Search

We present an optical method that combines confocal microscopy with position modulation to perform axial tracking and topographic imaging of fluorescent surfaces. Using a remote focusing system, the confocal observation volume is oscillated in the axial direction. The resulting modulation of the detected signal is used as a feedback to precisely control the distance to an object of interest. The accuracy of this method is theoretically analyzed and the axial-locking accuracy is experimentally evaluated. Topographic imaging is demonstrated on fluorescently coated beads and fixed cells. This microscope allows for nanometric topography or tracking of dynamic fluorescent surfaces.

An M13 bacteriophage-based Förster resonance energy transfer (FRET) system is developed to estimate intermolecular distance at the nanoscale using a complex of CdSSe/ZnS nanocrystal quantum dots, genetically engineered M13 bacteriophages labeled with fluorescein isothiocyanate and trinitrotoluene (TNT) as an inhibitor. In the absence of trinitrotoluene, it is observed that a significant spectral shift from blue to green occur, which represents efficient energy transfer through dipole-dipole coupling between donor and acceptor, or FRET-on mode. On the other hand, in the presence of trinitrotoluene, the energy transfer is suppressed, since the donor-to-acceptor intermolecular distance is detuned by the specific capturing of TNT by the M13 bacteriophage, denoted as FRET-off mode. These noble features are confirmed by changes in the fluorescence intensity and the fluorescence decay curve. TNT addition to our system results in reducing the total energy transfer efficiency considerably from 16.1% to 7.6% compared to that in the non-TNT condition, while the exciton decay rate is significantly enhanced. In particular, we confirm that the energy transfer efficiency satisfies the original intermolecular distance dependence of FRET. The relative donor-to-acceptor distance is changed from 70.03 Å to 80.61 Å by inclusion of TNT.

We have employed a variable stripe length method in order to measure the optical gain of GaAs/AlGaAs quantum rings. Although the large lateral diameter of quantum rings ( ∼ 50 nm) with a few nm size distribution is expected to cause a small spectral inhomogeneity ( ∼ 1 %), a broad gain width ( ∼ 300 meV) was observed. This result was attributed to a variation of the vertical heights and variations in localized states that exhibit crescent shaped wavefunctions, whereby the energy levels are distributed over a broad spectral range. When the excitation intensity is decreased, irregular peaks appear in the gain spectrum gradually. Similar phenomena were also observed as the temperature increased. We conclude that excited carriers in quantum rings are distributed stochastically at various localized states and that the population inversion is sensitive to both excitation intensity and temperature.

We find that the emission from laterally coupled quantum dots is strongly polarized along the coupled direction [1\documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$$\bar 1$$\end{document}1¯0], and its polarization anisotropy can be shaped by changing the orientation of the polarized excitation. When the nonresonant excitation is linearly polarized perpendicular to the coupled direction [110], excitons (X1 and X2) and local biexcitons (X1X1 and X2X2) from the two separate quantum dots (QD1 and QD2) show emission anisotropy with a small degree of polarization (10%). On the other hand, when the excitation polarization is parallel to the coupled direction [1\documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$$\bar 1$$\end{document}1¯0], the polarization anisotropy of excitons, local biexcitons, and coupled biexcitons (X1X2) is enhanced with a degree of polarization of 74%. We also observed a consistent anisotropy in the time-resolved photoluminescence. The decay rate of the polarized photoluminescence intensity along the coupled direction is relatively high, but the anisotropic decay rate can be modified by changing the orientation of the polarized excitation. An energy difference is also observed between the polarized emission spectra parallel and perpendicular to the coupled direction, and it increases by up to three times by changing the excitation polarization orientation from [110] to [1\documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$$\bar 1$$\end{document}1¯0]. These results suggest that the dipole–dipole interaction across the two separate quantum dots is mediated and that the anisotropic wavefunctions of the excitons and biexcitons are shaped by the excitation polarization., Quantum dots: coupled control New information storage technologies could use polarized light to control the optical properties of coupled quantum dots. The idea of combining quantum dots – nanoscale semiconductor crystals – into coupled pairs has attracted great attention due to the increased number of exotic quantum states that can be realized for storing data. Robert Taylor at the University of Oxford, UK, with co-workers in China and Korea, directed polarized laser light onto coupled gallium arsenide quantum dots to induce photoluminescence. They found that the emitted light showed very different characteristics depending on whether the excitation was parallel or at right angles to the line formed by the two dots. This ‘optical shaping’ reflects different arrangements of excitons – bound states of electrons and holes – in the coupled dots, and could open new avenues for data storage and thermoelectric energy harvesting.

We found that optical Aharonov–Bohm oscillations in a single GaAs/GaAlAs quantum ring can be controlled by excitation intensity. With a weak excitation intensity of 1.2 kW cm–2, the optical Aharonov–Bohm oscillation period of biexcitons was observed to be half that of excitons in accordance with the period expected for a two-exciton Wigner molecule. When the excitation intensity is increased by an order of magnitude (12 kW cm–2), a gradual deviation of the Wigner molecule condition occurs with decreased oscillation periods and diamagnetic coefficients for both excitons and biexcitons along with a spectral shift. These results suggest that the effective orbit radii and rim widths of electrons and holes in a single quantum ring can be modified by light intensity via photoexcited carriers, which are possibly trapped at interface defects resulting in a local electric field.

We have performed time-resolved photoluminescence of dilute GaAs/AlGaAs quantum rings for increasing excitation and temperature. Although a large distance between quantum rings (200 ± 50 nm) prevents a ring-to-ring carrier transport, a decay time difference over the wide spectrum and its change became significant with increased excitation and temperature. Those results were explained in terms of an internal relaxation of the fine levels in a quantum ring structure. As carrier injection is increased, the carrier relaxation of high energy levels becomes enhanced possibly via the state-filling effect and Auger scattering. We also found that the population decay of low energy levels slows down due to a carrier feeding, but the net population of intermediate levels become nearly constant due to a balanced carrier transfer in between the high and low energy levels. For increased temperature, we observed a photoluminescence quenching at the high energy levels as a consequence of a thermal escape from the shallow potential depth.

We have considered optical nonlinearities of coupled quantum dots theoretically, where an exciton dipole-dipole interaction is mediated between the adjacent large and small quantum dots. For increasing a pump pulse area in resonance with the large quantum dot exciton the induced nonlinear refractive index of the small quantum dot exciton has been obtained. As the exciton dipole-dipole interaction depends on the relative orientation of two exciton dipoles, the optical nonlinearities for the directions parallel and perpendicular to the coupling axis of the two quantum dots are compared. The directional imbalance of optical nonlinearities in coupled quantum dots can be utilized for a polarization phase modulator by controlling a pump pulse area and propagation length.

We recently implemented highly sensitive detection systems for photo-sensitizing potassium ions (K+) based on two-step F&ouml, rster resonance energy transfer (FRET). As a successive study for quantitative understanding of energy transfer processes in terms of the exciton population, we investigated the fluorescence decay dynamics in conjugated polymers and an aptamer-based 6-carboxyfluorescein (6-FAM)/6-carboxytetramethylrhodamine (TAMRA) complex. In the presence of K+ ions, the Guanine-rich aptamer enabled efficient two-step resonance energy transfer from conjugated polymers to dyed pairs of 6-FAM and TAMRA through the G-quadruplex phase. Although the fluorescence decay time of TAMRA barely changed, the fluorescence intensity was significantly increased. We also found that 6-FAM showed a decreased exciton population due the compensation of energy transfer to TAMRA by FRET from conjugated polymers, but a fluorescence quenching also occurred concomitantly. Consequently, the fluorescence intensity of TAMRA showed a 4-fold enhancement, where the initial transfer efficiency (~300%) rapidly saturated within ~0.5 ns and the plateau of transfer efficiency (~230%) remained afterward.

A green emitting Ba1.98SiO4−δN2/3δ:Eu0.02 phosphor with an appreciable intensity was synthesized using the gas-reduction–nitridation (GRN) method. SEM revealed agglomerated Ba1.98SiO4−δN2/3δ:Eu0.02 particles with irregular morphologies and a primary particle size of 1–2.5 μm. The phosphor showed emission lines of Eu2+ corresponding to the 4f65d1 → 4f7 transition under 370 nm excitation. As the GRN process was conducted to incorporate N3− into the lattice, both the excitation and emission intensity of Ba1.98SiO4−δN2/3δ:Eu0.02 were enhanced greatly compared to Ba1.98SiO4:Eu0.02. The decay time of Ba1.98SiO4−δN2/3δ:Eu0.02 showed that N entered the Ba1.98SiO4:Eu0.02 lattices to replace O to form a NO point defect. The electroluminescence intensity of Ba1.98SiO4−δN2/3δ:Eu0.02 at 503 nm increased with increasing forward bias current. Intense green LEDs were fabricated by coating the synthesized phosphors on the cap of the near-ultraviolet InGaN LEDs (λem = 375 nm). Overall, this phosphor appears to be a promising candidate for solid-state lighting applications.

Generally confinement size is considered to determine the dimensionality of nanostructures. While the exciton Bohr radius is used as a criterion to define either weak or strong confinement in optical experiments, the binding energy of confined excitons is difficult to measure experimentally. One alternative is to use the temperature dependence of the radiative recombination time, which has been employed previously in quantum wells and quantum wires. A one-dimensional loop structure is often assumed to model quantum rings, but this approximation ceases to be valid when the rim width becomes comparable to the ring radius. We have evaluated the density of states in a single quantum ring by measuring the temperature dependence of the radiative recombination of excitons, where the photoluminescence decay time as a function of temperature was calibrated by using the low temperature integrated intensity and linewidth. We conclude that the quasi-continuous finely-spaced levels arising from the rotation energy give rise to a quasi-one-dimensional density of states, as long as the confined exciton is allowed to rotate around the opening of the anisotropic ring structure, which has a finite rim width.

We demonstrate that the Stimulated Emission Depletion (STED) concept, which is usually invoked for fluorescence, can be extended to photoacoustic effects. When two-nanosecond pulses of exciting and stimulating light are synchronized, 80% of the acoustic signal generated through excited state absorption (ESA) can be quenched. Regarding the cross-sections for stimulated emission and ESA, a model gives a good order of magnitude in the depletion efficiency. The transient molecular orientation, usually measured via the fluorescence anisotropy, can be accessed in photoacoustic when STED is implemented.

We find that the exciton dipole–dipole interaction in a single laterally coupled GaAs/AlGaAs quantum dot structure can be controlled by the linear polarization of a nonresonant optical excitation. When the excitation intensity is increased with the linearly polarized light parallel to the lateral coupling direction [11̅0], excitons (X1 and X2) and local biexcitons (X1X1 and X2X2) of the two separate quantum dots (QD1 and QD2) show a redshift along with coupled biexcitons (X1X2), while neither coupled biexcitons nor a redshift are observed when the polarization of the exciting beam is perpendicular to the coupling direction. The polarization dependence and the redshift are attributed to an optical nonlinearity in the exciton Förster resonant energy transfer interaction, whereby exciton population transfer between the two quantum dots also becomes significant with increasing excitation intensity. We have further distinguished coupled biexcitons from local biexcitons by their large diamagnetic coefficient.

The dynamics of carriers in GaN epilayers is investigated using femtosecond pump-probe spectroscopy. After the residual chirp on the continuum probe is removed, the normalized difference spectra (NDS) for different probe energies are synchronized, recovering the full time resolution of our laser pulse. Our Monte-Carlo simulation agrees well with the unchirped NDS spectrum, which shows the development of the carrier distribution at early times, where phonon satellites are seen, together with a strong non-thermal electron distribution in the region of the LO-phonon energy arising from the remarkably strong electron-LO phonon interaction. Employing a new technique which involves the integration of the normalized NDS multiplied by the corresponding energy, a measure of the mean energy of the carriers in non-thermal states is obtained. By comparing the time-dependent energy loss with the theoretical energy loss rate, we estimate the effective temperature of the phonon modes as well as the population of phonons. © 2005 Elsevier B.V. All rights reserved.

Polarization modulation in CdSe quantum dots is presented in the framework of the optically-induced nonlinearities of spin dichroism. The real and the imaginary parts of the phase retardation, which are induced from the nonlinear refractive index of the spin-degenerate fine states, are shown spectrally. The polarization modulation is also described in terms of the Jones vector, where the spectral dependences of the amplitude and phase are shown. The optically-induced elliptical polarization of a Gaussian pulse in a feasible condition of multi-quantum dot-layers is predicted precisely in terms of the rotational and the elliptical angles for increasing pulse area up to π, which is also mapped on a the normalized Poincare sphere.

We report all-optical polarization switching based on resonant excitation of spin-polarized e-h pairs in CdSe nanocrystal quantum dots at room temperature. Pump-probe experiments have been performed using the same and the opposite configurations of circular polarizations. Comparing the co- and the cross-circular polarization cases, it is quite evident that selectively-excited spins are flipped to a balanced state within 1 ps and that during this time, the two spin states are equally populated. The all-optical switching results are found to be in close agreement with pump-probe experimental results. The optical switching technique proposed in the present investigation should be extremely useful for future ultrafast terabit communication systems.

The optical modal gain spectrum for a ZnO thin film was measured by using a variable stripe length method. Using the dierential equation for amplified spontaneous emission in a stripe geometry, we obtained stripe-length-dependent gain spectra, which enabled us to investigate the gain saturation in long stripe lengths. When the stripe was shorter than the saturation length, our analysis was in a good agreement with the gain obtained by commonly-used analysis [1]. For intermediate density ( nMott). Both gains saturate with increasing stripe length, but the electron-hole plasma becomes relatively dominant for long stripe lengths ( 1000 µm) while the exciton-exciton scattering is relatively suppressed. This result suggests that exciton-exciton scattering gain saturation is more vulnerable to increase in the stripe length increase since the excitonic stimulated emission occurs on a coherence scale of the localized area.

Radiative and non-radiative recombination processes of free excitons in GaN have been investigated in terms of exciton-polariton and bound exciton by using pump-probe technique. The initial non-radiative trapping process ( 40ps) of the resonantly-excited free excitons was attributed to generation of the bound excitons, in good agreement with the coupled rate equations in the four energy levels. As free excitons are released from the bound excitons due to thermal excitation, the activation energy for donor-bound exciton ( Eact = 16.3 ± 5.2 meV) was estimated by temperature-dependent photoluminescence measurements. A comparison of the reflectance spectrum at 4K with the exciton-polariton model enabled us to obtain the exciton-polariton dispersion with oscillator parameters such as resonance energy, polarizibility, and damping linewidth. The radiative recombination time of the activated free excitons ( 305ps) was observed to be comparable to the theoretical exciton-polariton decay time near the bottleneck regime ( 297ps), in which a significant group velocity reduction is seen.

A novel multi-functional dual-layer polymer electrolyte was prepared by impregnating the interconnected pores with an ethylene carbonate (EC)/dimethyl carbonate (DMC)/lithium hexafluorophosphate (LiPF6) solution. An incompatible layer is based on a microporous polyethylene (PE) and a compatible layer, based on a poly(vinylidenefluoride-co-hexafluoropropylene) (P(VdF-co-HFP)) is sub-microporous and compatible with an electrolyte solution. The Li electrode/the dual-layer polymer electrolyte/Li[Ni0.15Li0.23Mn0.62]O2 cell showed stable cycle performance under prolonged cycle number. This behavior is due to the enhanced compatibility between the matrix polymer and the liquid electrolytes within the submicroporous compatible layer, which could lead to a controlled Li+ deposition on the Li anode surface by forming homegeneous electrolyte zone near the anode.

International audience; We report a novel optical resolution photoacoustic microscopy concept to obtain an axial resolution only by optical methods. The photoacoustic signal is generated through a non-radiative relaxation from a level that is populated by excited state absorption. This two-step excitation process of a single laser enables to achieve an optical sectioning without any acoustic selectivity, whereby a full optical resolution photoacoustic microscopy is obtained. We bring a proof of this concept using Rhodamine and Zinc Tetraphenylporphyrin dyes known for their efficient excited state absorption process.In vivo sub-femtoliter resolution photoacoustic microscopy with higher frame rates," Sci. Rep. 5, 15421 (2015). 13. Y. Yamaoka, M. Nambu, and T. Takamatsu, "Fine depth resolution of two-photon absorption-induced photoacoustic microscopy using low-frequency bandpass filtering," Opt.

A single In 0.49 Ga 0.51 P quantum well sandwiched by In 0.49 Ga 0.51 P/In 0.49 (Ga 0.6 Al 0.4 ) 0.51 P digital alloy structures was investigated in terms of optical modal gain, where gain saturation effects were also considered for both changes in wavelength and stripe length by using a modal gain contour map analysis. We found the gain threshold density is considerably lower by an order of magnitude when compared to the Mott density (∼2 × 10 12 cm −2 ), which can be attributed to a carrier-harvesting effect through the mini-band of the digital alloy.

The Temperature dependence of the exciton radiative decay time in ZnO nanorods has been investigated, which is associated with the density of states for the intra-relaxation of thermally excited excitons. The photoluminescence decay time was calibrated by using the photoluminescence intensity in order to obtain the radiative decay time. In the absence of an external magnetic field, we have confirmed that the radiative decay time increased with temperature in a similar manner to that seen in bulk material (similar to T-1.5). Under an external magnetic field of 6T parallel to the c-axis, we found that the power coefficient of the radiative decay time with temperature decreased (similar to T-1.3) when compared to that in the absence of a magnetic field. This result can be attributed to an enhancement of the effective mass perpendicular to the magnetic field and a redshift of the center-of-mass exciton as a consequence of perturbation effects in the weak-field regime. (C) 2014 Optical Society of America

We propose an amplified all-optical polarization phase modulator assisted by a local surface plasmon in Au-hybrid CdSe quantum dots. When the local surface plasmon of a spherical Au quantum dot is in resonance with the exciton energy level of a CdSe quantum dot, a significant enhancement of the linear and nonlinear refractive index is found in both the real and imaginary terms via the interaction with the dipole field of the local surface plasmon. Given a gating pulse intensity, an elliptical polarization induced by the phase retardation is described in terms of elliptical and rotational angles. In the case that a larger excitation than the bleaching intensity is applied, the signal light can be amplified due to the presence of gain in the CdSe quantum dot. This enables a longer propagation of the signal light relative to the metal loss, resulting in more feasible polarization modulation. (C) 2012 Optical Society of America

A way of analyzing the data in a variable stripe length method gain experiment is presented. We confirm that the stripe length dependence of the gain in In0.02Ga0.98N/In0.16Ga0.84N multiple quantum wells is caused by the change of the chemical potential along the excited stripe due to the interaction of the carrier and photon densities, and the gain threshold density is estimated. A trial function assuming a Lorentzian line shape for the stripe length dependence of the gain is compared with the edge emission intensity as a function of the stripe length. This is found to fit very well with our data, even beyond the saturation region. © 2001 American Institute of Physics.

The dynamics of carriers in GaN epilayers is investigated by using femtosecond pump-probe spectroscopy. After the residual chirp on the continuum probe is removed, the normalized difference spectra (NDS) for different probe energies are synchronized, recovering the full time resolution of our laser pulse. Our Monte-Carlo simulation agrees well with the unchirped NDS spectrum, which shows the development of the carrier distribution at early times, where phonon satellites are seen, together with a strong non-thermal electron distribution in the region of the LO-phonon energy arising from the remark-ably strong electron-LO phonon interaction. By employing a new technique which involves the integration of the normalized NDS multiplied by the corresponding energy, a measure of the mean energy of the carriers in non-thermal states is obtained. By comparing the time-dependent energy loss with the theoretical energy loss rate, we estimate the effective temperature of the phonon modes as well as the population of phonons.

Energy relaxation of optically-generated hot carriers in ZnO is explored theoretically as a function of time. Cooling curves are extracted from the energy loss rates obtained by using the Kogan formula extended to a degenerate electron-hole hot plasma at low lattice temperatures. The energy losses of the carriers by various carrier-phonon interactions are taken into account. The screening of the carrier-phonon interactions is included within the random phase approximation. We observed an initial slow energy relaxation process followed by a rapid relaxation at both high and low carrier temperatures. The dominant relaxation process at the earlier cooling stage in the temperature range 10 2 K Tc 10 3 K is the excitations of optical phonons. The energy relaxation in the low carrier temperature range (Tc 10 2 K) is determined mainly by acoustic phonon scattering. The initial relaxation time of ZnO is found to be on the order of femtoseconds. The relaxation time is increased by a factor of ten if carrier screening eects are taken into account, irrespective of the initial carrier temperature.

not Available.

Transient gain spectra were measured for an In0.02Ga0.98N / In0.16Ga0.84N multiple quantum well by using the variable-stripe-length method (VSLM) in combination with the ultrafast optical Kerr-gate (OKG) technique. Gain dynamics were measured for a range of excitation lengths from short (50 mu m) to long (350 mu m) stripes with the sample under femtosecond photoexcitation. Analysis of the temporal behaviour of gain and chemical potential suggests that stimulated emission originates from a photoexcited electron-hole plasma at early times; at later times, localized states dominate as the electron-hole plasma becomes exhausted. Gain reduction at early times is attributable to coupling of the electron-hole plasma with photons along the stripe, whilst localized states are less susceptible to gain saturation.