Light-matter coupling between the molecular dipole transitions and a confined electromagnetic field provides the ability to control the fundamental properties of coupled matter. The use of tunable optical microcavities for electromagnetic field confinement allows one to affect the coupled state properties in a controllable manner, whereas the coupling strength in this system strongly depends on the transition dipole moment and a mode volume of the cavity. In this study we have demonstrated controllable emission of Rhodamine 6G organic molecules with relatively low and unoriented dipole moments in a strong coupling regime by placing them into a tunable Fabry-Perot microcavity.
Photonic crystals doped with fluorescent nanoparticles offer a plenty of interesting applications in photonics, laser
physics, and biosensing. Understanding of the mechanisms and effects of modulation of the photoluminescent properties
of photonic crystals by varying the depth of nanoparticle penetration should promote targeted development of
nanocrystal-doped photonic crystals with desired optical and morphological properties. Here, we have investigated the
penetration of semiconductor quantum dots (QDs) into porous silicon photonic crystals and performed experimental
analysis and theoretical modeling of the effects of the depth of nanoparticle penetration on the photoluminescent
properties of this photonic system. For this purpose, we fabricated porous silicon microcavities with an eigenmode width
not exceeding 10 nm at a wavelength of 620 nm. CdSe/CdS/ZnS QDs fluorescing at 617 nm with a quantum yield of
about 70% and a width at half-height of about 40 nm were used in the study. Confocal microscopy and scanning electron
microscopy were used to estimate the depth of penetration of QDs into the porous silicon structure; the
photoluminescence spectra, kinetics, and angular fluorescence distribution were also analyzed. Enhancement of QD
photoluminescence at the microcavity eigenmode wavelength was observed. Theoretical modeling of porous silicon
photonic crystals doped with QDs was performed using the finite-difference time-domain (FDTD) approach. Theoretical
modeling has predicted, and the experiments have confirmed, that even a very limited depth of nanoparticle penetration
into photonic crystals, not exceeding the first Bragg mirror of the microcavity, leads to significant changes in the QD
luminescence spectrum determined by the modulation of the local density of photonic states in the microcavity. At the
same time, complete and uniform filling of a photonic crystal with nanoparticles does not enhance this effect, which is as
strong as in the case of a very limited depth of nanoparticle penetration. Our results will help to choose the best
technology for fabrication of efficient sensor systems based on porous silicon photonic crystals doped with fluorescent
nanoparticles.
Combination of nanometer-scale 3D structural analysis with optical characterization of the same material is a challenging task. Its results may be important for nanophotonics, materials science, and quality control. We have developed a new technique for complementary high-resolution structural and optical characterization followed by optical spectroscopic and microscopic measurements accompanied by reconstruction of the 3D structure in the same area of the sample. The 3D structure is reconstructed by combination of ultramicrotomic and SPM techniques allowing the study of the 3D distribution of implanted nanoparticles and their effect on the matrix structure. The combination of scanning probe nanotomography (SPN) and optical microspectroscopy makes it possible to direct estimate how the 3D structural characteristics of materials affect their macroscopic optical properties. The technique developed has been applied to the engineering of materials made from cholesteric liquid crystals and fluorescent quantum dots (QDs). These materials permit photochemical patterning and image recording through the changes in the dissymmetry factor of circular polarization of QD emission. The differences in the polarisation images and morphological characteristics of the liquid crystal matrix have proved to be correlated with the arrangement of the areas of homogeneous distribution and nonhomogeneous clustering of QDs. The reconstruction of the 3D structure of the liquid crystal matrix in the areas of homogeneous QD distribution has shown that QDs embedded into cholesteric liquid crystal matrices do not perturb their periodic planar texture. The combined optical/SPM/ultramicrotome technique will be indispensable for evaluating the effects of inorganic nanoparticles on the organisation of organic and liquid crystal matrices, biomedical materials, cells, and tissues.
Optical materials based on cholesteric liquid crystals (LCs) doped with fluorescent CdSe/ZnS quantum dots (QDs) have been developed and demonstrated to have a wide photonic band gap. It has been shown that the fluorescence emission of QDs embedded in LCs is circularly polarized and that the dissymmetry factor of this polarization may be optically or electrically controlled via conformational changes in the helical structure of the LC matrix. The possibility of photochemical patterning or image recording using these materials has been demonstrated; the recorded information can be read through changes in the dissymmetry factor of circular polarization of QDs emission. The developed photo- and electro-active materials with a controlled degree of fluorescence circular polarization may be used as on-demand single photon sources in photonics, optoelectronics, and quantum cryptography, as well as for development of nanophotonic systems capable of low-threshold lasing.
Monodispersed semiconductor nanocrystals or quantum dots (QDs) specifically immobilized on the surface of purple
membranes (PMs) containing bacteriorhodopsin (bR) can harvest light in the UV to blue region, which cannot be
absorbed efficiently by the PMs alone, and transfer the harvested energy to the retinal chromophores of bR via highly
efficient Förster resonance energy transfer (FRET). CdTe or CdSe/ZnS QDs with a quantum yield as high as 70% have
been used to estimate different parameters characterizing the improvement of the bR biological function caused by
nanocrystals. AFM examination has shown that the most FRET-efficient QD–PM hybrid structures are characterized by
the highest level of QD ordering; hence, AFM imaging of bR–PM hybrid materials provides the basis for optimization of
the assembly design in order to engineer bio-hybrid structures with advanced optical and photovoltaic properties.
Oriented bR-containing proteoliposomes tagged with QDs at a QD-to-bR molar ratio of up to 1:5 have been engineered
and used to analyze the photoresponse, with the bR proton pumping considerably increased. Finally, the kinetics of the
potential/current generation in films of oriented bR containing or not containing QDs have been analyzed. Incorporation
of QDs resulted in an increase in the potential/current generation rate and in an almost fourfold increase in the rate of Mform
formation. Thus, the improvement of the bR native function by QDs may be caused by two reasons: an extension of
the range of utilized light and an increase in the rate of the bR photocycle.
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