Semiconductor quantum dots (QDs) feature high values of the two-photon absorption (TPA) cross-sections, enabling their applications in biosensing and nonlinear optoelectronics. However, the efficient QD photoluminescence (PL) intensity caused by TPA requires high-intensity laser excitation which hinders these applications. Placing the QDs in the micro- or nanocavities leads to a change in their PL properties. Particularly, near plasmon nanoparticles (open nanocavities) the local field may be enhanced by the localized plasmons, which will lead to an increase of the TPA efficiency. Alternatively, placing QDs in a photonic crystal may boost an increase of their PL quantum yield due to the Purcell effect and also increase their PL intensity at the photonic mode wavelength due to the redistribution of the density of photonic states. In this study, we have fabricated thin-film hybrid materials based on QDs placed near plasmonic nanoparticles or in the photonic crystal. We have demonstrated a 4.3-fold increase of the radiative recombination rate of QDs in the photonic crystal cavity under the two-photon excitation, resulting in the increase of the PL quantum yield. In turn, the coating of the QDs films with the gold nanorods led to the 12-fold increase in TPA at the maximum of the plasmon spectrum. Our results pave the way to a strong increase of the PL efficiency of the QDs under two-photon excitation for their applications in biosensing and nonlinear optoelectronics.
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.
We demonstrate a new way for detection ultralow concentration of explosives in this study. It combines an ion mobility spectrometry (IMS) and a promising method of laser desorption/ionization on silicon (DIOS). The DIOS is widely used in mass spectrometry due to the possibility of small molecule detection and high sensitivity. It is known that IMS based on laser ion source is a power method for the fast detection of ultralow concentration of organic molecules. However requirement of using high energy pulse ultraviolet laser increases weight and size of the device. The use of DIOS in an ion source of IMS could decrease energy pulse requirements and allows one to construct both compact and high sensitive device for analyzing gas and liquid probes. On the other hand mechanisms of DIOS in gas media is poorly studied, especially in case of nitroaromatic compounds. The investigation of the desorption/ionization on porous silicon (pSi) surface of nitroaromatic compounds has been carried out for 2,4,6-trinitrotoluene (TNT) using IMS and mass spectrometry (MS). It has been demonstrated that TNT ion formation in a gas medium is a complicated process and includes both an electron emission from the pSi surface with subsequent ion-molecular reactions in a gas phase and a proton transfer between pSi surface and TNT molecule.
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.
It is known that manufacturing and applications of photonic crystals is currently an area of much interest. One of the
focuses of special attention in this area is various microcavity (MC) devices. Porous silicon is one of the most promising
materials for manufacturing such devices because it is simple to prepare, its optical parameters are precisely controllable,
and it has an enormous surface area. This allows to inject different kinds of luminophores into porous silicon MC
devices. Apparently, semiconductor quantum dots (QDs) are among the most interesting of them. QDs are characterized
by a wide absorbance spectrum, large absorption cross-section, high quantum yield, and excellent photostability. To date,
there have been few studies on QD injection into porous silicon photonic structures. In addition, many structures used
lack the desired characteristics; the depth of QD penetration also remains a question. This is the first study to analyze the
photoluminescence spectrum and kinetics of QDs in a high-quality porous silicon MC. A drastic narrowing of the
luminescence spectrum has been observed after QD injection. We have found that the MC morphology considerably
affects the penetration of QDs. The kinetics of photoluminescence has also been investigated. Measurements have shown
a decrease in the QD characteristic photoluminescence decay time after QD injection into a porous silicon MC compared
with the QD photoluminescence decay time in a toluene solution. However, we have not observed a significant
difference between the photoluminescence decay times of QDs in an MC and in single-layer porous silicon.
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