamics to individual QDs.T his correlation also permits the interpretation of the PL data within the context of the three-dimensional structure provided by cryo-ET.F igure 4a nd Supplementary Video S2 show the overlay of several recovered in-plane excitation dipoles with their corresponding three-dimensional cryo-ET reconstructions.…”