Addition of Zinc Sulfide Shells to Semiconducting Nanoparticles and its Effect on the Nanoparticle Fluorescence Emission Properties

The addition of a ZnS shell to CdSe and CdS quantum dot cores was explored using various methods. Spectrophotometry was used to assess the success of ZnS overcoating, which produces both an increase in overall fluorescence and decrease in particle size distribution. A new method was developed, involving preheating of the zinc and sulfide precursor solutions, resulting in CdSe(ZnS) particles with improved fluorescence and a more uniform shell coating from oleylamine-capped CdSe core particles.

Influence of different storage methods on laser fluorescence values: a two-year study

The aim of this study was to assess the influence on the infrared laser fluorescence response of some storage methods commonly used in dental research. Forty extracted permanent teeth, selected from a pool of frozen teeth, were divided into four groups of 10. Three groups were stored at 4 degrees C in 1% chloramine, 10% formalin or 0.02% thymol solution. The fourth group was stored at -20 degrees C (no storage solution added). Fluorescence measurements were performed at 14, 77, 113, 168, 232, 486 and 737 days. After 2 years, significant decreases in fluorescence (p<0.01) for the samples in formalin (-60%), chloramine (-72%) and thymol (-54%) were observed. The frozen teeth showed a slight but non-significant increase in fluorescence of 5% (p>0.01). Storing solutions have a significant influence on the fluorescence yield. Samples used for in vitro purposes stored frozen do not significantly change their fluorescence response. Thus, cut-off values obtained under the latter conditions could be extrapolated to the in vivo situation.

Iron X-ray fluorescence (XRF) scannings of ODP Holes 165-1001A and 171-1050C

Abstract: Ocean Drilling Program Sites 1001A (Caribbean Sea) and 1050C (western North Atlantic) display obliquity and precession cycles throughout polarity zone C27 of the late Danian stage (earliest Cenozoic time). Sliding-window spectra analysis and direct cycle counting on downhole logs and high-resolution Fe variations at both sites yield the equivalent of 35-36 obliquity cycles. This cycle-tuned duration for polarity chron C27 of 1.45 Ma (applying a modern mean obliquity period of 40.4 ka) is consistent with trends from astronomical tuning of early Danian polarity chron C29 and 40Ar/39Ar age calibration of the Campanian-Maastrichtian magnetic polarity time scale. The cycle-tuned Danian stage (sensu Berggren et al. 1995, in SEPM Special Publications, 54, 129-212) spans 3.65 Ma (65.5-61.85 Ma). Spreading rates on a reference South Atlantic synthetic profile display progressive slowing during the Maastrichtian to Danian stages, then remained relatively constant through late Palaeocene and early Eocene time.

O 1s excitation and ionization processes in the CO2 molecule studied via detection of low-energy fluorescence emission

Oxygen 1s excitation and ionization processes in the CO2 molecule have been studied with dispersed and non-dispersed fluorescence spectroscopy as well as with the vacuum ultraviolet (VUV) photon?photoion coincidence technique. The intensity of the neutral O emission line at 845 nm shows particular sensitivity to core-to-Rydberg excitations and core?valence double excitations, while shape resonances are suppressed. In contrast, the partial fluorescence yield in the wavelength window 300?650 nm and the excitation functions of selected O+ and C+ emission lines in the wavelength range 400?500 nm display all of the absorption features. The relative intensity of ionic emission in the visible range increases towards higher photon energies, which is attributed to O 1s shake-off photoionization. VUV photon?photoion coincidence spectra reveal major contributions from the C+ and O+ ions and a minor contribution from C2+. No conclusive changes in the intensity ratios among the different ions are observed above the O 1s threshold. The line shape of the VUV?O+ coincidence peak in the mass spectrum carries some information on the initial core excitation

Realistic detailed balance study of the quantum efficiency of quantum dot solar cells

An attractive but challenging technology for high efficiency solar energy conversion is the intermediate band solar cell (IBSC), whose theoretical efficiency limit is 63%, yet which has so far failed to yield high efficiencies in practice. The most advanced IBSC technology is that based on quantum dots (QDs): the QD-IBSC. In this paper, k·p calculations of photon absorption in the QDs are combined with a multi-level detailed balance model. The model has been used to reproduce the measured quantum efficiency of a real QD-IBSC and its temperature dependence. This allows the analysis of individual sub-bandgap transition currents, which has as yet not been possible experimentally, yielding a deeper understanding of the failure of current QD-IBSCs. Based on the agreement with experimental data, the model is believed to be realistic enough to evaluate future QD-IBSC proposals.

Fluorescence and photobleaching dynamics of single light-harvesting complexes

Single light-harvesting complexes LH-2 from Rhodopseudomonas acidophila were immobilized on various charged surfaces under physiological conditions. Polarized light experiments showed that the complexes were situated on the surface as nearly upright cylinders. Their fluorescence lifetimes and photobleaching properties were obtained by using a confocal fluorescence microscope with picosecond time resolution. Initially all molecules fluoresced with a lifetime of 1 ± 0.2 ns, similar to the bulk value. The photobleaching of one bacteriochlorophyll molecule from the 18-member assembly caused the fluorescence to switch off completely, because of trapping of the mobile excitations by energy transfer. This process was linear in light intensity. On continued irradiation the fluorescence often reappeared, but all molecules did not show the same behavior. Some LH-2 complexes displayed a variation of their quantum yields that was attributed to photoinduced confinement of the excited states and thereby a diminution of the superradiance. Others showed much shorter lifetimes caused by excitation energy traps that are only ≈3% efficient. On repeated excitation some molecules entered a noisy state where the fluorescence switched on and off with a correlation time of ≈0.1 s. About 490 molecules were examined.

Fluorescence correlation spectroscopy reveals fast optical excitation-driven intramolecular dynamics of yellow fluorescent proteins

Fast excitation-driven fluctuations in the fluorescence emission of yellow-shifted green fluorescent protein mutants T203Y and T203F, with S65G/S72A, are discovered in the 10−6–10−3-s time range, by using fluorescence correlation spectroscopy at 10−8 M. This intensity-dependent flickering is conspicuous at high pH, with rate constants independent of pH and viscosity with a minor temperature effect. The mean flicker rate increases linearly with excitation intensity for at least three decades, but the mean dark fraction of the molecules undergoing these dynamics is independent of illumination intensity over ≈6 × 102 to 5 × 106 W/cm2. These results suggest that optical excitation establishes an equilibration between two molecular states of different spectroscopic properties that are coupled only via the excited state as a gateway. This reversible excitation-driven transition has a quantum efficiency of ≈10−3. Dynamics of external protonation, reversibly quenching the fluorescence, are also observed at low pH in the 10- to 100-μs time range. The independence of these two bright–dark flicker processes implies the existence of at least two separate dark states of these green fluorescent protein mutants. Time-resolved fluorescence measurements reveal a single exponential decay of the excited state population with 3.8-ns lifetime, after 500-nm excitation, that is pH independent. Our fluorescence correlation spectroscopy results are discussed in terms of recent theoretical studies that invoke isomerization of the chromophore as a nonradiative channel of the excited state relaxation.

Mapping Intercellular CO2 Mole Fraction (Ci) in Rosa rubiginosa Leaves Fed with Abscisic Acid by Using Chlorophyll Fluorescence Imaging1 : Significance of Ci Estimated from Leaf Gas Exchange

Imaging of photochemical yield of photosystem II (PSII) computed from leaf chlorophyll fluorescence images and gas-exchange measurements were performed on Rosa rubiginosa leaflets during abscisic acid (ABA) addition. In air ABA induced a decrease of both the net CO2 assimilation (An) and the stomatal water vapor conductance (gs). After ABA treatment, imaging in transient nonphotorespiratory conditions (0.1% O2) revealed a heterogeneous decrease of PSII photochemical yield. This decline was fully reversed by a transient high CO2 concentration (7400 μmol mol−1) in the leaf atmosphere. It was concluded that ABA primarily affected An by decreasing the CO2 supply at ribulose-1,5-bisphosphate carboxylase/oxygenase. Therefore, the An versus intercellular mole fraction (Ci) relationship was assumed not to be affected by ABA, and images of Ci and gs were constructed from images of PSII photochemical yield under nonphotorespiratory conditions. The distribution of gs remained unimodal following ABA treatment. A comparison of calculations of Ci from images and gas exchange in ABA-treated leaves showed that the overestimation of Ci estimated from gas exchange was only partly due to heterogeneity. This overestimation was also attributed to the cuticular transpiration, which largely affects the calculation of the leaf conductance to CO2, when leaf conductance to water is low.

Optical initialization, readout, and dynamics of a Mn spin in a quantum dot

We have investigated the spin preparation efficiency by optical pumping of individual Mn atoms embedded in CdTe/ZnTe quantum dots. Monitoring the time dependence of the intensity of the fluorescence during the resonant optical pumping process in individual quantum dots allows to directly probe the dynamics of the initialization of the Mn spin. This technique presents the convenience of including preparation and readout of the Mn spin in the same step. Our measurements demonstrate that Mn spin initialization, at zero magnetic field, can reach an efficiency of 75% and occurs in the tens of nanoseconds range when a laser resonantly drives at saturation one of the quantum-dot transition. We observe that the efficiency of optical pumping changes from dot-to-dot and is affected by a magnetic field of a few tens of millitesla applied in Voigt or Faraday configuration. This is attributed to the local strain distribution at the Mn location which predominantly determines the dynamics of the Mn spin under weak magnetic field. The spectral distribution of the spin-flip-scattered photons from quantum dots presenting a weak optical pumping efficiency reveals a significant spin relaxation for the exciton split in the exchange field of the Mn spin.

Quantum interference effects in a cavity QED system

We consider the effect of quantum interference on population distribution and photon statistics of a cavity field interacting with dressed states of a strongly driven three-level atom. We analyse three coupling configurations of the cavity field to the driven atom, with the cavity frequency tuned to the outer Rabi sideband, the inner Rabi sideband and the central frequency of the 'singly dressed' three-level atom. The quantum doubly dressed states for each configuration are identified and the population distribution and photon statistics are interpreted in terms of transitions among these dressed states and their populations. We find that the population distribution depends strongly on quantum interference and the cavity damping. For the cavity field tuned to the outer or inner Rabi sidebands the cavity damping induces transitions between the dressed states which are forbidden for the ordinary spontaneous emission. Moreover, we find that in the case of the cavity field coupled to the inner Rabi sideband the population distribution is almost Poissonian with a large average number of photons that can be controlled by quantum interference. This system can be considered as a one-atom dressed-state laser with controlled intensity.

Simulating quantum interference in a three-level system with perpendicular transition dipole moments

We consider a three-level V-type atomic system with the ground state coupled by a laser field to only one of the excited states, and with the two excited states coupled together by a dc field. Although the dipole moments of the two dipole-allowed transitions are assumed perpendicular, we demonstrate that this system emulates to a large degree a three-level system with parallel dipole moments-the latter being a system that exhibits quantum interference and displays a number of interesting features. As examples, we show that the system can produce extremely large values for the intensity-intensity correlation function, and that its resonance fluorescence spectrum can display ultranarrow lines. The dressed states for this system are identified, and the spectral features are interpreted in terms of transitions among these dressed states. We also show that this system is capable of exhibiting considerable squeezing.

73 nm wavelength tuning from a frequency-doubled quantum-dot laser in PPKTP waveguides

A compact all-room-temperature CW 73-nm tunable laser source in the visible spectral region (574nm-647nm) has been demonstrated by frequency-doubling of a broadly-tunable InAs/GaAs quantum dot external-cavity diode laser in periodically-poled potassium titanyl phosphate waveguides with a maximum output power in excess of 12mW and a maximum conversion efficiency exceeding 10%. Three waveguides with different cross-sectional areas (4×4μm2, 3×5μm2 and 2x6μm2) were investigated. Introduction - Development of compact broadly tunable laser sources in the visible spectral region is currently very attractive area of research with applications ranging from photomedicine and biophotonics to confocal fluorescence microscopy and laser projection displays. In this respect, semiconductor lasers with their small size, high efficiency, reliability and low cost are very promising for realization of such sources by frequency­doubling of the infrared light in nonlinear crystal waveguides. Furthermore, the wide tunability offered by quantum-dot (QD) external-cavity diode lasers (ECDL), due to the temperature insensibility and broad gain bandwidth [1,2], is very promising for the development of tunable visible laser sources [3,4]. In this work we show a compact green-to-red tunable all­room-temperature CW laser source using a frequency-doubled InAs/GaAs QD-ECDL in periodically-poled potassium titanyl phosphate (PPKTP) crystal waveguides. This laser source generates frequency-doubled light over the 574nm-647nm wavelength range utilizing the significant difference in the effective refractive indices of high-order and low-order modes in multimode waveguides [3]. Experimental results - Experimental setup used in this work was similar to that described in [3] and consisted of a QD gain chip in the quasi­Littrow configuration and a PPKTP waveguide. Coarse wavelength tuning of the QD-ECDL between 1140 nm and 1300 nm at 20°C was possible for pump current of 1.5 A. The laser output was coupled into the PPKTP waveguide using an AR-coated 40x aspheric lens (NA ~ 0.55). The PPKTP frequency-doubling crystal (not AR coated) used in our work was 18 mm in length and was periodically poled for SHG (with the poling period of ~ 11.574 11m). The crystal contained 3 different waveguides with cross-sectional areas of ~ 4x4 11m2, 3x5 11m2 and 2x6 11m2. Both the pump laser and the PPKTP crystal were operating at room temperature. The waveguides with cross-sectional areas of 4x411m2, 3x511m2 and 2x611m2 demonstrated the tunability in the wavelength ranges of 577nm - 647nm, 576nm -643nm and 574nm - 641nm, respectively, with a maximum output power of 12.04mW at 606 nm Conclusion - We demonstrated a compact all-room-temperature broadly­tunable laser source operating in the visible spectral region between 574nm and 647nm. This laser source is based on second harmonic generation in PPKTP waveguides with different cross-sectional areas using an InAs/GaAs QD-ECDL References [I] E.U. Rafailov, M.A. Cataluna, and W. Sibbett, Nat. Phot. 1,395 (2007). [2] K.A. Fedorova, M.A. Cataluna, I. Krestnikov, D. Livshits, and E.U. Rafailov, Opt. Express 18(18), 19438-19443 (2010). [3] K.A. Fedorova, G.S. Sokolovskii, P.R. Battle, D.A. Livshits, and E.U. Rafailov, Laser Phys. Lett. 9, 790-795 (2012). [4] K.A. Fedorova,G.S. Sokolovskii, D.T. Nikitichev, P.R. Battle, I.L. Krestnikov, D.A. Livshits, and E.U. Rafailov, Opt. Lett. 38(15), 2835-2837 (2013) © 2014 IEEE.

Conjugated Quantum Dots Inhibit the Amyloid β (1–42) Fibrillation Process

Nanoparticles have enormous potential in diagnostic and therapeutic studies. We have demonstrated that the amyloid beta mixed with and conjugated to dihydrolipoic acid- (DHLA) capped CdSe/ZnS quantum dots (QDs) of size approximately 2.5 nm can be used to reduce the fibrillation process. Transmission electron microscopy (TEM) and atomic force microscopy (AFM) were used as tools for analysis of fibrillation. There is a significant change in morphology of fibrils when amyloid β (1–42) (Aβ (1–42)) is mixed or conjugated to the QDs. The length and the width of the fibrils vary under modified conditions. Thioflavin T (ThT) fluorescence supports the decrease in fibril formation in presence of DHLA-capped QDs.