A versatile tunable microcavity for investigation of light-matter interaction.

Light-matter interaction between a molecular ensemble and a confined electromagnetic field is a promising area of research, as it allows light-control of the properties of coupled matter. The common way to achieve coupling is to place an ensemble of molecules or quantum emitters into a cavity. In this approach, light-matter coupling is evidenced by modification of the spectral response of the emitter, which depends on the strength of interaction between emitter and cavity modes. However, there is not yet a user-friendly approach that allows the study of a large number of different and replaceable samples in a wide optical range using the same resonator. Here, we present the design of such a device that can speed up and facilitate investigation of light-matter interaction ranging from weak to strong coupling regimes in ultraviolet-visible and infrared (IR) spectral regions. The device is based on a tunable unstable λ/2 Fabry-Pérot microcavity consisting of plane and convex mirrors that satisfy the plane-parallelism condition at least at one point of the curved mirror and minimize the mode volume. Fine tuning of the microcavity length is provided by a Z-piezopositioner in a range up to 10 µm with a step of several nm. This design makes a device a versatile instrument that ensures easy finding of optimal conditions for light-matter interaction for almost any sample in both visible and IR areas, enabling observation of both electronic and vibrational couplings with microcavity modes thus paving the way to investigation of various coupling effects including Raman scattering enhancement, modification of chemical reactivity rate, lasing, and long-distance nonradiative energy transfer.

An instrumental approach to combining confocal microspectroscopy and 3D scanning probe nanotomography.

In the past decade correlative microscopy, which combines the potentials of different types of high-resolution microscopies with a variety of optical microspectroscopy techniques, has been attracting increasing attention in material science and biological research. One of outstanding solutions in this area is the combination of scanning probe microscopy (SPM), which provides data on not only the topography, but also the spatial distribution of a wide range of physical properties (elasticity, conductivity, etc.), with ultramicrotomy, allowing 3D multiparametric examination of materials. The combination of SPM and ultramicrotomy (scanning probe nanotomography) is very appropriate for characterization of soft multicompound nanostructurized materials, such as polymer matrices and microstructures doped with different types of nanoparticles (magnetic nanoparticles, quantum dots, nanotubes, etc.), and biological materials. A serious problem of this technique is a lack of chemical and optical characterization tools, which may be solved by using optical microspectroscopy. Here, we report the development of an instrumental approach to combining confocal microspectroscopy and 3D scanning probe nanotomography in a single apparatus. This approach retains all the advantages of SPM and upright optical microspectroscopy and allows 3D multiparametric characterization using both techniques. As the first test of the system developed, we have performed correlative characterization of the morphology and the magnetic and fluorescent properties of fluorescent magnetic microspheres doped with a fluorescent dye and magnetic nanoparticles. The results of this study can be used to obtain 3D volume images of a specimen for most high-resolution near-field scanning probe microscopies: SNOM, TERS, AFM-IR, etc. This approach will result in development of unique techniques combining the advantages of SPM (nanoscale morphology and a wide range of physical parameters) and high-resolution optical microspectroscopy (nanoscale chemical mapping and optical properties) and allowing simultaneous 3D measurements.

A novel design of a scanning probe microscope integrated with an ultramicrotome for serial block-face nanotomography.

We present a new concept of a combined scanning probe microscope (SPM)/ultramicrotome apparatus. It enables "slice-and-view" scanning probe nanotomography measurements and 3D reconstruction of the bulk sample nanostructure from series of SPM images after consecutive ultrathin sections. The sample is fixed on a flat XYZ scanning piezostage mounted on the ultramicrotome arm. The SPM measuring head with a cantilever tip and a laser-photodiode tip detection system approaches the sample for SPM measurements of the block-face surface immediately after the ultramicrotome sectioning is performed. The SPM head is moved along guides that are also fixed on the ultramicrotome arm. Thereby, relative dysfunctional displacements of the tip, the sample, and the ultramicrotome knife are minimized. The design of the SPM head enables open frontal optical access to the sample block-face adapted for high-resolution optical lenses for correlative SPM/optical microscopy applications. The new system can be used in a wide range of applications for the study of 3D nanostructures of biological objects, biomaterials, polymer nanocomposites, and nanohybrid materials in various SPM and optical microscopy measuring modes.

Combined scanning probe nanotomography and optical microspectroscopy: a correlative technique for 3D characterization of nanomaterials.

Combination of 3D structural analysis with optical characterization of the same sample area on the nanoscale is a highly demanded approach in nanophotonics, materials science, and quality control of nanomaterial. We have developed a correlative microscopy technique where the 3D structure of the sample is reconstructed on the nanoscale by means of a "slice-and-view" combination of ultramicrotomy and scanning probe microscopy (scanning probe nanotomography, SPNT), and its optical characteristics are analyzed using microspectroscopy. This approach has been used to determine the direct quantitative relationship of the 3D structural characteristics of nanovolumes of materials with their microscopic optical properties. This technique has been applied to 3D structural and optical characterization of a hybrid material consisting of cholesteric liquid crystals doped with fluorescent quantum dots (QDs) that can be used for photochemical patterning and image recording through the changes in the dissymmetry factor of the circular polarization of QD emission. The differences in the polarization images and fluorescent spectra of this hybrid material have proved to be correlated with the arrangement of the areas of homogeneous distribution and heterogeneous clustering of QDs. The reconstruction of the 3D nanostructure of the liquid crystal matrix in the areas of homogeneous QDs distribution has shown that QDs do not perturb the periodic planar texture of the cholesteric liquid crystal matrix, whereas QD clusters do perturb it. The combined microspectroscopy-nanotomography technique will be important for evaluating the effects of nanoparticles on the structural organization of organic and liquid crystal matrices and biomedical materials, as well as quality control of nanotechnology fabrication processes and products.