High Photoluminescence Quantum Yield in Band Gap Tunable Bromide Containing Mixed Halide Perovskites

DOE PAGES

Sutter-Fella, Carolin M.; Li, Yanbo; Amani, Matin; ...

2015-12-21

Hybrid organic-inorganic halide perovskite based semiconductor materials are attractive for use in a wide range of optoelectronic devices because they combine the advantages of suitable optoelectronic attributes and simultaneously low-cost solution processability. Here, we present a two-step low-pressure vapor-assisted solution process to grow high quality homogeneous CH 3NH 3PbI 3-xBr x perovskite films over the full band gap range of 1.6-2.3 eV. Photoluminescence light-in versus light-out characterization techniques are used to provide new insights into the optoelectronic properties of Br-containing hybrid organic-inorganic perovskites as a function of optical carrier injection by employing pump-powers over a 6 orders of magnitude dynamicmore » range. The internal luminescence quantum yield of wide band gap perovskites reaches impressive values up to 30%. This high quantum yield translates into substantial quasi-Fermi level splitting and high "luminescence or optically implied" open-circuit voltage. Most importantly, both attributes, high internal quantum yield and high optically implied open-circuit voltage, are demonstrated over the entire band gap range (1.6 eV ≤ E g ≤ 2.3 eV). These results establish the versatility of Br-containing perovskite semiconductors for a variety of applications and especially for the use as high-quality top cell in tandem photovoltaic devices in combination with industry dominant Si bottom cells. (Figure Presented).« less

State-selected chemical reaction dynamics at the S matrix level - Final-state specificities of near-threshold processes at low and high energies

NASA Technical Reports Server (NTRS)

Chatfield, David C.; Truhlar, Donald G.; Schwenke, David W.

1992-01-01

State-to-state reaction probabilities are found to be highly final-state specific at state-selected threshold energies for the reactions O + H2 yield OH + H and H + H2 yield H2 + H. The study includes initial rotational states with quantum numbers 0-15, and the specificity is especially dramatic for the more highly rotationally excited reactants. The analysis is based on accurate quantum mechanical reactive scattering calculations. Final-state specificity is shown in general to increase with the rotational quantum number of the reactant diatom, and the trends are confirmed for both zero and nonzero values of the total angular momentum.

A Phosphine-Free Route to Size-Adjustable CdSe and CdSe/CdS Core-Shell Quantum Dots for White-Light-Emitting Diodes.

PubMed

Zhang, Yugang; Li, Guopeng; Zhang, Ting; Song, Zihang; Wang, Hui; Zhang, Zhongping; Jiang, Yang

2018-03-01

The selenium dioxide was used as the precursor to synthesize wide-size-ranged CdSe quantum dots (2.4-5.7 nm) via hot-injection route. The CdSe quantum dots are featured with high crystalline, monodisperse, zinc blende structure and wide emission region (530-635 nm). In order to improve the stability and quantum yield, a phosphine-free single-molecular precursor approach is used to obtain CdSe/CdS core/shell quantum dots. The CdSe/CdS quantum dots are highly fluorescent with quantum yield up to 65%, and persist the good monodispersity and high crystallinity. Moreover, the quantum dots white light-emitting-diodes are fabricated by using the resultant red emission core/shell quantum dots and Y3Al5O12:Ce3+ yellow phosphors as color-conversion layers on a blue InGaN chip. The prepared light-emitting-diodes show good performance with CIE-1931 coordinated of (0.3583, 0.3349), an Ra of 92.9, and a Tc of 4410 K at 20 mA, which indicate that the combination of red-emission QDs and yellow phophors as a promising approach to obtain warm WLEDs with good color rendering.

Towards efficient solar hydrogen production by intercalated carbon nitride photocatalyst.

PubMed

Gao, Honglin; Yan, Shicheng; Wang, Jiajia; Huang, Yu An; Wang, Peng; Li, Zhaosheng; Zou, Zhigang

2013-11-07

The development of efficient photocatalytic material for converting solar energy to hydrogen energy as viable alternatives to fossil-fuel technologies is expected to revolutionize energy shortage and environment issues. However, to date, the low quantum yield for solar hydrogen production over photocatalysts has hindered advances in the practical applications of photocatalysis. Here, we show that a carbon nitride intercalation compound (CNIC) synthesized by a simple molten salt route is an efficient polymer photocatalyst with a high quantum yield. We found that coordinating the alkali metals into the C-N plane of carbon nitride will induce the un-uniform spatial charge distribution. The electrons are confined in the intercalated region while the holes are in the far intercalated region, which promoted efficient separation of photogenerated carriers. The donor-type alkali metal ions coordinating into the nitrogen pots of carbon nitrides increase the free carrier concentration and lead to the formation of novel nonradiative paths. This should favor improved transport of the photogenerated electron and hole and decrease the electron-hole recombination rate. As a result, the CNIC exhibits a quantum yield as high as 21.2% under 420 nm light irradiation for solar hydrogen production. Such high quantum yield opens up new opportunities for using cheap semiconducting polymers as energy transducers.

High quantum-yield phosphors via quantum splitting and upconversion

NASA Astrophysics Data System (ADS)

Jeong, Joayoung

The Gd3+ ion has been used to induce quantum splitting in luminescent materials by using cross-relaxation energy transfer (CRET). In Nd:LiGdF4, quantum splitting results from a two-step CRET between Gd3+ and Nd3+, first involving a transition 6G→6I on Gd3+ and an excitation within the 4f3 configuration of Nd3+ followed by a second CRET that brings Gd3+ to 6P7/2. The excited Nd3+ ion rapidly relaxes nonradiatively to the emitting 4F3/2. The excited Gd3+ ion then transfers its energy back to Nd3+, which gives rise to the second photon. The result is a quantum yield of 1.05 +/- 0.35 with emission in the NIR following excitation at 175 nm. GdF3:Pr3+, Eu 3+ also exhibits quantum splitting, but only at very low concentration of Pr3+ (0.3%) and Eu3+ (0.2%), resulting in a quantum yield of approximately 20% under 160-nm excitation. Host intrinsic emission via a self-trapped exciton (STE) was also examined as a means to sensitize Gd3+ emission. The material ScPO4:Gd 3+ exhibits a high absolute quantum yield of 0.9 +/- 0.2 under 170-nm excitation, demonstrating a potentially new and efficient pathway for exciting quantum splitting phosphors. Single crystals of the material GdZrF7 were grown, and its structure was established via single-crystal X-ray diffraction methods. Doped samples of GdZrF7:Yb3+, Er3+ exhibit bright up-conversion luminescence with light output that is up to twice that of a commercial material based on the host Gd2O2S. When doped with Eu3+, the fluoride also emits a nearly white color under vacuum ultraviolet excitation with an absolute quantum yield near 0.9. The new compound Gd4.67(SiO4)3S was synthesized and studied. The structure was established via single-crystal X-ray methods, and the luminescence of Tb3+ samples was investigated.

Transparent Ultra-High-Loading Quantum Dot/Polymer Nanocomposite Monolith for Gamma Scintillation.

PubMed

Liu, Chao; Li, Zhou; Hajagos, Tibor Jacob; Kishpaugh, David; Chen, Dustin Yuan; Pei, Qibing

2017-06-27

Spectroscopic gamma-photon detection has widespread applications for research, defense, and medical purposes. However, current commercial detectors are either prohibitively expensive for wide deployment or incapable of producing the characteristic gamma photopeak. Here we report the synthesis of transparent, ultra-high-loading (up to 60 wt %) Cd x Zn 1-x S/ZnS core/shell quantum dot/polymer nanocomposite monoliths for gamma scintillation by in situ copolymerization of the partially methacrylate-functionalized quantum dots in a monomer solution. The efficient Förster resonance energy transfer of the high-atomic-number quantum dots to lower-band-gap organic dyes enables the extraction of quantum-dot-borne excitons for photon production, resolving the problem of severe light yield deterioration found in previous nanoparticle-loaded scintillators. As a result, the nanocomposite scintillator exhibited simultaneous improvements in both light yield (visible photons produced per MeV of gamma-photon energy) and gamma attenuation. With these enhancements, a 662 keV Cs-137 gamma photopeak with 9.8% resolution has been detected using a 60 wt % quantum-dot nanocomposite scintillator, demonstrating the potential of such a nanocomposite system in the development of high-performance low-cost spectroscopic gamma detectors.

Luminescent carbon quantum dots with high quantum yield as a single white converter for white light emitting diodes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Feng, X. T.; Zhang, Y.; Liu, X. G., E-mail: liuxuguang@tyut.edu.cn

Carbon quantum dots (CQDs) with high quantum yield (51.4%) were synthesized by a one-step hydrothermal method using thiosalicylic acid and ethylenediamine as precursor. The CQDs have the average diameter of 2.3 nm and possess excitation-independent emission wavelength in the range from 320 to 440 nm excitation. Under an ultraviolet (UV) excitation, the CQDs aqueous solutions emit bright blue fluorescence directly and exhibit broad emission with a high spectral component ratio of 67.4% (blue to red intensity to total intensity). We applied the CQDs as a single white-light converter for white light emitting diodes (WLEDs) using a UV-LED chip as the excitation lightmore » source. The resulted WLED shows superior performance with corresponding color temperature of 5227 K and the color coordinates of (0.34, 0.38) belonging to the white gamut.« less

Efficient Carrier Multiplication in Colloidal Silicon Nanorods

DOE PAGES

Stolle, Carl Jackson; Lu, Xiaotang; Yu, Yixuan; ...

2017-08-01

In this study, auger recombination lifetimes, absorption cross sections, and the quantum yields of carrier multiplication (CM), or multiexciton generation (MEG), were determined for solvent-dispersed silicon (Si) nanorods using transient absorption spectroscopy (TAS). Nanorods with an average diameter of 7.5 nm and aspect ratios of 6.1, 19.3, and 33.2 were examined. Colloidal Si nanocrystals of similar diameters were also studied for comparison. The nanocrystals and nanorods were passivated with organic ligands by hydrosilylation to prevent surface oxidation and limit the effects of surface trapping of photoexcited carriers. All samples used in the study exhibited relatively efficient photoluminescence. The Auger lifetimesmore » increased with nanorod length, and the nanorods exhibited higher CM quantum yield and efficiency than the nanocrystals with a similar band gap energy E g. Beyond a critical length, the CM quantum yield decreases. Finally, nanorods with the aspect ratio of 19.3 had the highest CM quantum yield of 1.6 ± 0.2 at 2.9E g, which corresponded to a multiexciton yield that was twice as high as observed for the spherical nanocrystals.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Stolle, Carl Jackson; Lu, Xiaotang; Yu, Yixuan

In this study, auger recombination lifetimes, absorption cross sections, and the quantum yields of carrier multiplication (CM), or multiexciton generation (MEG), were determined for solvent-dispersed silicon (Si) nanorods using transient absorption spectroscopy (TAS). Nanorods with an average diameter of 7.5 nm and aspect ratios of 6.1, 19.3, and 33.2 were examined. Colloidal Si nanocrystals of similar diameters were also studied for comparison. The nanocrystals and nanorods were passivated with organic ligands by hydrosilylation to prevent surface oxidation and limit the effects of surface trapping of photoexcited carriers. All samples used in the study exhibited relatively efficient photoluminescence. The Auger lifetimesmore » increased with nanorod length, and the nanorods exhibited higher CM quantum yield and efficiency than the nanocrystals with a similar band gap energy E g. Beyond a critical length, the CM quantum yield decreases. Finally, nanorods with the aspect ratio of 19.3 had the highest CM quantum yield of 1.6 ± 0.2 at 2.9E g, which corresponded to a multiexciton yield that was twice as high as observed for the spherical nanocrystals.« less

Optomechanical Control of Quantum Yield in Trans-Cis Ultrafast Photoisomerization of a Retinal Chromophore Model.

PubMed

Valentini, Alessio; Rivero, Daniel; Zapata, Felipe; García-Iriepa, Cristina; Marazzi, Marco; Palmeiro, Raúl; Fdez Galván, Ignacio; Sampedro, Diego; Olivucci, Massimo; Frutos, Luis Manuel

2017-03-27

The quantum yield of a photochemical reaction is one of the most fundamental quantities in photochemistry, as it measures the efficiency of the transduction of light energy into chemical energy. Nature has evolved photoreceptors in which the reactivity of a chromophore is enhanced by its molecular environment to achieve high quantum yields. The retinal chromophore sterically constrained inside rhodopsin proteins represents an outstanding example of such a control. In a more general framework, mechanical forces acting on a molecular system can strongly modify its reactivity. Herein, we show that the exertion of tensile forces on a simplified retinal chromophore model provokes a substantial and regular increase in the trans-to-cis photoisomerization quantum yield in a counterintuitive way, as these extension forces facilitate the formation of the more compressed cis photoisomer. A rationale for the mechanochemical effect on this photoisomerization mechanism is also proposed. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Synthesis of Nitrogen- and Chlorine-Doped Graphene Quantum Dots for Cancer Cell Imaging.

PubMed

Nafiujjaman, Md; Joon, Hwang; Kwak, Kwang Soo; Lee, Yong-Kyu

2018-06-01

In this study, we synthesized high quantum yield nitrogen and chlorine-doped graphene quantum dots (Cl-GQDs-N) for cancer cell imaging using simple and high production yield hydrothermal method from low-cost fructose. Prepared Cl-GQDs-N are about 30 nm in diameter and these Cl-GQDs-N display powerful blue color photoluminescence under the 365 nm UV lamp. We have further investigated their optical performances under various conditions. In vitro study shows no toxicity effect in normal and cancer cells treated with Cl-GQDs-N. Finally, we believe that our synthesized Cl-GQDs-N will bring more application opportunities in the field of bioimaging, optoelectronics and beyond.

Near-Unity Quantum Yields of Biexciton Emission from CdSe=CdS Nanocrystals Measured Using Single-Particle Spectroscopy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Park, Young-Shin; Malko, Anton V.; Vela, Javier

2011-05-03

Biexciton photoluminescence (PL) quantum yields (Q 2X) of individual CdSe/CdS core-shell nanocrystal quantum dots with various shell thicknesses are derived from independent PL saturation and two-photon correlation measurements. We observe a near-unity Q{sub 2X} for some nanocrystals with an ultrathick 19-monolayer shell. High Q 2X’s are, however, not universal and vary widely among nominally identical nanocrystals indicating a significant dependence of Q 2X upon subtle structural differences. Interestingly, our measurements indicate that high Q 2X’s are not required to achieve complete suppression of PL intensity fluctuations in individual nanocrystals.

Separation of photoactive conformers based on hindered diarylethenes: efficient modulation in photocyclization quantum yields.

PubMed

Li, Wenlong; Jiao, Changhong; Li, Xin; Xie, Yongshu; Nakatani, Keitaro; Tian, He; Zhu, Weihong

2014-04-25

Endowing both solvent independency and excellent thermal bistability, the benzobis(thiadiazole)-bridged diarylethene system provides an efficient approach to realize extremely high photocyclization quantum yields (Φo-c , up to 90.6 %) by both separating completely pure anti-parallel conformer and suppressing intramolecular charge transfer (ICT). © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Excitonic Emission of Monolayer Semiconductors Near-Field Coupled to High-Q Microresonators

NASA Astrophysics Data System (ADS)

Javerzac-Galy, Clément; Kumar, Anshuman; Schilling, Ryan D.; Piro, Nicolas; Khorasani, Sina; Barbone, Matteo; Goykhman, Ilya; Khurgin, Jacob B.; Ferrari, Andrea C.; Kippenberg, Tobias J.

2018-05-01

We present quantum yield measurements of single layer $\\textrm{WSe}_2$ (1L-$\\textrm{WSe}_2$) integrated with high-Q ($Q>10^6$) optical microdisk cavities, using an efficient ($\\eta>$90%) near-field coupling scheme based on a tapered optical fiber. Coupling of the excitonic emission is achieved by placing 1L-WSe$_2$ to the evanescent cavity field. This preserves the microresonator high intrinsic quality factor ($Q>10^6$) below the bandgap of 1L-WSe$_2$. The nonlinear excitation power dependence of the cavity quantum yield is in agreement with an exciton-exciton annihilation model. The cavity quantum yield is $\\textrm{QY}_\\textrm{c}\\sim10^{-3}$, consistent with operation in the \\textit{broad emitter} regime (i.e. the emission lifetime of 1L-WSe$_2$ is significantly shorter than the bare cavity decay time). This scheme can serve as a precise measurement tool for the excitonic emission of layered materials into cavity modes, for both in plane and out of plane excitation.

Photo-kinetics of photoinduced transformation reaction of methylene green with titanium trichloride in different solvents

NASA Astrophysics Data System (ADS)

Nadeem, Syed Muhammad Saqib; Saeed, Rehana

2017-08-01

The photo-kinetics of photoinduced transformation reaction of methylene green and titanium trichloride was investigated in water and different aqueous-alcoholic solvents. The reaction is pseudo-first order, dependent only on the concentration of titanium trichloride at fixed concentration of methylene green. The effect of water and aqueous-alcoholic solvents was studied in the acidic range from 4 to 7. It was observed that the quantum yield (φ) of reaction increased with increase in polarity of the solvent. The quantum yield (φ) was high in acidic condition and decreased with further increase in acidity. The quantum yield (φ) increased sharply with increase in concentration of titanium trichloride while it almost remained unaffected by change in concentration of methylene green. The addition of ions increased the quantum yield (φ) of reaction. The increase in temperature decreased the rate and quantum yield (φ) of reaction. An electron transfer mechanism for the reaction has been proposed in accordance with the kinetics of reaction. The absence of any reaction intermediate was confirmed by spectroscopic investigations. Activation energy ( E a) was calculated by Arrhenius relation. Thermodynamic parameters such as activation energy ( E a), enthalpy change (Δ H), free energy change (Δ G) and entropy change (Δ S) were also evaluated.

Fluorescence quantum yield of carbon dioxide for quantitative UV laser-induced fluorescence in high-pressure flames

NASA Astrophysics Data System (ADS)

Lee, T.; Bessler, W. G.; Yoo, J.; Schulz, C.; Jeffries, J. B.; Hanson, R. K.

2008-11-01

The fluorescence quantum yield for ultraviolet laser-induced fluorescence of CO2 is determined for selected excitation wavelengths in the range 215-250 nm. Wavelength-resolved laser-induced fluorescence (LIF) spectra of CO2, NO, and O2 are measured in the burned gases of a laminar CH4/air flame ( φ=0.9 and 1.1) at 20 bar with additional NO seeded into the flow. The fluorescence spectra are fit to determine the relative contribution of the three species to infer an estimate of fluorescence quantum yield for CO2 that ranges from 2-8×10-6 depending on temperature and excitation wavelength with an estimated uncertainty of ±0.5×10-6. The CO2 fluorescence signal increases linearly with gas pressure for flames with constant CO2 mole fraction for the 10 to 60 bar range, indicating that collisional quenching is not an important contributor to the CO2 fluorescence quantum yield. Spectral simulation calculations are used to choose two wavelengths for excitation of CO2, 239.34 and 242.14 nm, which minimize interference from LIF of NO and O2. Quantitative LIF images of CO2 are demonstrated using these two excitation wavelengths and the measured fluorescence quantum yield.

Photoisomerization of alfa calcidol by a sensitized quantum chain reaction.

PubMed

Estruch, Gastón A; Aramendía, Pedro F

2012-01-01

The production of vitamin D3 is a pharmaceutically relevant process, producing high added-value products. Precursors are extracts from vegetal origin but bearing mainly an E geometry in the 5,6 double bond. The synthesis of vitamin D3 (5-E-α-calcidol) with the correct Z stereochemistry in the 5,6 double bond from the E isomer using anthracene and triethylamine (TEA) as the sensitizer system was studied from the kinetic and mechanistic point of view. The sensitized isomerization of E-calcidol by irradiation of anthracene takes place only in deoxygenated solution and yields the Z isomer in ca 5% yield in the photostationary state. When TEA is added to the system, the E-Z reaction is not inhibited by oxygen any more, the quantum yield of photoisomerization to the Z isomer grows linearly with the concentration of E-calcidol, while conversions higher than 95% to the Z isomer are reached in the photostationary state and E-Z quantum yields as high as 45 at [E-calcidol] = 25 mM are reached. If TEA is replaced by 1,4-diazabicyclo[2.2.2]octane, the reaction rate drops to one-third at the same amine concentration. The observations can be explained by a quantum chain reaction mechanism. The high conversion achieved eliminates the need of isomer separation. © 2011 Wiley Periodicals, Inc. Photochemistry and Photobiology © 2011 The American Society of Photobiology.

Intense visible emission from ZnO/PAAX (X = H or Na) nanocomposite synthesized via a simple and scalable sol-gel method

NASA Astrophysics Data System (ADS)

Zhu, Y.; Apostoluk, A.; Gautier, P.; Valette, A.; Omar, L.; Cornier, T.; Bluet, J. M.; Masenelli-Varlot, K.; Daniele, S.; Masenelli, B.

2016-03-01

Intense visible nano-emitters are key objects for many technologies such as single photon source, bio-labels or energy convertors. Chalcogenide nanocrystals have ruled this domain for several decades. However, there is a demand for cheaper and less toxic materials. In this scheme, ZnO nanoparticles have appeared as potential candidates. At the nanoscale, they exhibit crystalline defects which can generate intense visible emission. However, even though photoluminescence quantum yields as high as 60% have been reported, it still remains to get quantum yield of that order of magnitude which remains stable over a long period. In this purpose, we present hybrid ZnO/polyacrylic acid (PAAH) nanocomposites, obtained from the hydrolysis of diethylzinc in presence of PAAH, exhibiting quantum yield systematically larger than 20%. By optimizing the nature and properties of the polymeric acid, the quantum yield is increased up to 70% and remains stable over months. This enhancement is explained by a model based on the hybrid type II heterostructure formed by ZnO/PAAH. The addition of PAAX (X = H or Na) during the hydrolysis of ZnEt2 represents a cost effective method to synthesize scalable amounts of highly luminescent ZnO/PAAX nanocomposites.

A general quantitative pH sensor developed with dicyandiamide N-doped high quantum yield graphene quantum dots.

PubMed

Wu, Zhu Lian; Gao, Ming Xuan; Wang, Ting Ting; Wan, Xiao Yan; Zheng, Lin Ling; Huang, Cheng Zhi

2014-04-07

A general quantitative pH sensor for environmental and intracellular applications was developed by the facile hydrothermal preparation of dicyandiamide (DCD) N-doped high quantum yield (QY) graphene quantum dots (GQDs) using citric acid (CA) as the carbon source. The obtained N-doped GQDs have excellent photoluminesence (PL) properties with a relatively high QY of 36.5%, suggesting that N-doped chemistry could promote the QY of carbon nanomaterials. The possible mechanism for the formation of the GQDs involves the CA self-assembling into a nanosheet structure through intermolecular H-bonding at the initial stage of the reaction, and then the pure graphene core with many function groups formed through the dehydration between the carboxyl and hydroxyl of the intermolecules under hydrothermal conditions. These N-doped GQDs have low toxicity, and are photostable and pH-sensitive between 1.81 to 8.96, giving a general pH sensor with a wide range of applications from real water to intracellular contents.

Quantum trajectories for high-order-harmonic generation from multiple rescattering events in the long-wavelength regime

NASA Astrophysics Data System (ADS)

He, Lixin; Li, Yang; Wang, Zhe; Zhang, Qingbin; Lan, Pengfei; Lu, Peixiang

2014-05-01

We have performed the quantum trajectory analysis for high-order-harmonic generation (HHG) with different driving laser wavelengths. By defining the ratio of HHG yields of the Nth and first rescattering events (YN/Y1), we quantitatively evaluate the HHG contributions from multiple rescatterings. The results show that the HHG yield ratio increases gradually with the increase of the laser wavelength, which demonstrates that high-order rescatterings provide ascendent contributions to HHG at longer wavelength. By calculating the classical electron trajectories, we find significant differences exist in the electron behaviors between the first and high-order rescatterings. Further investigations have demonstrated that the increasing HHG yield ratio is mainly attributed to the relatively smaller contributions from the short path of the first electron rescattering at longer laser wavelength.

Aqueous synthesis of highly luminescent AgInS2-ZnS quantum dots and their biological applications

NASA Astrophysics Data System (ADS)

Regulacio, Michelle D.; Win, Khin Yin; Lo, Seong Loong; Zhang, Shuang-Yuan; Zhang, Xinhai; Wang, Shu; Han, Ming-Yong; Zheng, Yuangang

2013-02-01

Highly emissive and air-stable AgInS2-ZnS quantum dots (ZAIS QDs) with quantum yields of up to 20% have been successfully synthesized directly in aqueous media in the presence of polyacrylic acid (PAA) and mercaptoacetic acid (MAA) as stabilizing and reactivity-controlling agents. The as-prepared water-dispersible ZAIS QDs are around 3 nm in size, possess the tetragonal chalcopyrite crystal structure, and exhibit long fluorescence lifetimes (>100 ns). In addition, these ZAIS QDs are found to exhibit excellent optical and colloidal stability in physiologically relevant pH values as well as very low cytotoxicity, which render them particularly suitable for biological applications. Their potential use in biological labelling of baculoviral vectors is demonstrated.Highly emissive and air-stable AgInS2-ZnS quantum dots (ZAIS QDs) with quantum yields of up to 20% have been successfully synthesized directly in aqueous media in the presence of polyacrylic acid (PAA) and mercaptoacetic acid (MAA) as stabilizing and reactivity-controlling agents. The as-prepared water-dispersible ZAIS QDs are around 3 nm in size, possess the tetragonal chalcopyrite crystal structure, and exhibit long fluorescence lifetimes (>100 ns). In addition, these ZAIS QDs are found to exhibit excellent optical and colloidal stability in physiologically relevant pH values as well as very low cytotoxicity, which render them particularly suitable for biological applications. Their potential use in biological labelling of baculoviral vectors is demonstrated. Electronic supplementary information (ESI) available: Quantum yields, EDX spectrum and photoluminescence decay curves. See DOI: 10.1039/c3nr34159c

Triazatruxene: A Rigid Central Donor Unit for a D-A3 Thermally Activated Delayed Fluorescence Material Exhibiting Sub-Microsecond Reverse Intersystem Crossing and Unity Quantum Yield via Multiple Singlet-Triplet State Pairs.

PubMed

Dos Santos, Paloma L; Ward, Jonathan S; Congrave, Daniel G; Batsanov, Andrei S; Eng, Julien; Stacey, Jessica E; Penfold, Thomas J; Monkman, Andrew P; Bryce, Martin R

2018-06-01

By inverting the common structural motif of thermally activated delayed fluorescence materials to a rigid donor core and multiple peripheral acceptors, reverse intersystem crossing (rISC) rates are demonstrated in an organic material that enables utilization of triplet excited states at faster rates than Ir-based phosphorescent materials. A combination of the inverted structure and multiple donor-acceptor interactions yields up to 30 vibronically coupled singlet and triplet states within 0.2 eV that are involved in rISC. This gives a significant enhancement to the rISC rate, leading to delayed fluorescence decay times as low as 103.9 ns. This new material also has an emission quantum yield ≈1 and a very small singlet-triplet gap. This work shows that it is possible to achieve both high photoluminescence quantum yield and fast rISC in the same molecule. Green organic light-emitting diode devices with external quantum efficiency >30% are demonstrated at 76 cd m -2 .

The dissociative recombination of O2(+) - The quantum yield of O(1S) and O(1D)

NASA Technical Reports Server (NTRS)

Abreu, V. J.; Solomon, S. C.; Sharp, W. E.; Hays, P. B.

1983-01-01

Data from the visible airglow experiment on the Atmosphere Explorer-E satellite have been used to determine the quantum yield of O(1S) and O(1D) from the dissociative recombination of O2(+). A range of values between 0.09 and 0.23 has been obtained for the quantum yield of O(1S). It is shown that the quantum yield of O(1S) depends on the ratio of electron density to atomic oxygen density. This suggests that the quantum yield of O(1S) may depend on the degree of vibrational excitation of the recombining O2(+). The quantum yield of O(1D) has been measured to be 1.23 + or - 0.42, with no dependence on the electron-oxygen ratio.

Core/Shell NaGdF4:Nd3+/NaGdF4 Nanocrystals with Efficient Near-Infrared to Near-Infrared Downconversion Photoluminescence for Bioimaging Applications

PubMed Central

Chen, Guanying; Ohulchanskyy, Tymish Y.; Liu, Sha; Law, Wing-Cheung; Wu, Fang; Swihart, Mark T.; Ågren, Hans; Prasad, Paras N.

2012-01-01

We have synthesized core/shell NaGdF4:Nd3+/NaGdF4 nanocrystals with an average size of 15 nm and exceptionally high photoluminescence (PL) quantum yield. When excited at 740 nm, the nanocrystals manifest spectrally distinguished, near infrared to near infrared (NIR-to-NIR) downconversion PL peaked at ~900, ~1050, and ~1300 nm. The absolute quantum yield of NIR-to-NIR PL reached 40% for core-shell nanoparticles dispersed in hexane. Time-resolved PL measurements revealed that this high quantum yield was achieved through suppression of nonradiative recombination originating from surface states and cross relaxations between dopants. NaGdF4:Nd3+/NaGdF4 nanocrystals, synthesized in organic media, were further converted to be water-dispersible by eliminating the capping ligand of oleic acid. NIR-to-NIR PL bioimaging was demonstrated both in vitro and in vivo through visualization of the NIR-to-NIR PL at ~900 nm under incoherent lamp light excitation. The fact that both excitation and the PL of these nanocrystals are in the biological window of optical transparency, combined with their high quantum efficiency, spectral sharpness and photostability, makes these nanocrystals extremely promising as optical biomaging probes. PMID:22401578

Strongly Coupled Tin-Halide Perovskites to Modulate Light Emission: Tunable 550-640 nm Light Emission (FWHM 36-80 nm) with a Quantum Yield of up to 6.4.

PubMed

Chen, Min-Yi; Lin, Jin-Tai; Hsu, Chia-Shuo; Chang, Chung-Kai; Chiu, Ching-Wen; Chen, Hao Ming; Chou, Pi-Tai

2018-05-01

Colloidal perovskite quantum dots represent one of the most promising materials for applications in solar cells and photoluminescences. These devices require a low density of crystal defects and a high yield of photogenerated carriers, which are difficult to realize in tin-halide perovskite because of the intrinsic instability of tin during nucleation. Here, an enhancement in the luminescent property of tin-halide perovskite nanoplates (TPNPs) that are composed of strongly coupled layered structures with the chemical formula of PEA 2 SnX 4 (PEA = C 6 H 5 (CH 2 ) 2 NH 3 , X = Br, I) is reported. TPNPs (X = I) show an emission at a wavelength of 640 nm, with high quantum yield of 6.40 ± 0.14% and full width at half maximum (FWHM) as small as 36 nm. The presence of aliphatic carboxylic acid is found to play a key role in reducing the tin perovskite defect density, which significantly improves the emission intensity and stability of TPNPs. Upon mixing iodo- and bromo- precursors, the emission wavelength is successfully tuned from 640 nm (PEA 2 SnI 4 ) to 550 nm (PEA 2 SnBr 4 ), with a corresponding emission quantum yield and FWHM of 0.16-6.40% and 36-80 nm, respectively. The results demonstrate a major advance for the emission yield and tunability of tin-halide perovskites. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Accurate quantum yields by laser gain vs absorption spectroscopy - Investigation of Br/Br(asterisk) channels in photofragmentation of Br2 and IBr

NASA Technical Reports Server (NTRS)

Haugen, H. K.; Weitz, E.; Leone, S. R.

1985-01-01

Various techniques have been used to study photodissociation dynamics of the halogens and interhalogens. The quantum yields obtained by these techniques differ widely. The present investigation is concerned with a qualitatively new approach for obtaining highly accurate quantum yields for electronically excited states. This approach makes it possible to obtain an accuracy of 1 percent to 3 percent. It is shown that measurement of the initial transient gain/absorption vs the final absorption in a single time-resolved signal is a very accurate technique in the study of absolute branching fractions in photodissociation. The new technique is found to be insensitive to pulse and probe laser characteristics, molecular absorption cross sections, and absolute precursor density.

Sample-averaged biexciton quantum yield measured by solution-phase photon correlation.

PubMed

Beyler, Andrew P; Bischof, Thomas S; Cui, Jian; Coropceanu, Igor; Harris, Daniel K; Bawendi, Moungi G

2014-12-10

The brightness of nanoscale optical materials such as semiconductor nanocrystals is currently limited in high excitation flux applications by inefficient multiexciton fluorescence. We have devised a solution-phase photon correlation measurement that can conveniently and reliably measure the average biexciton-to-exciton quantum yield ratio of an entire sample without user selection bias. This technique can be used to investigate the multiexciton recombination dynamics of a broad scope of synthetically underdeveloped materials, including those with low exciton quantum yields and poor fluorescence stability. Here, we have applied this method to measure weak biexciton fluorescence in samples of visible-emitting InP/ZnS and InAs/ZnS core/shell nanocrystals, and to demonstrate that a rapid CdS shell growth procedure can markedly increase the biexciton fluorescence of CdSe nanocrystals.

Characterization of cap-shaped silver particles for surface-enhanced fluorescence effects.

PubMed

Yamaguchi, Tetsuji; Kaya, Takatoshi; Takei, Hiroyuki

2007-05-15

Surface-enhanced fluorescence has potentially many desirable properties as an analytical method for medical diagnostics, but the effect observed so far is rather modest and only in conjunction with fluorophores with low quantum yields. Coupled with the fact that preparation of suitable surfaces at low costs has been difficult, this has limited its utilities. Here we report a novel method for forming uniform and reproducible surfaces with respectable enhancement ratios even for high-quantum-yield fluorophores. Formation of dense surface-adsorbed latex spheres on a flat surface via partial aggregation, followed by evaporation of silver, results in a film consisting of cap-shaped silver particles at high densities. Binding of fluorescence biomolecules, either through physisorption or antigen-antibody reaction, was performed, and enhancements close to 50 have been observed with fluorophores such as R-phycoerythrin and Alexa 546-labeled, bovine serum albumin, both of which have quantum yields around 0.8. We attribute this to the unique shape of the silver particle and the presence of abundant gaps among adjacent particles at high densities. The effectiveness of the new surface is also demonstrated with IL-6 sandwich assays.

Improved Charge-Transfer Fluorescent Dyes

NASA Technical Reports Server (NTRS)

Meador, Michael

2005-01-01

Improved charge-transfer fluorescent dyes have been developed for use as molecular probes. These dyes are based on benzofuran nuclei with attached phenyl groups substituted with, variously, electron donors, electron acceptors, or combinations of donors and acceptors. Optionally, these dyes could be incorporated as parts of polymer backbones or as pendant groups or attached to certain surfaces via self-assembly-based methods. These dyes exhibit high fluorescence quantum yields -- ranging from 0.2 to 0.98, depending upon solvents and chemical structures. The wavelengths, quantum yields, intensities, and lifetimes of the fluorescence emitted by these dyes vary with (and, hence, can be used as indicators of) the polarities of solvents in which they are dissolved: In solvents of increasing polarity, fluorescence spectra shift to longer wavelengths, fluorescence quantum yields decrease, and fluorescence lifetimes increase. The wavelengths, quantum yields, intensities, and lifetimes are also expected to be sensitive to viscosities and/or glass-transition temperatures. Some chemical species -- especially amines, amino acids, and metal ions -- quench the fluorescence of these dyes, with consequent reductions in intensities, quantum yields, and lifetimes. As a result, the dyes can be used to detect these species. Another useful characteristic of these dyes is a capability for both two-photon and one-photon absorption. Typically, these dyes absorb single photons in the ultraviolet region of the spectrum (wavelengths < 400 nm) and emit photons in the long-wavelength ultraviolet, visible, and, when dissolved in some solvents, near-infrared regions. In addition, these dyes can be excited by two-photon absorption at near-infrared wavelengths (600 to 800 nm) to produce fluorescence spectra identical to those obtained in response to excitation by single photons at half the corresponding wavelengths (300 to 400 nm). While many prior fluorescent dyes exhibit high quantum yields, solvent-polarity- dependent fluorescence behavior, susceptibility to quenching by certain chemical species, and/or two-photon fluorescence, none of them has the combination of all of these attributes. Because the present dyes do have all of these attributes, they have potential utility as molecular probes in a variety of applications. Examples include (1) monitoring curing and deterioration of polymers; (2) monitoring protein expression; (3) high-throughput screening of drugs; (4) monitoring such chemical species as glucose, amines, amino acids, and metal ions; and (5) photodynamic therapy of cancers and other diseases.

Quantum Yield of Single Surface Plasmons Generated by a Quantum Dot Coupled with a Silver Nanowire.

PubMed

Li, Qiang; Wei, Hong; Xu, Hongxing

2015-12-09

The interactions between surface plasmons (SPs) in metal nanostructures and excitons in quantum emitters (QEs) lead to many interesting phenomena and potential applications that are strongly dependent on the quantum yield of SPs. The difficulty in distinguishing all the possible exciton recombination channels hinders the experimental determination of SP quantum yield. Here, we experimentally measured for the first time the quantum yield of single SPs generated by the exciton-plasmon coupling in a system composed of a single quantum dot and a silver nanowire (NW). By utilizing the SP guiding property of the NW, the decay rates of all the exciton recombination channels, i.e., direct free space radiation channel, SP generation channel, and nonradiative damping channel, are quantitatively obtained. It is determined that the optimum emitter-NW coupling distance for the largest SP quantum yield is about 10 nm, resulting from the different distance-dependent decay rates of the three channels. These results are important for manipulating the coupling between plasmonic nanostructures and QEs and developing on-chip quantum plasmonic devices for potential nanophotonic and quantum information applications.

Action spectra of photosystems II and I and quantum yield of photosynthesis in leaves in State 1.

PubMed

Laisk, Agu; Oja, Vello; Eichelmann, Hillar; Dall'Osto, Luca

2014-02-01

The spectral global quantum yield (YII, electrons/photons absorbed) of photosystem II (PSII) was measured in sunflower leaves in State 1 using monochromatic light. The global quantum yield of PSI (YI) was measured using low-intensity monochromatic light flashes and the associated transmittance change at 810nm. The 810-nm signal change was calibrated based on the number of electrons generated by PSII during the flash (4·O2 evolution) which arrived at the PSI donor side after a delay of 2ms. The intrinsic quantum yield of PSI (yI, electrons per photon absorbed by PSI) was measured at 712nm, where photon absorption by PSII was small. The results were used to resolve the individual spectra of the excitation partitioning coefficients between PSI (aI) and PSII (aII) in leaves. For comparison, pigment-protein complexes for PSII and PSI were isolated, separated by sucrose density ultracentrifugation, and their optical density was measured. A good correlation was obtained for the spectral excitation partitioning coefficients measured by these different methods. The intrinsic yield of PSI was high (yI=0.88), but it absorbed only about 1/3 of quanta; consequently, about 2/3 of quanta were absorbed by PSII, but processed with the low intrinsic yield yII=0.63. In PSII, the quantum yield of charge separation was 0.89 as detected by variable fluorescence Fv/Fm, but 29% of separated charges recombined (Laisk A, Eichelmann H and Oja V, Photosynth. Res. 113, 145-155). At wavelengths less than 580nm about 30% of excitation is absorbed by pigments poorly connected to either photosystem, most likely carotenoids bound in pigment-protein complexes. Copyright © 2013 Elsevier B.V. All rights reserved.

Adaptation to high CO2 concentration in an optimal environment: radiation capture, canopy quantum yield and carbon use efficiency

NASA Technical Reports Server (NTRS)

Monje, O.; Bugbee, B.

1998-01-01

The effect of elevated [CO2] on wheat (Triticum aestivum L. Veery 10) productivity was examined by analysing radiation capture, canopy quantum yield, canopy carbon use efficiency, harvest index and daily C gain. Canopies were grown at either 330 or 1200 micromoles mol-1 [CO2] in controlled environments, where root and shoot C fluxes were monitored continuously from emergence to harvest. A rapidly circulating hydroponic solution supplied nutrients, water and root zone oxygen. At harvest, dry mass predicted from gas exchange data was 102.8 +/- 4.7% of the observed dry mass in six trials. Neither radiation capture efficiency nor carbon use efficiency were affected by elevated [CO2], but yield increased by 13% due to a sustained increase in canopy quantum yield. CO2 enrichment increased root mass, tiller number and seed mass. Harvest index and chlorophyll concentration were unchanged, but CO2 enrichment increased average life cycle net photosynthesis (13%, P < 0.05) and root respiration (24%, P < 0.05). These data indicate that plant communities adapt to CO2 enrichment through changes in C allocation. Elevated [CO2] increases sink strength in optimal environments, resulting in sustained increases in photosynthetic capacity, canopy quantum yield and daily C gain throughout the life cycle.

Fluorescent porous silicon biological probes with high quantum efficiency and stability.

PubMed

Tu, Chang-Ching; Chou, Ying-Nien; Hung, Hsiang-Chieh; Wu, Jingda; Jiang, Shaoyi; Lin, Lih Y

2014-12-01

We demonstrate porous silicon biological probes as a stable and non-toxic alternative to organic dyes or cadmium-containing quantum dots for imaging and sensing applications. The fluorescent silicon quantum dots which are embedded on the porous silicon surface are passivated with carboxyl-terminated ligands through stable Si-C covalent bonds. The porous silicon bio-probes have shown photoluminescence quantum yield around 50% under near-UV excitation, with high photochemical and thermal stability. The bio-probes can be efficiently conjugated with antibodies, which is confirmed by a standard enzyme-linked immunosorbent assay (ELISA) method.

Sample-Averaged Biexciton Quantum Yield Measured by Solution-Phase Photon Correlation

DOE PAGES

Beyler, Andrew P.; Bischof, Thomas S.; Cui, Jian; ...

2014-11-19

The brightness of nanoscale optical materials such as semiconductor nanocrystals is currently limited in high excitation flux applications by inefficient multiexciton fluorescence. We have devised a solution-phase photon correlation measurement that can conveniently and reliably measure the average biexciton-to-exciton quantum yield ratio of an entire sample without user selection bias. This technique can be used to investigate the multiexciton recombination dynamics of a broad scope of synthetically underdeveloped materials, including those with low exciton quantum yields and poor fluorescence stability. Here in this study, we have applied this method to measure weak biexciton fluorescence in samples of visible-emitting InP/ZnS andmore » InAs/ZnS core/shell nanocrystals, and to demonstrate that a rapid CdS shell growth procedure can markedly increase the biexciton fluorescence of CdSe nanocrystals.« less

Sample-Averaged Biexciton Quantum Yield Measured by Solution-Phase Photon Correlation

PubMed Central

Beyler, Andrew P.; Bischof, Thomas S.; Cui, Jian; Coropceanu, Igor; Harris, Daniel K.; Bawendi, Moungi G.

2015-01-01

The brightness of nanoscale optical materials such as semiconductor nanocrystals is currently limited in high excitation flux applications by inefficient multiexciton fluorescence. We have devised a solution-phase photon correlation measurement that can conveniently and reliably measure the average biexciton-to-exciton quantum yield ratio of an entire sample without user selection bias. This technique can be used to investigate the multiexciton recombination dynamics of a broad scope of synthetically underdeveloped materials, including those with low exciton quantum yields and poor fluorescence stability. Here, we have applied this method to measure weak biexciton fluorescence in samples of visible-emitting InP/ZnS and InAs/ZnS core/shell nanocrystals, and to demonstrate that a rapid CdS shell growth procedure can markedly increase the biexciton fluorescence of CdSe nanocrystals. PMID:25409496

Green, Rapid, and Universal Preparation Approach of Graphene Quantum Dots under Ultraviolet Irradiation.

PubMed

Zhu, Jinli; Tang, Yanfeng; Wang, Gang; Mao, Jiarong; Liu, Zhiduo; Sun, Tongming; Wang, Miao; Chen, Da; Yang, Yucheng; Li, Jipeng; Deng, Yuan; Yang, Siwei

2017-04-26

It is of great significance and importance to explore a mild, clean, and highly efficient universal approach for the synthesis of graphene quantum dots. Herein, we introduced a new green, rapid, and universal preparation approach for graphene quantum dots via the free-radical polymerization of oxygen-containing aromatic compounds under ultraviolet irradiation. This approach had a high yield (86%), and the byproducts are only H 2 O and CO 2 . The obtained graphene quantum dots were well-crystallized and showed remarkable optical and biological properties. The colorful, different-sized graphene quantum dots can be used in fluorescent bioimaging in vitro and in vivo. This approach is suitable not only for the preparation of graphene quantum dots but also for heteroatom-doped graphene quantum dots.

High-Z Nanoparticle/Polymer Nanocomposites for Gamma-Ray Scintillation Detectors

NASA Astrophysics Data System (ADS)

Liu, Chao

An affordable and reliable solution for spectroscopic gamma-ray detection has long been sought after due to the needs from research, defense, and medical applications. Scintillators resolve gamma energy by proportionally converting a single high-energy photon into a number of photomultiplier-tube-detectable low-energy photons, which is considered a more affordable solution for general purposes compared to the delicate semiconductor detectors. An ideal scintillator should simultaneously exhibit the following characteristics: 1) high atomic number (Z) for high gamma stopping power and photoelectron production; 2) high light yield since the energy resolution is inversely proportional to the square root of light yield; 3) short emission decay lifetime; and 4) low cost and scalable production. However, commercial scintillators made from either inorganic single crystals or plastics fail to satisfy all requirements due to their intrinsic material properties and fabrication limitations. The concept of adding high-Z constituents into plastic scintillators to harness high Z, low cost, and fast emission in the resulting nanocomposite scintillators is not new in and of itself. Attempts have been made by adding organometallics, quantum dots, and scintillation nanocrystals into the plastic matrix. High-Z organometallics have long been used to improve the Z of plastic scintillators; however, their strong spin-orbit coupling effect entails careful triplet energy matching using expensive triplet emitters to avoid severe quenching of the light yield. On the other hand, reported quantum dot- and nanocrystal-polymer nanocomposites suffer from moderate Z and high optical loss due to aggregation and self-absorption at loadings higher than 10 wt%, limiting their potential for practical application. This dissertation strives to improve the performance of nanoparticle-based nanocomposite scintillators. One focus is to synthesize transparent nanocomposites with higher loadings of high-Z inorganic nanoparticles. A facile single-precursor method is first developed to synthesize HfO2 nanoparticles, the highest-Z simple oxide with band gap larger than polyvinyltoluene, with uniform size distribution around 5 nm. A nanoparticle-surface-modification protocol is then developed for the fabrication of transparent nanocomposite monoliths with high nanoparticle loadings (up to 40 wt%). Using this method, transparent HfO2-loaded blue-emitting nanocomposite scintillators (2 mm thick, transmittance at 550 nm >75%) have been fabricated capable of producing a full energy photopeak for 662 keV gamma rays, with the best deconvoluted photopeak energy resolution < 8%, representing a significant improvement over previous nanoparticle-based nanocomposite scintillators. Although the HfO2 work represents a great improvement over previous reports, it is also found in this system that the light yield deteriorates at higher nanoparticle loadings. This is attributed to the trapping of fast electron energy deposited in the non-emitting nanoparticles. To overcome this deterioration issue, a revisit to the previously proposed quantum-dot-loaded nanocomposite scintillator is made with significant improvements. Transparent, ultra-high-loading (up to 60 wt%) CdxZn1-xS/ZnS core/shell quantum dot/polymer nanocomposite monoliths are first synthesized by in situ copolymerization of the partially mathacrylate-functionalized quantum dots in a monomer solution. With efficient Forster resonance energy transfer from the high-atomic-number quantum dots to lower-band-gap organic dyes, quantum-dot-borne excitons are extracted for photon production. The resulting nanocomposites thus exhibit unprecedented simultaneous enhancements in both light yield (visible photons produced per MeV of gamma photon energy) and gamma attenuation power. In a best demonstration, a 60 wt% quantum-dot nanocomposite scintillator exhibits a light yield of 9255 photons/MeV and a photopeak resolution of 9.8% under 662 keV Cs-137 gamma irradiation, demonstrating the potential of this model system for future high-performance low-cost spectroscopic gamma detectors.

Size-Dependent Biexciton Quantum Yields and Carrier Dynamics of Quasi-Two-Dimensional Core/Shell Nanoplatelets

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ma, Xuedan; Diroll, Benjamin T.; Cho, Wooje

Quasi-two-dimensional nanoplatelets (NPLs) possess fundamentally different excitonic properties from zero-dimensional quantum dots. We study lateral size-dependent photon emission statistics and carrier dynamics of individual NPLs using second-order photon correlation (g( 2)(τ)) spectroscopy and photoluminescence (PL) intensity-dependent lifetime analysis. Room-temperature radiative lifetimes of NPLs can be derived from maximum PL intensity periods in PL time traces. It first decreases with NPL lateral size and then stays constant, deviating from the electric dipole approximation. Analysis of the PL time traces further reveals that the single exciton quantum yield in NPLs decreases with NPL lateral size and increases with protecting shell thickness, indicatingmore » the importance of surface passivation on NPL emission quality. Second-order photon correlation (g( 2)(τ)) studies of single NPLs show that the biexciton quantum yield is strongly dependent on the lateral size and single exciton quantum yield of the NPLs. In large NPLs with unity single exciton quantum yield, the corresponding biexciton quantum yield can reach unity. In conclusion, these findings reveal that by careful growth control and core–shell material engineering, NPLs can be of great potential for light amplification and integrated quantum photonic applications.« less

Size-Dependent Biexciton Quantum Yields and Carrier Dynamics of Quasi-Two-Dimensional Core/Shell Nanoplatelets

DOE PAGES

Ma, Xuedan; Diroll, Benjamin T.; Cho, Wooje; ...

2017-08-08

Quasi-two-dimensional nanoplatelets (NPLs) possess fundamentally different excitonic properties from zero-dimensional quantum dots. We study lateral size-dependent photon emission statistics and carrier dynamics of individual NPLs using second-order photon correlation (g( 2)(τ)) spectroscopy and photoluminescence (PL) intensity-dependent lifetime analysis. Room-temperature radiative lifetimes of NPLs can be derived from maximum PL intensity periods in PL time traces. It first decreases with NPL lateral size and then stays constant, deviating from the electric dipole approximation. Analysis of the PL time traces further reveals that the single exciton quantum yield in NPLs decreases with NPL lateral size and increases with protecting shell thickness, indicatingmore » the importance of surface passivation on NPL emission quality. Second-order photon correlation (g( 2)(τ)) studies of single NPLs show that the biexciton quantum yield is strongly dependent on the lateral size and single exciton quantum yield of the NPLs. In large NPLs with unity single exciton quantum yield, the corresponding biexciton quantum yield can reach unity. In conclusion, these findings reveal that by careful growth control and core–shell material engineering, NPLs can be of great potential for light amplification and integrated quantum photonic applications.« less

Violet-to-Blue Gain and Lasing from Colloidal CdS Nanoplatelets: Low-Threshold Stimulated Emission Despite Low Photoluminescence Quantum Yield

DOE Office of Scientific and Technical Information (OSTI.GOV)

Diroll, Benjamin T.; Talapin, Dmitri V.; Schaller, Richard D.

Amplified spontaneous emission (ASE) and lasing from solution-processed materials are demonstrated in the challenging violet-to-blue (430–490 nm) spectral region for colloidal nanoplatelets of CdS and newly synthesized core/shell CdS/ZnS nanoplatelets. Despite modest band-edge photoluminescence quantum yields of 2% or less for single excitons, which we show results from hole trapping, the samples exhibit low ASE thresholds. Furthermore, four-monolayer CdS samples show ASE at shorter wavelengths than any reported film of colloidal quantum-confined material. This work underlines that low quantum yields for single excitons do not necessarily lead to a poor gain medium. The low ASE thresholds originate from negligible dispersionmore » in thickness, large absorption cross sections of 2.8 × 10–14 cm–2, and rather slow (150 to 300 ps) biexciton recombination. We show that under higher-fluence excitation, ASE can kinetically outcompete hole trapping. Using nanoplatelets as the gain medium, lasing is observed in a linear optical cavity. This work confirms the fundamental advantages of colloidal quantum well structures as gain media, even in the absence of high photoluminescence efficiency.« less

Stable CdS QDs with intense broadband photoluminescence and high quantum yields

NASA Astrophysics Data System (ADS)

Mandal, Abhijit; Saha, Jony; De, Goutam

2011-11-01

Aqueous synthesis of CdS quantum dots (QDs) using thiolactic acid (TLA) as a capping agent was reported. These QDs exhibited excellent colloidal and photostability over a span of 2 years and showed intense broadband and almost white photoluminescence suitable for solid state lighting devices. The photoluminescence (PL) property of the aqueous CdS QDs is optimized by adjusting various processing parameters. The highest quantum yield (QY) achieved for TLA capped CdS QDs of average size 3.5 nm was ˜50%. Luminescence lifetime measurements of CdS-TLA QDs indicated longer lifetimes and a larger contribution of the surface-related emission, indicating removal of quenching defects.

Absolute I(asterisk) quantum yields for the ICN A state by diode laser gain-vs-absorption spectroscopy

NASA Technical Reports Server (NTRS)

Hess, Wayne P.; Leone, Stephen R.

1987-01-01

Absolute I(asterisk) quantum yields have been measured as a function of wavelength for room temperature photodissociation of the ICN A state continuum. The yields are obtained by the technique of time-resolved diode laser gain-vs-absorption spectroscopy. Quantum yields are evaluated at seven wavelengths from 248 to 284 nm. The yield at 266 nm is 66.0 + or - 2 percent and it falls off to 53.4 + or - 2 percent and 44.0 + or - 4 percent at 284 and 248 nm, respectively. The latter values are significantly higher than those obtained by previous workers using infrared fluorescence. Estimates of I(asterisk) quantum yields obtained from analysis of CN photofragment rotational distributions, as discussed by other workers, are in good agreement with the I(asterisk) yields reported here. The results are considered in conjunction with recent theoretical and experimental work on the CN rotational distributions and with previous I(asterisk) quantum yield results.

Peptide-Decorated Tunable-Fluorescence Graphene Quantum Dots.

PubMed

Sapkota, Bedanga; Benabbas, Abdelkrim; Lin, Hao-Yu Greg; Liang, Wentao; Champion, Paul; Wanunu, Meni

2017-03-22

We report here the synthesis of graphene quantum dots with tunable size, surface chemistry, and fluorescence properties. In the size regime 15-35 nm, these quantum dots maintain strong visible light fluorescence (mean quantum yield of 0.64) and a high two-photon absorption (TPA) cross section (6500 Göppert-Mayer units). Furthermore, through noncovalent tailoring of the chemistry of these quantum dots, we obtain water-stable quantum dots. For example, quantum dots with lysine groups bind strongly to DNA in solution and inhibit polymerase-based DNA strand synthesis. Finally, by virtue of their mesoscopic size, the quantum dots exhibit good cell permeability into living epithelial cells, but they do not enter the cell nucleus.

Protein-induced Photophysical Changes to the Amyloid Indicator Dye Thioflavin T

DOE Office of Scientific and Technical Information (OSTI.GOV)

L Wolfe; M Calabrese; A Nath

2011-12-31

The small molecule thioflavin T (ThT) is a defining probe for the identification and mechanistic study of amyloid fiber formation. As such, ThT is fundamental to investigations of serious diseases such as Alzheimer's disease, Parkinson disease, and type II diabetes. For each disease, a different protein undergoes conformational conversion to a {beta}-sheet rich fiber. The fluorescence of ThT exhibits an increase in quantum yield upon binding these fibers. Despite its widespread use, the structural basis for binding specificity and for the changes to the photophysical properties of ThT remain poorly understood. Here, we report the co-crystal structures of ThT withmore » two alternative states of {beta}-2 microglobulin ({beta}2m); one monomeric, the other an amyloid-like oligomer. In the latter, the dye intercalates between {beta}-sheets orthogonal to the {beta}-strands. Importantly, the fluorophore is bound in such a manner that a photophysically relevant torsion is limited to a range of angles generally associated with low, not high, quantum yield. Quantum mechanical assessment of the fluorophore shows the electronic distribution to be strongly stabilized by aromatic interactions with the protein. Monomeric {beta}2m gives little increase in ThT fluorescence despite showing three fluorophores, at two binding sites, in configurations generally associated with high quantum yield. Our efforts fundamentally extend existing understanding about the origins of amyloid-induced photophysical changes. Specifically, the {beta}-sheet interface that characterizes amyloid acts both sterically and electronically to stabilize the fluorophore's ground state electronic distribution. By preventing the fluorophore from adopting its preferred excited state configuration, nonradiative relaxation pathways are minimized and quantum yield is increased.« less

Protein-induced photophysical changes to the amyloid indicator dye thioflavin T

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wolfe, Leslie S.; Calabrese, Matthew F.; Nath, Abhinav

2010-10-04

The small molecule thioflavin T (ThT) is a defining probe for the identification and mechanistic study of amyloid fiber formation. As such, ThT is fundamental to investigations of serious diseases such as Alzheimer's disease, Parkinson disease, and type II diabetes. For each disease, a different protein undergoes conformational conversion to a {beta}-sheet rich fiber. The fluorescence of ThT exhibits an increase in quantum yield upon binding these fibers. Despite its widespread use, the structural basis for binding specificity and for the changes to the photophysical properties of ThT remain poorly understood. Here, we report the co-crystal structures of ThT withmore » two alternative states of {beta}-2 microglobulin ({beta}2m); one monomeric, the other an amyloid-like oligomer. In the latter, the dye intercalates between {beta}-sheets orthogonal to the {beta}-strands. Importantly, the fluorophore is bound in such a manner that a photophysically relevant torsion is limited to a range of angles generally associated with low, not high, quantum yield. Quantum mechanical assessment of the fluorophore shows the electronic distribution to be strongly stabilized by aromatic interactions with the protein. Monomeric {beta}2m gives little increase in ThT fluorescence despite showing three fluorophores, at two binding sites, in configurations generally associated with high quantum yield. Our efforts fundamentally extend existing understanding about the origins of amyloid-induced photophysical changes. Specifically, the {beta}-sheet interface that characterizes amyloid acts both sterically and electronically to stabilize the fluorophore's ground state electronic distribution. By preventing the fluorophore from adopting its preferred excited state configuration, nonradiative relaxation pathways are minimized and quantum yield is increased.« less

The effect of axial ligands on the quantum yield of singlet oxygen of new silicon phthalocyanine

NASA Astrophysics Data System (ADS)

Lv, Huafei; Zhang, Xuemei; Yu, Xinxin; Pan, Sujuan; Xie, Shusen; Yang, Hongqin; Peng, Yiru

2016-10-01

The singlet oxygen (1O2) production abilitity is an important factor to assess their potential as effective of photosensitizers. In this paper, the 1O2 production rate, production rate constant and quantum yield of silicon(IV) phthalocyanine axially bearing 1-3 generation dendritic substituents were evaluated by a high performance liquid chromatographic method. The results show that the 1O2 production rate and production rate constant of these compounds increase gradually with dendritic generations increase. And the 1O2 quantum yield of silicon(IV) phthalocyanine with first generation dendritic ligand was the highest. This may be due to the isolation effect of the dendritic ligands on the phthalocyanine core. The parameters of the observed 1O2 production properties will provide valuable data for these dendrimer phthalocyanines as promising photosensitizer in PDT application.

Lunisolar tidal force and its relationship to chlorophyll fluorescence in Arabidopsis thaliana.

PubMed

Fisahn, Joachim; Klingelé, Emile; Barlow, Peter

2015-01-01

The yield of chlorophyll fluorescence Ft was measured in leaves of Arabidopsis thaliana over periods of several days under conditions of continuous illumination (LL) without the application of saturating light pulses. After linearization of the time series of the chlorophyll fluorescence yield (ΔFt), oscillations became apparent with periodicities in the circatidal range. Alignments of these linearized time series ΔFt with the lunisolar tidal acceleration revealed high degrees of synchrony and phase congruence. Similar congruence with the lunisolar tide was obtained with the linearized quantum yield of PSII (ΔФII), recorded after application of saturating light pulses. These findings strongly suggest that there is an exogenous timekeeper which is a stimulus for the oscillations detected in both the linearized yield of chlorophyll fluorescence (ΔFt) and the linearized quantum yield of PSII (ΔФII).

Lunisolar tidal force and its relationship to chlorophyll fluorescence in Arabidopsis thaliana

PubMed Central

Fisahn, Joachim; Klingelé, Emile; Barlow, Peter

2015-01-01

The yield of chlorophyll fluorescence Ft was measured in leaves of Arabidopsis thaliana over periods of several days under conditions of continuous illumination (LL) without the application of saturating light pulses. After linearization of the time series of the chlorophyll fluorescence yield (ΔFt), oscillations became apparent with periodicities in the circatidal range. Alignments of these linearized time series ΔFt with the lunisolar tidal acceleration revealed high degrees of synchrony and phase congruence. Similar congruence with the lunisolar tide was obtained with the linearized quantum yield of PSII (ΔФII), recorded after application of saturating light pulses. These findings strongly suggest that there is an exogenous timekeeper which is a stimulus for the oscillations detected in both the linearized yield of chlorophyll fluorescence (ΔFt) and the linearized quantum yield of PSII (ΔФII). PMID:26376108

High yield and ultrafast sources of electrically triggered entangled-photon pairs based on strain-tunable quantum dots.

PubMed

Zhang, Jiaxiang; Wildmann, Johannes S; Ding, Fei; Trotta, Rinaldo; Huo, Yongheng; Zallo, Eugenio; Huber, Daniel; Rastelli, Armando; Schmidt, Oliver G

2015-12-01

Triggered sources of entangled photon pairs are key components in most quantum communication protocols. For practical quantum applications, electrical triggering would allow the realization of compact and deterministic sources of entangled photons. Entangled-light-emitting-diodes based on semiconductor quantum dots are among the most promising sources that can potentially address this task. However, entangled-light-emitting-diodes are plagued by a source of randomness, which results in a very low probability of finding quantum dots with sufficiently small fine structure splitting for entangled-photon generation (∼10(-2)). Here we introduce strain-tunable entangled-light-emitting-diodes that exploit piezoelectric-induced strains to tune quantum dots for entangled-photon generation. We demonstrate that up to 30% of the quantum dots in strain-tunable entangled-light-emitting-diodes emit polarization-entangled photons. An entanglement fidelity as high as 0.83 is achieved with fast temporal post selection. Driven at high speed, that is 400 MHz, strain-tunable entangled-light-emitting-diodes emerge as promising devices for high data-rate quantum applications.

Highly Luminescent Phase-Stable CsPbI3 Perovskite Quantum Dots Achieving Near 100% Absolute Photoluminescence Quantum Yield.

PubMed

Liu, Feng; Zhang, Yaohong; Ding, Chao; Kobayashi, Syuusuke; Izuishi, Takuya; Nakazawa, Naoki; Toyoda, Taro; Ohta, Tsuyoshi; Hayase, Shuzi; Minemoto, Takashi; Yoshino, Kenji; Dai, Songyuan; Shen, Qing

2017-10-24

Perovskite quantum dots (QDs) as a new type of colloidal nanocrystals have gained significant attention for both fundamental research and commercial applications owing to their appealing optoelectronic properties and excellent chemical processability. For their wide range of potential applications, synthesizing colloidal QDs with high crystal quality is of crucial importance. However, like most common QD systems such as CdSe and PbS, those reported perovskite QDs still suffer from a certain density of trapping defects, giving rise to detrimental nonradiative recombination centers and thus quenching luminescence. In this paper, we show that a high room-temperature photoluminescence quantum yield of up to 100% can be obtained in CsPbI 3 perovskite QDs, signifying the achievement of almost complete elimination of the trapping defects. This is realized with our improved synthetic protocol that involves introducing organolead compound trioctylphosphine-PbI 2 (TOP-PbI 2 ) as the reactive precursor, which also leads to a significantly improved stability for the resulting CsPbI 3 QD solutions. Ultrafast kinetic analysis with time-resolved transient absorption spectroscopy evidence the negligible electron or hole-trapping pathways in our QDs, which explains such a high quantum efficiency. We expect the successful synthesis of the "ideal" perovskite QDs will exert profound influence on their applications to both QD-based light-harvesting and -emitting devices.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sutter-Fella, Carolin M.; Li, Yanbo; Amani, Matin

Hybrid organic-inorganic halide perovskite based semiconductor materials are attractive for use in a wide range of optoelectronic devices because they combine the advantages of suitable optoelectronic attributes and simultaneously low-cost solution processability. Here, we present a two-step low-pressure vapor-assisted solution process to grow high quality homogeneous CH 3NH 3PbI 3-xBr x perovskite films over the full band gap range of 1.6-2.3 eV. Photoluminescence light-in versus light-out characterization techniques are used to provide new insights into the optoelectronic properties of Br-containing hybrid organic-inorganic perovskites as a function of optical carrier injection by employing pump-powers over a 6 orders of magnitude dynamicmore » range. The internal luminescence quantum yield of wide band gap perovskites reaches impressive values up to 30%. This high quantum yield translates into substantial quasi-Fermi level splitting and high "luminescence or optically implied" open-circuit voltage. Most importantly, both attributes, high internal quantum yield and high optically implied open-circuit voltage, are demonstrated over the entire band gap range (1.6 eV ≤ E g ≤ 2.3 eV). These results establish the versatility of Br-containing perovskite semiconductors for a variety of applications and especially for the use as high-quality top cell in tandem photovoltaic devices in combination with industry dominant Si bottom cells. (Figure Presented).« less

Note: Measuring instrument of singlet oxygen quantum yield in photodynamic effects

NASA Astrophysics Data System (ADS)

Li, Zhongwei; Zhang, Pengwei; Zang, Lixin; Qin, Feng; Zhang, Zhiguo; Zhang, Hongli

2017-06-01

Using diphenylisobenzofuran (C20H14O) as a singlet oxygen (1O2) reporter, a comparison method, which can be used to measure the singlet oxygen quantum yield (ΦΔ) of the photosensitizer quantitatively, is presented in this paper. Based on this method, an automatic measuring instrument of singlet oxygen quantum yield is developed. The singlet oxygen quantum yield of the photosensitizer hermimether and aloe-emodin is measured. It is found that the measuring results are identical to the existing ones, which verifies the validity of the measuring instrument.

High Quantum Yield Blue Emission from Lead-Free Inorganic Antimony Halide Perovskite Colloidal Quantum Dots.

PubMed

Zhang, Jian; Yang, Ying; Deng, Hui; Farooq, Umar; Yang, Xiaokun; Khan, Jahangeer; Tang, Jiang; Song, Haisheng

2017-09-26

Colloidal quantum dots (QDs) of lead halide perovskite have recently received great attention owing to their remarkable performances in optoelectronic applications. However, their wide applications are hindered from toxic lead element, which is not environment- and consumer-friendly. Herein, we utilized heterovalent substitution of divalent lead (Pb 2+ ) with trivalent antimony (Sb 3+ ) to synthesize stable and brightly luminescent Cs 3 Sb 2 Br 9 QDs. The lead-free, full-inorganic QDs were fabricated by a modified ligand-assisted reprecipitation strategy. A photoluminescence quantum yield (PLQY) was determined to be 46% at 410 nm, which was superior to that of other reported halide perovskite QDs. The PL enhancement mechanism was unraveled by surface composition derived quantum-well band structure and their large exciton binding energy. The Br-rich surface and the observed 530 meV exciton binding energy were proposed to guarantee the efficient radiative recombination. In addition, we can also tune the inorganic perovskite QD (Cs 3 Sb 2 X 9 ) emission wavelength from 370 to 560 nm via anion exchange reactions. The developed full-inorganic lead-free Sb-perovskite QDs with high PLQY and stable emission promise great potential for efficient emission candidates.

Perovskite Quantum Dots with Near Unity Solution and Neat-Film Photoluminescent Quantum Yield by Novel Spray Synthesis.

PubMed

Dai, Shu-Wen; Hsu, Bo-Wei; Chen, Chien-Yu; Lee, Chia-An; Liu, Hsiao-Yun; Wang, Hsiao-Fang; Huang, Yu-Ching; Wu, Tien-Lin; Manikandan, Arumugam; Ho, Rong-Ming; Tsao, Cheng-Si; Cheng, Chien-Hong; Chueh, Yu-Lun; Lin, Hao-Wu

2018-02-01

In this study, a novel perovskite quantum dot (QD) spray-synthesis method is developed by combining traditional perovskite QD synthesis with the technique of spray pyrolysis. By utilizing this new technique, the synthesis of cubic-shaped perovskite QDs with a homogeneous size of 14 nm is demonstrated, which shows an unprecedented stable absolute photoluminescence quantum yield ≈100% in the solution and even in the solid-state neat film. The highly emissive thin films are integrated with light emission devices (LEDs) and organic light emission displays (OLEDs). The color conversion type QD-LED (ccQD-LED) hybrid devices exhibit an extremely saturated green emission, excellent external quantum efficiency of 28.1%, power efficiency of 121 lm W -1 , and extraordinary forward-direction luminescence of 8 500 000 cd m -2 . The conceptual ccQD-OLED hybrid display also successfully demonstrates high-definition still images and moving pictures with a 119% National Television System Committee 1931 color gamut and 123% Digital Cinema Initiatives-P3 color gamut. These very-stable, ultra-bright perovskite QDs have the properties necessary for a variety of useful applications in optoelectronics. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Remarkably high apparent quantum yield of the overall photocatalytic H2O splitting achieved by utilizing Zn ion added Ga2O3 prepared using dilute CaCl2 solution.

PubMed

Sakata, Yoshihisa; Hayashi, Takuya; Yasunaga, Ryō; Yanaga, Nobuyuki; Imamura, Hayao

2015-08-21

Remarkably high photocatalytic activity for the overall H2O splitting, where the activity was 32 mmol h(-1) for H2 production and 16 mmol h(-1) for O2 production under irradiation from a 450 W high-pressure Hg lamp and the apparent quantum yield (AQY) was 71% under irradiation at 254 nm, was achieved by utilizing a Rh(0.5)Cr(1.5)O3(Rh; 0.5 wt%)/Zn(3 mol%)-Ga2O3 photocatalyst when Ga2O3 was prepared using dilute CaCl2 aqueous solution having a concentration of 0.001 mol l(-1).

Lanthanide complexes with 2-(tosylamino)benzylidene-N-benzoylhydrazone, which exhibit high NIR emission.

PubMed

Utochnikova, V V; Kovalenko, A D; Burlov, A S; Marciniak, L; Ananyev, I V; Kalyakina, A S; Kurchavov, N A; Kuzmina, N P

2015-07-28

New NIR emitting materials were found among the lanthanide complexes with 2-(tosylamino)benzylidene-N-benzoylhydrazone. Complexes of Nd(3+), Er(3+) and Yb(3+), as well as Eu(3+), Gd(3+) and Lu(3+), were synthesized for the first time. Owing to the absence of vibration quenching the ytterbium complex was found to exhibit a photoluminescence quantum yield of 1.4%. Since the sensitization efficiency was calculated to be 55%, the losses in the quantum yield are probably due to Yb-Yb resonant energy transfer.

Method for resurrecting negative electron affinity photocathodes after exposure to an oxidizing gas

DOEpatents

Mulhollan, Gregory A; Bierman, John C

2012-10-30

A method by which negative electron affinity photocathodes (201), single crystal, amorphous, or otherwise ordered, can be made to recover their quantum yield following exposure to an oxidizing gas has been discovered. Conventional recovery methods employ the use of cesium as a positive acting agent (104). In the improved recovery method, an electron beam (205), sufficiently energetic to generate a secondary electron cloud (207), is applied to the photocathode in need of recovery. The energetic beam, through the high secondary electron yield of the negative electron affinity surface (203), creates sufficient numbers of low energy electrons which act on the reduced-yield surface so as to negate the effects of absorbed oxidizing atoms thereby recovering the quantum yield to a pre-decay value.

Connectivity is a Poor Indicator of Fast Quantum Search

NASA Astrophysics Data System (ADS)

Meyer, David A.; Wong, Thomas G.

2015-03-01

A randomly walking quantum particle evolving by Schrödinger's equation searches on d -dimensional cubic lattices in O (√{N }) time when d ≥5 , and with progressively slower runtime as d decreases. This suggests that graph connectivity (including vertex, edge, algebraic, and normalized algebraic connectivities) is an indicator of fast quantum search, a belief supported by fast quantum search on complete graphs, strongly regular graphs, and hypercubes, all of which are highly connected. In this Letter, we show this intuition to be false by giving two examples of graphs for which the opposite holds true: one with low connectivity but fast search, and one with high connectivity but slow search. The second example is a novel two-stage quantum walk algorithm in which the walking rate must be adjusted to yield high search probability.

Photodynamic therapy potential of thiol-stabilized CdTe quantum dot-group 3A phthalocyanine conjugates (QD-Pc).

PubMed

Tekdaş, Duygu Aydın; Durmuş, Mahmut; Yanık, Hülya; Ahsen, Vefa

2012-07-01

Thiol stabilized CdTe quantum dot (QD) nanoparticles were synthesized in aqueous phase and were used as energy donors to tetra-triethyleneoxythia substituted aluminum, gallium and indium phthalocyanines through fluorescence resonance energy transfer (FRET). Energy transfer occurred from the QDs to phthalocyanines upon photoexcitation of the QDs. An enhancement in efficiency of energy transfer with the nature of the carboxylic thiol stabilizer on the QDs was observed. As a result of the nanoparticle and the phthalocyanine mixing, the photoluminescence efficiency of the phthalocyanine moieties in the mixtures does not strictly follow the quantum yields of the bare phthalocyanines. The photochemistry study of phthalocyanines in the presence of the QDs revealed high singlet oxygen quantum yield, hence the possibility of using QDs in combination with phthalocyanines as photosensitizers in photodynamic therapy of cancer. The fluorescence of the CdTe quantum dots-phthalocyanine conjugates (QDs-Pc) were effectively quenched by addition of 1,4-benzoquinone. Copyright © 2012 Elsevier B.V. All rights reserved.

Quantum Yields in Mixed-Conifer Forests and Ponderosa Pine Plantations

NASA Astrophysics Data System (ADS)

Wei, L.; Marshall, J. D.; Zhang, J.

2008-12-01

Most process-based physiological models require canopy quantum yield of photosynthesis as a starting point to simulate carbon sequestration and subsequently gross primary production (GPP). The quantum yield is a measure of photosynthetic efficiency expressed in moles of CO2 assimilated per mole of photons absorbed; the process is influenced by environmental factors. In the summer 2008, we measured quantum yields on both sun and shade leaves for four conifer species at five sites within Mica Creek Experimental Watershed (MCEW) in northern Idaho and one conifer species at three sites in northern California. The MCEW forest is typical of mixed conifer stands dominated by grand fir (Abies grandis (Douglas ex D. Don) Lindl.). In northern California, the three sites with contrasting site qualities are ponderosa pine (Pinus ponderosa C. Lawson var. ponderosa) plantations that were experimentally treated with vegetation control, fertilization, and a combination of both. We found that quantum yields in MCEW ranged from ~0.045 to ~0.075 mol CO2 per mol incident photon. However, there were no significant differences between canopy positions, or among sites or tree species. In northern California, the mean value of quantum yield of three sites was 0.051 mol CO2/mol incident photon. No significant difference in quantum yield was found between canopy positions, or among treatments or sites. The results suggest that these conifer species maintain relatively consistent quantum yield in both MCEW and northern California. This consistency simplifies the use of a process-based model to accurately predict forest productivity in these areas.

Fluorenyl benzothiadiazole and benzoselenadiazole near-IR fluorescent probes for two-photon fluorescence imaging (Conference Presentation)

NASA Astrophysics Data System (ADS)

Belfield, Kevin D.; Yao, Sheng; Kim, Bosung; Yue, Xiling

2016-03-01

Imaging biological samples with two-photon fluorescence (2PF) microscopy has the unique advantage of resulting high contrast 3D resolution subcellular image that can reach up to several millimeters depth. 2PF probes that absorb and emit at near IR region need to be developed. Two-photon excitation (2PE) wavelengths are less concerned as 2PE uses wavelengths doubles the absorption wavelength of the probe, which means 2PE wavelengths for probes even with absorption at visible wavelength will fall into NIR region. Therefore, probes that fluoresce at near IR region with high quantum yields are needed. A series of dyes based on 5-thienyl-2, 1, 3-benzothiadiazole and 5-thienyl-2, 1, 3-benzoselenadiazole core were synthesized as near infrared two-photon fluorophores. Fluorescence maxima wavelengths as long as 714 nm and fluorescence quantum yields as high as 0.67 were achieved. The fluorescence quantum yields of the dyes were nearly constant, regardless of solvents polarity. These diazoles exhibited large Stokes shift (<114nm), high two-photon absorption cross sections (up to 2,800 GM), and high two-photon fluorescence figure of merit (FM , 1.04×10-2 GM). Cells incubated on a 3D scaffold with one of the new probes (encapsulated in Pluronic micelles) exhibited bright fluorescence, enabling 3D two-photon fluorescence imaging to a depth of 100 µm.

Absolute 1* quantum yields for the ICN A state by diode laser gain versus absorption spectroscopy

NASA Technical Reports Server (NTRS)

Hess, Wayne P.; Leone, Stephen R.

1987-01-01

Absolute I* quantum yields were measured as a function of wavelength for room temperature photodissociation of the ICN A state continuum. The temperature yields are obtained by the technique of time-resolved diode laser gain-versus-absorption spectroscopy. Quantum yields are evaluated at seven wavelengths from 248 to 284 nm. The yield at 266 nm is 66.0 +/- 2% and it falls off to 53.4 +/- 2% and 44.0 +/- 4% at 284 and 248 respectively. The latter values are significantly higher than those obtained by previous workers using infrared fluorescence. Estimates of I* quantum yields obtained from analysis of CN photofragment rotational distributions, as discussed by other workers, are in good agreement with the I* yields. The results are considered in conjunction with recent theoretical and experimental work on the CN rotational distributions and with previous I* yield results.

Luminescence and luminescence quenching of highly efficient Y2Mo4O15:Eu3+ phosphors and ceramics

PubMed Central

Janulevicius, Matas; Marmokas, Paulius; Misevicius, Martynas; Grigorjevaite, Julija; Mikoliunaite, Lina; Sakirzanovas, Simas; Katelnikovas, Arturas

2016-01-01

A good LED phosphor must possess strong enough absorption, high quantum yields, colour purity, and quenching temperatures. Our synthesized Y2Mo4O15:Eu3+ phosphors possess all of these properties. Excitation of these materials with near-UV or blue radiation yields bright red emission and the colour coordinates are relatively stable upon temperature increase. Furthermore, samples doped with 50% Eu3+ showed quantum yields up to 85%, what is suitable for commercial application. Temperature dependent emission spectra revealed that heavily Eu3+ doped phosphors possess stable emission up to 400 K and lose half of the efficiency only at 515 K. In addition, ceramic disks of Y2Mo4O15:75%Eu3+ phosphor with thickness of 0.71 and 0.98 mm were prepared and it turned out that they efficiently convert radiation of 375 and 400 nm LEDs to the red light, whereas combination with 455 nm LED yields purple colour. PMID:27180941

Luminescence and luminescence quenching of highly efficient Y2Mo4O15:Eu(3+) phosphors and ceramics.

PubMed

Janulevicius, Matas; Marmokas, Paulius; Misevicius, Martynas; Grigorjevaite, Julija; Mikoliunaite, Lina; Sakirzanovas, Simas; Katelnikovas, Arturas

2016-05-16

A good LED phosphor must possess strong enough absorption, high quantum yields, colour purity, and quenching temperatures. Our synthesized Y2Mo4O15:Eu(3+) phosphors possess all of these properties. Excitation of these materials with near-UV or blue radiation yields bright red emission and the colour coordinates are relatively stable upon temperature increase. Furthermore, samples doped with 50% Eu(3+) showed quantum yields up to 85%, what is suitable for commercial application. Temperature dependent emission spectra revealed that heavily Eu(3+) doped phosphors possess stable emission up to 400 K and lose half of the efficiency only at 515 K. In addition, ceramic disks of Y2Mo4O15:75%Eu(3+) phosphor with thickness of 0.71 and 0.98 mm were prepared and it turned out that they efficiently convert radiation of 375 and 400 nm LEDs to the red light, whereas combination with 455 nm LED yields purple colour.

Room temperature synthesis of pH-switchable polyaniline quantum dots as a turn-on fluorescent probe for acidic biotarget labeling.

PubMed

Liu, Yanfeng; Ding, Yin; Gou, Huilin; Huang, Xin; Zhang, Guiyang; Zhang, Qi; Liu, Yunzhong; Meng, Zhen; Xi, Kai; Jia, Xudong

2018-04-05

The synthesis of well-defined light-element-derived quantum dots (LEQDs) with advanced optical properties under mild conditions is highly desirable yet challenging. Here, a polyaniline (PANI) structure is introduced into carbon-rich LEQDs to yield well-defined, fluorescent polyaniline quantum dots (PAQDs), PAQD24, through a one-pot room temperature reaction. The mild synthetic conditions effectively minimize the defects introduced during the conventional synthesis and endow PAQD24 with desirable optical properties, including a narrow emission band (full width at half maximum = 55 nm), an optimal quantum yield of 32.5% and two-photon fluorescence. Furthermore, the bandgap of PAQD24 is highly sensitive toward pH variations in the near-neutral region, due to the proton doping and dedoping of the PANI structure. Such unique properties together with its fine bio-compatibility enable the application of this material as a turn-on fluorescent probe for the labeling of acidic biotargets from sub-cellular to organ levels, providing potential applications in diagnosis and surgery guidance for certain diseases.

High quantum yield of the Egyptian blue family of infrared phosphors (MCuSi4O10, M = Ca, Sr, Ba)

NASA Astrophysics Data System (ADS)

Berdahl, Paul; Boocock, Simon K.; Chan, George C.-Y.; Chen, Sharon S.; Levinson, Ronnen M.; Zalich, Michael A.

2018-05-01

The alkaline earth copper tetra-silicates, blue pigments, are interesting infrared phosphors. The Ca, Sr, and Ba variants fluoresce in the near-infrared (NIR) at 909, 914, and 948 nm, respectively, with spectral widths on the order of 120 nm. The highest quantum yield ϕ reported thus far is ca. 10%. We use temperature measurements in sunlight to determine this parameter. The yield depends on the pigment loading (mass per unit area) ω with values approaching 100% as ω → 0 for the Ca and Sr variants. Although maximum quantum yield occurs near ω = 0, maximum fluorescence occurs near ω = 70 g m-2, at which ϕ = 0.7. The better samples show fluorescence decay times in the range of 130 to 160 μs. The absorbing impurity CuO is often present. Good phosphor performance requires long fluorescence decay times and very low levels of parasitic absorption. The strong fluorescence enhances prospects for energy applications such as cooling of sunlit surfaces (to reduce air conditioning requirements) and luminescent solar concentrators.

Highly Sensitive Detection of Glucose by a "Turn-Off-On" Fluorescent Probe Using Gadolinium-Doped Carbon Dots and Carbon Microparticles.

PubMed

Hu, Meixin; Qi, Jianrong; Ruan, Jing; Shen, Guangxia

2018-06-01

Carbon dots, as a potential substitute for semiconductor quantum dots, have drawn great interest in recent years. The preparation of fluorescent carbon dots has been made easy with many significant advances, but the complicated purifying processes, low quantum yield, and blue emission wavelength still limit its wider application in biosensors, biomedicine, and photonic devices. Here we report a strategy to synthesis Gd-doped carbon dots (Gd-Cdots) of super-high quantum yield with a microwave assisted hydrothermal method. The Gd-Cdots, with a diameter of 47∼8 nm, can be purified easily with conventional centrifugal techniques. Carbon microparticles (CMPs) have also been synthesized with a similar procedure. Meanwhile, we demonstrated a novel "turn-off-on" fluorescent biosensor, which has been developed for highly sensitive detection of glucose using Gd-doped carbon dots as probes. The proposed biosensor has exhibited low-cost and non-toxic properties, with high sensitivity and good specificity. In addition, the results in real blood samples further confirmed it as a promising application in diabetes diagnosis.

Degradation Mechanisms in Blue Phosphorescent Organic Light-Emitting Devices by Exciton-Polaron Interactions: Loss in Quantum Yield versus Loss in Charge Balance.

PubMed

Zhang, Yingjie; Aziz, Hany

2017-01-11

We study the relative importance of deterioration of material quantum yield and charge balance to the electroluminescence stability of PHOLEDs, with a special emphasis on blue devices. Investigations show that the quantum yields of both host and emitter in the emission layer degrade due to exciton-polaron interactions and that the deterioration in material quantum yield plays the primary role in device degradation under operation. On the other hand, the results show that the charge balance factor is also affected by exciton-polaron interactions but only plays a secondary role in determining device stability. Finally, we show that the degradation mechanisms in blue PHOLEDs are fundamentally the same as those in green PHOLEDs. The limited stability of the blue devices is a result of faster deterioration in the quantum yield of the emitter.

Comparisons of Photosynthetic Responses of Xanthium strumarium and Helianthus annuus to Chronic and Acute Water Stress in Sun and Shade 1

PubMed Central

Ben, Gui-Ying; Osmond, C. Barry; Sharkey, Thomas D.

1987-01-01

We have examined the effects of mild, chronic water stress and acute water stress on two water stress sensitive plants, Xanthium strumarium and Helianthus annuus. Using a combination of the leaf disc O2 electrode to measure the light responses of photosynthesis and 77 K fluorescence to monitor damage to the primary photochemistry, we have found the following: (a) The CO2 saturated rate of photosynthesis at high light is the most water stress sensitive parameter measured. (b) The apparent quantum yield (moles O2 per mole photons) was slightly, if at all, affected by mild water stress (>−1.5 megapascals). (c) Severe water stress (<−1.5 megapascals) reduced the quantum yield of photosynthesis regardless of whether the stress was applied in sun or shade. The light independent reduction of quantum yield was not associated with a reduction in 77 K fluorescence (Fv/Fm) indicating that the quantum yield reduction was not the result of damage to primary photochemistry. (d) The diel fluctuation in 77 K fluorescence seen in sun-exposed control leaves was greatly exaggerated in water stressed leaves because of enhanced decline in 77 K fluorescence in the morning. The rate of recovery was similar in both control and water stressed leaves. Shaded leaves showed no change in 77 K fluorescence regardless of whether water stress was imposed or not. (e) The water stress sensitive plants used in these experiments did not recover from acute water stress severe enough to reduce the quantum yield or chronic water stress which lasted long enough that light dependent damage to primary photochemistry occurred. PMID:16665465

Comparisons of Photosynthetic Responses of Xanthium strumarium and Helianthus annuus to Chronic and Acute Water Stress in Sun and Shade.

PubMed

Ben, G Y; Osmond, C B; Sharkey, T D

1987-06-01

We have examined the effects of mild, chronic water stress and acute water stress on two water stress sensitive plants, Xanthium strumarium and Helianthus annuus. Using a combination of the leaf disc O(2) electrode to measure the light responses of photosynthesis and 77 K fluorescence to monitor damage to the primary photochemistry, we have found the following: (a) The CO(2) saturated rate of photosynthesis at high light is the most water stress sensitive parameter measured. (b) The apparent quantum yield (moles O(2) per mole photons) was slightly, if at all, affected by mild water stress (>-1.5 megapascals). (c) Severe water stress (<-1.5 megapascals) reduced the quantum yield of photosynthesis regardless of whether the stress was applied in sun or shade. The light independent reduction of quantum yield was not associated with a reduction in 77 K fluorescence (F(v)/F(m)) indicating that the quantum yield reduction was not the result of damage to primary photochemistry. (d) The diel fluctuation in 77 K fluorescence seen in sun-exposed control leaves was greatly exaggerated in water stressed leaves because of enhanced decline in 77 K fluorescence in the morning. The rate of recovery was similar in both control and water stressed leaves. Shaded leaves showed no change in 77 K fluorescence regardless of whether water stress was imposed or not. (e) The water stress sensitive plants used in these experiments did not recover from acute water stress severe enough to reduce the quantum yield or chronic water stress which lasted long enough that light dependent damage to primary photochemistry occurred.

Aptamer-Modified Semiconductor Quantum Dots for Biosensing Applications

PubMed Central

Wen, Lin; Qiu, Liping; Wu, Yongxiang; Hu, Xiaoxiao; Zhang, Xiaobing

2017-01-01

Semiconductor quantum dots have attracted extensive interest in the biosensing area because of their properties, such as narrow and symmetric emission with tunable colors, high quantum yield, high stability and controllable morphology. The introduction of various reactive functional groups on the surface of semiconductor quantum dots allows one to conjugate a spectrum of ligands, antibodies, peptides, or nucleic acids for broader and smarter applications. Among these ligands, aptamers exhibit many advantages including small size, high chemical stability, simple synthesis with high batch-to-batch consistency and convenient modification. More importantly, it is easy to introduce nucleic acid amplification strategies and/or nanomaterials to improve the sensitivity of aptamer-based sensing systems. Therefore, the combination of semiconductor quantum dots and aptamers brings more opportunities in bioanalysis. Here we summarize recent advances on aptamer-functionalized semiconductor quantum dots in biosensing applications. Firstly, we discuss the properties and structure of semiconductor quantum dots and aptamers. Then, the applications of biosensors based on aptamer-modified semiconductor quantum dots by different signal transducing mechanisms, including optical, electrochemical and electrogenerated chemiluminescence approaches, is discussed. Finally, our perspectives on the challenges and opportunities in this promising field are provided. PMID:28788080

Aptamer-Modified Semiconductor Quantum Dots for Biosensing Applications.

PubMed

Wen, Lin; Qiu, Liping; Wu, Yongxiang; Hu, Xiaoxiao; Zhang, Xiaobing

2017-07-28

Semiconductor quantum dots have attracted extensive interest in the biosensing area because of their properties, such as narrow and symmetric emission with tunable colors, high quantum yield, high stability and controllable morphology. The introduction of various reactive functional groups on the surface of semiconductor quantum dots allows one to conjugate a spectrum of ligands, antibodies, peptides, or nucleic acids for broader and smarter applications. Among these ligands, aptamers exhibit many advantages including small size, high chemical stability, simple synthesis with high batch-to-batch consistency and convenient modification. More importantly, it is easy to introduce nucleic acid amplification strategies and/or nanomaterials to improve the sensitivity of aptamer-based sensing systems. Therefore, the combination of semiconductor quantum dots and aptamers brings more opportunities in bioanalysis. Here we summarize recent advances on aptamer-functionalized semiconductor quantum dots in biosensing applications. Firstly, we discuss the properties and structure of semiconductor quantum dots and aptamers. Then, the applications of biosensors based on aptamer-modified semiconductor quantum dots by different signal transducing mechanisms, including optical, electrochemical and electrogenerated chemiluminescence approaches, is discussed. Finally, our perspectives on the challenges and opportunities in this promising field are provided.

Efficient nanosecond photoluminescence from infrared PbS quantum dots coupled to plasmonic nanoantennas

DOE PAGES

Akselrod, Gleb M.; Weidman, Mark C.; Li, Ying; ...

2016-09-13

Infrared (IR) light sources with high modulation rates are critical components for on-chip optical communications. Lead-based colloidal quantum dots are promising nonepitaxial materials for use in IR light-emitting diodes, but their slow photoluminescence lifetime is a serious limitation. Here we demonstrate coupling of PbS quantum dots to colloidal plasmonic nanoantennas based on film-coupled metal nanocubes, resulting in a dramatic 1300-fold reduction in the emission lifetime from the microsecond to the nanosecond regime. This lifetime reduction is primarily due to a 1100-fold increase in the radiative decay rate owing to the high quantum yield (65%) of the antenna. The short emissionmore » lifetime is accompanied by high antenna quantum efficiency and directionality. Lastly, this nonepitaxial platform points toward GHz frequency, electrically modulated, telecommunication wavelength light-emitting diodes and single-photon sources.« less

Graphene quantum dots as enhanced plant growth regulators: effects on coriander and garlic plants.

PubMed

Chakravarty, Disha; Erande, Manisha B; Late, Dattatray J

2015-10-01

We report investigations on the use of graphene quantum dots for growth enhancement in coriander (Coriandrum sativam L.) and garlic (Allium sativum) plants. The as-received seeds of coriander and garlic were treated with 0.2 mg mL(-1) of graphene quantum dots for 3 h before planting. Graphene quantum dots enhanced the growth rate in coriander and garlic plants, including leaves, roots, shoots, flowers and fruits, when the seeds were treated with graphene quantum dots. Our investigations open up the opportunity to use graphene quantum dots as plant growth regulators that can be used in a variety of other food plants for high yield. © 2015 Society of Chemical Industry.

Nonlinear quantum Rabi model in trapped ions

NASA Astrophysics Data System (ADS)

Cheng, Xiao-Hang; Arrazola, Iñigo; Pedernales, Julen S.; Lamata, Lucas; Chen, Xi; Solano, Enrique

2018-02-01

We study the nonlinear dynamics of trapped-ion models far away from the Lamb-Dicke regime. This nonlinearity induces a blockade on the propagation of quantum information along the Hilbert space of the Jaynes-Cummings and quantum Rabi models. We propose to use this blockade as a resource for the dissipative generation of high-number Fock states. Also, we compare the linear and nonlinear cases of the quantum Rabi model in the ultrastrong and deep strong-coupling regimes. Moreover, we propose a scheme to simulate the nonlinear quantum Rabi model in all coupling regimes. This can be done via off-resonant nonlinear red- and blue-sideband interactions in a single trapped ion, yielding applications as a dynamical quantum filter.

Amine-Reactive Fluorene Probes: Synthesis, Optical Characterization, Bioconjugation, and Two-Photon Fluorescence Imaging

PubMed Central

2008-01-01

With the increasing demand for confocal and two-photon fluorescence imaging, the availability of reactive probes that possess high two-photon absorptivity, high fluorescence quantum yield, and high photostability is of paramount importance. To address the demand for better-performing probes, we prepared two-photon absorbing amine-reactive fluorenyl-based probes 2-(9,9-bis(2-(2-methoxyethoxy)ethyl)-2-isothiocyanato-9H-fluoren-7-yl)benzothiazole (1) and 2-(4-(2-(9,9-bis(2-(2-ethoxyethoxy)ethyl)-2-isothiocyanato-9H-fluoren-7-yl)vinyl)phenyl)benzothiazole (2), incorporating the isothiocyanate as a reactive linker. Probe design was augmented by integrating high optical nonlinearities, increased hydrophilicity, and coupling with reactive functional groups for specific targeting of biomolecules, assuring a better impact on two-photon fluorescence microscopy (2PFM) imaging. The isothiocyanate (NCS) derivatives were conjugated with cyclic peptide RGDfK and Reelin protein. The study of the chemical and photophysical properties of the new labeling reagents, as well as the conjugates, is described. The conjugates displayed high chemical stability and photostability. The NCS derivatives had low fluorescence quantum yields, while their bioconjugates exhibited high fluorescence quantum yields, essentially “lighting up” after conjugation. Conventional and 2PFM imaging and fluorescence lifetime imaging (FLIM) of HeLa, NT2, and H1299 cells, incubated with two-photon absorbing amine-reactive probe (1), RGDfK-dye conjugate (7), and Reelin-dye conjugate (6), was demonstrated. PMID:19090700

New anthracene derivatives as triplet acceptors for efficient green-to-blue low-power upconversion.

PubMed

Liang, Zuo-Qin; Sun, Bin; Ye, Chang-Qing; Wang, Xiao-Mei; Tao, Xu-Tang; Wang, Qin-Hua; Ding, Ping; Wang, Bao; Wang, Jing-Jing

2013-10-21

Three new anthracene derivatives [2-chloro-9,10-dip-tolylanthracene (DTACl), 9,10-dip-tolylanthracene-2-carbonitrile (DTACN), and 9,10-di(naphthalen-1-yl)anthracene-2-carbonitrile (DNACN)] were synthesized as triplet acceptors for low-power upconversion. Their linear absorption, single-photon-excited fluorescence, and upconversion fluorescence properties were studied. The acceptors exhibit high fluorescence yields in DMF. Selective excitation of the sensitizer Pd(II)octaethylporphyrin (PdOEP) in solution containing DTACl, DTACN, or DNA-CN at 532 nm with an ultralow excitation power density of 0.5 W cm(-2) results in anti-Stokes blue emission. The maximum upconversion quantum yield (Φ(UC) =17.4%) was obtained for the couple PdOEP/DTACl. In addition, the efficiency of the triplet-triplet energy transfer process was quantitatively studied by quenching experiments. Experimental results revealed that a highly effective acceptor for upconversion should combine high fluorescence quantum yields with efficient quenching of the sensitizer triplet. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Quantum radiation reaction in laser-electron-beam collisions.

PubMed

Blackburn, T G; Ridgers, C P; Kirk, J G; Bell, A R

2014-01-10

It is possible using current high-intensity laser facilities to reach the quantum radiation reaction regime for energetic electrons. An experiment using a wakefield accelerator to drive GeV electrons into a counterpropagating laser pulse would demonstrate the increase in the yield of high-energy photons caused by the stochastic nature of quantum synchrotron emission: we show that a beam of 10(9) 1 GeV electrons colliding with a 30 fs laser pulse of intensity 10(22)  W cm(-2) will emit 6300 photons with energy greater than 700 MeV, 60× the number predicted by classical theory.

Photoswitchable Fluorescent Diarylethene Derivatives with Thiophene 1,1-Dioxide Groups: Effect of Alkyl Substituents at the Reactive Carbons

PubMed Central

Sumi, Takaki; Irie, Masahiro

2017-01-01

Photoswitching and fluorescent properties of sulfone derivatives of 1,2-bis(2-alkyl-4-methyl-5-phenyl-3-thienyl)perfluorocyclopentene, 1–5, having methyl, ethyl, n-propyl, i-propyl, and i-butyl substituents at the reactive carbons (2- and 2′-positions) of the thiophene 1,1-dioxide rings were studied. Diarylethenes 1–5 underwent isomerization reactions between open-ring and closed-ring forms upon alternate irradiation with ultraviolet (UV) and visible light and showed fluorescence in the closed-ring forms. The alkyl substitution at the reactive carbons affects the fluorescent property of the closed-ring isomers. The closed-ring isomers 2b–5b with ethyl, n-propyl, i-propyl, and i-butyl substituents show higher fluorescence quantum yields than 1b with methyl substituents. In polar solvents, the fluorescence quantum yield of 1b markedly decreases, while 2b–5b maintain the relatively high fluorescence quantum yields. Although the cycloreversion quantum yields of the derivatives with methyl, ethyl, n-propyl, and i-propyl substituents are quite low and in the order of 10−5, introduction of i-butyl substituents was found to increase the yield up to the order of 10−3. These results indicate that appropriate alkyl substitution at the reactive carbons is indispensable for properly controlling the photoswitching and fluorescent properties of the photoswitchable fluorescent diarylethenes, which are potentially applicable to super-resolution fluorescence microscopies. PMID:28869489

CW-pumped telecom band polarization entangled photon pair generation in a Sagnac interferometer.

PubMed

Li, Yan; Zhou, Zhi-Yuan; Ding, Dong-Sheng; Shi, Bao-Sen

2015-11-02

Polarization entangled photon pair source is widely used in many quantum information processing applications such as teleportation, quantum communications, quantum computation and high precision quantum metrology. We report on the generation of a continuous-wave pumped 1550 nm polarization entangled photon pair source at telecom wavelength using a type-II periodically poled KTiOPO(4) (PPKTP) crystal in a Sagnac interferometer. Hong-Ou-Mandel (HOM) interference measurement yields signal and idler photon bandwidth of 2.4 nm. High quality of entanglement is verified by various kinds of measurements, for example two-photon interference fringes, Bell inequality and quantum states tomography. The source can be tuned over a broad range against temperature or pump power without loss of visibilities. This source will be used in our future experiments such as generation of orbital angular momentum entangled source at telecom wavelength for quantum frequency up-conversion, entanglement based quantum key distributions and many other quantum optics experiments at telecom wavelengths.

Enhancing the photon-extraction efficiency of site-controlled quantum dots by deterministically fabricated microlenses

NASA Astrophysics Data System (ADS)

Kaganskiy, Arsenty; Fischbach, Sarah; Strittmatter, André; Rodt, Sven; Heindel, Tobias; Reitzenstein, Stephan

2018-04-01

We report on the realization of scalable single-photon sources (SPSs) based on single site-controlled quantum dots (SCQDs) and deterministically fabricated microlenses. The fabrication process comprises the buried-stressor growth technique complemented with low-temperature in-situ electron-beam lithography for the integration of SCQDs into microlens structures with high yield and high alignment accuracy. The microlens-approach leads to a broadband enhancement of the photon-extraction efficiency of up to (21 ± 2)% and a high suppression of multi-photon events with g (2)(τ = 0) < 0.06 without background subtraction. The demonstrated combination of site-controlled growth of QDs and in-situ electron-beam lithography is relevant for arrays of efficient SPSs which, can be applied in photonic quantum circuits and advanced quantum computation schemes.

Carrier Multiplication in Quantum Dots within the Framework of Two Competing Energy Relaxation Mechanisms.

PubMed

Stewart, John T; Padilha, Lazaro A; Bae, Wan Ki; Koh, Weon-Kyu; Pietryga, Jeffrey M; Klimov, Victor I

2013-06-20

The realization of high-yield, low-threshold carrier multiplication (CM) in semiconductor quantum dots (QDs) is a promising step toward third-generation photovoltaics (PV). Recent studies of QD solar cells have shown that CM can indeed produce greater-than-unity quantum efficiencies in photon-to-charge-carrier conversion, establishing the relevance of this process to practical PV technologies. While being appreciable, the reported CM yields are still not high enough for a significant increase in the power conversion efficiency over traditional bulk materials. At present, the design of nanomaterials with improved CM is hindered by a poor understanding of the mechanism underlying this process. Here, we present a possible solution to this problem by introducing a model that treats CM as a competition between impact-ionization-like scattering and non-CM energy losses. Importantly, it allows for evaluation of expected CM yields from fairly straightforward measurements of Auger recombination (inverse of CM) and near-band-edge carrier cooling. The validation of this model via a comparative CM study of PbTe, PbSe, and PbS QDs suggests that it indeed represents a predictive capability, which might help in the development of nanomaterials with improved CM performance.

Ultrafast and Efficient Transport of Hot Plasmonic Electrons by Graphene for Pt Free, Highly Efficient Visible-Light Responsive Photocatalyst.

PubMed

Kumar, Dinesh; Lee, Ahreum; Lee, Taegon; Lim, Manho; Lim, Dong-Kwon

2016-03-09

We report that reduced graphene-coated gold nanoparticles (r-GO-AuNPs) are excellent visible-light-responsive photocatalysts for the photoconversion of CO2 into formic acid (HCOOH). The wavelength-dependent quantum and chemical yields of HCOOH shows a significant contribution of plasmon-induced hot electrons for CO2 photoconversion. Furthermore, the presence and reduced state of the graphene layers are critical parameters for the efficient CO2 photoconversion because of the electron mobility of graphene. With an excellent selectivity toward HCOOH (>90%), the quantum yield of HCOOH using r-GO-AuNPs is 1.52%, superior to that of Pt-coated AuNPs (quantum yield: 1.14%). This indicates that r-GO is a viable alternative to platinum metal. The excellent colloidal stability and photocatalytic stability of r-GO-AuNPs enables CO2 photoconversion under more desirable reaction conditions. These results highlight the role of reduced graphene layers as highly efficient electron acceptors and transporters to facilitate the use of hot electrons for plasmonic photocatalysts. The femtosecond transient spectroscopic analysis also shows 8.7 times higher transport efficiency of hot plasmonic electrons in r-GO-AuNPs compared with AuNPs.

Fluorescence Quantum Yield Measurements of Fluorescent Proteins: A Laboratory Experiment for a Biochemistry or Molecular Biophysics Laboratory Course

ERIC Educational Resources Information Center

Wall, Kathryn P.; Dillon, Rebecca; Knowles, Michelle K.

2015-01-01

Fluorescent proteins are commonly used in cell biology to assess where proteins are within a cell as a function of time and provide insight into intracellular protein function. However, the usefulness of a fluorescent protein depends directly on the quantum yield. The quantum yield relates the efficiency at which a fluorescent molecule converts…

Coherent quantum dynamics of a superconducting flux qubit.

PubMed

Chiorescu, I; Nakamura, Y; Harmans, C J P M; Mooij, J E

2003-03-21

We have observed coherent time evolution between two quantum states of a superconducting flux qubit comprising three Josephson junctions in a loop. The superposition of the two states carrying opposite macroscopic persistent currents is manipulated by resonant microwave pulses. Readout by means of switching-event measurement with an attached superconducting quantum interference device revealed quantum-state oscillations with high fidelity. Under strong microwave driving, it was possible to induce hundreds of coherent oscillations. Pulsed operations on this first sample yielded a relaxation time of 900 nanoseconds and a free-induction dephasing time of 20 nanoseconds. These results are promising for future solid-state quantum computing.

Investigations of quantum pendulum dynamics in a spin-1 BEC

NASA Astrophysics Data System (ADS)

Hoang, Thai; Gerving, Corey; Land, Ben; Anquez, Martin; Hamley, Chris; Chapman, Michael

2013-05-01

We investigate the quantum spin dynamics of a spin-1 BEC initialized to an unstable critical point of the dynamical phase space. The subsequent evolution of the collective states of the system is analogous to an inverted simple pendulum in the quantum limit and yields non-classical states with quantum correlations. For short evolution times in the low depletion limit, we observe squeezed states and for longer times beyond the low depletion limit we observe highly non-Gaussian distributions. C.D. Hamley, C.S. Gerving, T.M. Hoang, E.M. Bookjans, and M.S. Chapman, ``Spin-Nematic Squeezed Vacuum in a Quantum Gas,'' Nature Physics 8, 305-308 (2012).

Tradeoffs between oscillator strength and lifetime in terahertz quantum cascade lasers

DOE PAGES

Chan, Chun Wang I.; Albo, Asaf; Hu, Qing; ...

2016-11-14

Contemporary research into diagonal active region terahertz quantum cascade lasers for high temperature operation has yielded little success. We present evidence that the failure of high diagonality alone as a design strategy is due to a fundamental trade-off between large optical oscillator strength and long upper-level lifetime. Here, we hypothesize that diagonality needs to be paired with increased doping in order to succeed, and present evidence that highly diagonal designs can benefit from much higher doping than normally found in terahertz quantum cascade lasers. In assuming the benefits of high diagonality paired with high doping, we also highlight important challengesmore » that need to be overcome, specifically the increased importance of carrier induced band-bending and impurity scattering.« less

A high quantum yield molecule-protein complex fluorophore for near-infrared II imaging

PubMed Central

Antaris, Alexander L.; Chen, Hao; Diao, Shuo; Ma, Zhuoran; Zhang, Zhe; Zhu, Shoujun; Wang, Joy; Lozano, Alexander X.; Fan, Quli; Chew, Leila; Zhu, Mark; Cheng, Kai; Hong, Xuechuan; Dai, Hongjie; Cheng, Zhen

2017-01-01

Fluorescence imaging in the second near-infrared window (NIR-II) allows visualization of deep anatomical features with an unprecedented degree of clarity. NIR-II fluorophores draw from a broad spectrum of materials spanning semiconducting nanomaterials to organic molecular dyes, yet unfortunately all water-soluble organic molecules with >1,000 nm emission suffer from low quantum yields that have limited temporal resolution and penetration depth. Here, we report tailoring the supramolecular assemblies of protein complexes with a sulfonated NIR-II organic dye (CH-4T) to produce a brilliant 110-fold increase in fluorescence, resulting in the highest quantum yield molecular fluorophore thus far. The bright molecular complex allowed for the fastest video-rate imaging in the second NIR window with ∼50-fold reduced exposure times at a fast 50 frames-per-second (FPS) capable of resolving mouse cardiac cycles. In addition, we demonstrate that the NIR-II molecular complexes are superior to clinically approved ICG for lymph node imaging deep within the mouse body. PMID:28524850

Synthesis and spectroscopic properties of some new difluoroboron bis-β-diketonate derivatives.

PubMed

Pi, Yan; Wang, Dun-Jia; Liu, Hua; Hu, Yan-Jun; Wei, Xian-Hong; Zheng, Jing

2014-10-15

Six new bis-β-diketones (RCOCH2CO-C7H7N-COCH2COR) were synthesized from 3,5-diacetyl-2,6-dimethylpyridine via Claisen condensation with the corresponding esters, and then reacted with boron trifluoride etherate to afford difluoroboron bis-β-diketonate derivatives. Their spectroscopic properties were investigated by UV-vis, FTIR, (1)H NMR and fluorescence spectroscopic techniques. It was found that these boron complexes exhibited violet or blue fluorescence emission at 422-445nm and possessed high extinction coefficients. The results indicate that the extending π-conjugation can increase the fluorescence intensity and quantum yield for these boron complexes. Especially, the compound 2b displayed the stronger fluorescence intensity and the highest fluorescence quantum yield (Φu=0.94) in these boron compounds. However, compounds 2c and 2d had the lower fluorescence intensity and quantum yield as a result of the heavy atom effect of the chlorine atom in the molecules. Copyright © 2014 Elsevier B.V. All rights reserved.

Synthesis and spectroscopic properties of some new difluoroboron bis-β-diketonate derivatives

NASA Astrophysics Data System (ADS)

Pi, Yan; Wang, Dun-Jia; Liu, Hua; Hu, Yan-Jun; Wei, Xian-Hong; Zheng, Jing

2014-10-01

Six new bis-β-diketones (RCOCH2CO-C7H7N-COCH2COR) were synthesized from 3,5-diacetyl-2,6-dimethylpyridine via Claisen condensation with the corresponding esters, and then reacted with boron trifluoride etherate to afford difluoroboron bis-β-diketonate derivatives. Their spectroscopic properties were investigated by UV-vis, FTIR, 1H NMR and fluorescence spectroscopic techniques. It was found that these boron complexes exhibited violet or blue fluorescence emission at 422-445 nm and possessed high extinction coefficients. The results indicate that the extending π-conjugation can increase the fluorescence intensity and quantum yield for these boron complexes. Especially, the compound 2b displayed the stronger fluorescence intensity and the highest fluorescence quantum yield (Φu = 0.94) in these boron compounds. However, compounds 2c and 2d had the lower fluorescence intensity and quantum yield as a result of the heavy atom effect of the chlorine atom in the molecules.

A high quantum yield molecule-protein complex fluorophore for near-infrared II imaging

DOE Office of Scientific and Technical Information (OSTI.GOV)

Antaris, Alexander L.; Chen, Hao; Diao, Shuo

Fluorescence imaging in the second near-infrared window (NIR-II) allows visualization of deep anatomical features with an unprecedented degree of clarity. NIR-II fluorophores draw from a broad spectrum of materials spanning semiconducting nanomaterials to organic molecular dyes, yet unfortunately all water-soluble organic molecules with 41,000 nm emission suffer from low quantum yields that have limited temporal resolution and penetration depth. We report tailoring the supramolecular assemblies of protein complexes with a sulfonated NIR-II organic dye (CH-4T) to produce a brilliant 110-fold increase in fluorescence, resulting in the highest quantum yield molecular fluorophore thus far. The bright molecular complex allowed for themore » fastest video-rate imaging in the second NIR window with B50-fold reduced exposure times at a fast 50 frames-per-second (FPS) capable of resolving mouse cardiac cycles. Additionally, we demonstrate that the NIR-II molecular complexes are superior to clinically approved ICG for lymph node imaging deep within the mouse body.« less

A high quantum yield molecule-protein complex fluorophore for near-infrared II imaging

DOE PAGES

Antaris, Alexander L.; Chen, Hao; Diao, Shuo; ...

2017-05-19

Fluorescence imaging in the second near-infrared window (NIR-II) allows visualization of deep anatomical features with an unprecedented degree of clarity. NIR-II fluorophores draw from a broad spectrum of materials spanning semiconducting nanomaterials to organic molecular dyes, yet unfortunately all water-soluble organic molecules with 41,000 nm emission suffer from low quantum yields that have limited temporal resolution and penetration depth. We report tailoring the supramolecular assemblies of protein complexes with a sulfonated NIR-II organic dye (CH-4T) to produce a brilliant 110-fold increase in fluorescence, resulting in the highest quantum yield molecular fluorophore thus far. The bright molecular complex allowed for themore » fastest video-rate imaging in the second NIR window with B50-fold reduced exposure times at a fast 50 frames-per-second (FPS) capable of resolving mouse cardiac cycles. Additionally, we demonstrate that the NIR-II molecular complexes are superior to clinically approved ICG for lymph node imaging deep within the mouse body.« less

Determination of absolute chemiluminescence quantum yields for reactions of bis-(pentachlorophenyl) oxalate, hydrogen peroxide and fluorescent compounds.

PubMed

Catherall, C L; Palmer, T F; Cundall, R B

1989-01-01

Absolute chemiluminescence quantum yields (phi CL) for reactions of bis-(pentachlorophenyl) oxalate (PCPO), hydrogen peroxide (H2O2) and 9:10 diphenyl anthracene (DPA) have been determined. A fully corrected chemiluminescence monitoring spectrometer was calibrated for spectral sensitivity using the chemiluminescence of the bis-(pentachlorophenyl) oxalate system as a liquid light source, the total photon output of which had previously been determined by chemical actinometry. At high (PCPO)/(H2O2) ratios phi CL was found to be independent of PCPO and H2O2 concentrations.

Spectroscopy characterization and quantum yield determination of quantum dots

NASA Astrophysics Data System (ADS)

Contreras Ortiz, S. N.; Mejía Ospino, E.; Cabanzo, R.

2016-02-01

In this paper we show the characterization of two kinds of quantum dots: hydrophilic and hydrophobic, with core and core/shell respectively, using spectroscopy techniques such as UV-Vis, fluorescence and Raman. We determined the quantum yield in the quantum dots using the quinine sulphate as standard. This salt is commonly used because of its quantum yield (56%) and stability. For the CdTe excitation, we used a wavelength of 549nm and for the CdSe/ZnS excitation a wavelength of 527nm. The results show that CdSe/ZnS (49%) has better fluorescence, better quantum dots, and confirm the fluorescence result. The quantum dots have shown a good fluorescence performance, so this property will be used to replace dyes, with the advantage that quantum dots are less toxic than some dyes like the rhodamine. In addition, in this work we show different techniques to find the quantum dots emission: fluorescence spectrum, synchronous spectrum and Raman spectrum.

Efficient quantum computing using coherent photon conversion.

PubMed

Langford, N K; Ramelow, S; Prevedel, R; Munro, W J; Milburn, G J; Zeilinger, A

2011-10-12

Single photons are excellent quantum information carriers: they were used in the earliest demonstrations of entanglement and in the production of the highest-quality entanglement reported so far. However, current schemes for preparing, processing and measuring them are inefficient. For example, down-conversion provides heralded, but randomly timed, single photons, and linear optics gates are inherently probabilistic. Here we introduce a deterministic process--coherent photon conversion (CPC)--that provides a new way to generate and process complex, multiquanta states for photonic quantum information applications. The technique uses classically pumped nonlinearities to induce coherent oscillations between orthogonal states of multiple quantum excitations. One example of CPC, based on a pumped four-wave-mixing interaction, is shown to yield a single, versatile process that provides a full set of photonic quantum processing tools. This set satisfies the DiVincenzo criteria for a scalable quantum computing architecture, including deterministic multiqubit entanglement gates (based on a novel form of photon-photon interaction), high-quality heralded single- and multiphoton states free from higher-order imperfections, and robust, high-efficiency detection. It can also be used to produce heralded multiphoton entanglement, create optically switchable quantum circuits and implement an improved form of down-conversion with reduced higher-order effects. Such tools are valuable building blocks for many quantum-enabled technologies. Finally, using photonic crystal fibres we experimentally demonstrate quantum correlations arising from a four-colour nonlinear process suitable for CPC and use these measurements to study the feasibility of reaching the deterministic regime with current technology. Our scheme, which is based on interacting bosonic fields, is not restricted to optical systems but could also be implemented in optomechanical, electromechanical and superconducting systems with extremely strong intrinsic nonlinearities. Furthermore, exploiting higher-order nonlinearities with multiple pump fields yields a mechanism for multiparty mediation of the complex, coherent dynamics.

DNA nanosensor based on biocompatible graphene quantum dots and carbon nanotubes.

PubMed

Qian, Zhao Sheng; Shan, Xiao Yue; Chai, Lu Jing; Ma, Juan Juan; Chen, Jian Rong; Feng, Hui

2014-10-15

An ultrasensitive nanosensor based on fluorescence resonance energy transfer (FRET) between biocompatible graphene quantum dots and carbon nanotubes for DNA detection was reported. We take advantage of good biocompatibility and strong fluorescence of graphene quantum dots, base pairing specificity of DNA and unique fluorescence resonance energy transfer between graphene quantum dots and carbon nanotubes to achieve the analysis of low concentrations of DNA. Graphene quantum dots with high quantum yield up to 0.20 were prepared and served as the fluorophore of DNA probe. FRET process between graphene quantum dots-labeled probe and oxidized carbon nanotubes is easily achieved due to their efficient self-assembly through specific π-π interaction. This nanosensor can distinguish complementary and mismatched nucleic acid sequences with high sensitivity and good reproducibility. The detection method based on this nanosensor possesses a broad linear span of up to 133.0 nM and ultralow detection limit of 0.4 nM. The constructed nanosensor is expected to be highly biocompatible because of all its components with excellent biocompatibility. Copyright © 2014 Elsevier B.V. All rights reserved.

In vivo characterization of hair and skin derived carbon quantum dots with high quantum yield as long-term bioprobes in zebrafish

PubMed Central

Zhang, Jing-Hui; Niu, Aping; Li, Jing; Fu, Jian-Wei; Xu, Qun; Pei, De-Sheng

2016-01-01

Carbon quantum dots (CDs) were widely investigated because of their tunable fluorescence properties and low toxicity. However, so far there have been no reports on in vivo functional studies of hair and skin derived CDs. Here, hair derived CDs (HCDs) and skin derived CDs (SCDs) were produced by using human hair and pig skin as precursors. The quantum yields (QYs) of HCDs and SCDs were quite high, compared to citric acid derived CDs (CCDs). HCDs and SCDs possess optimal photostability, hypotoxicity and biocompatibility in zebrafish, indicating that HCDs and SCDs possess the capacity of being used as fluorescence probes for in vivo biological imaging. The long-time observation for fluorescence alternation of CDs in zebrafish and the quenching assay of CDs by ATP, NADH and Fe3+ ions demonstrated that the decaying process of CDs in vivo might be induced by the synergistic effect of the metabolism process. All results indicated that large batches and high QYs of CDs can be acquired by employing natural and nontoxic hair and skin as precursors. To our knowledge, this is the first time to report SCDs, in vivo comparative studies of HCDs, SCDs and CCDs as bioprobes, and explore their mechanism of photostability in zebrafish. PMID:27886267

In vivo characterization of hair and skin derived carbon quantum dots with high quantum yield as long-term bioprobes in zebrafish.

PubMed

Zhang, Jing-Hui; Niu, Aping; Li, Jing; Fu, Jian-Wei; Xu, Qun; Pei, De-Sheng

2016-11-25

Carbon quantum dots (CDs) were widely investigated because of their tunable fluorescence properties and low toxicity. However, so far there have been no reports on in vivo functional studies of hair and skin derived CDs. Here, hair derived CDs (HCDs) and skin derived CDs (SCDs) were produced by using human hair and pig skin as precursors. The quantum yields (QYs) of HCDs and SCDs were quite high, compared to citric acid derived CDs (CCDs). HCDs and SCDs possess optimal photostability, hypotoxicity and biocompatibility in zebrafish, indicating that HCDs and SCDs possess the capacity of being used as fluorescence probes for in vivo biological imaging. The long-time observation for fluorescence alternation of CDs in zebrafish and the quenching assay of CDs by ATP, NADH and Fe 3+ ions demonstrated that the decaying process of CDs in vivo might be induced by the synergistic effect of the metabolism process. All results indicated that large batches and high QYs of CDs can be acquired by employing natural and nontoxic hair and skin as precursors. To our knowledge, this is the first time to report SCDs, in vivo comparative studies of HCDs, SCDs and CCDs as bioprobes, and explore their mechanism of photostability in zebrafish.

In vivo characterization of hair and skin derived carbon quantum dots with high quantum yield as long-term bioprobes in zebrafish

NASA Astrophysics Data System (ADS)

Zhang, Jing-Hui; Niu, Aping; Li, Jing; Fu, Jian-Wei; Xu, Qun; Pei, De-Sheng

2016-11-01

Carbon quantum dots (CDs) were widely investigated because of their tunable fluorescence properties and low toxicity. However, so far there have been no reports on in vivo functional studies of hair and skin derived CDs. Here, hair derived CDs (HCDs) and skin derived CDs (SCDs) were produced by using human hair and pig skin as precursors. The quantum yields (QYs) of HCDs and SCDs were quite high, compared to citric acid derived CDs (CCDs). HCDs and SCDs possess optimal photostability, hypotoxicity and biocompatibility in zebrafish, indicating that HCDs and SCDs possess the capacity of being used as fluorescence probes for in vivo biological imaging. The long-time observation for fluorescence alternation of CDs in zebrafish and the quenching assay of CDs by ATP, NADH and Fe3+ ions demonstrated that the decaying process of CDs in vivo might be induced by the synergistic effect of the metabolism process. All results indicated that large batches and high QYs of CDs can be acquired by employing natural and nontoxic hair and skin as precursors. To our knowledge, this is the first time to report SCDs, in vivo comparative studies of HCDs, SCDs and CCDs as bioprobes, and explore their mechanism of photostability in zebrafish.

Arginine-glycine-aspartic acid-conjugated dendrimer-modified quantum dots for targeting and imaging melanoma.

PubMed

Li, Zhiming; Huang, Peng; Lin, Jing; He, Rong; Liu, Bing; Zhang, Xiaomin; Yang, Sen; Xi, Peng; Zhang, Xuejun; Ren, Qiushi; Cui, Daxiang

2010-08-01

Angiogenesis is essential for the development of malignant tumors and provides important targets for tumor diagnosis and therapy. Quantum dots have been broadly investigated for their potential application in cancer molecular imaging. In present work, CdSe quantum dots were synthesized, polyamidoamine dendrimers were used to modify surface of quantum dots and improve their solubility in water solution. Then, dendrimer-modified CdSe quantum dots were conjugated with arginine-glycine-aspartic acid (RGD) peptides. These prepared nanoprobes were injected into nude mice loaded with melanoma (A375) tumor xenografts via tail vessels, IVIS imaging system was used to image the targeting and bio-distribution of as-prepared nanoprobes. The dendrimer-modified quantum dots exhibit water-soluble, high quantum yield, and good biocompatibility. RGD-conjugated quantum dots can specifically target human umbilical vein endothelial cells (HUVEC) and A375 melanoma cells, as well as nude mice loaded with A735 melanoma cells. High-performance RGD-conjugated dendrimers modified quantum dot-based nanoprobes have great potential in application such as tumor diagnosis and therapy.

Mapping quantum yield for (Fe-Zn-Sn-Ti)Ox photoabsorbers using a high throughput photoelectrochemical screening system.

PubMed

Xiang, Chengxiang; Haber, Joel; Marcin, Martin; Mitrovic, Slobodan; Jin, Jian; Gregoire, John M

2014-03-10

Combinatorial synthesis and screening of light absorbers are critical to material discoveries for photovoltaic and photoelectrochemical applications. One of the most effective ways to evaluate the energy-conversion properties of a semiconducting light absorber is to form an asymmetric junction and investigate the photogeneration, transport and recombination processes at the semiconductor interface. This standard photoelectrochemical measurement is readily made on a semiconductor sample with a back-side metallic contact (working electrode) and front-side solution contact. In a typical combinatorial material library, each sample shares a common back contact, requiring novel instrumentation to provide spatially resolved and thus sample-resolved measurements. We developed a multiplexing counter electrode with a thin layer assembly, in which a rectifying semiconductor/liquid junction was formed and the short-circuit photocurrent was measured under chopped illumination for each sample in a material library. The multiplexing counter electrode assembly demonstrated a photocurrent sensitivity of sub-10 μA cm(-2) with an external quantum yield sensitivity of 0.5% for each semiconductor sample under a monochromatic ultraviolet illumination source. The combination of cell architecture and multiplexing allows high-throughput modes of operation, including both fast-serial and parallel measurements. To demonstrate the performance of the instrument, the external quantum yields of 1819 different compositions from a pseudoquaternary metal oxide library, (Fe-Zn-Sn-Ti)Ox, at 385 nm were collected in scanning serial mode with a throughput of as fast as 1 s per sample. Preliminary screening results identified a promising ternary composition region centered at Fe0.894Sn0.103Ti0.0034Ox, with an external quantum yield of 6.7% at 385 nm.

Co-reductive fabrication of carbon nanodots with high quantum yield for bioimaging of bacteria

PubMed Central

Wang, Jiajun; Liu, Xia; Milcovich, Gesmi; Chen, Tzu-Yu; Durack, Edel; Mallen, Sarah; Ruan, Yongming

2018-01-01

A simple and straightforward synthetic approach for carbon nanodots (C-dots) is proposed. The strategy is based on a one-step hydrothermal chemical reduction with thiourea and urea, leading to high quantum yield C-dots. The obtained C-dots are well-dispersed with a uniform size and a graphite-like structure. A synergistic reduction mechanism was investigated using Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy. The findings show that using both thiourea and urea during the one-pot synthesis enhances the luminescence of the generated C-dots. Moreover, the prepared C-dots have a high distribution of functional groups on their surface. In this work, C-dots proved to be a suitable nanomaterial for imaging of bacteria and exhibit potential for application in bioimaging thanks to their low cytotoxicity. PMID:29441259

Increasing selectivity for TNT-based explosive detection by synchronous luminescence and derivative spectroscopy with quantum yields of selected aromatic amines.

PubMed

Sheaff, Chrystal N; Eastwood, Delyle; Wai, Chien M

2007-01-01

The detection of explosive material is at the forefront of current analytical problems. A detection method is desired that is not restricted to detecting only explosive materials, but is also capable of identifying the origin and type of explosive. It is essential that a detection method have the selectivity to distinguish among compounds in a mixture of explosives. The nitro compounds found in explosives have low fluorescent yields or are considered to be non-fluorescent; however, after reduction, the amino compounds exhibit relatively high fluorescence. We discuss how to increase selectivity of explosive detection using fluorescence; this includes synchronous luminescence and derivative spectroscopy with appropriate smoothing. By implementing synchronous luminescence and derivative spectroscopy, we were able to resolve the reduction products of one major TNT-based explosive compound, 2,4-diaminotoluene, and the reduction products of other minor TNT-based explosives in a mixture. We also report for the first time the quantum yields of these important compounds. Relative quantum yields are useful in establishing relative fluorescence intensities and are an important spectroscopic measurement of molecules. Our approach allows for rapid, sensitive, and selective detection with the discrimination necessary to distinguish among various explosives.

Quantum Yields of Soluble and Particulate Material in the Ocean

DTIC Science & Technology

1999-09-30

and prospects. IEEE Transactions, 46(5): 825-829 In Press Moisan, T.A. & B.G. Mitchell UV Absorption by Mycosporine - like Amino Acids in Phaeocystis...were grown to evaluate the spectral quantum yield of in vivo chlorophyll a fluorescence. We determined that mycosporine amino acids with UV absorption...evaluate the role of photoprotective pigments, including mycosporine amino acids and the xanthophyll pigments in Phaeocystis, on the spectral quantum yield

Colloidal Spherical Quantum Wells with Near-Unity Photoluminescence Quantum Yield and Suppressed Blinking.

PubMed

Jeong, Byeong Guk; Park, Young-Shin; Chang, Jun Hyuk; Cho, Ikjun; Kim, Jai Kyeong; Kim, Heesuk; Char, Kookheon; Cho, Jinhan; Klimov, Victor I; Park, Philip; Lee, Doh C; Bae, Wan Ki

2016-10-02

Thick inorganic shell endows colloidal nanocrystals (NCs) with enhanced photochemical stability and suppression of photoluminescence intermittency (also known as blinking). However, the progress of using thick-shell heterostructure NCs in applications has been limited, due to low photoluminescence quantum yield (PL QY  60%) at room temperature. Here, we demonstrate thick-shell NCs with CdS/CdSe/CdS seed/spherical quantum well/shell (SQW) geometry that exhibit near-unity PL QY at room temperature and suppression of blinking. In SQW NCs, the lattice mismatch is diminished between the emissive CdSe layer and the surrounding CdS layers as a result of coherent strain, which suppresses the formation of misfit defects and consequently permits ~ 100% PL QY for SQW NCs with thick CdS shell (≥ 5 nm). High PL QY of thick-shell SQW NCs are preserved even in concentrated dispersion and in film under thermal stress, which makes them promising candidates for applications in solid-state lightings and luminescent solar concentrators.

Complex Chemical Reaction Networks from Heuristics-Aided Quantum Chemistry.

PubMed

Rappoport, Dmitrij; Galvin, Cooper J; Zubarev, Dmitry Yu; Aspuru-Guzik, Alán

2014-03-11

While structures and reactivities of many small molecules can be computed efficiently and accurately using quantum chemical methods, heuristic approaches remain essential for modeling complex structures and large-scale chemical systems. Here, we present a heuristics-aided quantum chemical methodology applicable to complex chemical reaction networks such as those arising in cell metabolism and prebiotic chemistry. Chemical heuristics offer an expedient way of traversing high-dimensional reactive potential energy surfaces and are combined here with quantum chemical structure optimizations, which yield the structures and energies of the reaction intermediates and products. Application of heuristics-aided quantum chemical methodology to the formose reaction reproduces the experimentally observed reaction products, major reaction pathways, and autocatalytic cycles.

The initiating radical yields and the efficiency of polymerization for various dental photoinitiators excited by different light curing units.

PubMed

Neumann, Miguel G; Schmitt, Carla C; Ferreira, Giovana C; Corrêa, Ivo C

2006-06-01

To evaluate the efficiency of the photopolymerization of dental resins it is necessary to know to what extent the light emitted by the light curing units is absorbed by the photoinitiators. On the other hand, the efficiency of the absorbed photons to produce species that launch the polymerization process is also of paramount importance. Therefore, the previously determined PAE (photon absorption efficiency) is used in conjunction with the polymerization quantum yields for the photoinitiators, in order to be able to compare the total process on an equivalent basis. This parameter can be used to identify the best performance for the photochemical process with specific photoinitiators. The efficiency of LED (Ultrablue IS) and QTH (Optilux 401) lamps were tested comparing their performances with the photoinitiators camphorquinone (CQ); phenylpropanedione (PPD); monoacylphosphine oxide (Lucirin TPO); and bisacylphosphine oxide (Irgacure 819). The extent of photopolymerization per absorbed photon was determined from the polymerization quantum yields obtained by using the photoinitiators to polymerize methyl methacrylate, and afterwards combined with the previously determined PAEs. Although CQ presents a rather low polymerization quantum yield, its photopolymerization efficiency is practically the highest when irradiated with the Ultrablue LED. On the other hand, Lucirin is much more efficient than the other photoinitiators when irradiated with a QTH lamp, due to its high quantum yield and the overlap between its absorption spectrum and the output of the visible lamp light. Difference in photopolymerization efficiencies arise when combinations of photoinitiators are used, and when LED sources are used in preference to QTH. Mechanistic understanding is essential to optimal initiator formulation.

Semiconductor Seeded Nanorods with Graded Composition Exhibiting High Quantum-Yield, High Polarization, and Minimal Blinking.

PubMed

Hadar, Ido; Philbin, John P; Panfil, Yossef E; Neyshtadt, Shany; Lieberman, Itai; Eshet, Hagai; Lazar, Sorin; Rabani, Eran; Banin, Uri

2017-04-12

Seeded semiconductor nanorods represent a unique family of quantum confined materials that manifest characteristics of mixed dimensionality. They show polarized emission with high quantum yield and fluorescence switching under an electric field, features that are desirable for use in display technologies and other optical applications. So far, their robust synthesis has been limited mainly to CdSe/CdS heterostructures, thereby constraining the spectral tunability to the red region of the visible spectrum. Herein we present a novel synthesis of CdSe/Cd 1-x Zn x S seeded nanorods with a radially graded composition that show bright and highly polarized green emission with minimal intermittency, as confirmed by ensemble and single nanorods optical measurements. Atomistic pseudopotential simulations elucidate the importance of the Zn atoms within the nanorod structure, in particular the effect of the graded composition. Thus, the controlled addition of Zn influences and improves the nanorods' optoelectronic performance by providing an additional handle to manipulate the degree confinement beyond the common size control approach. These nanorods may be utilized in applications that require the generation of a full, rich spectrum such as energy-efficient displays and lighting.

[Fluorescence spectra and quantum yield of TiO2 nanocrystals synthesized by alcohothermal method].

PubMed

Song, Cui-Hong; Li, Yan-Ting; Li, Jing; Wei, Yong-Ju; Hu, Yu-Zhu; Wei, Yu

2008-01-01

Fluorescence spectra and fluorescence quantum yield of TiO2 nanocrystals were studied. Using tetra n-butyl titanate as a starting material, a facile alcohothermal technique was used to synthesize TiO2 nanocrystals. As can be seen from the transmittance electron microscopy (TEM) image, TiO2 nanocrystals with a relatively uniform particle size distribution of < 10 nm are present in the transparent sol. The transparent sol presents a strong stable fluorescence emission with a maximum at 450 nm, which is greatly dependent on the size quantization effects, defect energy level and the surface state of TiO2 nanocrystals. The quantum yield (gamma) of TiO2 was determined by the relative comparison procedure, using freshly prepared analytical purity quinine sulfate in 0.05 mol x L(-1) H2SO4 as a relative quantum yield standard. The emission quantum yield of TiO2 nanocrystals prepared in alcoholic media was calculated to be about 0.20 at wavelengths ranging from 330 to 370 nm, which was much higher than the values reported in previous works. So, it is supposed that nano-TiO2 will be applied as a potential quantum dots fluorescence probe in biological analysis.

Aeronomical determinations of the quantum yields of O (1S) and O (1D) from dissociative recombination of O2(+)

NASA Technical Reports Server (NTRS)

Yee, Jeng-Hwa; Abreu, Vincent J.; Colwell, William B.

1989-01-01

Data from the visible-airglow experiment on the Atmosphere Explorer-E satellite have been used to determine the quantum yields of O (1S) and O (1D) from the dissociative recombination of O2(+) based on a constant total recombination rate from each vibrational level. A range of values between 0.05 and 0.18 has been obtained for the quantum yield of O (1S) and shows a positive correlation with the extent of the vibrational excitation of O2(+). The quantum yield of O (1D) has been measured to be 0.9 + or - 0.2, with no apparent dependence on the vibrational distribution of O2(+).

Tuning Single Quantum Dot Emission with a Micromirror.

PubMed

Yuan, Gangcheng; Gómez, Daniel; Kirkwood, Nicholas; Mulvaney, Paul

2018-02-14

The photoluminescence of single quantum dots fluctuates between bright (on) and dark (off) states, also termed fluorescence intermittency or blinking. This blinking limits the performance of quantum dot-based devices such as light-emitting diodes and solar cells. However, the origins of the blinking remain unresolved. Here, we use a movable gold micromirror to determine both the quantum yield of the bright state and the orientation of the excited state dipole of single quantum dots. We observe that the quantum yield of the bright state is close to unity for these single QDs. Furthermore, we also study the effect of a micromirror on blinking, and then evaluate excitation efficiency, biexciton quantum yield, and detection efficiency. The mirror does not modify the off-time statistics, but it does change the density of optical states available to the quantum dot and hence the on times. The duration of the on times can be lengthened due to an increase in the radiative recombination rate.

Why Do Simple Molecules with "Isolated" Phenyl Rings Emit Visible Light?

PubMed

Zhang, Haoke; Zheng, Xiaoyan; Xie, Ni; He, Zikai; Liu, Junkai; Leung, Nelson L C; Niu, Yingli; Huang, Xuhui; Wong, Kam Sing; Kwok, Ryan T K; Sung, Herman H Y; Williams, Ian D; Qin, Anjun; Lam, Jacky W Y; Tang, Ben Zhong

2017-11-15

π-Bonds connected with aromatic rings were generally believed as the standard structures for constructing highly efficient fluorophores. Materials without these typical structures, however, exhibited only low fluorescence quantum yields and emitted in the ultraviolet spectral region. In this work, three molecules, namely bis(2,4,5-trimethylphenyl)methane, 1,1,2,2-tetrakis(2,4,5-trimethylphenyl)ethane, and 1,1,2,2-tetraphenylethane, with nonconjugated structures and isolated phenyl rings were synthesized and their photophysical properties were systematically investigated. Interestingly, the emission spectra of these three molecules could be well extended to 600 nm with high solid-state quantum yields of up to 70%. Experimental and theoretical analyses proved that intramolecular through-space conjugation between the "isolated" phenyl rings played an important role for this abnormal phenomenon.

Chromophore-Based Luminescent Metal–Organic Frameworks as Lighting Phosphors

DOE PAGES

Lustig, William P.; Wang, Fangming; Teat, Simon J.; ...

2016-05-31

Here, energy-efficient solid-state-lighting (SSL) technologies are rapidly developing, but the lack of stable, high-performance rare-earth free phosphors may impede the growth of the SSL market. One possible alternative is organic phosphor materials, but these can suffer from lower quantum yields and thermal instability compared to rare-earth phosphors. However, if luminescent organic chromophores can be built into a rigid metal-organic framework, their quantum yields and thermal stability can be greatly improved. This Forum Article discusses the design of a group of such chromophore-based luminescent metal-organic frameworks with exceptionally high performance and rational control of the important parameters that influence their emissionmore » properties, including electronic structures of chromophore, coligands, metal ions, and guest molecule s.« less

Estimation of quantum yields of weak fluorescence from eosin Y dimers formed in aqueous solutions.

PubMed

Enoki, Masami; Katoh, Ryuzi

2018-05-17

We studied the weak fluorescence from the dimer of eosin Y (EY) in aqueous solutions. We used a newly developed ultrathin optical cell with a thickness ranging from of the order of microns to several hundreds of microns to successfully measure the fluorescence spectra of highly concentrated aqueous solutions of EY without artifacts caused by the reabsorption of fluorescence. The spectra we obtained were similar to the fluorescence spectrum of the EY monomer; almost no fluorescence was observed from the EY dimer. By a careful comparison of the spectra of solutions at low and high concentrations of EY, we succeeded in extracting the fluorescence spectrum of the EY dimer. The fluorescence quantum yield of the EY dimer was estimated to be 0.005.

Direct Generation and Detection of Quantum Correlated Photons with 3.2 um Wavelength Spacing.

PubMed

Sua, Yong Meng; Fan, Heng; Shahverdi, Amin; Chen, Jia-Yang; Huang, Yu-Ping

2017-12-13

Quantum correlated, highly non-degenerate photons can be used to synthesize disparate quantum nodes and link quantum processing over incompatible wavelengths, thereby constructing heterogeneous quantum systems for otherwise unattainable superior performance. Existing techniques for correlated photons have been concentrated in the visible and near-IR domains, with the photon pairs residing within one micron. Here, we demonstrate direct generation and detection of high-purity photon pairs at room temperature with 3.2 um wavelength spacing, one at 780 nm to match the rubidium D2 line, and the other at 3950 nm that falls in a transparent, low-scattering optical window for free space applications. The pairs are created via spontaneous parametric downconversion in a lithium niobate waveguide with specially designed geometry and periodic poling. The 780 nm photons are measured with a silicon avalanche photodiode, and the 3950 nm photons are measured with an upconversion photon detector using a similar waveguide, which attains 34% internal conversion efficiency. Quantum correlation measurement yields a high coincidence-to-accidental ratio of 54, which indicates the strong correlation with the extremely non-degenerate photon pairs. Our system bridges existing quantum technology to the challenging mid-IR regime, where unprecedented applications are expected in quantum metrology and sensing, quantum communications, medical diagnostics, and so on.

The use of dendrimers as high-performance shells for round-trip energy transfer: efficient trans-cis photoisomerization from an excited triplet state produced within a dendrimer shell.

PubMed

Miura, Yousuke; Momotake, Atsuya; Takeuchi, Keiichirou; Arai, Tatsuo

2011-01-01

A series of stilbene-cored poly(benzyl ether) dendrimers with benzophenone peripheries were synthesized and their photophysical and photochemical properties were studied. Fluorescence studies revealed that singlet-singlet energy transfer (SSET) from the stilbene core to the benzophenone units took place efficiently in dendrimers of all generations. Similarly, phosphorescence and time-resolved spectroscopic measurements indicated efficient triplet-triplet energy transfer (TTET) from the benzophenone periphery to the stilbene core. Upon excitation at 310 nm, the stilbene core isomerizes via an energy round trip within the dendrimer shell. The quantum yields for the energy round trip (Φ(ERT)), defined as the product of the quantum yields of SSET, intersystem crossing, and TTET (Φ(ERT) = Φ(SS)Φ(isc)Φ(TT)), were extremely high for all generations--99%, 95% and 94% for G1, G2, and G3, respectively--which means that the excitation energy of the dendrimer core was transferred to the dendrimer periphery and back to the core almost quantitatively. The quantum yield for photoisomerization of G1-G3 via an energy round trip was higher than for other stilbene-cored dendrimers, which mainly isomerize from the excited singlet state. Photostability in the dendrimers was also demonstrated and discussed.

Solvent Dependency in the Quantum Efficiency of 4-[(4-Aminophenyl)-(4-imino-1-cyclohexa-2, 5- dienylidene) methyl] Aniline Hydrochloride.

PubMed

Pathrose, Bini; Nampoori, V P N; Radhakrishnan, P; Sahira, H; Mujeeb, A

2015-05-01

In the present work dual beam thermal lens technique is used for studying the solvent dependency on the quantum efficiency of a novel dye used for biomedical applications. The role of solvent in the absolute fluorescence quantum yield of 4-[(4-Aminophenyl)-(4-imino-1-cyclohexa-2, 5- dienylidene) methyl] aniline hydrochloride is studied using thermal lens technique. It is observed that the variation in solvents and its concentration results considerable variations in the fluorescence quantum yield. These variations are due to the non-radiative relaxation of the absorbed energy and because of the different solvent properties. The highest quantum yield of the dye is observed in the polar protic solvent-water.

Quantum yield measurements of light-induced H₂ generation in a photosystem I-[FeFe]-H₂ase nanoconstruct.

PubMed

Applegate, Amanda M; Lubner, Carolyn E; Knörzer, Philipp; Happe, Thomas; Golbeck, John H

2016-01-01

The quantum yield for light-induced H2 generation was measured for a previously optimized bio-hybrid cytochrome c 6-crosslinked PSI(C13G)-1,8-octanedithiol-[FeFe]-H2ase(C97G) (PSI-H2ase) nanoconstruct. The theoretical quantum yield for the PSI-H2ase nanoconstruct is 0.50 molecules of H2 per photon absorbed, which equates to a requirement of two photons per H2 generated. Illumination of the PSI-H2ase nanoconstruct with visible light between 400 and 700 nm resulted in an average quantum yield of 0.10-0.15 molecules of H2 per photon absorbed, which equates to a requirement of 6.7-10 photons per H2 generated. A possible reason for the difference between the theoretical and experimental quantum yield is the occurrence of non-productive PSI(C13G)-1,8-octanedithiol-PSIC13G (PSI-PSI) conjugates, which would absorb light without generating H2. Assuming the thiol-Fe coupling is equally efficient at producing PSI-PSI conjugates as well as in producing PSI-H2ase nanoconstructs, the theoretical quantum yield would decrease to 0.167 molecules of H2 per photon absorbed, which equates to 6 photons per H2 generated. This value is close to the range of measured values in the current study. A strategy that purifies the PSI-H2ase nanoconstructs from the unproductive PSI-PSI conjugates or that incorporates different chemistries on the PSI and [FeFe]-H2ase enzyme sites could potentially allow the PSI-H2ase nanoconstruct to approach the expected theoretical quantum yield for light-induced H2 generation.

Photogeneration of reactive transient species upon irradiation of natural water samples: Formation quantum yields in different spectral intervals, and implications for the photochemistry of surface waters.

PubMed

Marchisio, Andrea; Minella, Marco; Maurino, Valter; Minero, Claudio; Vione, Davide

2015-04-15

Chromophoric dissolved organic matter (CDOM) in surface waters is a photochemical source of several transient species such as CDOM triplet states ((3)CDOM*), singlet oxygen ((1)O2) and the hydroxyl radical (OH). By irradiation of lake water samples, it is shown here that the quantum yields for the formation of these transients by CDOM vary depending on the irradiation wavelength range, in the order UVB > UVA > blue. A possible explanation is that radiation at longer wavelengths is preferentially absorbed by the larger CDOM fractions, which show lesser photoactivity compared to smaller CDOM moieties. The quantum yield variations in different spectral ranges were definitely more marked for (3)CDOM* and OH compared to (1)O2. The decrease of the quantum yields with increasing wavelength has important implications for the photochemistry of surface waters, because long-wavelength radiation penetrates deeper in water columns compared to short-wavelength radiation. The average steady-state concentrations of the transients ((3)CDOM*, (1)O2 and OH) were modelled in water columns of different depths, based on the experimentally determined wavelength trends of the formation quantum yields. Important differences were found between such modelling results and those obtained in a wavelength-independent quantum yield scenario. Copyright © 2015 Elsevier Ltd. All rights reserved.

Quantum Yield Heterogeneity among Single Nonblinking Quantum Dots Revealed by Atomic Structure-Quantum Optics Correlation

DOE PAGES

Orfield, Noah J.; McBride, James R.; Wang, Feng; ...

2016-02-05

Physical variations in colloidal nanostructures give rise to heterogeneity in expressed optical behavior. This correlation between nanoscale structure and function demands interrogation of both atomic structure and photophysics at the level of single nanostructures to be fully understood. In this paper, by conducting detailed analyses of fine atomic structure, chemical composition, and time-resolved single-photon photoluminescence data for the same individual nanocrystals, we reveal inhomogeneity in the quantum yields of single nonblinking “giant” CdSe/CdS core/shell quantum dots (g-QDs). We find that each g-QD possesses distinctive single exciton and biexciton quantum yields that result mainly from variations in the degree of charging,more » rather than from volume or structure inhomogeneity. We further establish that there is a very limited nonemissive “dark” fraction (<2%) among the studied g-QDs and present direct evidence that the g-QD core must lack inorganic passivation for the g-QD to be “dark”. Finally and therefore, in contrast to conventional QDs, ensemble photoluminescence quantum yield is principally defined by charging processes rather than the existence of dark g-QDs.« less

Cultivating Fluorescent Flowers with Highly Luminescent Carbon Dots Fabricated by a Double Passivation Method.

PubMed

Han, Shuai; Chang, Tao; Zhao, Haiping; Du, Huanhuan; Liu, Shan; Wu, Baoshuang; Qin, Shenjun

2017-07-07

In this work, we present the fabrication of highly luminescent carbon dots (CDs) by a double passivation method with the assistance of Ca(OH)₂. In the reaction process, Ca 2+ protects the active functional groups from overconsumption during dehydration and carbonization, and the electron-withdrawing groups on the CD surface are converted to electron-donating groups by the hydroxyl ions. As a result, the fluorescence quantum yield of the CDs was found to increase with increasing Ca(OH)₂ content in the reaction process. A blue-shift optical spectrum of the CDs was also found with increasing Ca(OH)₂ content, which could be attributed to the increasing of the energy gaps for the CDs. The highly photoluminescent CDs obtained (quantum yield: 86%) were used to cultivate fluorescent carnations by a water culture method, while the results of fluorescence microscopy analysis indicated that the CDs had entered the plant tissue structure.

Water-soluble multidentate polymers compactly coating Ag2S quantum dots with minimized hydrodynamic size and bright emission tunable from red to second near-infrared region.

PubMed

Gui, Rijun; Wan, Ajun; Liu, Xifeng; Yuan, Wen; Jin, Hui

2014-05-21

Hydrodynamic size-minimized quantum dots (QDs) have outstanding physicochemical properties for applications in multicolor molecular and cellular imaging at the level of single molecules and nanoparticles. In this study, we have reported the aqueous synthesis of Ag2S QDs by using thiol-based multidentate polymers as capping reagents. By regulating the composition of the precursors (AgNO3 and sulfur-N2H4·H2O complex) and multidentate polymers (poly(acrylic acid)-graft-cysteamine-graft-ethylenediamine), as well as the reaction time, Ag2S QDs (2.6-3.7 nm) are prepared, displaying tunable photoluminescence (PL) emission from red to the second near-infrared region (687-1096 nm). The small hydrodynamic thickness (1.6-1.9 nm) of the multidentate polymers yields a highly compact coating for the QDs, which results in the bright fluorescent QDs with high PL quantum yields (QYs: 14.2-16.4%). Experimental results confirm that the QDs have high PL stability and ultralow cytotoxicity, as well as high PLQYs and small hydrodynamic sizes (4.5-5.6 nm) similar to fluorescent proteins (27-30 kDa), indicating the feasibility of highly effective PL imaging in cells and living animals.

Combined low temperature-high light effects on gas exchange properties of jojoba leaves.

PubMed

Loreto, F; Bongi, G

1989-12-01

Jojoba (Simmondsia chinensis [Link] Schneider) is an important crop in desert climates. A relatively high frequency of periods of chilling and high photon flux density (PFD) in this environment makes photoinhibition likely, resulting in a reduction of assimilation capacity in overwintering leaves. This could explain the low net photosynthesis found in shoots from the field (4-6 micromoles per square meter per second) when compared to greenhouse grown plants (12-15 micromoles per square meter per second). The responses of photosynthesis and stomatal conductance to changes in absorbed PFD and in substomatal partial pressure of CO(2) were measured on jojoba leaves recovering from chilling temperature (4 degrees C) in high or low PFD. No measurable gas exchange was found immediately after chilling in either high or low PFD. For leaves chilled in low PFD, the original quantum yield was restored after 24 hours. The time course of recovery from chilling in high PFD was much longer. Quantum yield recovered to 60% of its original value in 72 hours but failed to recover fully after 1 week. Measurements of PSII chlorophyll fluorescence at 77 K showed that the reduced quantum yield was caused by photoinhibition. The ratio of variable to maximal fluorescence fell from a control level of 0.82 to 0.41 after the photoinhibitory treatment and recovery was slow. We also found a large increase in net assimilation rate and little closure of stomata as CO(2) was increased from ambient partial pressure of 35 to 85 pascals. For plants grown in full light, the increase in net assimilation rate was 100%. The photosynthetic response at high CO(2) concentration may constitute an ecological advantage of jojoba as a crop in the future.

Combined Low Temperature-High Light Effects on Gas Exchange Properties of Jojoba Leaves 1

PubMed Central

Loreto, Francesco; Bongi, Guido

1989-01-01

Jojoba (Simmondsia chinensis [Link] Schneider) is an important crop in desert climates. A relatively high frequency of periods of chilling and high photon flux density (PFD) in this environment makes photoinhibition likely, resulting in a reduction of assimilation capacity in overwintering leaves. This could explain the low net photosynthesis found in shoots from the field (4-6 micromoles per square meter per second) when compared to greenhouse grown plants (12-15 micromoles per square meter per second). The responses of photosynthesis and stomatal conductance to changes in absorbed PFD and in substomatal partial pressure of CO2 were measured on jojoba leaves recovering from chilling temperature (4°C) in high or low PFD. No measurable gas exchange was found immediately after chilling in either high or low PFD. For leaves chilled in low PFD, the original quantum yield was restored after 24 hours. The time course of recovery from chilling in high PFD was much longer. Quantum yield recovered to 60% of its original value in 72 hours but failed to recover fully after 1 week. Measurements of PSII chlorophyll fluorescence at 77 K showed that the reduced quantum yield was caused by photoinhibition. The ratio of variable to maximal fluorescence fell from a control level of 0.82 to 0.41 after the photoinhibitory treatment and recovery was slow. We also found a large increase in net assimilation rate and little closure of stomata as CO2 was increased from ambient partial pressure of 35 to 85 pascals. For plants grown in full light, the increase in net assimilation rate was 100%. The photosynthetic response at high CO2 concentration may constitute an ecological advantage of jojoba as a crop in the future. PMID:16667220

Tuning Optoelectronic Properties of the Graphene-Based Quantum Dots C16- xSi xH10 Family.

PubMed

Ramadan, F-Z; Ouarrad, H; Drissi, L B

2018-06-07

The electronic and optical properties of graphene-based quantum dots (QDs) are investigated using DFT and many-body perturbation theory. Formation energy, hardeness and electrophilicity show that all structures, from pyrene to silicene QD passing through 15 CSi QD configurations, are energetically and chemically stable. It is also found that they are reactive which implies their favorable character for the possible electronic transport and conductivity. The electronic and optical properties are very sensitive to the number and position of the substituted silicon atoms as well as the directions of the light polarization. Moreover, quantum confinement effects make the exciton binding energy of CSi quantum dots larger than those of their higher dimensional allotropes such as silicene, graphene, and SiC sheet and nanotube. It is also higher those of other shapes of quantum dots like hexagonal graphene QDs and can be tailored from the ultraviolet region to the visible one. The values of the singlet-triplet splitting determined for the X- and Y-light polarized indicate that all configurations have a high fluorescence quantum yield compared to the yield of typical semiconductors, which makes them very promising for various applications such as the light-emitting diode material and nanomedicine.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Peng; State Key Laboratory of Superhard Materials, College of Physics, Jilin University, Changchun 130012; Bai, Xue, E-mail: baix@jlu.edu.cn, E-mail: yuzhang@jlu.edu.cn

High quantum yield, narrow full width at half-maximum and tunable emission color of perovskite quantum dots (QDs) make this kind of material good prospects for light-emitting diodes (LEDs). However, the relatively poor stability under high temperature and air condition limits the device performance. To overcome this issue, the liquid-type packaging structure in combination with blue LED chip was employed to fabricate the fluorescent perovskite quantum dot-based LEDs. A variety of monochromatic LEDs with green, yellow, reddish-orange, and red emission were fabricated by utilizing the inorganic cesium lead halide perovskite quantum dots as the color-conversion layer, which exhibited the narrow fullmore » width at half-maximum (<35 nm), the relatively high luminous efficiency (reaching 75.5 lm/W), and the relatively high external quantum efficiency (14.6%), making it the best-performing perovskite LEDs so far. Compared to the solid state LED device, the liquid-type LED devices exhibited excellent color stability against the various working currents. Furthermore, we demonstrated the potential prospects of all-inorganic perovskite QDs for the liquid-type warm white LEDs.« less

On the minimum quantum requirement of photosynthesis.

PubMed

Zeinalov, Yuzeir

2009-01-01

An analysis of the shape of photosynthetic light curves is presented and the existence of the initial non-linear part is shown as a consequence of the operation of the non-cooperative (Kok's) mechanism of oxygen evolution or the effect of dark respiration. The effect of nonlinearity on the quantum efficiency (yield) and quantum requirement is reconsidered. The essential conclusions are: 1) The non-linearity of the light curves cannot be compensated using suspensions of algae or chloroplasts with high (>1.0) optical density or absorbance. 2) The values of the maxima of the quantum efficiency curves or the values of the minima of the quantum requirement curves cannot be used for estimation of the exact value of the maximum quantum efficiency and the minimum quantum requirement. The estimation of the maximum quantum efficiency or the minimum quantum requirement should be performed only after extrapolation of the linear part at higher light intensities of the quantum requirement curves to "0" light intensity.

Plasmonic enhancement of electroluminescence

NASA Astrophysics Data System (ADS)

Guzatov, D. V.; Gaponenko, S. V.; Demir, H. V.

2018-01-01

Here plasmonic effect specifically on electroluminescence (EL) is studied in terms of radiative and nonradiative decay rates for a dipole near a metal spherical nanoparticle (NP). Contribution from scattering is taken into account and is shown to play a decisive role in EL enhancement owing to pronounced size-dependent radiative decay enhancement and weak size effect on non-radiative counterpart. Unlike photoluminescence where local incident field factor mainly determines the enhancement possibility and level, EL enhancement is only possible by means of quantum yield rise, EL enhancement being feasible only for an intrinsic quantum yield Q0 < 1. The resulting plasmonic effect is independent of intrinsic emitter lifetime but is exclusively defined by the value of Q0, emission spectrum, NP diameter and emitter-metal spacing. For 0.1< Q0 < 0.25, Ag nanoparticles are shown to enhance LED/OLED intensity by several times over the whole visible whereas Au particles feature lower effect within the red-orange range only. Independently of positive effect on quantum yield, metal nanoparticles embedded in an electroluminescent device will improve its efficiency at high currents owing to enhanced overall recombination rate which will diminish manifestation of Auger processes. The latter are believed to be responsible for the known undesirable efficiency droop in semiconductor commercial quantum well based LEDs at higher current. For the same reason plasmonics can diminish quantum dot photodegradation from Auger process induced non-radiative recombination and photoionization thus opening a way to avoid negative Auger effects in emerging colloidal semiconductor LEDs.

pH-Induced transformation of ligated Au25 to brighter Au23 nanoclusters.

PubMed

Waszkielewicz, Magdalena; Olesiak-Banska, Joanna; Comby-Zerbino, Clothilde; Bertorelle, Franck; Dagany, Xavier; Bansal, Ashu K; Sajjad, Muhammad T; Samuel, Ifor D W; Sanader, Zeljka; Rozycka, Miroslawa; Wojtas, Magdalena; Matczyszyn, Katarzyna; Bonacic-Koutecky, Vlasta; Antoine, Rodolphe; Ozyhar, Andrzej; Samoc, Marek

2018-05-01

Thiolate-protected gold nanoclusters have recently attracted considerable attention due to their size-dependent luminescence characterized by a long lifetime and large Stokes shift. However, the optimization of nanocluster properties such as the luminescence quantum yield is still a challenge. We report here the transformation of Au25Capt18 (Capt labels captopril) nanoclusters occurring at low pH and yielding a product with a much increased luminescence quantum yield which we have identified as Au23Capt17. We applied a simple method of treatment with HCl to accomplish this transformation and we characterized the absorption and emission of the newly created ligated nanoclusters as well as their morphology. Based on DFT calculations we show which Au nanocluster size transformations can lead to highly luminescent species such as Au23Capt17.

Estimation of the quantum efficiency of the photodissociation of HbO2 and HbCO

NASA Astrophysics Data System (ADS)

Gisbrecht, A. I.; Mamilov, S. A.; Esman, S. S.; Asimov, M. M.

2016-01-01

The paper presents our results on the study of the efficiency of inter-fractional changes in hemoglobin molecules depending on the laser radiation parameters. The evaluation of the quantum efficiency of light interaction in vivo with oxyhemoglobin (HbO2) and carboxyhemoglobin (HbCO) in the blood at wavelengths for 525 and 605 nm is presented. The photodissociation yield of 11% for HbO2 and 79% for HbCO are measured at the wavelength of 525 nm and 10 % for HbO2 and 76 % for HbCO at a wavelength of 605 nm. Thus, the quantum yield of photodissociation of the HbCO is considerably higher, which ensures high efficiency of photodecomposition of the HbCO in the blood. The obtained results can be used in the clinical phototherapy practice for effective treatment of CO poisoning.

Novel highly luminescent amine-functionalized bridged silsesquioxanes

NASA Astrophysics Data System (ADS)

Pereira, Rui F. P.; Nunes, Sílvia C.; Toquer, Guillaume; Cardoso, Marita A.; Valente, Artur J. M.; Ferro, Marta C.; Silva, Maria M.; Carlos, Luís D.; Ferreira, Rute A. S.; de Zea Bermudez, Verónica

2017-12-01

Amine-functionalized bridged silsesquioxanes were synthesized from bis[(3-trimethoxysilyl)propyl] amine via a solvent-mediated route. BS-1 and BS-2 were obtained with neutral pH with sub- and stoichiometric amounts of water, respectively, and high tetrahydrofuran content. BS-3 was prepared with hyperstoichiometric water concentration, high tetrahydrofuran content and hydrochloric acid. BS-4 was synthesized with hyperstoichiometric water concentration, high ethanol content and sodium hydroxide. BS-1 and BS-2 were produced as transparent films, whereas BS-3 and BS-4 formed white powders. Face-to-face stacking of flat or folded lamellae yielded quasi-hydrophobic platelets with emission quantum yields of 0.05±0.01 (BS-1 and BS-2) or superhydrophilic onion-like nanoparticles with exciting emission quantum yields of 0.38±0.03 (BS-3) and 0.33±0.04 (BS-4), respectively. The latter two values are the largest ever reported for amine-functionalized siloxane-based hybrids lacking aromatic groups. Fast Grotthus proton hopping between =NH2+/=NH groups (BS-3) and =N-/=NH groups (BS-4), promoted by H+ and OH- ions, respectively, and aided by short amine-amine contacts provided by the onion-like morphology, account for this unique optical behavior.

Primary quantum yields of NO2 photodissociation

NASA Technical Reports Server (NTRS)

Gardner, Edward P.; Sperry, Paul D.; Calvert, Jack G.

1987-01-01

The quantum yields of formation of NO, O2, and NO2 loss are measured for NO2 vapor at low pressures (0.13-0.30 torr) irradiated at 334-405 nm wavelengths and temperature in the range 273-370 K in order to study the primary quantum efficiencies of NO2 photodecomposition. The temperature and wavelength dependences of the primary quantum efficiencies are examined. It is observed that the primary quantum efficiencies increase rapidly from near zero at 424 nm to near unity for excitation at wavelengths less than 394 nm. The theory of Pitts et al. (1964) that the energy deficiency for photodissociation of NO2 excited at wavelengths greater than 397.9 nm is due to the rotational and vibrational energy of the NO2 molecules is confirmed by the data. Values for the primary quantum yields of NO2 photodecomposition as a function of wavelength are presented.

Rose bengal in poly(2-hydroxyethyl methacrylate) thin films: self-quenching by photoactive energy traps

NASA Astrophysics Data System (ADS)

Ezquerra Riega, Sergio D.; Rodríguez, Hernán B.; San Román, Enrique

2017-03-01

The effect of dye concentration on the fluorescence,ΦF, and singlet molecular oxygen,ΦΔ, quantum yields of rose bengal loaded poly(2-hydroxyethyl methacrylate) thin films (∼200 nm thick) was investigated, with the aim of understanding the effect of molecular interactions on the photophysical properties of dyes in crowded constrained environments. Films were characterized by absorption and fluorescence spectroscopy, singlet molecular oxygen (1O2) production was quantified using a chemical monitor, and the triplet decay was determined by laser flash-photolysis. For the monomeric dilute dye, ΦF = 0.05 ± 0.01 and ΦΔ = 0.76 ± 0.14. The effect of humidity and the photostability of the dye were also investigated. Spectral changes in absorption and fluorescence in excess of 0.05 M and concentration self-quenching after 0.01 M are interpreted in the context of a quenching radius model. Calculations of energy migration and trapping rates were performed assuming random distribution of the dye. Best fits of fluorescence quantum yields with concentration are obtained in the whole concentration range with a quenching radius r Q = 1.5 nm, in the order of molecular dimensions. Agreement is obtained only if dimeric traps are considered photoactive, with an observed fluorescence quantum yield ratio ΦF,trap/ΦF,monomer ≈ 0.35. Fluorescent traps are capable of yielding triplet states and 1O2. Results show that the excited state generation efficiency, calculated as the product between the absorption factor and the fluorescence quantum yield, is maximized at around 0.15 M, a very high concentration for random dye distributions. Relevant information for the design of photoactive dyed coatings is provided.

Photosensitized electron transfer processes in SiO2 colloids and sodium lauryl sulfate micellar systems: Correlation of quantum yields with interfacial surface potentials

PubMed Central

Laane, Colja; Willner, Itamar; Otvos, John W.; Calvin, Melvin

1981-01-01

The effectiveness of negatively charged colloidal SiO2 particles in controlling photosensitized electron transfer reactions has been studied and compared with that of the negatively charged sodium lauryl sulfate (NaLauSO4) micellar system. In particular, the photosensitized reduction of the zwitterionic electron acceptor propylviologen sulfonate (PVS0) with tris(2,2′-bipyridinium)ruthenium(II) [Ru(bipy)32+] as the sensitizer and triethanolamine as the electron donor is found to have a quantum yield of 0.033 for formation of the radical anion (PVS[unk]) in the SiO2 colloid compared with 0.005 in the homogeneous system and 0.0086 in a NaLauSO4 micellar solution. The higher quantum yields obtained with the SiO2 colloidal system are attributed to substantial stabilization against back reaction of the intermediate photoproducts—i.e., Ru(bipy)33+ and PVS[unk]—by electrostatic repulsion of the reduced electron acceptor from the negatively charged particle surface. The binding properties of the SiO2 particles and NaLauSO4 micelles were investigated by flow dialysis. The results show that the sensitizer binds to both interfaces and that the SiO2 interface is characterized by a much higher surface potential than the micellar interface (≈-170 mV vs. -85 mV). The effect of ionic strength on the surface potential was estimated from the Gouy-Chapman theory, and the measured quantum yields of photosensitized electron transfer were correlated with surface potential at different ionic strengths. This correlation shows that the quantum yield is not affected by surface potentials smaller than ≈-40 mV. At larger potentials, the quantum yield increases rapidly. The quantum yield obtained in the micellar system at different strengths fits nicely on the correlation curve for the colloid SiO2 system. These results indicate that the surface potential is the dominant factor in the quantum yield improvement for PVS0 reduction. PMID:16593095

Tomographic imaging of flourescence resonance energy transfer in highly light scattering media

NASA Astrophysics Data System (ADS)

Soloviev, Vadim Y.; McGinty, James; Tahir, Khadija B.; Laine, Romain; Stuckey, Daniel W.; Mohan, P. Surya; Hajnal, Joseph V.; Sardini, Alessandro; French, Paul M. W.; Arridge, Simon R.

2010-02-01

Three-dimensional localization of protein conformation changes in turbid media using Förster Resonance Energy Transfer (FRET) was investigated by tomographic fluorescence lifetime imaging (FLIM). FRET occurs when a donor fluorophore, initially in its electronic excited state, transfers energy to an acceptor fluorophore in close proximity through non-radiative dipole-dipole coupling. An acceptor effectively behaves as a quencher of the donor's fluorescence. The quenching process is accompanied by a reduction in the quantum yield and lifetime of the donor fluorophore. Therefore, FRET can be localized by imaging changes in the quantum yield and the fluorescence lifetime of the donor fluorophore. Extending FRET to diffuse optical tomography has potentially important applications such as in vivo studies in small animal. We show that FRET can be localized by reconstructing the quantum yield and lifetime distribution from time-resolved non-invasive boundary measurements of fluorescence and transmitted excitation radiation. Image reconstruction was obtained by an inverse scattering algorithm. Thus we report, to the best of our knowledge, the first tomographic FLIM-FRET imaging in turbid media. The approach is demonstrated by imaging a highly scattering cylindrical phantom concealing two thin wells containing cytosol preparations of HEK293 cells expressing TN-L15, a cytosolic genetically-encoded calcium FRET sensor. A 10mM calcium chloride solution was added to one of the wells to induce a protein conformation change upon binding to TN-L15, resulting in FRET and a corresponding decrease in the donor fluorescence lifetime. The resulting fluorescence lifetime distribution, the quantum efficiency, absorption and scattering coefficients were reconstructed.

Improved photoluminescence quantum yield and stability of CdSe-TOP, CdSe-ODA-TOPO, CdSe/CdS and CdSe/EP nanocomposites

NASA Astrophysics Data System (ADS)

Wei, Shutian; Zhu, Zhilin; Wang, Zhixiao; Wei, Gugangfen; Wang, Pingjian; Li, Hai; Hua, Zhen; Lin, Zhonghai

2016-07-01

Size-controllable monodisperse CdSe nanocrystals with different organic capping were prepared based on the hot-injection method. The effective separation of nucleation and growth was achieved by rapidly mixing two highly reactive precursors. As a contrast, we prepared CdSe/CdS nanocrystals (NCs) successfully based on the selective ion layer adsorption and reaction (SILAR) technique. This inorganic capping obtained higher photoluminescence quantum yield (PLQY) of 59.3% compared with organic capping of 40.8%. Furthermore, the CdSe-epoxy resin (EP) composites were prepared by adopting a flexible ex situ method, and showed excellent stability in the ambient environment for one year. So the composites with both high PLQY of nanocrystals and excellent stability are very promising to device application.

Novel fully-BODIPY functionalized cyclotetraphosphazene photosensitizers having high singlet oxygen quantum yields

NASA Astrophysics Data System (ADS)

Şenkuytu, Elif; Eçik, Esra Tanrıverdi

2017-07-01

Novel fully-BODIPY functionalized dendrimeric cyclotetraphosphazenes (FBCP 1 and 2) have been synthesized and characterized by 1H, 13C and 31P NMR spectroscopies. The photophysical and photochemical properties of FBCP 1 and 2 are investigated in dichloromethane solution. The effectiveness of singlet oxygen generation was measured for FBCP 1 and 2 by UV-Vis spectra monitoring of the solution of 1,3-diphenylisobenzofuran (DPBF), which is a well-known trapping molecule used in detection of singlet oxygen. FBCP 1 and 2 show high molar extinction coefficients in the NIR region, good singlet oxygen quantum yields and appropriate photo degradation. The data presented in the work indicate that the dendrimeric cyclotetraphosphazenes are effective singlet oxygen photosensitizers that might be used for various areas of applications such as photodynamic therapy and photocatalysis.

Fluorescence quantum yield measurements of fluorescent proteins: a laboratory experiment for a biochemistry or molecular biophysics laboratory course.

PubMed

Wall, Kathryn P; Dillon, Rebecca; Knowles, Michelle K

2015-01-01

Fluorescent proteins are commonly used in cell biology to assess where proteins are within a cell as a function of time and provide insight into intracellular protein function. However, the usefulness of a fluorescent protein depends directly on the quantum yield. The quantum yield relates the efficiency at which a fluorescent molecule converts absorbed photons into emitted photons and it is necessary to know for assessing what fluorescent protein is the most appropriate for a particular application. In this work, we have designed an upper-level, biochemistry laboratory experiment where students measure the fluorescence quantum yields of fluorescent proteins relative to a standard organic dye. Four fluorescent protein variants, enhanced cyan fluorescent protein (ECFP), enhanced green fluorescent protein (EGFP), mCitrine, and mCherry, were used, however the methods described are useful for the characterization of any fluorescent protein or could be expanded to fluorescent quantum yield measurements of organic dye molecules. The laboratory is designed as a guided inquiry project and takes two, 4 hr laboratory periods. During the first day students design the experiment by selecting the excitation wavelength, choosing the standard, and determining the concentration needed for the quantum yield experiment that takes place in the second laboratory period. Overall, this laboratory provides students with a guided inquiry learning experience and introduces concepts of fluorescence biophysics into a biochemistry laboratory curriculum. © 2014 The International Union of Biochemistry and Molecular Biology.

Photochemical redox reactions of copper(II)-alanine complexes in aqueous solutions.

PubMed

Lin, Chen-Jui; Hsu, Chao-Sheng; Wang, Po-Yen; Lin, Yi-Liang; Lo, Yu-Shiu; Wu, Chien-Hou

2014-05-19

The photochemical redox reactions of Cu(II)/alanine complexes have been studied in deaerated solutions over an extensive range of pH, Cu(II) concentration, and alanine concentration. Under irradiation, the ligand-to-metal charge transfer results in the reduction of Cu(II) to Cu(I) and the concomitant oxidation of alanine, which produces ammonia and acetaldehyde. Molar absorptivities and quantum yields of photoproducts for Cu(II)/alanine complexes at 313 nm are characterized mainly with the equilibrium Cu(II) speciation where the presence of simultaneously existing Cu(II) species is taken into account. By applying regression analysis, individual Cu(I) quantum yields are determined to be 0.094 ± 0.014 for the 1:1 complex (CuL) and 0.064 ± 0.012 for the 1:2 complex (CuL2). Individual quantum yields of ammonia are 0.055 ± 0.007 for CuL and 0.036 ± 0.005 for CuL2. Individual quantum yields of acetaldehyde are 0.030 ± 0.007 for CuL and 0.024 ± 0.007 for CuL2. CuL always has larger quantum yields than CuL2, which can be attributed to the Cu(II) stabilizing effect of the second ligand. For both CuL and CuL2, the individual quantum yields of Cu(I), ammonia, and acetaldehyde are in the ratio of 1.8:1:0.7. A reaction mechanism for the formation of the observed photoproducts is proposed.

Noise induced quantum effects in photosynthetic complexes

NASA Astrophysics Data System (ADS)

Dorfman, Konstantin; Voronine, Dmitri; Mukamel, Shaul; Scully, Marlan

2012-02-01

Recent progress in coherent multidimensional optical spectroscopy revealed effects of quantum coherence coupled to population leading to population oscillations as evidence of quantum transport. Their description requires reevaluation of the currently used methods and approximations. We identify couplings between coherences and populations as the noise-induced cross-terms in the master equation generated via Agarwal-Fano interference that have been shown earlier to enhance the quantum yield in a photocell. We investigated a broad range of typical parameter regimes, which may be applied to a variety of photosynthetic complexes. We demonstrate that quantum coherence may be induced in photosynthetic complexes under natural conditions of incoherent light from the sun. This demonstrates that a photosynthetic reaction center may be viewed as a biological quantum heat engine that transforms high-energy thermal photon radiation into low entropy electron flux.

Quantum-dot-tagged microbeads for multiplexed optical coding of biomolecules.

PubMed

Han, M; Gao, X; Su, J Z; Nie, S

2001-07-01

Multicolor optical coding for biological assays has been achieved by embedding different-sized quantum dots (zinc sulfide-capped cadmium selenide nanocrystals) into polymeric microbeads at precisely controlled ratios. Their novel optical properties (e.g., size-tunable emission and simultaneous excitation) render these highly luminescent quantum dots (QDs) ideal fluorophores for wavelength-and-intensity multiplexing. The use of 10 intensity levels and 6 colors could theoretically code one million nucleic acid or protein sequences. Imaging and spectroscopic measurements indicate that the QD-tagged beads are highly uniform and reproducible, yielding bead identification accuracies as high as 99.99% under favorable conditions. DNA hybridization studies demonstrate that the coding and target signals can be simultaneously read at the single-bead level. This spectral coding technology is expected to open new opportunities in gene expression studies, high-throughput screening, and medical diagnostics.

Single photon emission from plasma treated 2D hexagonal boron nitride.

PubMed

Xu, Zai-Quan; Elbadawi, Christopher; Tran, Toan Trong; Kianinia, Mehran; Li, Xiuling; Liu, Daobin; Hoffman, Timothy B; Nguyen, Minh; Kim, Sejeong; Edgar, James H; Wu, Xiaojun; Song, Li; Ali, Sajid; Ford, Mike; Toth, Milos; Aharonovich, Igor

2018-05-03

Artificial atomic systems in solids are becoming increasingly important building blocks in quantum information processing and scalable quantum nanophotonic networks. Amongst numerous candidates, 2D hexagonal boron nitride has recently emerged as a promising platform hosting single photon emitters. Here, we report a number of robust plasma and thermal annealing methods for fabrication of emitters in tape-exfoliated hexagonal boron nitride (hBN) crystals. A two-step process comprising Ar plasma etching and subsequent annealing in Ar is highly robust, and yields an eight-fold increase in the concentration of emitters in hBN. The initial plasma-etching step generates emitters that suffer from blinking and bleaching, whereas the two-step process yields emitters that are photostable at room temperature with emission wavelengths greater than ∼700 nm. Density functional theory modeling suggests that the emitters might be associated with defect complexes that contain oxygen. This is further confirmed by generating the emitters via annealing hBN in air. Our findings advance the present understanding of the structure of quantum emitters in hBN and enhance the nanofabrication toolkit needed to realize integrated quantum nanophotonic circuits.

A highly efficient silole-containing dithienylethene with excellent thermal stability and fatigue resistance: a promising candidate for optical memory storage materials.

PubMed

Chan, Jacky Chi-Hung; Lam, Wai Han; Yam, Vivian Wing-Wah

2014-12-10

Diarylethene compounds are potential candidates for applications in optical memory storage systems and photoswitchable molecular devices; however, they usually show low photocycloreversion quantum yields, which result in ineffective erasure processes. Here, we present the first highly efficient photochromic silole-containing dithienylethene with excellent thermal stability and fatigue resistance. The photochemical quantum yields for photocyclization and photocycloreversion of the compound are found to be high and comparable to each other; the latter of which is rarely found in diarylethene compounds. These would give rise to highly efficient photoswitchable material with effective writing and erasure processes. Incorporation of the silole moiety as a photochromic dithienylethene backbone also was demonstrated to enhance the thermal stability of the closed form, in which the thermal backward reaction to the open form was found to be negligible even at 100 °C, which leads to a promising candidate for use as photoswitchable materials and optical memory storage.

Graphene quantum dots, graphene oxide, carbon quantum dots and graphite nanocrystals in coals

NASA Astrophysics Data System (ADS)

Dong, Yongqiang; Lin, Jianpeng; Chen, Yingmei; Fu, Fengfu; Chi, Yuwu; Chen, Guonan

2014-06-01

Six coal samples of different ranks have been used to prepare single-layer graphene quantum dots (S-GQDs). After chemical oxidation and a series of centrifugation separation, every coal could be treated into two fractions, namely, CoalA and CoalB. According to the characterization results of TEM, AFM, XRD, Raman and FTIR, CoalA was revealed to be mainly composed of S-GQDs, which have an average height of about 0.5 nm and an average plane dimension of about 10 nm. The obtained S-GQDs showed excitation-dependent fluorescence and excellent electrochemiluminescence. CoalB was found to be some other carbon-based nanomaterials (CNMs), including agglomerated GQDs, graphene oxide, carbon quantum dots and agglomerated carbon nanocrystals. Generally, low-ranked coals might be more suitable for the preparation of S-GQDs. The production yield of S-GQDs from the six investigated coals decreased from 56.30% to 14.66% when the coal rank increased gradually. In contrast, high-ranked coals had high production yield of CoalB and might be more suitable for preparing other CNMs that were contained in CoalB, although those CNMs were difficult to separate from each other in our experiment.Six coal samples of different ranks have been used to prepare single-layer graphene quantum dots (S-GQDs). After chemical oxidation and a series of centrifugation separation, every coal could be treated into two fractions, namely, CoalA and CoalB. According to the characterization results of TEM, AFM, XRD, Raman and FTIR, CoalA was revealed to be mainly composed of S-GQDs, which have an average height of about 0.5 nm and an average plane dimension of about 10 nm. The obtained S-GQDs showed excitation-dependent fluorescence and excellent electrochemiluminescence. CoalB was found to be some other carbon-based nanomaterials (CNMs), including agglomerated GQDs, graphene oxide, carbon quantum dots and agglomerated carbon nanocrystals. Generally, low-ranked coals might be more suitable for the preparation of S-GQDs. The production yield of S-GQDs from the six investigated coals decreased from 56.30% to 14.66% when the coal rank increased gradually. In contrast, high-ranked coals had high production yield of CoalB and might be more suitable for preparing other CNMs that were contained in CoalB, although those CNMs were difficult to separate from each other in our experiment. Electronic supplementary information (ESI) available: Elemental analysis results of coal samples, FTIR spectra of CoalA and CoalB, ECL responses of CoalA/S2O82-. See DOI: 10.1039/c4nr01482k

Polariton-Assisted Singlet Fission in Acene Aggregates.

PubMed

Martínez-Martínez, Luis A; Du, Matthew; F Ribeiro, Raphael; Kéna-Cohen, Stéphane; Yuen-Zhou, Joel

2018-04-19

Singlet fission is an important candidate to increase energy conversion efficiency in organic photovoltaics by providing a pathway to increase the quantum yield of excitons per photon absorbed in select materials. We investigate the dependence of exciton quantum yield for acenes in the strong light-matter interaction (polariton) regime, where the materials are embedded in optical microcavities. Starting from an open-quantum-systems approach, we build a kinetic model for time-evolution of species of interest in the presence of singlet quenchers and show that polaritons can decrease or increase exciton quantum yields compared to the cavity-free case. In particular, we find that hexacene, under the conditions of our model, can feature a higher yield than cavity-free pentacene when assisted by polaritonic effects. Similarly, we show that pentacene yield can be increased when assisted by polariton states. Finally, we address how various relaxation processes between bright and dark states in lossy microcavities affect polariton photochemistry. Our results also provide insights on how to choose microcavities to enhance similarly related chemical processes.

High performance, low dissipation quantum cascade lasers across the mid-IR range.

PubMed

Bismuto, Alfredo; Blaser, Stéphane; Terazzi, Romain; Gresch, Tobias; Muller, Antoine

2015-03-09

In this work, we present the development of low consumption quantum cascade lasers across the mid-IR range. In particular, short cavity single-mode lasers with optimised facet reflectivities have been fabricated from 4.5 to 9.2 μm. Threshold dissipated powers as low as 0.5 W were obtained in continuous wave operation at room temperature. In addition, the beneficial impact of reducing chip length on laser mounting yield is discussed. High power single-mode lasers from the same processed wafers are also presented.

Highly efficient exciplex organic light-emitting diodes using thermally activated delayed fluorescent emitters as donor and acceptor materials.

PubMed

Jeon, Sang Kyu; Yook, Kyoung Soo; Lee, Jun Yeob

2016-06-03

Highly efficient exciplex type organic light-emitting diodes were developed using thermally activated delayed fluorescent emitters as donors and acceptors of an exciplex. Blue emitting bis[4-(9,9-dimethyl-9,10-dihydroacridine)phenyl]sulfone (DMAC-DPS) was a donor and 9,9'-(5-(4,6-diphenyl-1,3,5-triazin-2-yl)-1,3-phenylene)bis(9H-carbazole) (DDCzTrz) and 9,9',9″-(5-(4,6-diphenyl-1,3,5-triazin-2-yl)benzene-1,2,3-triyl)tris(9H-carbazole) (TCzTrz) were acceptor materials. The exciplexes of DMAC-DPS:TCzTrz and DMAC-DPS:DDCzTrz resulted in high photoluminescence quantum yield and high quantum efficiency in the green exciplex organic light-emitting diodes. High quantum efficiencies of 13.4% and 15.3% were obtained in the DMAC-DPS:DDCzTrz and DMAC-DPS:TCzTrz exciplex devices.

Highly efficient exciplex organic light-emitting diodes using thermally activated delayed fluorescent emitters as donor and acceptor materials

NASA Astrophysics Data System (ADS)

Jeon, Sang Kyu; Yook, Kyoung Soo; Lee, Jun Yeob

2016-06-01

Highly efficient exciplex type organic light-emitting diodes were developed using thermally activated delayed fluorescent emitters as donors and acceptors of an exciplex. Blue emitting bis[4-(9,9-dimethyl-9,10-dihydroacridine)phenyl]sulfone (DMAC-DPS) was a donor and 9,9‧-(5-(4,6-diphenyl-1,3,5-triazin-2-yl)-1,3-phenylene)bis(9H-carbazole) (DDCzTrz) and 9,9‧,9″-(5-(4,6-diphenyl-1,3,5-triazin-2-yl)benzene-1,2,3-triyl)tris(9H-carbazole) (TCzTrz) were acceptor materials. The exciplexes of DMAC-DPS:TCzTrz and DMAC-DPS:DDCzTrz resulted in high photoluminescence quantum yield and high quantum efficiency in the green exciplex organic light-emitting diodes. High quantum efficiencies of 13.4% and 15.3% were obtained in the DMAC-DPS:DDCzTrz and DMAC-DPS:TCzTrz exciplex devices.

High-Performance Blue-Excitable Yellow Phosphor Obtained from an Activated Solvochromic Bismuth-Fluorophore Metal–Organic Framework

DOE PAGES

Deibert, Benjamin J.; Velasco, Ever; Liu, Wei; ...

2016-06-23

Here, we report the synthesis, structure, and photoluminescence properties of a new bismuth based luminescent metal-organic framework (LMOF). The framework is comprised of a 9-coordinated Bi 3+ building unit and 4', 4''', 4''''', 4'''''''-(ethene-1,1,2,2-tetrayl)tetrakis([1,1'-biphenyl]-4-carboxylic acid) (H 4tcbpe) organic linker, which has strong yellow aggregation induced emission (AIE). The structure can be viewed as two interpenetrated 4,4-anionic nets that are stabilized by K + ions forming one-dimensional helical inorganic chains by connecting bismuth nodes through shared oxygen bonds. The as-made LMOF has a bluish emission centered at 459 nm with an internal quantum yield of 57% when excited at 360 nm.more » The emission properties of the LMOF were found to be highly solvochromic with respect to DMF. Upon partial solvent removal, the framework undergoes significant red-shifting to a greenish emission centered at 500 nm. Complete removal of DMF results in additional red-shifting fluorescence coupled with structural changes. The resulting material has strong blue-excitable (455 nm) yellow emission centered at 553 nm, with a quantum yield of 74%, which is maintained after heating in air for 5 days at 90°C. This is the second highest quantum yield value for blue-excited yellow emission among all reported LMOFs.« less

High-Performance Blue-Excitable Yellow Phosphor Obtained from an Activated Solvochromic Bismuth-Fluorophore Metal–Organic Framework

DOE Office of Scientific and Technical Information (OSTI.GOV)

Deibert, Benjamin J.; Velasco, Ever; Liu, Wei

Here, we report the synthesis, structure, and photoluminescence properties of a new bismuth based luminescent metal-organic framework (LMOF). The framework is comprised of a 9-coordinated Bi 3+ building unit and 4', 4''', 4''''', 4'''''''-(ethene-1,1,2,2-tetrayl)tetrakis([1,1'-biphenyl]-4-carboxylic acid) (H 4tcbpe) organic linker, which has strong yellow aggregation induced emission (AIE). The structure can be viewed as two interpenetrated 4,4-anionic nets that are stabilized by K + ions forming one-dimensional helical inorganic chains by connecting bismuth nodes through shared oxygen bonds. The as-made LMOF has a bluish emission centered at 459 nm with an internal quantum yield of 57% when excited at 360 nm.more » The emission properties of the LMOF were found to be highly solvochromic with respect to DMF. Upon partial solvent removal, the framework undergoes significant red-shifting to a greenish emission centered at 500 nm. Complete removal of DMF results in additional red-shifting fluorescence coupled with structural changes. The resulting material has strong blue-excitable (455 nm) yellow emission centered at 553 nm, with a quantum yield of 74%, which is maintained after heating in air for 5 days at 90°C. This is the second highest quantum yield value for blue-excited yellow emission among all reported LMOFs.« less

Light propagation and fluorescence quantum yields in liquid scintillators

NASA Astrophysics Data System (ADS)

Buck, C.; Gramlich, B.; Wagner, S.

2015-09-01

For the simulation of the scintillation and Cherenkov light propagation in large liquid scintillator detectors a detailed knowledge about the absorption and emission spectra of the scintillator molecules is mandatory. Furthermore reemission probabilities and quantum yields of the scintillator components influence the light propagation inside the liquid. Absorption and emission properties are presented for liquid scintillators using 2,5-Diphenyloxazole (PPO) and 4-bis-(2-Methylstyryl)benzene (bis-MSB) as primary and secondary wavelength shifter. New measurements of the quantum yields for various aromatic molecules are shown.

Compact and highly stable quantum dots through optimized aqueous phase transfer

NASA Astrophysics Data System (ADS)

Tamang, Sudarsan; Beaune, Grégory; Poillot, Cathy; De Waard, Michel; Texier-Nogues, Isabelle; Reiss, Peter

2011-03-01

A large number of different approaches for the aqueous phase transfer of quantum dots have been proposed. Surface ligand exchange with small hydrophilic thiols, such as L-cysteine, yields the lowest particle hydrodynamic diameter. However, cysteine is prone to dimer formation, which limits colloidal stability. We demonstrate that precise pH control during aqueous phase transfer dramatically increases the colloidal stability of InP/ZnS quantum dots. Various bifunctional thiols have been applied. The formation of disulfides, strongly diminishing the fluorescence QY has been prevented through addition of appropriate reducing agents. Bright InP/ZnS quantum dots with a hydrodynamic diameter <10 nm and long-term stability have been obtained. Finally we present in vitro studies of the quantum dots functionalized with the cell-penetrating peptide maurocalcine.

Complete Quantum Control of a Single Silicon-Vacancy Center in a Diamond Nanopillar

NASA Astrophysics Data System (ADS)

Zhang, Jingyuan Linda; Lagoudakis, Konstantinos G.; Tzeng, Yan-Kai; Dory, Constantin; Radulaski, Marina; Kelaita, Yousif; Shen, Zhi-Xun; Melosh, Nicholas A.; Chu, Steven; Vuckovic, Jelena

Coherent quantum control of a quantum bit (qubit) is an important step towards its use in a quantum network. SiV- center in diamond offers excellent physical qualities such as low inhomogeneous broadening, fast photon emission, and a large Debye-Waller factor, while the fast spin manipulation and techniques to extend the spin coherence time are under active investigation. Here, we demonstrate full coherent control over the state of a single SiV- center in a diamond nanopillar using ultrafast optical pulses. The high quality of the chemical vapor deposition grown SiV- centers allows us to coherently manipulate and quasi-resonantly read out the state of the single SiV- center. Moreover, the SiV- centers being coherently controlled are integrated into diamond nanopillar arrays in a site-controlled, individually addressable manner with high yield, low strain, and high spectral stability, which paves the way for scalable on chip optically accessible quantum system in a quantum photonic network. Financial support is provided by the DOE Office of Basic Energy Sciences, Division of Materials Sciences through Stanford Institute for Materials and Energy Sciences (SIMES) under contract DE-AC02-76SF00515.

Low temperature synthesis of silicon quantum dots with plasma chemistry control in dual frequency non-thermal plasmas.

PubMed

Sahu, Bibhuti Bhusan; Yin, Yongyi; Han, Jeon Geon; Shiratani, Masaharu

2016-06-21

The advanced materials process by non-thermal plasmas with a high plasma density allows the synthesis of small-to-big sized Si quantum dots by combining low-temperature deposition with superior crystalline quality in the background of an amorphous hydrogenated silicon nitride matrix. Here, we make quantum dot thin films in a reactive mixture of ammonia/silane/hydrogen utilizing dual-frequency capacitively coupled plasmas with high atomic hydrogen and nitrogen radical densities. Systematic data analysis using different film and plasma characterization tools reveals that the quantum dots with different sizes exhibit size dependent film properties, which are sensitively dependent on plasma characteristics. These films exhibit intense photoluminescence in the visible range with violet to orange colors and with narrow to broad widths (∼0.3-0.9 eV). The observed luminescence behavior can come from the quantum confinement effect, quasi-direct band-to-band recombination, and variation of atomic hydrogen and nitrogen radicals in the film growth network. The high luminescence yields in the visible range of the spectrum and size-tunable low-temperature synthesis with plasma and radical control make these quantum dot films good candidates for light emitting applications.

Far-infrared response of spherical quantum dots: Dielectric effects and the generalized Kohn's theorem

NASA Astrophysics Data System (ADS)

Movilla, J. L.; Planelles, J.

2007-05-01

The influence of the dielectric environment on the far-infrared (FIR) absorption spectra of two-electron spherical quantum dots is theoretically studied. Effective mass and envelope function approaches with realistic steplike confining potentials are used. Special attention is paid to absorptions that are induced by the electron-electron interaction. High confining barriers make the FIR absorption coefficients almost independent of the quantum dot dielectric environment. Low barrier heights and strong dielectric mismatches preserve the strong fundamental (Kohn) mode but yield the cancellation of excited absorptions, thus monitoring dielectrically induced phase transitions from volume to surface states.

Analysis of the external and internal quantum efficiency of multi-emitter, white organic light emitting diodes

NASA Astrophysics Data System (ADS)

Furno, Mauro; Rosenow, Thomas C.; Gather, Malte C.; Lüssem, Björn; Leo, Karl

2012-10-01

We report on a theoretical framework for the efficiency analysis of complex, multi-emitter organic light emitting diodes (OLEDs). The calculation approach makes use of electromagnetic modeling to quantify the overall OLED photon outcoupling efficiency and a phenomenological description for electrical and excitonic processes. From the comparison of optical modeling results and measurements of the total external quantum efficiency, we obtain reliable estimates of internal quantum yield. As application of the model, we analyze high-efficiency stacked white OLEDs and comment on the various efficiency loss channels present in the devices.

Nano-patterned superconducting surface for high quantum efficiency cathode

DOEpatents

Hannon, Fay; Musumeci, Pietro

2017-03-07

A method for providing a superconducting surface on a laser-driven niobium cathode in order to increase the effective quantum efficiency. The enhanced surface increases the effective quantum efficiency by improving the laser absorption of the surface and enhancing the local electric field. The surface preparation method makes feasible the construction of superconducting radio frequency injectors with niobium as the photocathode. An array of nano-structures are provided on a flat surface of niobium. The nano-structures are dimensionally tailored to interact with a laser of specific wavelength to thereby increase the electron yield of the surface.

Quantum mechanics: The Bayesian theory generalized to the space of Hermitian matrices

NASA Astrophysics Data System (ADS)

Benavoli, Alessio; Facchini, Alessandro; Zaffalon, Marco

2016-10-01

We consider the problem of gambling on a quantum experiment and enforce rational behavior by a few rules. These rules yield, in the classical case, the Bayesian theory of probability via duality theorems. In our quantum setting, they yield the Bayesian theory generalized to the space of Hermitian matrices. This very theory is quantum mechanics: in fact, we derive all its four postulates from the generalized Bayesian theory. This implies that quantum mechanics is self-consistent. It also leads us to reinterpret the main operations in quantum mechanics as probability rules: Bayes' rule (measurement), marginalization (partial tracing), independence (tensor product). To say it with a slogan, we obtain that quantum mechanics is the Bayesian theory in the complex numbers.

Intermediate quantum maps for quantum computation

NASA Astrophysics Data System (ADS)

Giraud, O.; Georgeot, B.

2005-10-01

We study quantum maps displaying spectral statistics intermediate between Poisson and Wigner-Dyson. It is shown that they can be simulated on a quantum computer with a small number of gates, and efficiently yield information about fidelity decay or spectral statistics. We study their matrix elements and entanglement production and show that they converge with time to distributions which differ from random matrix predictions. A randomized version of these maps can be implemented even more economically and yields pseudorandom operators with original properties, enabling, for example, one to produce fractal random vectors. These algorithms are within reach of present-day quantum computers.

Quantum Yields of CAM Plants Measured by Photosynthetic O2 Exchange 1

PubMed Central

Adams, William W.; Nishida, Kojiro; Osmond, C. Barry

1986-01-01

The quantum yield of photosynthetic O2 exchange was measured in eight species of leaf succulents representative of both malic enzyme type and phosphoenolpyruvate carboxykinase type CAM plants. Measurements were made at 25°C and CO2 saturation using a leaf disc O2 electrode system, either during or after deacidification. The mean quantum yield was 0.095 ± 0.012 (sd) moles O2 per mole quanta, which compared with 0.094 ± 0.006 (sd) moles O2 per mole quanta for spinach leaf discs measured under the same conditions. There were no consistent differences in quantum yield between decarboxylation types or during different phases of CAM metabolism. On the basis of current notions of compartmentation of CAM biochemistry, our observations are interpreted to indicate that CO2 refixation is energetically independent of gluconeogenesis during deacidification. PMID:16664793

Beyond the Fermi liquid paradigm: Hidden Fermi liquids

PubMed Central

Jain, J. K.; Anderson, P. W.

2009-01-01

An intense investigation of possible non-Fermi liquid states of matter has been inspired by two of the most intriguing phenomena discovered in the past quarter century, namely, high-temperature superconductivity and the fractional quantum Hall effect. Despite enormous conceptual strides, these two fields have developed largely along separate paths. Two widely employed theories are the resonating valence bond theory for high-temperature superconductivity and the composite fermion theory for the fractional quantum Hall effect. The goal of this perspective article is to note that they subscribe to a common underlying paradigm: They both connect these exotic quantum liquids to certain ordinary Fermi liquids residing in unphysical Hilbert spaces. Such a relation yields numerous nontrivial experimental consequences, exposing these theories to rigorous and definitive tests. PMID:19506260

Structural Investigation of Cesium Lead Halide Perovskites for High-Efficiency Quantum Dot Light-Emitting Diodes.

PubMed

Le, Quyet Van; Kim, Jong Beom; Kim, Soo Young; Lee, Byeongdu; Lee, Dong Ryeol

2017-09-07

We have investigated the effect of reaction temperature of hot-injection method on the structural properties of CsPbX 3 (X: Br, I, Cl) perovskite nanocrystals (NCs) using small- and wide-angle X-ray scattering. It is confirmed that the size of the NCs decreased as the reaction temperature decreased, resulting in stronger quantum confinement. The cubic-phase perovskite NCs formed despite the fact that the reaction temperatures increased from 140 to 180 °C; however, monodispersive NC cubes that are required for densely packing self-assembly film were formed only at lower temperatures. From the X-ray scattering measurements, the spin-coated film from more monodispersive perovskite nanocubes synthesized at lower temperatures resulted in more preferred orientation. This dense-packing perovskite film with preferred orientation yielded efficient light-emitting diode (LED) performance. Thus the dense-packing structure of NC assemblies formed after spin-coating should be considered for high-efficient LEDs based on perovskite quantum dots in addition to quantum confinement effect of the quantum dots.

Solid-state ensemble of highly entangled photon sources at rubidium atomic transitions

NASA Astrophysics Data System (ADS)

Zopf, Michael; Keil, Robert; Chen, Yan; HöFer, Bianca; Zhang, Jiaxiang; Ding, Fei; Schmidt, Oliver G.

Semiconductor InAs/GaAs quantum dots grown by the Stranski-Krastanov method are among the leading candidates for the deterministic generation of polarization entangled photon pairs. Despite remarkable progress in the last twenty years, many challenges still remain for this material, such as the extremely low yield (< 1% quantum dots can emit entangled photons), the low degree of entanglement, and the large wavelength distribution. Here we show that, with an emerging family of GaAs/AlGaAs quantum dots grown by droplet etching and nanohole infilling, it is possible to obtain a large ensemble (close to 100%) of polarization-entangled photon emitters on a wafer without any post-growth tuning. Under pulsed resonant two-photon excitation, all measured quantum dots emit single pairs of entangled photons with ultra-high purity, high degree of entanglement (fidelity up to F=0.91, with a record high concurrence C=0.90), and ultra-narrow wavelength distribution at rubidium transitions. Therefore, a solid-state quantum repeater - among many other key enabling quantum photonic elements - can be practically implemented with this new material. Financially supported by BMBF Q.Com-H (16KIS0106) and the Euro- pean Union Seventh Framework Programme 209 (FP7/2007-2013) under Grant Agreement No. 601126 210 (HANAS).

Synthesis of Cd-free InP/ZnS Quantum Dots Suitable for Biomedical Applications.

PubMed

Ellis, Matthew A; Grandinetti, Giovanna; Fichter, Katye M; Fichter, Kathryn M

2016-02-06

Fluorescent nanocrystals, specifically quantum dots, have been a useful tool for many biomedical applications. For successful use in biological systems, quantum dots should be highly fluorescent and small/monodisperse in size. While commonly used cadmium-based quantum dots possess these qualities, they are potentially toxic due to the possible release of Cd(2+) ions through nanoparticle degradation. Indium-based quantum dots, specifically InP/ZnS, have recently been explored as a viable alternative to cadmium-based quantum dots due to their relatively similar fluorescence characteristics and size. The synthesis presented here uses standard hot-injection techniques for effective nanoparticle growth; however, nanoparticle properties such as size, emission wavelength, and emission intensity can drastically change due to small changes in the reaction conditions. Therefore, reaction conditions such temperature, reaction duration, and precursor concentration should be maintained precisely to yield reproducible products. Because quantum dots are not inherently soluble in aqueous solutions, they must also undergo surface modification to impart solubility in water. In this protocol, an amphiphilic polymer is used to interact with both hydrophobic ligands on the quantum dot surface and bulk solvent water molecules. Here, a detailed protocol is provided for the synthesis of highly fluorescent InP/ZnS quantum dots that are suitable for use in biomedical applications.

Synthesis of Cd-free InP/ZnS Quantum Dots Suitable for Biomedical Applications

PubMed Central

Ellis, Matthew A.; Grandinetti, Giovanna; Fichter, Katye M.

2016-01-01

Fluorescent nanocrystals, specifically quantum dots, have been a useful tool for many biomedical applications. For successful use in biological systems, quantum dots should be highly fluorescent and small/monodisperse in size. While commonly used cadmium-based quantum dots possess these qualities, they are potentially toxic due to the possible release of Cd2+ ions through nanoparticle degradation. Indium-based quantum dots, specifically InP/ZnS, have recently been explored as a viable alternative to cadmium-based quantum dots due to their relatively similar fluorescence characteristics and size. The synthesis presented here uses standard hot-injection techniques for effective nanoparticle growth; however, nanoparticle properties such as size, emission wavelength, and emission intensity can drastically change due to small changes in the reaction conditions. Therefore, reaction conditions such temperature, reaction duration, and precursor concentration should be maintained precisely to yield reproducible products. Because quantum dots are not inherently soluble in aqueous solutions, they must also undergo surface modification to impart solubility in water. In this protocol, an amphiphilic polymer is used to interact with both hydrophobic ligands on the quantum dot surface and bulk solvent water molecules. Here, a detailed protocol is provided for the synthesis of highly fluorescent InP/ZnS quantum dots that are suitable for use in biomedical applications. PMID:26891282

Montelukast photodegradation: elucidation of Ф-order kinetics, determination of quantum yields and application to actinometry.

PubMed

Maafi, Mounir; Maafi, Wassila

2014-08-25

A recently developed Ф-order semi-emperical integrated rate-law for photoreversible AB(2Ф) reactions has been successfully applied to investigate Montelukast sodium (Monte) photodegradation kinetics in ethanol. The model equations also served to propose a new stepwise kinetic elucidation method valid for any AB(2Ф) system and its application to the determination of Monte's forward (Ф(λ(irr))(A-->B)) and reverse (Ф(λ(irr))(B-->A)) quantum yields at various irradiation wavelengths. It has been found that Ф(λ(irr))(A-->B) undergoes a 15-fold increase with wavelength between 220 and 360 nm, with the spectral section 250-360 nm representing Monte effective photodegradation causative range. The reverse quantum yield values were generally between 12 and 54% lower than those recorded for Ф(λ(irr))(A-->B), with the trans-isomer (Monte) converting almost completely to its cis-counterpart at high irradiation wavelengths. Furthermore, the potential use of Monte as an actinometer has been investigated, and an actinometric method was proposed. This study demonstrated the usefulness of Monte for monochromatic light actinometry for the dynamic range 258-380 nm. Copyright © 2014 Elsevier B.V. All rights reserved.

Multiple exciton generation for photoelectrochemical hydrogen evolution reactions with quantum yields exceeding 100%

DOE PAGES

Yan, Yong; Crisp, Ryan W.; Gu, Jing; ...

2017-04-03

Multiple exciton generation (MEG) in quantum dots (QDs) has the potential to greatly increase the power conversion efficiency in solar cells and in solar-fuel production. During the MEG process, two electron-hole pairs (excitons) are created from the absorption of one high-energy photon, bypassing hot-carrier cooling via phonon emission. Here we demonstrate that extra carriers produced via MEG can be used to drive a chemical reaction with quantum efficiency above 100%. We developed a lead sulfide (PbS) QD photoelectrochemical cell that is able to drive hydrogen evolution from aqueous Na 2S solution with a peak external quantum efficiency exceeding 100%. QDmore » photoelectrodes that were measured all demonstrated MEG when the incident photon energy was larger than 2.7 times the bandgap energy. Finally, our results demonstrate a new direction in exploring high-efficiency approaches to solar fuels.« less

Secure self-calibrating quantum random-bit generator

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fiorentino, M.; Santori, C.; Spillane, S. M.

2007-03-15

Random-bit generators (RBGs) are key components of a variety of information processing applications ranging from simulations to cryptography. In particular, cryptographic systems require 'strong' RBGs that produce high-entropy bit sequences, but traditional software pseudo-RBGs have very low entropy content and therefore are relatively weak for cryptography. Hardware RBGs yield entropy from chaotic or quantum physical systems and therefore are expected to exhibit high entropy, but in current implementations their exact entropy content is unknown. Here we report a quantum random-bit generator (QRBG) that harvests entropy by measuring single-photon and entangled two-photon polarization states. We introduce and implement a quantum tomographicmore » method to measure a lower bound on the 'min-entropy' of the system, and we employ this value to distill a truly random-bit sequence. This approach is secure: even if an attacker takes control of the source of optical states, a secure random sequence can be distilled.« less

Single-particle tracking of quantum dot-conjugated prion proteins inside yeast cells

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tsuji, Toshikazu; Kawai-Noma, Shigeko; Pack, Chan-Gi

2011-02-25

Research highlights: {yields} We develop a method to track a quantum dot-conjugated protein in yeast cells. {yields} We incorporate the conjugated quantum dot proteins into yeast spheroplasts. {yields} We track the motions by conventional or 3D tracking microscopy. -- Abstract: Yeast is a model eukaryote with a variety of biological resources. Here we developed a method to track a quantum dot (QD)-conjugated protein in the budding yeast Saccharomyces cerevisiae. We chemically conjugated QDs with the yeast prion Sup35, incorporated them into yeast spheroplasts, and tracked the motions by conventional two-dimensional or three-dimensional tracking microscopy. The method paves the way towardmore » the individual tracking of proteins of interest inside living yeast cells.« less

High Throughput, High Yield Fabrication of High Quantum Efficiency Back-Illuminated Photon Counting, Far UV, UV, and Visible Detector Arrays

NASA Technical Reports Server (NTRS)

Nikzad, Shouleh; Hoenk, M. E.; Carver, A. G.; Jones, T. J.; Greer, F.; Hamden, E.; Goodsall, T.

2013-01-01

In this paper we discuss the high throughput end-to-end post fabrication processing of high performance delta-doped and superlattice-doped silicon imagers for UV, visible, and NIR applications. As an example, we present our results on far ultraviolet and ultraviolet quantum efficiency (QE) in a photon counting, detector array. We have improved the QE by nearly an order of magnitude over microchannel plates (MCPs) that are the state-of-the-art UV detectors for many NASA space missions as well as defense applications. These achievements are made possible by precision interface band engineering of Molecular Beam Epitaxy (MBE) and Atomic Layer Deposition (ALD).

Quantum logic using correlated one-dimensional quantum walks

NASA Astrophysics Data System (ADS)

Lahini, Yoav; Steinbrecher, Gregory R.; Bookatz, Adam D.; Englund, Dirk

2018-01-01

Quantum Walks are unitary processes describing the evolution of an initially localized wavefunction on a lattice potential. The complexity of the dynamics increases significantly when several indistinguishable quantum walkers propagate on the same lattice simultaneously, as these develop non-trivial spatial correlations that depend on the particle's quantum statistics, mutual interactions, initial positions, and the lattice potential. We show that even in the simplest case of a quantum walk on a one dimensional graph, these correlations can be shaped to yield a complete set of compact quantum logic operations. We provide detailed recipes for implementing quantum logic on one-dimensional quantum walks in two general cases. For non-interacting bosons—such as photons in waveguide lattices—we find high-fidelity probabilistic quantum gates that could be integrated into linear optics quantum computation schemes. For interacting quantum-walkers on a one-dimensional lattice—a situation that has recently been demonstrated using ultra-cold atoms—we find deterministic logic operations that are universal for quantum information processing. The suggested implementation requires minimal resources and a level of control that is within reach using recently demonstrated techniques. Further work is required to address error-correction.

Stabilization of the Simplest Criegee Intermediate from the Reaction between Ozone and Ethylene: A High-Level Quantum Chemical and Kinetic Analysis of Ozonolysis.

PubMed

Nguyen, Thanh Lam; Lee, Hyunwoo; Matthews, Devin A; McCarthy, Michael C; Stanton, John F

2015-06-04

The fraction of the collisionally stabilized Criegee species CH2OO produced from the ozonolysis of ethylene is calculated using a two-dimensional (E, J)-grained master equation technique and semiclassical transition-state theory based on the potential energy surface obtained from high-accuracy quantum chemical calculations. Our calculated yield of 42 ± 6% for the stabilized CH2OO agrees well, within experimental error, with available (indirect) experimental results. Inclusion of angular momentum in the master equation is found to play an essential role in bringing the theoretical results into agreement with the experiment. Additionally, yields of HO and HO2 radical products are predicted to be 13 ± 6% and 17 ± 6%, respectively. In the kinetic simulation, the HO radical product is produced mostly from the stepwise decomposition mechanism of primary ozonide rather than from dissociation of hot CH2OO.

High-Fidelity Single-Shot Toffoli Gate via Quantum Control.

PubMed

Zahedinejad, Ehsan; Ghosh, Joydip; Sanders, Barry C

2015-05-22

A single-shot Toffoli, or controlled-controlled-not, gate is desirable for classical and quantum information processing. The Toffoli gate alone is universal for reversible computing and, accompanied by the Hadamard gate, forms a universal gate set for quantum computing. The Toffoli gate is also a key ingredient for (nontopological) quantum error correction. Currently Toffoli gates are achieved by decomposing into sequentially implemented single- and two-qubit gates, which require much longer times and yields lower overall fidelities compared to a single-shot implementation. We develop a quantum-control procedure to construct a single-shot Toffoli gate for three nearest-neighbor-coupled superconducting transmon systems such that the fidelity is 99.9% and is as fast as an entangling two-qubit gate under the same realistic conditions. The gate is achieved by a nongreedy quantum control procedure using our enhanced version of the differential evolution algorithm.

Fabrication of highly fluorescent graphene quantum dots using L-glutamic acid for in vitro/in vivo imaging and sensing.

PubMed

Wu, Xu; Tian, Fei; Wang, Wenxue; Chen, Jiao; Wu, Min; Zhao, Julia Xiaojun

2013-08-21

A facile bottom-up method for the synthesis of highly fluorescent graphene quantum dots (GQDs) has been developed using a one-step pyrolysis of a natural amino acid, L-glutamic acid, with the assistance of a simple heating mantle device. The developed GQDs showed strong blue, green and red luminescence under the irradiation of ultra-violet, blue and green light, respectively. Moreover, the GQDs emitted near-infrared (NIR) fluorescence in the range of 800-850 nm with the excitation-dependent manner. This NIR fluorescence has a large Stokes shift of 455 nm, providing significant advantage for sensitive determination and imaging of biological targets. The fluorescence properties of the GQDs, such as quantum yields, fluorescence life time, and photostability, were measured and the fluorescence quantum yield was as high as 54.5 %. The morphology and composites of the GQDs were characterized using TEM, SEM, EDS, and FT-IR. The feasibility of using the GQDs as a fluorescent biomarker was investigated through in vitro and in vivo fluorescence imaging. The results showed that the GQDs could be a promising candidate for bioimaging. Most importantly, compared to the traditional quantum dots (QDs), the GQDs is chemically inert. Thus, the potential toxicity of the intrinsic heavy metal in the traditional QDs would not be a concern for GQDs. In addition, the GQDs possessed an intrinsic peroxidase-like catalytic activity that was similar to the graphene sheets and carbon nanotubes. Coupled with 2,2'-azino-bis(3-ethylbenzothiazoline-6-sulphonic acid) (ABTS), the GQDs can be used for the sensitive detection of hydrogen peroxide with a limit of detection of 20 μM.

Fabrication of highly fluorescent graphene quantum dots using L-glutamic acid for in vitro/in vivo imaging and sensing

PubMed Central

Wu, Xu; Tian, Fei; Wang, Wenxue; Chen, Jiao; Wu, Min; Zhao, Julia Xiaojun

2013-01-01

A facile bottom-up method for the synthesis of highly fluorescent graphene quantum dots (GQDs) has been developed using a one-step pyrolysis of a natural amino acid, L-glutamic acid, with the assistance of a simple heating mantle device. The developed GQDs showed strong blue, green and red luminescence under the irradiation of ultra-violet, blue and green light, respectively. Moreover, the GQDs emitted near-infrared (NIR) fluorescence in the range of 800–850 nm with the excitation-dependent manner. This NIR fluorescence has a large Stokes shift of 455 nm, providing significant advantage for sensitive determination and imaging of biological targets. The fluorescence properties of the GQDs, such as quantum yields, fluorescence life time, and photostability, were measured and the fluorescence quantum yield was as high as 54.5 %. The morphology and composites of the GQDs were characterized using TEM, SEM, EDS, and FT-IR. The feasibility of using the GQDs as a fluorescent biomarker was investigated through in vitro and in vivo fluorescence imaging. The results showed that the GQDs could be a promising candidate for bioimaging. Most importantly, compared to the traditional quantum dots (QDs), the GQDs is chemically inert. Thus, the potential toxicity of the intrinsic heavy metal in the traditional QDs would not be a concern for GQDs. In addition, the GQDs possessed an intrinsic peroxidase-like catalytic activity that was similar to the graphene sheets and carbon nanotubes. Coupled with 2,2′-azino-bis(3-ethylbenzothiazoline-6-sulphonic acid) (ABTS), the GQDs can be used for the sensitive detection of hydrogen peroxide with a limit of detection of 20 μM. PMID:23997934

Comparison of femtosecond laser and continuous wave UV sources for protein-nucleic acid crosslinking.

PubMed

Fecko, Christopher J; Munson, Katherine M; Saunders, Abbie; Sun, Guangxing; Begley, Tadhg P; Lis, John T; Webb, Watt W

2007-01-01

Crosslinking proteins to the nucleic acids they bind affords stable access to otherwise transient regulatory interactions. Photochemical crosslinking provides an attractive alternative to formaldehyde-based protocols, but irradiation with conventional UV sources typically yields inadequate product amounts. Crosslinking with pulsed UV lasers has been heralded as a revolutionary technique to increase photochemical yield, but this method had only been tested on a few protein-nucleic acid complexes. To test the generality of the yield enhancement, we have investigated the benefits of using approximately 150 fs UV pulses to crosslink TATA-binding protein, glucocorticoid receptor and heat shock factor to oligonucleotides in vitro. For these proteins, we find that the quantum yields (and saturating yields) for forming crosslinks using the high-peak intensity femtosecond laser do not improve on those obtained with low-intensity continuous wave (CW) UV sources. The photodamage to the oligonucleotides and proteins also has comparable quantum yields. Measurements of the photochemical reaction yields of several small molecules selected to model the crosslinking reactions also exhibit nearly linear dependences on UV intensity instead of the previously predicted quadratic dependence. Unfortunately, these results disprove earlier assertions that femtosecond pulsed laser sources provide significant advantages over CW radiation for protein-nucleic acid crosslinking.

Production yield of rare-earth ions implanted into an optical crystal

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kornher, Thomas, E-mail: t.kornher@physik.uni-stuttgart.de; Xia, Kangwei; Kolesov, Roman

2016-02-01

Rare-earth (RE) ions doped into desired locations of optical crystals might enable a range of novel integrated photonic devices for quantum applications. With this aim, we have investigated the production yield of cerium and praseodymium by means of ion implantation. As a measure, the collected fluorescence intensity from both implanted samples and single centers was used. With a tailored annealing procedure for cerium, a yield up to 53% was estimated. Praseodymium yield amounts up to 91%. Such high implantation yield indicates a feasibility of creation of nanopatterned rare-earth doping and suggests strong potential of RE species for on-chip photonic devices.

A Quick and Parallel Analytical Method Based on Quantum Dots Labeling for ToRCH-Related Antibodies

NASA Astrophysics Data System (ADS)

Yang, Hao; Guo, Qing; He, Rong; Li, Ding; Zhang, Xueqing; Bao, Chenchen; Hu, Hengyao; Cui, Daxiang

2009-12-01

Quantum dot is a special kind of nanomaterial composed of periodic groups of II-VI, III-V or IV-VI materials. Their high quantum yield, broad absorption with narrow photoluminescence spectra and high resistance to photobleaching, make them become a promising labeling substance in biological analysis. Here, we report a quick and parallel analytical method based on quantum dots for ToRCH-related antibodies including Toxoplasma gondii, Rubella virus, Cytomegalovirus and Herpes simplex virus type 1 (HSV1) and 2 (HSV2). Firstly, we fabricated the microarrays with the five kinds of ToRCH-related antigens and used CdTe quantum dots to label secondary antibody and then analyzed 100 specimens of randomly selected clinical sera from obstetric outpatients. The currently prevalent enzyme-linked immunosorbent assay (ELISA) kits were considered as “golden standard” for comparison. The results show that the quantum dots labeling-based ToRCH microarrays have comparable sensitivity and specificity with ELISA. Besides, the microarrays hold distinct advantages over ELISA test format in detection time, cost, operation and signal stability. Validated by the clinical assay, our quantum dots-based ToRCH microarrays have great potential in the detection of ToRCH-related pathogens.

Cultivating Fluorescent Flowers with Highly Luminescent Carbon Dots Fabricated by a Double Passivation Method

PubMed Central

Chang, Tao; Zhao, Haiping; Du, Huanhuan; Liu, Shan; Wu, Baoshuang; Qin, Shenjun

2017-01-01

In this work, we present the fabrication of highly luminescent carbon dots (CDs) by a double passivation method with the assistance of Ca(OH)2. In the reaction process, Ca2+ protects the active functional groups from overconsumption during dehydration and carbonization, and the electron-withdrawing groups on the CD surface are converted to electron-donating groups by the hydroxyl ions. As a result, the fluorescence quantum yield of the CDs was found to increase with increasing Ca(OH)2 content in the reaction process. A blue-shift optical spectrum of the CDs was also found with increasing Ca(OH)2 content, which could be attributed to the increasing of the energy gaps for the CDs. The highly photoluminescent CDs obtained (quantum yield: 86%) were used to cultivate fluorescent carnations by a water culture method, while the results of fluorescence microscopy analysis indicated that the CDs had entered the plant tissue structure. PMID:28686178

Bulk crystalline optomechanics

NASA Astrophysics Data System (ADS)

Renninger, W. H.; Kharel, P.; Behunin, R. O.; Rakich, P. T.

2018-06-01

Control of long-lived, high-frequency phonons using light offers a path towards creating robust quantum links, and could lead to tools for precision metrology with applications to quantum information processing. Optomechanical systems based on bulk acoustic-wave resonators are well suited for this goal in light of their high quality factors, and because they do not suffer from surface interactions as much as their microscale counterparts. However, so far these phonons have been accessible only electromechanically, using piezoelectric interactions. Here, we demonstrate customizable optomechanical coupling to macroscopic phonon modes of a bulk acoustic-wave resonator at cryogenic temperatures. These phonon modes, which are formed by shaping the surfaces of a crystal into a plano-convex phononic resonator, yield appreciable optomechanical coupling rates, providing access to high acoustic quality factors (4.2 × 107) at high phonon frequencies (13 GHz). This simple approach, which uses bulk properties rather than nanostructural control, is appealing for the ability to engineer optomechanical systems at high frequencies that are robust against thermal decoherence. Moreover, we show that this optomechanical system yields a unique form of dispersive symmetry-breaking that enables phonon heating or cooling without an optical cavity.

Rapid microwave-assisted synthesis of highly luminescent nitrogen-doped carbon dots for white light-emitting diodes

NASA Astrophysics Data System (ADS)

Wang, Yaling; Zheng, Jingxia; Wang, Junli; Yang, Yongzhen; Liu, Xuguang

2017-11-01

Highly luminescent nitrogen-doped carbon dots (N-CDs) were synthesized rapidly by one-step microwave-assisted hydrothermal method using citric acid as carbon source and ethylenediamine as dopant. The influences of reaction temperature, reaction time and raw material ratio on the fluorescence performance of N-CDs were investigated. Then N-CDs with the highest quantum yield were selected as fluorescent materials for fabricating white light-emitting diodes (LEDs). Highly luminescent N-CDs with the quantum yield of 75.96% and blue-to-red spectral composition of 51.48% were obtained at the conditions of 180 °C, 8 min and the molar ratio of citric acid to ethylenediamine 2:1. As-prepared highly luminescent N-CDs have an average size of 6.06 nm, possess extensive oxygen- and nitrogen-containing functional groups on their surface, and exhibit strong absorption in ultraviolet region. White LEDs based on the highly luminescent N-CDs emit warm white light with color coordinates of (0.42, 0.40) and correlated color temperature of 3416 K.

Photoelectric Effect: Back to Basics.

ERIC Educational Resources Information Center

Powell, R. A.

1978-01-01

Presents a simplified theoretical analysis of the variation of quantum yield with photon energy in the photoelectric experiment. Describes a way to amplify the experiment and make it more instructive to advanced students through the measurement of quantum yield of a photo cell. (GA)

DETERMINATION OF APPARENT QUANTUM YIELD SPECTRA FOR THE FORMATION OF BIOLOGICALLY LABILE PHOTOPRODUCTS

EPA Science Inventory

Quantum yield spectra for the photochemical formation of biologically labile photoproducts from dissolved organic matter (DOM) have not been available previously, although they would greatly facilitate attempts to model photoproduct formation rates across latitudinal, seasonal, a...

Control of the external photoluminescent quantum yield of emitters coupled to nanoantenna phased arrays

DOE Office of Scientific and Technical Information (OSTI.GOV)

Guo, Ke; Verschuuren, Marc A.; Lozano, Gabriel

2015-08-21

Optical losses in metals represent the largest limitation to the external quantum yield of emitters coupled to plasmonic antennas. These losses can be at the emission wavelength, but they can be more important at shorter wavelengths, i.e., at the excitation wavelength of the emitters, where the conductivity of metals is usually lower. We present accurate measurements of the absolute external photoluminescent quantum yield of a thin layer of emitting material deposited over a periodic nanoantenna phased array. Emission and absorptance measurements of the sample are performed using a custom-made setup including an integrating sphere and variable angle excitation. The measurementsmore » reveal a strong dependence of the external quantum yield on the angle at which the optical field excites the sample. Such behavior is attributed to the coupling between far-field illumination and near-field excitation mediated by the collective resonances supported by the array. Numerical simulations confirm that the inherent losses associated with the metal can be greatly reduced by selecting an optimum angle of illumination, which boosts the light conversion efficiency in the emitting layer. This combined experimental and numerical characterization of the emission from plasmonic arrays reveals the need to carefully design the illumination to achieve the maximum external quantum yield.« less

Multiple exciton generation in cluster-free alloy Cd(x)Hg(1-x)Te colloidal quantum dots synthesized in water.

PubMed

Kershaw, Stephen V; Kalytchuk, Sergii; Zhovtiuk, Olga; Shen, Qing; Oshima, Takuya; Yindeesuk, Witoon; Toyoda, Taro; Rogach, Andrey L

2014-12-21

A number of different composition CdxHg1-xTe alloy quantum dots have been synthesized using a modified aqueous synthesis and ion exchange method. The benefits of good stoichiometric control and high emission quantum yield were retained whilst also ensuring that the tendency to form gel-like clusters and adsorb excess cations in the stabilizing ligand shells was mitigated using a sequestering method to remove excess ionic material during and after the synthesis. This was highly desirable for ultrafast carrier dynamics measurements, avoiding strong photocharging effects which may mask fundamental carrier signals. Transient grating measurements revealed a composition dependent carrier multiplication process which competes with phonon mediated carrier cooling to deplete the initial hot carrier population. The interplay between these two mechanisms is strongly dependent on the electron effective mass which in these alloys has a marked composition dependence and may be considerably lower than the hole effective mass. For a composition x = 0.52 we measured a maximum carrier multiplication quantum yield of 199 ± 19% with pump photon energy 3 times the bandgap energy, Eg, whilst the threshold energy is calculated to be just 2.15Eg. There is some evidence to suggest an impact ionization process analogous to the inverse Auger S mechanism seen in bulk CdxHg1-xTe.

High-efficiency organic glass scintillators

DOE Office of Scientific and Technical Information (OSTI.GOV)

Feng, Patrick L.; Carlson, Joseph S.

A new family of neutron/gamma discriminating scintillators is disclosed that comprises stable organic glasses that may be melt-cast into transparent monoliths. These materials have been shown to provide light yields greater than solution-grown trans-stilbene crystals and efficient PSD capabilities when combined with 0.01 to 0.05% by weight of the total composition of a wavelength-shifting fluorophore. Photoluminescence measurements reveal fluorescence quantum yields that are 2 to 5 times greater than conventional plastic or liquid scintillator matrices, which accounts for the superior light yield of these glasses. The unique combination of high scintillation light-yields, efficient neutron/gamma PSD, and straightforward scale-up via melt-castingmore » distinguishes the developed organic glasses from existing scintillators.« less

Fixed-node quantum Monte Carlo

NASA Astrophysics Data System (ADS)

Anderson, James B.

Quantum Monte Carlo methods cannot at present provide exact solutions of the Schrödinger equation for systems with more than a few electrons. But, quantum Monte Carlo calculations can provide very low energy, highly accurate solutions for many systems ranging up to several hundred electrons. These systems include atoms such as Be and Fe, molecules such as H2O, CH4, and HF, and condensed materials such as solid N2 and solid silicon. The quantum Monte Carlo predictions of their energies and structures may not be `exact', but they are the best available. Most of the Monte Carlo calculations for these systems have been carried out using approximately correct fixed nodal hypersurfaces and they have come to be known as `fixed-node quantum Monte Carlo' calculations. In this paper we review these `fixed node' calculations and the accuracies they yield.

Quantum-locked key distribution at nearly the classical capacity rate.

PubMed

Lupo, Cosmo; Lloyd, Seth

2014-10-17

Quantum data locking is a protocol that allows for a small secret key to (un)lock an exponentially larger amount of information, hence yielding the strongest violation of the classical one-time pad encryption in the quantum setting. This violation mirrors a large gap existing between two security criteria for quantum cryptography quantified by two entropic quantities: the Holevo information and the accessible information. We show that the latter becomes a sensible security criterion if an upper bound on the coherence time of the eavesdropper's quantum memory is known. Under this condition, we introduce a protocol for secret key generation through a memoryless qudit channel. For channels with enough symmetry, such as the d-dimensional erasure and depolarizing channels, this protocol allows secret key generation at an asymptotic rate as high as the classical capacity minus one bit.

Fluorescent quantum dot hydrophilization with PAMAM dendrimer

NASA Astrophysics Data System (ADS)

Potapkin, Dmitry V.; Geißler, Daniel; Resch-Genger, Ute; Goryacheva, Irina Yu.

2016-05-01

Polyamidoamine (PAMAM) dendrimers were used to produce CdSe core/multi-shell fluorescent quantum dots (QDs) which are colloidally stable in aqueous solutions. The size, charge, and optical properties of QDs functionalized with the 4th (G4) and 5th (G5) generation of PAMAM were compared with amphiphilic polymer-covered QDs and used as criteria for the evaluation of the suitability of both water solubilization methods. As revealed by dynamic and electrophoretic light scattering (DLS and ELS), the hydrodynamic sizes of the QDs varied from 30 to 65 nm depending on QD type and dendrimer generation, with all QDs displaying highly positive surface charges, i.e., zeta potentials of around +50 mV in water. PAMAM functionalization yielded stable core/multi-shell QDs with photoluminescence quantum yields ( Φ) of up to 45 %. These dendrimer-covered QDs showed a smaller decrease in their Φ upon phase transfer compared with QDs made water soluble via encapsulation with amphiphilic brush polymer bearing polyoxyethylene/polyoxypropylene chains.

Temperature dependence of tris(2,2'-bipyridine) ruthenium (II) device characteristics

NASA Astrophysics Data System (ADS)

Slinker, Jason D.; Malliaras, George G.; Flores-Torres, Samuel; Abruña, Héctor D.; Chunwachirasiri, Withoon; Winokur, Michael J.

2004-04-01

We have investigated the temperature dependence of the current, radiance, and efficiency from electroluminescent devices based on [Ru(bpy)3]2+(PF6-)2, where bpy is 2,2'-bipyridine. We find that the current increases monotonically with temperature from 200 to 380 K, while the radiance reaches a maximum near room temperature. For temperatures greater than room temperature, an irreversible, current-induced degradation occurs with thermal cycling that diminishes both the radiance and the photoluminescence (PL) quantum yield, but does not affect the current. The temperature dependence of the external quantum efficiency is fully accounted for by the dependence of the PL quantum yield as measured from the emissive area of the device. This implies that the contacts remain ohmic throughout the temperature range investigated. The quenching of the PL with temperature was attributed to thermal activation to a nonradiative d-d transition. The temperature dependence of the current shows a complex behavior in which transport appears to be thermally activated, with distinct low-temperature and high-temperature regimes.

Phosphorescent Iridium(III) Complexes Bearing Fluorinated Aromatic Sulfonyl Group with Nearly Unity Phosphorescent Quantum Yields and Outstanding Electroluminescent Properties.

PubMed

Zhao, Jiang; Yu, Yue; Yang, Xiaolong; Yan, Xiaogang; Zhang, Huiming; Xu, Xianbin; Zhou, Guijiang; Wu, Zhaoxin; Ren, Yixia; Wong, Wai-Yeung

2015-11-11

A series of heteroleptic functional Ir(III) complexes bearing different fluorinated aromatic sulfonyl groups has been synthesized. Their photophysical features, electrochemical behaviors, and electroluminescent (EL) properties have been characterized in detail. These complexes emit intense yellow phosphorescence with exceptionally high quantum yields (ΦP > 0.9) at room temperature, and the emission maxima of these complexes can be finely tuned depending upon the number of the fluorine substituents on the pendant phenyl ring of the sulfonyl group. Furthermore, the electrochemical properties and electron injection/transporting (EI/ET) abilities of these Ir(III) phosphors can also be effectively tuned by the fluorinated aromatic sulfonyl group to furnish some desired characters for enhancing the EL performance. Hence, the maximum luminance efficiency (ηL) of 81.2 cd A(-1), corresponding to power efficiency (ηP) of 64.5 lm W(-1) and external quantum efficiency (ηext) of 19.3%, has been achieved, indicating the great potential of these novel phosphors in the field of organic light-emitting diodes (OLEDs). Furthermore, a clear picture has been drawn for the relationship between their optoelectronic properties and chemical structures. These results should provide important information for developing highly efficient phosphors.

Facile consecutive solvothermal growth of highly fluorescent InP/ZnS core/shell quantum dots using a safer phosphorus source.

PubMed

Byun, Ho-June; Song, Woo-Seuk; Yang, Heesun

2011-06-10

The work presents a facile, stepwise synthetic approach for the production of highly fluorescent InP/ZnS core/shell quantum dots (QDs) by using a safer phosphorus (P) precursor. First, InP quantum dots (QDs) were solvothermally prepared at 180 °C for 24 h by using a P source of P(N(CH(3))(2))(3). The as-grown InP QDs were consecutively placed in another solvothermal condition for ZnS shell overcoating. In contrast to the almost non-fluorescent InP QDs, due to their highly defective surface states, the ZnS-coated InP QDs were highly fluorescent as a result of effective surface passivation. After the shell growth, the resulting InP/ZnS core/shell QDs were subjected to a size-sorting processing, by which red- to green-emitting QDs with quantum yields (QYs) of 24-60% were produced. Solvothermal shell growth parameters such as the reaction time and Zn/In solution concentration ratio were varied and optimized toward the highest QYs of core/shell QDs.

Facile consecutive solvothermal growth of highly fluorescent InP/ZnS core/shell quantum dots using a safer phosphorus source

NASA Astrophysics Data System (ADS)

Byun, Ho-June; Song, Woo-Seuk; Yang, Heesun

2011-06-01

The work presents a facile, stepwise synthetic approach for the production of highly fluorescent InP/ZnS core/shell quantum dots (QDs) by using a safer phosphorus (P) precursor. First, InP quantum dots (QDs) were solvothermally prepared at 180 °C for 24 h by using a P source of P(N(CH3)2)3. The as-grown InP QDs were consecutively placed in another solvothermal condition for ZnS shell overcoating. In contrast to the almost non-fluorescent InP QDs, due to their highly defective surface states, the ZnS-coated InP QDs were highly fluorescent as a result of effective surface passivation. After the shell growth, the resulting InP/ZnS core/shell QDs were subjected to a size-sorting processing, by which red- to green-emitting QDs with quantum yields (QYs) of 24-60% were produced. Solvothermal shell growth parameters such as the reaction time and Zn/In solution concentration ratio were varied and optimized toward the highest QYs of core/shell QDs.

High-power lightweight external-cavity quantum cascade lasers

NASA Astrophysics Data System (ADS)

Day, Timothy; Takeuchi, Eric B.; Weida, Miles; Arnone, David; Pushkarsky, Michael; Boyden, David; Caffey, David

2009-05-01

Commercially available quantum cascade gain media has been integrated with advanced coating and die attach technologies, mid-IR micro-optics and telecom-style assembly and packaging to yield cutting edge performance. When combined into Daylight's external-cavity quantum cascade laser (ECqcL) platform, multi-Watt output power has been obtained. Daylight will describe their most recent results obtained from this platform, including high cw power from compact hermetically sealed packages and narrow spectral linewidth devices. Fiber-coupling and direct amplitude modulation from such multi-Watt lasers will also be described. In addition, Daylight will present the most recent results from their compact, portable, battery-operated "thermal laser pointers" that are being used for illumination and aiming applications. When combined with thermal imaging technology, such devices provide significant benefits in contrast and identification.

Size-controlled synthesis of ZnO quantum dots in microreactors

NASA Astrophysics Data System (ADS)

Schejn, Aleksandra; Frégnaux, Mathieu; Commenge, Jean-Marc; Balan, Lavinia; Falk, Laurent; Schneider, Raphaël

2014-04-01

In this paper, we report on a continuous-flow microreactor process to prepare ZnO quantum dots (QDs) with widely tunable particle size and photoluminescence emission wavelengths. X-ray diffraction, electron diffraction, UV-vis, photoluminescence and transmission electron microscopy measurements were used to characterize the synthesized ZnO QDs. By varying operating conditions (temperature, flow rate) or the capping ligand, ZnO QDs with diameters ranging from 3.6 to 5.2 nm and fluorescence maxima from 500 to 560 nm were prepared. Results obtained show that low reaction temperatures (20 or 35 °C), high flow rates and the use of propionic acid as a stabilizing agent are favorable for the production of ZnO QDs with high photoluminescence quantum yields (up to 30%).

One-pot synthesis of polythiol ligand for highly bright and stable hydrophilic quantum dots toward bioconjugate formation

NASA Astrophysics Data System (ADS)

Dezhurov, Sergey V.; Krylsky, Dmitry V.; Rybakova, Anastasia V.; Ibragimova, Sagila A.; Gladyshev, Pavel P.; Vasiliev, Alexey A.; Morenkov, Oleg S.

2018-03-01

A fast and efficient one-pot synthesis of thiol-terminated poly(vinylpirrolidone-co-maleic anhydride-co-ethylene glycol dimethacrylate) based heterobifunctional polymer (PTVP) has been developed. The polymer was used for the modification of quantum dots (QDs) to prepare water soluble and stable QDs with emission quantum yield as high as 80%. Using carbodiimide method, PTVP-capped red light-emitting QDs were conjugated to model monoclonal antibodies specific to glycoprotein B (gB) of Aujeszky’s disease virus (ADV) and successfully used in the lateral flow assay (LFA) for the detection of ADV gB in biological fluids. A comparative analysis of the sensitivity of the method was carried out using three types of QDs emitting in the red and far-red region.

Simple Microwave-Assisted Synthesis of Amphiphilic Carbon Quantum Dots from A3/B2 Polyamidation Monomer Set.

PubMed

Choi, Yujin; Jo, Seongho; Chae, Ari; Kim, Young Kwang; Park, Jeong Eun; Lim, Donggun; Park, Sung Young; In, Insik

2017-08-23

Highly fluorescent and amphiphilic carbon quantum dots (CQDs) were prepared by microwave-assisted pyrolysis of citric acid and 4,7,10-trioxa-1,13-tridecanediamine (TTDDA), which functioned as an A 3 and B 2 polyamidation type monomer set. Gram quantities of fluorescent CQDs were easily obtained within 5 min of microwave heating using a household microwave oven. Because of the dual role of TTDDA, both as a constituting monomer and as a surface passivation agent, TTDDA-based CQDs showed a high fluorescence quantum yield of 29% and amphiphilic solubility in various polar and nonpolar solvents. These properties enable the wide application of TTDDA-based CQDs as nontoxic bioimaging agents, nanofillers for polymer composites, and down-converting layers for enhancing the efficiency of Si solar cells.

Chemically Triggered Formation of Two-Dimensional Epitaxial Quantum Dot Superlattices.

PubMed

Walravens, Willem; De Roo, Jonathan; Drijvers, Emile; Ten Brinck, Stephanie; Solano, Eduardo; Dendooven, Jolien; Detavernier, Christophe; Infante, Ivan; Hens, Zeger

2016-07-26

Two dimensional superlattices of epitaxially connected quantum dots enable size-quantization effects to be combined with high charge carrier mobilities, an essential prerequisite for highly performing QD devices based on charge transport. Here, we demonstrate that surface active additives known to restore nanocrystal stoichiometry can trigger the formation of epitaxial superlattices of PbSe and PbS quantum dots. More specifically, we show that both chalcogen-adding (sodium sulfide) and lead oleate displacing (amines) additives induce small area epitaxial superlattices of PbSe quantum dots. In the latter case, the amine basicity is a sensitive handle to tune the superlattice symmetry, with strong and weak bases yielding pseudohexagonal or quasi-square lattices, respectively. Through density functional theory calculations and in situ titrations monitored by nuclear magnetic resonance spectroscopy, we link this observation to the concomitantly different coordination enthalpy and ligand displacement potency of the amine. Next to that, an initial ∼10% reduction of the initial ligand density prior to monolayer formation and addition of a mild, lead oleate displacing chemical trigger such as aniline proved key to induce square superlattices with long-range, square micrometer order; an effect that is the more pronounced the larger the quantum dots. Because the approach applies to PbS quantum dots as well, we conclude that it offers a reproducible and rational method for the formation of highly ordered epitaxial quantum dot superlattices.

Quantum dots/silica/polymer nanocomposite films with high visible light transmission and UV shielding properties

NASA Astrophysics Data System (ADS)

Mumin, Md Abdul; Xu, William Z.; Charpentier, Paul A.

2015-08-01

The dispersion of light-absorbing inorganic nanomaterials in transparent plastics such as poly(ethylene-co-vinyl acetate) (PEVA) is of enormous current interest in emerging solar materials, including photovoltaic (PV) modules and commercial greenhouse films. Nanocrystalline semiconductor or quantum dots (QDs) have the potential to absorb UV light and selectively emit visible light, which can control plant growth in greenhouses or enhance PV panel efficiencies. This work provides a new and simple approach for loading mesoporous silica-encapsulated QDs into PEVA. Highly luminescent CdS and CdS-ZnS core-shell QDs with 5 nm size were synthesized using a modified facile approach based on pyrolysis of the single-molecule precursors and capping the CdS QDs with a thin layer of ZnS. To make both the bare and core-shell structure QDs more resistant against photochemical reactions, a mesoporous silica layer was grown on the QDs through a reverse microemulsion technique based on hydrophobic interactions. By careful experimental tuning, this encapsulation technique enhanced the quantum yield (˜65%) and photostability compared to the bare QDs. Both the encapsulated bare and core-shell QDs were then melt-mixed with EVA pellets using a mini twin-screw extruder and pressed into thin films with controlled thickness. The results demonstrated for the first time that mesoporous silica not only enhanced the quantum yield and photostability of the QDs but also improved the compatibility and dispersibility of QDs throughout the PEVA films. The novel light selective films show high visible light transmission (˜90%) and decreased UV transmission (˜75%).

Quantum dots/silica/polymer nanocomposite films with high visible light transmission and UV shielding properties.

PubMed

Mumin, Md Abdul; Xu, William Z; Charpentier, Paul A

2015-08-07

The dispersion of light-absorbing inorganic nanomaterials in transparent plastics such as poly(ethylene-co-vinyl acetate) (PEVA) is of enormous current interest in emerging solar materials, including photovoltaic (PV) modules and commercial greenhouse films. Nanocrystalline semiconductor or quantum dots (QDs) have the potential to absorb UV light and selectively emit visible light, which can control plant growth in greenhouses or enhance PV panel efficiencies. This work provides a new and simple approach for loading mesoporous silica-encapsulated QDs into PEVA. Highly luminescent CdS and CdS-ZnS core-shell QDs with 5 nm size were synthesized using a modified facile approach based on pyrolysis of the single-molecule precursors and capping the CdS QDs with a thin layer of ZnS. To make both the bare and core-shell structure QDs more resistant against photochemical reactions, a mesoporous silica layer was grown on the QDs through a reverse microemulsion technique based on hydrophobic interactions. By careful experimental tuning, this encapsulation technique enhanced the quantum yield (∼65%) and photostability compared to the bare QDs. Both the encapsulated bare and core-shell QDs were then melt-mixed with EVA pellets using a mini twin-screw extruder and pressed into thin films with controlled thickness. The results demonstrated for the first time that mesoporous silica not only enhanced the quantum yield and photostability of the QDs but also improved the compatibility and dispersibility of QDs throughout the PEVA films. The novel light selective films show high visible light transmission (∼90%) and decreased UV transmission (∼75%).

Engineering triangular carbon quantum dots with unprecedented narrow bandwidth emission for multicolored LEDs.

PubMed

Yuan, Fanglong; Yuan, Ting; Sui, Laizhi; Wang, Zhibin; Xi, Zifan; Li, Yunchao; Li, Xiaohong; Fan, Louzhen; Tan, Zhan'ao; Chen, Anmin; Jin, Mingxing; Yang, Shihe

2018-06-08

Carbon quantum dots (CQDs) have emerged as promising materials for optoelectronic applications on account of carbon's intrinsic merits of high stability, low cost, and environment-friendliness. However, the CQDs usually give broad emission with full width at half maximum exceeding 80 nm, which fundamentally limit their display applications. Here we demonstrate multicolored narrow bandwidth emission (full width at half maximum of 30 nm) from triangular CQDs with a quantum yield up to 54-72%. Detailed structural and optical characterizations together with theoretical calculations reveal that the molecular purity and crystalline perfection of the triangular CQDs are key to the high color-purity. Moreover, multicolored light-emitting diodes based on these CQDs display good stability, high color-purity, and high-performance with maximum luminance of 1882-4762 cd m -2 and current efficiency of 1.22-5.11 cd A -1 . This work will set the stage for developing next-generation high-performance CQDs-based light-emitting diodes.

Photosynthetic Physiological Response of Radix Isatidis (Isatis indigotica Fort.) Seedlings to Nicosulfuron

PubMed Central

Ning, Na; Wen, Yinyuan; Dong, Shuqi; Yin, Meiqiang; Guo, Meijun; Wang, Binqiang; Feng, Lei; Guo, Pingyi

2014-01-01

Radix Isatidis (Isatis indigotica Fort.) is one of the most important traditional Chinese medicine plants. However, there is no suitable herbicide used for weed control in Radix Isatidis field during postemergence stage. To explore the safety of sulfonylurea herbicide nicosulfuron on Radix Isatidis (Isatis indigotica Fort.) seedlings and the photosynthetic physiological response of the plant to the herbicide, biological mass, leaf area, photosynthetic pigment content, photosynthetic rate, chlorophyll fluorescence characteristics, and P700 parameters of Radix Isatidis seedlings were analyzed 10 d after nicosulfuron treatment at 5th leaf stage in this greenhouse research. The results showed that biological mass, total chlorophyll, chlorophyll a, and carotenoids content, photosynthetic rate, stomatal conductance, PS II maximum quantum yield, PS II effective quantum yield, PS II electron transport rate, photochemical quenching, maximal P700 change, photochemical quantum yield of PS I, and PS I electron transport rate decreased with increasing herbicide concentrations, whereas initial fluorescence, quantum yield of non-regulated energy dissipation in PS II and quantum yield of non-photochemical energy dissipation due to acceptor side limitation in PS I increased. It suggests that nicosulfuron ≥1 mg L−1 causes the damage of chloroplast, PS II and PS I structure. Electron transport limitations in PS I receptor side, and blocked dark reaction process may be the main cause of the significantly inhibited growth and decreased photosynthetic rate of Radix Isatidis seedlings. PMID:25165819

Synthesis, characterization and photophysical-theoretical analysis of compounds A-π-D. 1. Effect of alkyl-phenyl substituted amines in photophysical properties

NASA Astrophysics Data System (ADS)

Ortega, E.; Montecinos, R.; Cattin, L.; Díaz, F. R.; del Valle, M. A.; Bernède, J. C.

2017-08-01

The study of new dipolar A-π-D molecules, which have an acceptor (A) and donor (D) charge joined by a conjugate bridge, have been an attention focus in the recent years due their different properties. In the current work, a molecular system has been modified in order to compare the effect on properties, such as quantum yield. Thus, two series were generated (alkyl- and alkoxy-substituted) to determine if molecules with tertiary asymmetric amines change their optical properties and whether quantum yield is affected. The different products have been characterized by several techniques such as UV-Vis spectrophotometry, elemental analysis, NMR, FT-IR, mass spectroscopy and fluorescence spectroscopy. Furthermore, their behavior in eight organic solvents, dichloromethane, tetrahydrofuran, ethyl acetate, 1,4-dioxane, acetone, acetonitrile, dimethylformamide and dimethylsulfoxide were experimentally and theoretically studied. The quantum yields were higher for the alkyl-substituted series. Theoretically, the dihedral angles formed between the tertiary amine and carbonyl group moieties have a correlation with quantum yield values, helping to explain why they are higher in non-polar solvents. Consequently, the maximum quantum yield was obtained with (E)-2-cyano-3-(5-((E)-2-(9,9-diethyl-7-(methyl(phenyl)amino)-9H-fluoren-2-yl) vinyl)thiophen-2-yl)acrylic acid (M8-1) in 1,4-dioxane, reaching 98.8%.

Simulation of a broadband nano-biosensor based on an onion-like quantum dot-quantum well structure

DOE Office of Scientific and Technical Information (OSTI.GOV)

Absalan, H; SalmanOgli, A; Rostami, R

The fluorescence resonance energy transfer is studied between modified quantum-dots and quantum-wells used as a donor and an acceptor. Because of the unique properties of quantum dots, including diverse surface modification flexibility, bio-compatibility, high quantum yields and wide absorption, their use as nano-biosensors and bio-markers used in diagnosis of cancer is suggested. The fluorescence resonance energy transfer is simulated in a quantum dot-quantum well system, where the energy can flow from donor to acceptor. If the energy transfer can be either turned on or off by a specific interaction, such as interaction with any dyes, a molecular binding event ormore » a cleavage reaction, a sensor can be designed (under assumption that the healthy cells have a known effect or unyielding effect on output parameters while cancerous cells, due to their pandemic optical properties, can impact the fluorescence resonance energy transfer parameters). The developed nano-biosensor can operate in a wide range of wavelengths (310 - 760 nm). (laser applications in biology and medicine)« less

Quantum corrections crossover and ferromagnetism in magnetic topological insulators.

PubMed

Bao, Lihong; Wang, Weiyi; Meyer, Nicholas; Liu, Yanwen; Zhang, Cheng; Wang, Kai; Ai, Ping; Xiu, Faxian

2013-01-01

Revelation of emerging exotic states of topological insulators (TIs) for future quantum computing applications relies on breaking time-reversal symmetry and opening a surface energy gap. Here, we report on the transport response of Bi2Te3 TI thin films in the presence of varying Cr dopants. By tracking the magnetoconductance (MC) in a low doping regime we observed a progressive crossover from weak antilocalization (WAL) to weak localization (WL) as the Cr concentration increases. In a high doping regime, however, increasing Cr concentration yields a monotonically enhanced anomalous Hall effect (AHE) accompanied by an increasing carrier density. Our results demonstrate a possibility of manipulating bulk ferromagnetism and quantum transport in magnetic TI, thus providing an alternative way for experimentally realizing exotic quantum states required by spintronic applications.

A fluorescent nanosensor based on graphene quantum dots-aptamer probe and graphene oxide platform for detection of lead (II) ion.

PubMed

Qian, Zhao Sheng; Shan, Xiao Yue; Chai, Lu Jing; Chen, Jian Rong; Feng, Hui

2015-06-15

The sensitive detection of heavy metal ions in the organism and aquatic ecosystem using nanosensors based on environment friendly and biocompatible materials still remains a challenge. A fluorescent turn-on nanosensor for lead (II) detection based on biocompatible graphene quantum dots and graphene oxide by employment of Pb(2+)-induced G-quadruplex formation was reported. Graphene quantum dots with high quantum yield, good biocompatibility were prepared and served as the fluorophore of Pb(2+) probe. Fluorescence turn-off of graphene quantum dots is easily achieved through efficient photoinduced electron transfer between graphene quantum dots and graphene oxide, and subsequent fluorescence turn-on process is due to the formation of G-quadraplex aptamer-Pb(2+) complex triggered by the addition of Pb(2+). This nanosensor can distinguish Pb(2+) ion from other ions with high sensitivity and good reproducibility. The detection method based on this nanosensor possesses a fast response time of one minute, a broad linear span of up to 400.0 nM and ultralow detection limit of 0.6 nM. Copyright © 2015 Elsevier B.V. All rights reserved.

The Application of Fluorescent Quantum Dots to Confocal, Multiphoton, and Electron Microscopic Imaging

PubMed Central

Deerinck, Thomas J.

2009-01-01

Fluorescent quantum dots are emerging as an important tool for imaging cells and tissues, and their unique optical and physical properties have captured the attention of the research community. The most common types of commercially available quantum dots consist of a nanocrystalline semiconductor core composed of cadmium selenide with a zinc sulfide capping layer and an outer polymer layer to facilitate conjugation to targeting biomolecules such as immunoglobulins. They exhibit high fluorescent quantum yields and have large absorption cross-sections, possess excellent photostability, and can be synthesized so that their narrow-band fluorescence emission can occur in a wide spectrum of colors. These properties make them excellent candidates for serving as multiplexing molecular beacons using a variety of imaging modalities including highly correlated microscopies. Whereas much attention has been focused on quantum-dot applications for live-cell imaging, we have sought to characterize and exploit their utility for enabling simultaneous multiprotein immunolabeling in fixed cells and tissues. Considerations for their application to immunolabeling for correlated light and electron microscopic analysis are discussed. PMID:18337229

Controllable Synthesis of Highly Luminescent Boron Nitride Quantum Dots.

PubMed

Li, Hongling; Tay, Roland Yingjie; Tsang, Siu Hon; Zhen, Xu; Teo, Edwin Hang Tong

2015-12-22

Boron nitride quantum dots (BNQDs), as a new member of heavy metal-free quantum dots, have aroused great interest in fundamental research and practical application due to their unique physical/chemical properties. However, it is still a challenge to controllably synthesize high-quality BNQDs with high quantum yield (QY), uniform size and strong fluorescent. In this work, BNQDs have been successfully fabricated by the liquid exfoliation and the subsequent solvothermal process with respect to its facileness and easy large scale up. Importantly, BNQDs with high-quality can be controllably obtained by adjusting the synthetic parameters involved in the solvothermal process including filling factor, synthesis temperature, and duration time. Encouragingly, the as-prepared BNQDs possess strong blue luminescence with QY as high as 19.5%, which can be attributed to the synergetic effect of size, surface chemistry and edge defects. In addition, this strategy presented here provides a new reference for the controllable synthesis of other heavy metal-free QDs. Furthermore, the as-prepared BNQDs are non-toxic to cells and exhibit nanosecond-scaled lifetimes, suggesting they have great potential biological and optoelectronic applications. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Optimally stopped variational quantum algorithms

NASA Astrophysics Data System (ADS)

Vinci, Walter; Shabani, Alireza

2018-04-01

Quantum processors promise a paradigm shift in high-performance computing which needs to be assessed by accurate benchmarking measures. In this article, we introduce a benchmark for the variational quantum algorithm (VQA), recently proposed as a heuristic algorithm for small-scale quantum processors. In VQA, a classical optimization algorithm guides the processor's quantum dynamics to yield the best solution for a given problem. A complete assessment of the scalability and competitiveness of VQA should take into account both the quality and the time of dynamics optimization. The method of optimal stopping, employed here, provides such an assessment by explicitly including time as a cost factor. Here, we showcase this measure for benchmarking VQA as a solver for some quadratic unconstrained binary optimization. Moreover, we show that a better choice for the cost function of the classical routine can significantly improve the performance of the VQA algorithm and even improve its scaling properties.

Ultra-broadband photodetectors based on epitaxial graphene quantum dots

NASA Astrophysics Data System (ADS)

El Fatimy, Abdel; Nath, Anindya; Kong, Byoung Don; Boyd, Anthony K.; Myers-Ward, Rachael L.; Daniels, Kevin M.; Jadidi, M. Mehdi; Murphy, Thomas E.; Gaskill, D. Kurt; Barbara, Paola

2018-03-01

Graphene is an ideal material for hot-electron bolometers due to its low heat capacity and weak electron-phonon coupling. Nanostructuring graphene with quantum-dot constrictions yields detectors of electromagnetic radiation with extraordinarily high intrinsic responsivity, higher than 1×109 V W-1 at 3 K. The sensing mechanism is bolometric in nature: the quantum confinement gap causes a strong dependence of the electrical resistance on the electron temperature. Here, we show that this quantum confinement gap does not impose a limitation on the photon energy for light detection and these quantum-dot bolometers work in a very broad spectral range, from terahertz through telecom to ultraviolet radiation, with responsivity independent of wavelength. We also measure the power dependence of the response. Although the responsivity decreases with increasing power, it stays higher than 1×108 V W-1 in a wide range of absorbed power, from 1 pW to 0.4 nW.

Do the cations in clay and the polymer matrix affect quantum dot fluorescent properties?

PubMed

Wei, Wenjun; Liu, Cui; Liu, Jiyan; Liu, Xueqing; Zou, Linling; Cai, Shaojun; Shi, Hong; Cao, Yuan-Cheng

2016-06-01

This paper studied the effects of cations and polymer matrix on the fluorescent properties of quantum dots (QDs). The results indicated that temperature has a greater impact on fluorescence intensity than clay cations (mainly K(+) and Na(+) ). Combined fluorescence lifetime and steady-state spectrometer tests showed that QD lifetimes all decreased when the cation concentration was increased, but the quantum yields were steady at various cation concentrations of 0, 0.05, 0.5 and 1 M. Poly(ethylene oxide) (PEO), poly(vinyl alcohol) (PVA) and diepoxy resin were used to study the effects of polymers on QD lifetime and quantum yield. The results showed that the lifetime for QDs 550 nm in PEO and PVA was 17.33 and 17.12 ns, respectively; for the epoxy resin, the lifetime was 0.74 ns, a sharp decrease from 24.47 ns. The quantum yield for QDs 550 nm changed from 34.22% to 7.45% and 7.81% in PEO and PVA, respectively; for the epoxy resin the quantum yield was 2.25%. QDs 580 nm and 620 nm showed the same results as QDs 550 nm. This study provides useful information on the design, synthesis and application of QDs-polymer luminescent materials. Copyright © 2015 John Wiley & Sons, Ltd. Copyright © 2015 John Wiley & Sons, Ltd.

ABSORBANCE, ABSORPTION COEFFICIENT, AND APPARENT QUANTUM YIELD: A COMMENT ON AMBIGUITY IN THE USE OF THESE OPTICAL CONCEPTS

EPA Science Inventory

Several important optical terms such as "absorbance" and "absorption coefficient" are frequently used ambiguously in the current peer-reviewed literature. Since they are important terms that are required to derive other quantities such as the "apparent quantum yield" of photoprod...

Unusually high fluorescence quantum yield of a homopolyfluorenylazomethine--towards a universal fluorophore.

PubMed

Mallet, Charlotte; Bolduc, Andréanne; Bishop, Sophie; Gautier, Yohan; Skene, W G

2014-11-28

The absolute fluorescence quantum yield (Φfl) of a polyfluorenyl azomethine homopolymer was measured as a function of solvent polarity. The solvent induced and temperature dependent fluorescence of the homopolymer were also investigated and they were compared to the corresponding monomer and copolymer. The Φfl of the homopolymer was consistent (45-70%), regardless of solvent polarity with Stokes shifts up to 7460 cm(-1) in ethanol. In contrast, the Φfl of its corresponding monomer decreased from 60% in ethanol to 1% in toluene, whereas a Φfl < 5% for its analogous copolymer was measured. Moderate fluorescence yields (Φfl ≈ 25%) were also possible in thin film when co-depositing the homopolymer with PMMA. Cryofluorescence was used to probe the excited state deactivation modes. Deactivation by internal conversion was found to compete with fluorescence. The fluorescence deactivation pathways of the homopolymer and its corresponding monomer could be suppressed at 77 K, resulting in fluorescence turn-on. Both fluorophores were found to detect nitroaromatics.

High-fidelity gates in quantum dot spin qubits

PubMed Central

Koh, Teck Seng; Coppersmith, S. N.; Friesen, Mark

2013-01-01

Several logical qubits and quantum gates have been proposed for semiconductor quantum dots controlled by voltages applied to top gates. The different schemes can be difficult to compare meaningfully. Here we develop a theoretical framework to evaluate disparate qubit-gating schemes on an equal footing. We apply the procedure to two types of double-dot qubits: the singlet–triplet and the semiconducting quantum dot hybrid qubit. We investigate three quantum gates that flip the qubit state: a DC pulsed gate, an AC gate based on logical qubit resonance, and a gate-like process known as stimulated Raman adiabatic passage. These gates are all mediated by an exchange interaction that is controlled experimentally using the interdot tunnel coupling g and the detuning ϵ, which sets the energy difference between the dots. Our procedure has two steps. First, we optimize the gate fidelity (f) for fixed g as a function of the other control parameters; this yields an that is universal for different types of gates. Next, we identify physical constraints on the control parameters; this yields an upper bound that is specific to the qubit-gate combination. We show that similar gate fidelities should be attainable for singlet-triplet qubits in isotopically purified Si, and for hybrid qubits in natural Si. Considerably lower fidelities are obtained for GaAs devices, due to the fluctuating magnetic fields ΔB produced by nuclear spins. PMID:24255105

Cs4PbBr6/CsPbBr3 Perovskite Composites with Near-Unity Luminescence Quantum Yield: Large-Scale Synthesis, Luminescence and Formation Mechanism, and White Light-Emitting Diode Application.

PubMed

Chen, Ya-Meng; Zhou, Yang; Zhao, Qing; Zhang, Jun-Ying; Ma, Ju-Ping; Xuan, Tong-Tong; Guo, Shao-Qiang; Yong, Zi-Jun; Wang, Jing; Kuroiwa, Yoshihiro; Moriyoshi, Chikako; Sun, Hong-Tao

2018-05-09

All-inorganic perovskites have emerged as a new class of phosphor materials owing to their outstanding optical properties. Zero-dimensional inorganic perovskites, in particular the Cs 4 PbBr 6 -related systems, are inspiring intensive research owing to the high photoluminescence quantum yield (PLQY) and good stability. However, synthesizing such perovskites with high PLQYs through an environment-friendly, cost-effective, scalable, and high-yield approach remains challenging, and their luminescence mechanisms has been elusive. Here, we report a simple, scalable, room-temperature self-assembly strategy for the synthesis of Cs 4 PbBr 6 /CsPbBr 3 perovskite composites with near-unity PLQY (95%), high product yield (71%), and good stability using low-cost, low-toxicity chemicals as precursors. A broad range of experimental and theoretical characterizations suggest that the high-efficiency PL originates from CsPbBr 3 nanocrystals well passivated by the zero-dimensional Cs 4 PbBr 6 matrix that forms based on a dissolution-crystallization process. These findings underscore the importance in accurately identifying the phase purity of zero-dimensional perovskites by synchrotron X-ray technique to gain deep insights into the structure-property relationship. Additionally, we demonstrate that green-emitting Cs 4 PbBr 6 /CsPbBr 3 , combined with red-emitting K 2 SiF 6 :Mn 4+ , can be used for the construction of WLEDs. Our work may pave the way for the use of such composite perovskites as highly luminescent emitters in various applications such as lighting, displays, and other optoelectronic and photonic devices.

Solving Quantum Ground-State Problems with Nuclear Magnetic Resonance

PubMed Central

Li, Zhaokai; Yung, Man-Hong; Chen, Hongwei; Lu, Dawei; Whitfield, James D.; Peng, Xinhua; Aspuru-Guzik, Alán; Du, Jiangfeng

2011-01-01

Quantum ground-state problems are computationally hard problems for general many-body Hamiltonians; there is no classical or quantum algorithm known to be able to solve them efficiently. Nevertheless, if a trial wavefunction approximating the ground state is available, as often happens for many problems in physics and chemistry, a quantum computer could employ this trial wavefunction to project the ground state by means of the phase estimation algorithm (PEA). We performed an experimental realization of this idea by implementing a variational-wavefunction approach to solve the ground-state problem of the Heisenberg spin model with an NMR quantum simulator. Our iterative phase estimation procedure yields a high accuracy for the eigenenergies (to the 10−5 decimal digit). The ground-state fidelity was distilled to be more than 80%, and the singlet-to-triplet switching near the critical field is reliably captured. This result shows that quantum simulators can better leverage classical trial wave functions than classical computers PMID:22355607

Self-consistent projection operator theory in nonlinear quantum optical systems: A case study on degenerate optical parametric oscillators

NASA Astrophysics Data System (ADS)

Degenfeld-Schonburg, Peter; Navarrete-Benlloch, Carlos; Hartmann, Michael J.

2015-05-01

Nonlinear quantum optical systems are of paramount relevance for modern quantum technologies, as well as for the study of dissipative phase transitions. Their nonlinear nature makes their theoretical study very challenging and hence they have always served as great motivation to develop new techniques for the analysis of open quantum systems. We apply the recently developed self-consistent projection operator theory to the degenerate optical parametric oscillator to exemplify its general applicability to quantum optical systems. We show that this theory provides an efficient method to calculate the full quantum state of each mode with a high degree of accuracy, even at the critical point. It is equally successful in describing both the stationary limit and the dynamics, including regions of the parameter space where the numerical integration of the full problem is significantly less efficient. We further develop a Gaussian approach consistent with our theory, which yields sensibly better results than the previous Gaussian methods developed for this system, most notably standard linearization techniques.

Black hole firewalls require huge energy of measurement

NASA Astrophysics Data System (ADS)

Hotta, Masahiro; Matsumoto, Jiro; Funo, Ken

2014-06-01

The unitary moving mirror model is one of the best quantum systems for checking the reasoning of the original firewall paradox of Almheiri et al. [J. High Energy Phys. 02 (2013) 062] in quantum black holes. Though the late-time part of radiations emitted from the mirror is fully entangled with the early part, no firewall exists with a deadly, huge average energy flux in this model. This is because the high-energy entanglement structure of the discretized systems in almost maximally entangled states is modified so as to yield the correct description of low-energy effective field theory. Furthermore, the strong subadditivity paradox of firewalls is resolved using nonlocality of general one-particle states and zero-point fluctuation entanglement. Due to the Reeh-Schlieder theorem in quantum field theory, another firewall paradox is inevitably raised with quantum remote measurements in the model. We resolve this paradox from the viewpoint of the energy cost of measurements. No firewall appears, as long as the energy for the measurement is much smaller than the ultraviolet cutoff scale.

Solvent-Controlled Synthesis of Highly Luminescent Carbon Dots with a Wide Color Gamut and Narrowed Emission Peak Widths.

PubMed

Ding, Hui; Wei, Ji-Shi; Zhang, Peng; Zhou, Zi-Yuan; Gao, Qing-Yu; Xiong, Huan-Ming

2018-05-01

Carbon dots (CDs) have tremendous potential applications in bioimaging, biomedicine, and optoelectronics. By far, it is still difficult to produce photoluminescence (PL) tunable CDs with high quantum yield (QY) across the entire visible spectrum and narrow the emission peak widths of CDs close to those of typical quantum dots. In this work, a series of CDs with tunable emission from 443 to 745 nm, quantum yield within 13-54%, and narrowed full width at half maximum (FWHM) from 108 to 55 nm, are obtained by only adjusting the reaction solvents in a one-pot solvothermal route. The distinct optical features of these CDs are based on their differences in the particle size, and the content of graphitic nitrogen and oxygen-containing functional groups, which can be modulated by controlling the dehydration and carbonization processes during solvothermal reactions. Blue, green, yellow, red, and even pure white light emitting films (Commission Internationale de L'Eclairage (CIE)= 0.33, 0.33, QY = 39%) are prepared by dispersing one or three kinds of CDs into polyvinyl alcohol with appropriate ratios. The near-infrared emissive CDs are excellent fluorescent probes for both in vitro and in vivo bioimaging because of their high QY in water, long-term stability, and low cytotoxicity. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Brightly Luminescent and Color-Tunable Colloidal CH3NH3PbX3 (X = Br, I, Cl) Quantum Dots: Potential Alternatives for Display Technology.

PubMed

Zhang, Feng; Zhong, Haizheng; Chen, Cheng; Wu, Xian-gang; Hu, Xiangmin; Huang, Hailong; Han, Junbo; Zou, Bingsuo; Dong, Yuping

2015-04-28

Organometal halide perovskites are inexpensive materials with desirable characteristics of color-tunable and narrow-band emissions for lighting and display technology, but they suffer from low photoluminescence quantum yields at low excitation fluencies. Here we developed a ligand-assisted reprecipitation strategy to fabricate brightly luminescent and color-tunable colloidal CH3NH3PbX3 (X = Br, I, Cl) quantum dots with absolute quantum yield up to 70% at room temperature and low excitation fluencies. To illustrate the photoluminescence enhancements in these quantum dots, we conducted comprehensive composition and surface characterizations and determined the time- and temperature-dependent photoluminescence spectra. Comparisons between small-sized CH3NH3PbBr3 quantum dots (average diameter 3.3 nm) and corresponding micrometer-sized bulk particles (2-8 μm) suggest that the intense increased photoluminescence quantum yield originates from the increase of exciton binding energy due to size reduction as well as proper chemical passivations of the Br-rich surface. We further demonstrated wide-color gamut white-light-emitting diodes using green emissive CH3NH3PbBr3 quantum dots and red emissive K2SiF6:Mn(4+) as color converters, providing enhanced color quality for display technology. Moreover, colloidal CH3NH3PbX3 quantum dots are expected to exhibit interesting nanoscale excitonic properties and also have other potential applications in lasers, electroluminescence devices, and optical sensors.

Structural Basis for Near Unity Quantum Yield Core/Shell Nanostructures

DOE Office of Scientific and Technical Information (OSTI.GOV)

McBride, James; Treadway, Joe; Pennycook, Stephen J

2006-01-01

Aberration-corrected Z-contrast scanning transmission electron microscopy of core/shell nanocrystals shows clear correlations between structure and quantum efficiency. Uniform shell coverage is obtained only for a graded CdS/ZnS shell material and is found to be critical to achieving near 100% quantum yield. The sublattice sensitivity of the images confirms that preferential growth takes place on the anion-terminated surfaces. This explains the three-dimensional "nanobullet" shape observed in the case of core/shell nanorods.

Nanostructured organosilicon luminophores as a new concept of nanomaterials for highly efficient down-conversion of light

NASA Astrophysics Data System (ADS)

Ponomarenko, Sergey A.; Surin, Nikolay M.; Borshchev, Oleg V.; Skorotetcky, Maxim S.; Muzafarov, Aziz M.

2015-10-01

Nanostructured organosilicon luminophores (NOLs) are branched molecular structures having two types of covalently bonded via silicon atoms organic luminophores with efficient Förster energy transfer between them. They combine the best properties of organic luminophores and inorganic quantum dots: high absorption cross-section, excellent photoluminescence quantum yield, fast luminescence decay time, good processability and low toxicity. A smart choice of organic luminophores allowed us to design and synthesize a library of NOLs, absorbing from VUV to visible region and emitting at the desired wavelengths from 390 to 650 nm. They can be used as unique wavelength shifters in plastic scintillators and other applications.

Experimental observation of four-photon entangled Dicke state with high fidelity.

PubMed

Kiesel, N; Schmid, C; Tóth, G; Solano, E; Weinfurter, H

2007-02-09

We present the experimental observation of the symmetric four-photon entangled Dicke state with two excitations |D_{4};{(2)}. A simple experimental setup allowed quantum state tomography yielding a fidelity as high as 0.844+/-0.008. We study the entanglement persistency of the state using novel witness operators and focus on the demonstration of a remarkable property: depending on the orientation of a measurement on one photon, the remaining three photons are projected into both inequivalent classes of genuine tripartite entanglement, the Greenberger-Horne-Zeilinger and W class. Furthermore, we discuss possible applications of |D_{4};{(2)} in quantum communication.

Extremely low amplified spontaneous emission threshold and blue electroluminescence from a spin-coated octafluorene neat film

NASA Astrophysics Data System (ADS)

Kim, D.-H.; Sandanayaka, A. S. D.; Zhao, L.; Pitrat, D.; Mulatier, J. C.; Matsushima, T.; Andraud, C.; Ribierre, J. C.; Adachi, C.

2017-01-01

We report on the photophysical, amplified spontaneous emission (ASE), and electroluminescence properties of a blue-emitting octafluorene derivative in spin-coated films. The neat film shows an extremely low ASE threshold of 90 nJ/cm2, which is related to its high photoluminescence quantum yield of 87% and its large radiative decay rate of 1.7 × 109 s-1. Low-threshold organic distributed feedback semiconductor lasers and fluorescent organic light-emitting diodes with a maximum external quantum efficiency as high as 4.4% are then demonstrated, providing evidence that this octafluorene derivative is a promising candidate for organic laser applications.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chen Lin; Chen Yixin

We show that no universal quantum cloning machine exists that can broadcast an arbitrary mixed qubit with a constant fidelity. Based on this result, we investigate the dependent quantum cloner in the sense that some parameter of the input qubit {rho}{sub s}({theta},{omega},{lambda}) is regarded as constant in the fidelity. For the case of constant {omega}, we establish the 1{yields}2 optimal symmetric dependent cloner with a fidelity 1/2. It is also shown that the 1{yields}M optimal quantum cloning machine for pure qubits is also optimal for mixed qubits, when {lambda} is the unique parameter in the fidelity. For general N{yields}M broadcastingmore » of mixed qubits, the situation is very different.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bisio, Alessandro; D'Ariano, Giacomo Mauro; Perinotti, Paolo

We analyze quantum algorithms for cloning of a quantum measurement. Our aim is to mimic two uses of a device performing an unknown von Neumann measurement with a single use of the device. When the unknown device has to be used before the bipartite state to be measured is available we talk about 1{yields}2 learning of the measurement, otherwise the task is called 1{yields}2 cloning of a measurement. We perform the optimization for both learning and cloning for arbitrary dimension d of the Hilbert space. For 1{yields}2 cloning we also propose a simple quantum network that achieves the optimal fidelity.more » The optimal fidelity for 1{yields}2 learning just slightly outperforms the estimate and prepare strategy in which one first estimates the unknown measurement and depending on the result suitably prepares the duplicate.« less

Highly Efficient Carbon Dots with Reversibly Switchable Green-Red Emissions for Trichromatic White Light-Emitting Diodes.

PubMed

Yuan, Biao; Guan, Shanyue; Sun, Xingming; Li, Xiaoming; Zeng, Haibo; Xie, Zheng; Chen, Ping; Zhou, Shuyun

2018-05-09

Carbon dots (CDs) have potentials to be utilized in optoelectronic devices, bioimaging, and photocatalysis. The majority of the current CDs with high quantum yield to date were limited in the blue light emission region. Herein, on the basis of surface electron-state engineering, we report a kind of CDs with reversible switching ability between green and red photoluminescence with a quantum yield (QY) of both up to 80%. Highly efficient green and red solid-state luminescence is realized by doping CDs into a highly transparent matrix of methyltriethoxysilane and 3-triethoxysilylpropylamine to form CDs/gel glasses composites with QYs of 80 and 78%. The CDs/gel glasses show better transmittance in visible light bands and excellent thermal stability. A blue-pumped CDs/gel glasses phosphor-based trichromatic white light-emitting diode (WLED) is realized, whose color rendering index is 92.9. The WLED gets the highest luminous efficiency of 71.75 lm W -1 in CDs-based trichromatic WLEDs. This work opens a door for developing highly efficient green- and red-emissive switching CDs which were used as phosphors for WLEDs and have the tendency for applications in other fields, such as sensing, bioimaging, and photocatalysis.

Growth of Nanosized Single Crystals for Efficient Perovskite Light-Emitting Diodes.

PubMed

Lee, Seungjin; Park, Jong Hyun; Nam, Yun Seok; Lee, Bo Ram; Zhao, Baodan; Di Nuzzo, Daniele; Jung, Eui Dae; Jeon, Hansol; Kim, Ju-Young; Jeong, Hu Young; Friend, Richard H; Song, Myoung Hoon

2018-04-24

Organic-inorganic hybrid perovskites are emerging as promising emitting materials due to their narrow full-width at half-maximum emissions, color tunability, and high photoluminescence quantum yields (PLQYs). However, the thermal generation of free charges at room temperature results in a low radiative recombination rate and an excitation-intensity-dependent PLQY, which is associated with the trap density. Here, we report perovskite films composed of uniform nanosized single crystals (average diameter = 31.7 nm) produced by introducing bulky amine ligands and performing the growth at a lower temperature. By effectively controlling the crystal growth, we maximized the radiative bimolecular recombination yield by reducing the trap density and spatially confining the charges. Finally, highly bright and efficient green emissive perovskite light-emitting diodes that do not suffer from electroluminescence blinking were achieved with a luminance of up to 55 400 cd m -2 , current efficiency of 55.2 cd A -1 , and external quantum efficiency of 12.1%.

Substituent effect on photophysical properties of bi-1,3,4-oxadiazole derivatives in solution

NASA Astrophysics Data System (ADS)

Chen, Fangyi; Tian, Taiji; Zhao, Chengxiao; Bai, Binglian; Li, Min; Wang, Haitao

2016-04-01

A series of phenyl substituted bi-1,3,4-oxadiazole derivatives were designed and synthesized; the effect of substituent on the photophysical properties and molecular electronic structures was fully studied by the combination of experimental techniques and theoretical calculations. Compared to parent compound without any substituent (BOXD), fluoro-substituent shows little effect on the absorption and emission spectra, whilst a little larger spectral red-shift could be observed for methoxy-, nitro-substituted derivatives and thienyl-substituted bi-1,3,4-oxadiazole (TBOXD). These spectral changes can be well explained by theoretically calculated HOMO and LUMO energy level changes. All these molecules show high fluorescence quantum yield except for nitro-substituted derivative in dilute solutions. The quantum yield of BOXD changes with the concentration and exhibits a high value at the concentrated solution. This work revealed the influence of substituent on the photophysical properties of bi-1,3,4-oxadizaole derivatives in dilute solutions and provided guidance for designing molecules with potential application.

Arene-Inserted Extended Germa[n]pericyclynes: Synthesis, Structure, and Phosphorescence Properties.

PubMed

Tanimoto, Hiroki; Mori, Junta; Ito, Shunichiro; Nishiyama, Yasuhiro; Morimoto, Tsumoru; Tanaka, Kazuo; Chujo, Yoshiki; Kakiuchi, Kiyomi

2017-07-26

This report describes the synthesis and characterization of arene-inserted extended (ArEx) germa[n]pericyclynes composed of germanium and 1,4-diethynylbenzene units. These novel cyclic germanium-π unit materials were synthesized with diethynylbenzene and germanium dichloride. X-ray crystallographic analysis revealed their structures, and the planar conformation of ArEx germa[4]pericyclyne along with the regular aromatic rings. UV/Vis absorption spectra and fluorescence emission spectra showed considerably unique and highly improved character compared to previously reported germa[n]pericyclynes. Even in the absence of transition metal components, phosphorescence emissions were observed, and the emission lifetimes were dramatically improved. ArEx germa[n]pericyclynes showed high photoluminescence quantum yields, whereas low photoluminescence quantum yields were observed for acyclic compounds. Density functional theory calculations show delocalized orbitals between skipped alkyne units through a germanium tether, and an increase in the HOMO energy level, leading to a small HOMO-LUMO energy gap. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Double labelling of intracellular mitochondria and nucleolus using thiophene pyridium salt with high quantum yield as biosensor and its application in stimulated emission depletion nanoscopy.

PubMed

Tian, Xiaohe; Wang, Hui; Zhang, Qiong; Zhang, Mingzhu; Zhu, Yingzhong; Chen, Yan; Wu, Jieying; Tian, Yupeng

2018-05-30

Probe for dual-site target distinct subcellular compartments from cytosol and nucleus is an attractive approach, however, which was scarcely reported. Herein, a series of small-molecular thiophene pyridium salt derivatives (MitoNuc1-4) possessing water-soluble, high quantum yield and two-photon activity were rationally designed, and their structures were crystallographic confirmed. Systematic photophysical and biological imaging property investigations were carried out for them. It was found that MitoNuc1-4 exhibit two-photon absorption properties in the near infrared region, and MitoNuc1 has membrane permeability and cationic nature, rendering it to be double labelling of mitochondria and nucleolus in living cells with superb photo-stability and non-invasiveness. It also demonstrated that MitoNuc1 in living cells can monitor mitochondrial division in real time and revealed nucleolar ultrastructure under stimulated emission depletion nanoscopy. Copyright © 2017 Elsevier B.V. All rights reserved.

Fluctuations in coral health of four common inshore reef corals in response to seasonal and anthropogenic changes in water quality.

PubMed

Browne, Nicola K; Tay, Jason K L; Low, Jeffrey; Larson, Ole; Todd, Peter A

2015-04-01

Environmental drivers of coral condition (maximum quantum yield, symbiont density, chlorophyll a content and coral skeletal growth rates) were assessed in the equatorial inshore coastal waters of Singapore, where the amplitude of seasonal variation is low, but anthropogenic influence is relatively high. Water quality variables (sediments, nutrients, trace metals, temperature, light) explained between 52 and 83% of the variation in coral condition, with sediments and light availability as key drivers of foliose corals (Merulina ampliata, Pachyseris speciosa), and temperature exerting a greater influence on a branching coral (Pocillopora damicornis). Seasonal reductions in water quality led to high chlorophyll a concentrations and maximum quantum yields in corals, but low growth rates. These marginal coral communities are potentially vulnerable to climate change, hence, we propose water quality thresholds for coral growth with the aim of mitigating both local and global environmental impacts. Copyright © 2015 Elsevier Ltd. All rights reserved.

Synthesis and spectral characterization of environmentally responsive fluorescent deoxycytidine analogs

PubMed Central

Elmehriki, Adam AH; Suchý, Mojmír; Chicas, Kirby J; Wojciechowski, Filip; Hudson, Robert HE

2014-01-01

Herein, we describe the synthesis and spectroscopic properties of five novel pyrrolodeoxycytidine analogs, and the related 5-(1-pyrenylethynyl)-2’-deoxycytidine analog; as well as fluorescence characterization of 5-(p-methoxyphenylethynyl)-2’-deoxyuridine. Within this series of compounds, rigidification of the structure from 6-phenylpyrrolodeoxycytidine to 5,6-benzopyrroldeoxycytidine made remarkable improvement of the fluorescence quantum yield (Φ ~1, EtOH) and substantially increased the Stokes shift. Exchange of the phenyl group of 6-phenylpyrrolodeoxycytidine for other heterocycles (benzofuryl or indolyl) produced an increase in the extinction coefficient at the excitation wavelength while preserving high quantum yields. The steady-state fluorescence response to the environment was determined by sensitivity of Stokes shift to solvent polarity. The effect of solvent polarity on fluorescence emission intensity was concurrently examined and showed that 5,6-benzopyrrolodeoxycytidine is highly sensitive to the presence of water. On the other hand, the previously synthesized 5-(p-methoxyphenylethynyl)-2’-deoxyuridine was found to be sensitive to solvent viscosity indicating molecular rotor behavior. PMID:25483932

Influence of quantum dot's quantum yield to chemiluminescent resonance energy transfer.

PubMed

Wang, Hai-Qiao; Li, Yong-Qiang; Wang, Jian-Hao; Xu, Qiao; Li, Xiu-Qing; Zhao, Yuan-Di

2008-03-03

The resonance energy transfer between chemiluminescence donor (luminol-H2O2 system) and quantum dots (QDs, emission at 593 nm) acceptors (CRET) was investigated. The resonance energy transfer efficiencies were compared while the oil soluble QDs, water soluble QDs (modified with thioglycolate) and QD-HRP conjugates were used as acceptor. The fluorescence of QD can be observed in the three cases, indicating that the CRET occurs while QD acceptor in different status was used. The highest CRET efficiency (10.7%) was obtained in the case of oil soluble QDs, and the lowest CRET efficiency (2.7%) was observed in the QD-HRP conjugates case. This result is coincident with the quantum yields of the acceptors (18.3% and 0.4%). The same result was observed in another similar set of experiment, in which the amphiphilic polymer modified QDs (emission at 675 nm) were used. It suggests that the quantum yield of the QD in different status is the crucial factor to the CRET efficiency. Furthermore, the multiplexed CRET between luminol donor and three different sizes QD acceptors was observed simultaneously. This work will offer useful support for improving the CRET studies based on quantum dots.

The Effect of Correlated Energetic Disorder on Charge Transport in Organic Semiconductors

NASA Astrophysics Data System (ADS)

Allen, Jonathan; Röding, Sebastian; Cherqui, Charles; Dunlap, David

2012-10-01

In their 1995 paper describing a Monte Carlo simulation for dissociation of an electron-hole pair in the presence of Gaussian energetic disorder, Albrect and Bäassler reported a surprising result. They found that increasing the width σ of the energetic disorder increases the quantum yield φ. They attributed this behavior to the tendency for energy fluctuations to compete against the Coulombic pair attraction, driving the electron-hole pair apart at short distances where, without disorder, recombination would be almost certain. We have expanded upon this notion, and introduced spatial correlation into the energetic disorder. By correlating the energetic disorder, we have demonstrated even larger quantum yields in simulation, attributable to the tendency of correlation to drive the charges further apart spatially than merely random disorder. Our results generally support the findings of Greenham et al. in that a larger correlation radius gives a larger quantum yield. In addition to larger quantum yield, we believe that correlated disorder could be used to create pathways for charge transport within a material, allowing the charge carrier behavior to be tuned.

A highly fluorescent hydrophilic ionic liquid as a potential probe for the sensing of biomacromolecules.

PubMed

Chen, Xu-Wei; Liu, Jia-Wei; Wang, Jian-Hua

2011-02-17

With respect to the conventional imidazolium ionic liquids which generally create very weak fluorescence with quantum yields at extremely low levels of 0.005-0.02, a symmetrical hydrophilic ionic liquid 1,3-butylimidazolium chloride (BBimCl) was found to be highly fluorescent with λ(em) at 388 nm when excited at λ(ex) < 340 nm. The very high quantum yield of BBimCl in aqueous medium, derived to be 0.523 when excited at 315 nm, was attributed to its symmetrical plane conjugating structure. In the presence of hemoglobin, the fluorescence of BBimCl could be significantly quenched, resulting from the coordinating interaction between the iron atom in the heme group of hemoglobin and the cationic imidazolium moiety. This feature of the present hydrophilic ionic liquid makes it a promising fluorescence probe candidate for the sensitive sensing of hemoglobin. A linear regression was observed within 3 × 10(-7) to 5 × 10(-6) mol L(-1) for hemoglobin, and a detection limit of 7.3 × 10(-8) mol L(-1) was derived.

Probing quantum Hall states with single-electron transistors at high magnetic fields

NASA Astrophysics Data System (ADS)

Gustafsson, Martin; Yankowitz, Matthew; Forsythe, Carlos; Zhu, Xiaoyang; Dean, Cory

The sequence of fractional quantum Hall states in graphene is not yet fully understood, largely due to disorder-induced limitations of conventional transport studies. Measurements of magnetotransport in other 2D crystals are further complicated by the difficulties in making ohmic contact to the materials. On the other hand, bulk electronic compressibility can provide clear signatures of the integer and fractional quantum Hall effects, does not require ohmic contact, and can be localized to regions of low disorder. The single-electron transistor (SET) is a suitable tool for such experiments due to its small size and high charge sensitivity, which allow electric fields penetrating the 2D electron system to be detected locally and with high fidelity. Here we report studies of exfoliated 2D van der Waals materials fully encapsulated in flakes of hexagonal boron nitride. SETs are fabricated lithographically on top of the encapsulation, yielding a structure which lends itself to experiments at high electric and magnetic fields. We demonstrate the method on monolayer graphene, where we observe fractional quantum Hall states at all filling factors ν = n / 3 up to n = 17 and extract their associated energy gaps for magnetic fields up to 31 tesla.

Effects of concentrations of sodium chloride on photosynthesis, antioxidative enzymes, growth and fiber yield of hybrid ramie.

PubMed

Huang, Chengjian; Wei, Gang; Jie, Yucheng; Wang, Longchang; Zhou, Hangfei; Ran, Chunyan; Huang, Zaocun; Jia, Huijuan; Anjum, Shakeel Ahmad

2014-03-01

Ramie (Boehmeria nivea L.) is one of the oldest and most important fiber crops in China due to the comfortable textile of its fine fiber. Increased ramie fiber demand brings ramie cultivation to salt-affected regions. The aim of this research was to determine morphological, physiological and biochemical responses of ramie by subjecting plants to varying concentrations of NaCl (0, 2, 4, 6 and 8 g NaCl/kg dry soil) at vigorous growth stage for 10 and 20 days. Results indicated that salinity stress substantially inhibited the growth of hybrid ramie plants and led to remarkable decline in fiber yield. However, when grown at 2 g NaCl/kg growth and fiber yield were similar to non-saline control. In addition, chlorophyll fluorescence and gas exchange parameters were correlated with growth and yield response. Salt treatments promoted a subsequent decrease in maximum quantum efficiency of PSII photochemistry (Fv/Fm), quantum efficiency of open PSII reaction centers (Fv'/Fm') and quantum yield of PSII (φPSII) while non-photochemical quenching (NPQ) changed conversely. Photochemical quenching (qP) and electron transport rate of PSII (ETR) increased at 2 and 4 g NaCl/kg then decreased at 6 and 8 g NaCl/kg. Substantial decline in the PSII activity at high salinity was associated with the loss of chlorophyll contents. Moreover, marked decrease in net photosynthetic rate (A), transpiration rate (E), stomatal conductance (gs) was also recorded. Nonetheless, intercellular CO2 (Ci) decreased at low salt stress, subsequently increased at high salt stress while water use efficiency (WUE) and instantaneous water use efficiency (WUEi) altered in opposite direction. Substantial decrease of photosynthesis at high salinity was due to non-stomatal factors. Furthermore, salinity stress led to decrease of proteins and accumulation of proline and malondialdehyde (MDA), as well as enhanced activities of superoxide dismutase (SOD, EC 1.15.1.1) and peroxidase (POD, EC 1.11.1.6), whereas, catalase (CAT, EC 1.11.1.7) enhanced at low salinity, decreased at high salinity. Nonetheless, these changes were closely related with the severity and duration of the salinity stress and their interaction. The results suggested a certain tolerance to salinity stress for hybrid ramie. This meets the essential condition for utilization in salinity-prone environments. Copyright © 2014 Elsevier Masson SAS. All rights reserved.

Measurement of fluorophore concentrations and fluorescence quantum yield in tissue-simulating phantoms using three diffusion models of steady-state spatially resolved fluorescence.

PubMed

Diamond, Kevin R; Farrell, Thomas J; Patterson, Michael S

2003-12-21

Steady-state diffusion theory models of fluorescence in tissue have been investigated for recovering fluorophore concentrations and fluorescence quantum yield. Spatially resolved fluorescence, excitation and emission reflectance Carlo simulations, and measured using a multi-fibre probe on tissue-simulating phantoms containing either aluminium phthalocyanine tetrasulfonate (AlPcS4), Photofrin meso-tetra-(4-sulfonatophenyl)-porphine dihydrochloride The accuracy of the fluorophore concentration and fluorescence quantum yield recovered by three different models of spatially resolved fluorescence were compared. The models were based on: (a) weighted difference of the excitation and emission reflectance, (b) fluorescence due to a point excitation source or (c) fluorescence due to a pencil beam excitation source. When literature values for the fluorescence quantum yield were used for each of the fluorophores, the fluorophore absorption coefficient (and hence concentration) at the excitation wavelength (mu(a,x,f)) was recovered with a root-mean-square accuracy of 11.4% using the point source model of fluorescence and 8.0% using the more complicated pencil beam excitation model. The accuracy was calculated over a broad range of optical properties and fluorophore concentrations. The weighted difference of reflectance model performed poorly, with a root-mean-square error in concentration of about 50%. Monte Carlo simulations suggest that there are some situations where the weighted difference of reflectance is as accurate as the other two models, although this was not confirmed experimentally. Estimates of the fluorescence quantum yield in multiple scattering media were also made by determining mu(a,x,f) independently from the fitted absorption spectrum and applying the various diffusion theory models. The fluorescence quantum yields for AlPcS4 and TPPS4 were calculated to be 0.59 +/- 0.03 and 0.121 +/- 0.001 respectively using the point source model, and 0.63 +/- 0.03 and 0.129 +/- 0.002 using the pencil beam excitation model. These results are consistent with published values.

Accuracy of quantum sensors measuring yield photon flux and photosynthetic photon flux

NASA Technical Reports Server (NTRS)

Barnes, C.; Tibbitts, T.; Sager, J.; Deitzer, G.; Bubenheim, D.; Koerner, G.; Bugbee, B.; Knott, W. M. (Principal Investigator)

1993-01-01

Photosynthesis is fundamentally driven by photon flux rather than energy flux, but not all absorbed photons yield equal amounts of photosynthesis. Thus, two measures of photosynthetically active radiation have emerged: photosynthetic photon flux (PPF), which values all photons from 400 to 700 nm equally, and yield photon flux (YPF), which weights photons in the range from 360 to 760 nm according to plant photosynthetic response. We selected seven common radiation sources and measured YPF and PPF from each source with a spectroradiometer. We then compared these measurements with measurements from three quantum sensors designed to measure YPF, and from six quantum sensors designed to measure PPF. There were few differences among sensors within a group (usually <5%), but YPF values from sensors were consistently lower (3% to 20%) than YPF values calculated from spectroradiometric measurements. Quantum sensor measurements of PPF also were consistently lower than PPF values calculated from spectroradiometric measurements, but the differences were <7% for all sources, except red-light-emitting diodes. The sensors were most accurate for broad-band sources and least accurate for narrow-band sources. According to spectroradiometric measurements, YPF sensors were significantly less accurate (>9% difference) than PPF sensors under metal halide, high-pressure sodium, and low-pressure sodium lamps. Both sensor types were inaccurate (>18% error) under red-light-emitting diodes. Because both YPF and PPF sensors are imperfect integrators, and because spectroradiometers can measure photosynthetically active radiation much more accurately, researchers should consider developing calibration factors from spectroradiometric data for some specific radiation sources to improve the accuracy of integrating sensors.

Cooperating or fighting with control noise in the optimal manipulation of quantum dynamics

NASA Astrophysics Data System (ADS)

Shuang, Feng; Rabitz, Herschel

2004-11-01

This paper investigates the impact of control field noise on the optimal manipulation of quantum dynamics. Simulations are performed on several multilevel quantum systems with the goal of population transfer in the presence of significant control noise. The noise enters as run-to-run variations in the control amplitude and phase with the observation being an ensemble average over many runs as is commonly done in the laboratory. A genetic algorithm with an improved elitism operator is used to find the optimal field that either fights against or cooperates with control field noise. When seeking a high control yield it is possible to find fields that successfully fight with the noise while attaining good quality stable results. When seeking modest control yields, fields can be found which are optimally shaped to cooperate with the noise and thereby drive the dynamics more efficiently. In general, noise reduces the coherence of the dynamics, but the results indicate that population transfer objectives can be met by appropriately either fighting or cooperating with noise, even when it is intense.

Cooperating or fighting with control noise in the optimal manipulation of quantum dynamics.

PubMed

Shuang, Feng; Rabitz, Herschel

2004-11-15

This paper investigates the impact of control field noise on the optimal manipulation of quantum dynamics. Simulations are performed on several multilevel quantum systems with the goal of population transfer in the presence of significant control noise. The noise enters as run-to-run variations in the control amplitude and phase with the observation being an ensemble average over many runs as is commonly done in the laboratory. A genetic algorithm with an improved elitism operator is used to find the optimal field that either fights against or cooperates with control field noise. When seeking a high control yield it is possible to find fields that successfully fight with the noise while attaining good quality stable results. When seeking modest control yields, fields can be found which are optimally shaped to cooperate with the noise and thereby drive the dynamics more efficiently. In general, noise reduces the coherence of the dynamics, but the results indicate that population transfer objectives can be met by appropriately either fighting or cooperating with noise, even when it is intense.

Controllable synthesis of dual emissive Ag:InP/ZnS quantum dots with high fluorescence quantum yield

NASA Astrophysics Data System (ADS)

Yang, Wu; He, Guoxing; Mei, Shiliang; Zhu, Jiatao; Zhang, Wanlu; Chen, Qiuhang; Zhang, Guilin; Guo, Ruiqian

2017-11-01

Dual emissive Cd-free quantum dots (QDs) are in great demand for various applications. However, their synthesis has been faced with challenges. Here, we demonstrate the dual emissive Ag:InP/ZnS core/shell QDs with the excellent photoluminescence quantum yield (PL QY) up to 75% and their PL dependence on the reaction temperature, reaction time, the different ZnX2 (X = I, Cl, and Br) precursors, the ratio of In/Zn and the Ag dopant concentration. The as-prepared Ag:InP/ZnS QDs exhibit dual emission with one peak position of about 492 nm owing to the intrinsic emission, and the other peak position of about 575 nm resulting from Ag-doped emission. These dual emissive QDs are integrated with the commercial GaN-based blue LEDs, and the simulation results show that the Ag:InP/ZnS QDs-based white LEDs could realize bright natural white-lights with the luminous efficacy (LE) of 94.2-98.4 lm/W, the color rendering index (CRI) of 82-83 and the color quality scale (CQS) of 82-83 at different correlated color temperatures (CCT). This unique combination of the above properties makes this new class of dual emissive QDs attractive for white LED applications.

Cryogenic on-chip multiplexer for the study of quantum transport in 256 split-gate devices

NASA Astrophysics Data System (ADS)

Al-Taie, H.; Smith, L. W.; Xu, B.; See, P.; Griffiths, J. P.; Beere, H. E.; Jones, G. A. C.; Ritchie, D. A.; Kelly, M. J.; Smith, C. G.

2013-06-01

We present a multiplexing scheme for the measurement of large numbers of mesoscopic devices in cryogenic systems. The multiplexer is used to contact an array of 256 split gates on a GaAs/AlGaAs heterostructure, in which each split gate can be measured individually. The low-temperature conductance of split-gate devices is governed by quantum mechanics, leading to the appearance of conductance plateaux at intervals of 2e2/h. A fabrication-limited yield of 94% is achieved for the array, and a "quantum yield" is also defined, to account for disorder affecting the quantum behaviour of the devices. The quantum yield rose from 55% to 86% after illuminating the sample, explained by the corresponding increase in carrier density and mobility of the two-dimensional electron gas. The multiplexer is a scalable architecture, and can be extended to other forms of mesoscopic devices. It overcomes previous limits on the number of devices that can be fabricated on a single chip due to the number of electrical contacts available, without the need to alter existing experimental set ups.

Absorption and emission behaviour of trans- p-coumaric acid in aqueous solutions and some organic solvents

NASA Astrophysics Data System (ADS)

Putschögl, M.; Zirak, P.; Penzkofer, A.

2008-01-01

The absorption and fluorescence behaviour of trans- p-coumaric acid ( trans-4-hydroxycinnamic acid) is investigated in buffered aqueous solution over a wide range from pH 1 to pH 12, in un-buffered water, and in some organic solvents. Absorption cross-section spectra, fluorescence quantum distributions, fluorescence quantum yields, and degrees of fluorescence polarisation are measured. p-Coumaric acid exists in different ionic forms in aqueous solution depending on the pH. There is an equilibrium between the neutral form ( p-CAH 2) and the single anionic form ( p-CAH -) at low pH (p Kna ≈ 4.9), and between the single anionic and the double anionic form ( p-CA 2-) at high pH (p Kaa ≈ 9.35). In the organic solvents studied trans- p-coumaric acid is dissolved in its neutral form. The fluorescence quantum yield of trans- p-coumaric acid in aqueous solution is ϕF ≈ 1.4 × 10 -4 for the neutral and the single anionic form, while it is ϕF ≈ 1.3 × 10 -3 for the double anionic form. For trans- p-coumaric acid in organic solvents fluorescence quantum yields in the range from 4.8 × 10 -5 (acetonitrile) to 1.5 × 10 -4 (glycerol) were measured. The fluorescence spectra are 7700-10,000 cm -1 Stokes shifted in aqueous solution, and 5400-8200 cm -1 Stokes shifted in the studied organic solvents. Decay paths responsible for the low fluorescence quantum yields are discussed (photo-isomerisation and internal conversion for p-CA 2-, solvent-assisted intra-molecular charge-transfer or ππ ∗ to nπ ∗ transfer and internal conversion for p-CAH 2 and p-CAH -). The solvent dependence of the first ππ ∗ electronic transition frequency and of the fluorescence Stokes shift of p-CAH 2 is discussed in terms of polar solute-solvent interaction effects. Thereby the ground-state and excite-state molecular dipole moments are extracted.

Rigidifying fluorescent linkers by metal-organic framework formation for fluorescence blue shift and quantum yield enhancement.

PubMed

Wei, Zhangwen; Gu, Zhi-Yuan; Arvapally, Ravi K; Chen, Ying-Pin; McDougald, Roy N; Ivy, Joshua F; Yakovenko, Andrey A; Feng, Dawei; Omary, Mohammad A; Zhou, Hong-Cai

2014-06-11

We demonstrate that rigidifying the structure of fluorescent linkers by structurally constraining them in metal-organic frameworks (MOFs) to control their conformation effectively tunes the fluorescence energy and enhances the quantum yield. Thus, a new tetraphenylethylene-based zirconium MOF exhibits a deep-blue fluorescent emission at 470 nm with a unity quantum yield (99.9 ± 0.5%) under Ar, representing ca. 3600 cm(-1) blue shift and doubled radiative decay efficiency vs the linker precursor. An anomalous increase in the fluorescence lifetime and relative intensity takes place upon heating the solid MOF from cryogenic to ambient temperatures. The origin of these unusual photoluminescence properties is attributed to twisted linker conformation, intramolecular hindrance, and framework rigidity.

The reaction of NH2 with NO2

NASA Technical Reports Server (NTRS)

Jayanty, R. K. M.; Simonaitis, R.; Heicklen, J.

1976-01-01

Ammonia (NH3) was photolyzed at 213.9 nm in the presence of NO2 at 25 C in order to study the reactions of NH2 with NO2. The products included NO, with a quantum yield of 1.0. The other measured products of the reaction were N2 and N2O with respective quantum yields of 0.94 plus or minus 0.10 and 0.3 in the presence of small amounts of He and 0.65 plus or minus 0.15 and 0.13 in the presence of a large excess of He. The quantum yield for NO2 consumption was 6.0 plus or minus 2.0 in the absence of He. These results are explained in terms of various reactions.

Deterministic quantum teleportation with atoms.

PubMed

Riebe, M; Häffner, H; Roos, C F; Hänsel, W; Benhelm, J; Lancaster, G P T; Körber, T W; Becher, C; Schmidt-Kaler, F; James, D F V; Blatt, R

2004-06-17

Teleportation of a quantum state encompasses the complete transfer of information from one particle to another. The complete specification of the quantum state of a system generally requires an infinite amount of information, even for simple two-level systems (qubits). Moreover, the principles of quantum mechanics dictate that any measurement on a system immediately alters its state, while yielding at most one bit of information. The transfer of a state from one system to another (by performing measurements on the first and operations on the second) might therefore appear impossible. However, it has been shown that the entangling properties of quantum mechanics, in combination with classical communication, allow quantum-state teleportation to be performed. Teleportation using pairs of entangled photons has been demonstrated, but such techniques are probabilistic, requiring post-selection of measured photons. Here, we report deterministic quantum-state teleportation between a pair of trapped calcium ions. Following closely the original proposal, we create a highly entangled pair of ions and perform a complete Bell-state measurement involving one ion from this pair and a third source ion. State reconstruction conditioned on this measurement is then performed on the other half of the entangled pair. The measured fidelity is 75%, demonstrating unequivocally the quantum nature of the process.

Photoinhibition of Photosystems I and II Using Chlorophyll Fluorescence Measurements

ERIC Educational Resources Information Center

Quiles, Maria Jose

2005-01-01

In this study the photoinhibition of photosystems (PS) I and II caused by exposure to high intensity light in oat ("Avena sativa," var Prevision) is measured by the emission of chlorophyll fluorescence in intact leaves adapted to darkness. The maximal quantum yield of PS II was lower in plants grown under high light intensity than in plants grown…

A single thiazole orange molecule forms an exciplex in a DNA i-motif.

PubMed

Xu, Baochang; Wu, Xiangyang; Yeow, Edwin K L; Shao, Fangwei

2014-06-18

A fluorescent exciplex of thiazole orange (TO) is formed in a single-dye conjugated DNA i-motif. The exciplex fluorescence exhibits a large Stokes shift, high quantum yield, robust response to pH oscillation and little structural disturbance to the DNA quadruplex, which can be used to monitor the folding of high-order DNA structures.

One-pot synthesis of highly luminescent InP/ZnS nanocrystals without precursor injection.

PubMed

Li, Liang; Reiss, Peter

2008-09-03

InP/ZnS core/shell nanocrystals are prepared using a single-step heating-up method relying on the difference in reactivity of the applied InP and ZnS precursors. The obtained particles exhibit size-dependent emission in the range of 480-590 nm, a fluorescence quantum yield of 50-70%, and high photostability.

Diboron compound-based organic light-emitting diodes with high efficiency and reduced efficiency roll-off

NASA Astrophysics Data System (ADS)

Wu, Tien-Lin; Huang, Min-Jie; Lin, Chih-Chun; Huang, Pei-Yun; Chou, Tsu-Yu; Chen-Cheng, Ren-Wu; Lin, Hao-Wu; Liu, Rai-Shung; Cheng, Chien-Hong

2018-04-01

Organic light-emitting diodes (OLEDs) based on thermally activated delayed fluorescence (TADF) materials are promising for the realization of highly efficient light emitters. However, such devices have so far suffered from efficiency roll-off at high luminance. Here, we report the design and synthesis of two diboron-based molecules, CzDBA and tBuCzDBA, which show excellent TADF properties and yield efficient OLEDs with very low efficiency roll-off. These donor-acceptor-donor (D-A-D) type and rod-like compounds concurrently generate TADF with a photoluminescence quantum yield of 100% and an 84% horizontal dipole ratio in the thin film. A green OLED based on CzDBA exhibits a high external quantum efficiency of 37.8 ± 0.6%, a current efficiency of 139.6 ± 2.8 cd A-1 and a power efficiency of 121.6 ± 3.1 lm W-1 with an efficiency roll-off of only 0.3% at 1,000 cd m-2. The device has a peak emission wavelength of 528 nm and colour coordinates of the Commission International de ĺEclairage (CIE) of (0.31, 0.61), making it attractive for colour-display applications.

AgCl-doped CdSe quantum dots with near-IR photoluminescence.

PubMed

Kotin, Pavel Aleksandrovich; Bubenov, Sergey Sergeevich; Mordvinova, Natalia Evgenievna; Dorofeev, Sergey Gennadievich

2017-01-01

We report the synthesis of colloidal CdSe quantum dots doped with a novel Ag precursor: AgCl. The addition of AgCl causes dramatic changes in the morphology of synthesized nanocrystals from spherical nanoparticles to tetrapods and finally to large ellipsoidal nanoparticles. Ellipsoidal nanoparticles possess an intensive near-IR photoluminescence ranging up to 0.9 eV (ca. 1400 nm). In this article, we explain the reasons for the formation of the ellipsoidal nanoparticles as well as the peculiarities of the process. The structure, Ag content, and optical properties of quantum dots are also investigated. The optimal conditions for maximizing both the reaction yield and IR photoluminescence quantum yield are found.

Structural control of InP/ZnS core/shell quantum dots enables high-quality white LEDs.

PubMed

Kumar, Baskaran Ganesh; Sadeghi, Sadra; Melikov, Rustamzhon; Aria, Mohammad Mohammadi; Jalali, Houman Bahmani; Ow-Yang, Cleva W; Nizamoglu, Sedat

2018-08-24

Herein, we demonstrate that the structural and optical control of InP-based quantum dots (QDs) can lead to high-performance light-emitting diodes (LEDs). Zinc sulphide (ZnS) shells passivate the InP QD core and increase the quantum yield in green-emitting QDs by 13-fold and red-emitting QDs by 8-fold. The optimised QDs are integrated in the liquid state to eliminate aggregation-induced emission quenching and we fabricated white LEDs with a warm, neutral and cool-white appearance by the down-conversion mechanism. The QD-functionalized white LEDs achieve luminous efficiency (LE) up to 14.7 lm W -1 and colour-rendering index up to 80. The structural and optical control of InP/ZnS core/shell QDs enable 23-fold enhancement in LE of white LEDs compared to ones containing only QDs of InP core.

Highly luminescent S,N co-doped carbon quantum dots-sensitized chemiluminescence on luminol-H2 O2 system for the determination of ranitidine.

PubMed

Chen, Jianqiu; Shu, Juan; Chen, Jiao; Cao, Zhiran; Xiao, An; Yan, Zhengyu

2017-05-01

S,N co-doped carbon quantum dots (N,S-CQDs) with super high quantum yield (79%) were prepared by the hydrothermal method and characterized by transmission electron microscopy, photoluminescence, UV-Vis spectroscopy and Fourier transformed infrared spectroscopy. N,S-CQDs can enhance the chemiluminescence intensity of a luminol-H 2 O 2 system. The possible mechanism of the luminol-H 2 O 2 -(N,S-CQDs) was illustrated by using chemiluminescence, photoluminescence and ultraviolet analysis. Ranitidine can quench the chemiluminescence intensity of a luminol-H 2 O 2 -N,S-CQDs system. So, a novel flow-injection chemiluminescence method was designed to determine ranitidine within a linear range of 0.5-50 μg ml -1 and a detection limit of 0.12 μg ml -1 . The method shows promising application prospects. Copyright © 2016 John Wiley & Sons, Ltd.

High power cascade diode lasers emitting near 2 μm

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hosoda, Takashi; Feng, Tao; Shterengas, Leon, E-mail: leon.shterengas@stonybrook.edu

2016-03-28

High-power two-stage cascade GaSb-based type-I quantum well diode lasers emitting near 2 μm were designed and fabricated. Coated devices with cavity length of 3 mm generated about 2 W of continuous wave power from 100-μm-wide aperture at the current of 6 A. The power conversion efficiency peaked at 20%. Carrier recycling between quantum well gain stages was realized using band-to-band tunneling in GaSb/AlSb/InAs heterostructure complemented with optimized electron and hole injector regions. Design optimization eliminated parasitic optical absorption and thermionic emission, and included modification of the InAs quantum wells of electron and composition and doping profile of hole injectors. Utilization of the cascade pumpingmore » scheme yielded 2 μm lasers with improved output power and efficiency compared to existing state-of-the-art diodes.« less

High Operating Temperature Midwave Quantum Dot Barrier Infrared Detector (QD-BIRD)

NASA Technical Reports Server (NTRS)

Ting, David Z.; Soibel, Alexander; Hill, Cory J.; Keo, Sam A.; Mumolo, Jason M.; Gunapala, Sarath D.

2012-01-01

The nBn or XBn barrier infrared detector has the advantage of reduced dark current resulting from suppressed Shockley-Read-Hall (SRH) recombination and surface leakage. High performance detectors and focal plane arrays (FPAs) based on InAsSb absorber lattice matched to GaSb substrate, with a matching AlAsSb unipolar electron barrier, have been demonstrated. The band gap of lattice-matched InAsSb yields a detector cutoff wavelength of approximately 4.2 ??m when operating at 150K. We report results on extending the cutoff wavelength of midwave barrier infrared detectors by incorporating self-assembled InSb quantum dots into the active area of the detector. Using this approach, we were able to extend the detector cutoff wavelength to 6 ?m, allowing the coverage of the full midwave infrared (MWIR) transmission window. The quantum dot barrier infrared detector (QD-BIRD) shows infrared response at temperatures up to 225 K.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dehesa, J.S.; Martinez-Finkelshtein, A.; Sorokin, V.N.

The asymptotics of the Boltzmann-Shannon information entropy as well as the Renyi entropy for the quantum probability density of a single-particle system with a confining (i.e., bounded below) power-type potential V(x)=x{sup 2k} with k is a member of N and x is a member of R, is investigated in the position and momentum spaces within the semiclassical (WKB) approximation. It is found that for highly excited states both physical entropies, as well as their sum, have a logarithmic dependence on its quantum number not only when k=1 (harmonic oscillator), but also for any fixed k. As a by-product, the extremalmore » case k{yields}{infinity} (the infinite well potential) is also rigorously analyzed. It is shown that not only the position-space entropy has the same constant value for all quantum states, which is a known result, but also that the momentum-space entropy is constant for highly excited states.« less

Versatile Tri(pyrazolyl)phosphanes as Phosphorus Precursors for the Synthesis of Highly Emitting InP/ZnS Quantum Dots.

PubMed

Panzer, René; Guhrenz, Chris; Haubold, Danny; Hübner, René; Gaponik, Nikolai; Eychmüller, Alexander; Weigand, Jan J

2017-11-13

Tri(pyrazolyl)phosphanes (5 R1,R2 ) are utilized as an alternative, cheap and low-toxic phosphorus source for the convenient synthesis of InP/ZnS quantum dots (QDs). From these precursors, remarkably long-term stable stock solutions (>6 months) of P(OLA) 3 (OLAH=oleylamine) are generated from which the respective pyrazoles are conveniently recovered. P(OLA) 3 acts simultaneously as phosphorus source and reducing agent in the synthesis of highly emitting InP/ZnS core/shell QDs. These QDs are characterized by a spectral range between 530-620 nm and photoluminescence quantum yields (PL QYs) between 51-62 %. A proof-of-concept white light-emitting diode (LED) applying the InP/ZnS QDs as a color-conversion layer was built to demonstrate their applicability and processibility. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

High-fidelity gates in quantum dot spin qubits.

PubMed

Koh, Teck Seng; Coppersmith, S N; Friesen, Mark

2013-12-03

Several logical qubits and quantum gates have been proposed for semiconductor quantum dots controlled by voltages applied to top gates. The different schemes can be difficult to compare meaningfully. Here we develop a theoretical framework to evaluate disparate qubit-gating schemes on an equal footing. We apply the procedure to two types of double-dot qubits: the singlet-triplet and the semiconducting quantum dot hybrid qubit. We investigate three quantum gates that flip the qubit state: a DC pulsed gate, an AC gate based on logical qubit resonance, and a gate-like process known as stimulated Raman adiabatic passage. These gates are all mediated by an exchange interaction that is controlled experimentally using the interdot tunnel coupling g and the detuning [Symbol: see text], which sets the energy difference between the dots. Our procedure has two steps. First, we optimize the gate fidelity (f) for fixed g as a function of the other control parameters; this yields an f(opt)(g) that is universal for different types of gates. Next, we identify physical constraints on the control parameters; this yields an upper bound f(max) that is specific to the qubit-gate combination. We show that similar gate fidelities (~99:5%) should be attainable for singlet-triplet qubits in isotopically purified Si, and for hybrid qubits in natural Si. Considerably lower fidelities are obtained for GaAs devices, due to the fluctuating magnetic fields ΔB produced by nuclear spins.

Quantum logic between remote quantum registers

NASA Astrophysics Data System (ADS)

Yao, N. Y.; Gong, Z.-X.; Laumann, C. R.; Bennett, S. D.; Duan, L.-M.; Lukin, M. D.; Jiang, L.; Gorshkov, A. V.

2013-02-01

We consider two approaches to dark-spin-mediated quantum computing in hybrid solid-state spin architectures. First, we review the notion of eigenmode-mediated unpolarized spin-chain state transfer and extend the analysis to various experimentally relevant imperfections: quenched disorder, dynamical decoherence, and uncompensated long-range coupling. In finite-length chains, the interplay between disorder-induced localization and decoherence yields a natural optimal channel fidelity, which we calculate. Long-range dipolar couplings induce a finite intrinsic lifetime for the mediating eigenmode; extensive numerical simulations of dipolar chains of lengths up to L=12 show remarkably high fidelity despite these decay processes. We further briefly consider the extension of the protocol to bosonic systems of coupled oscillators. Second, we introduce a quantum mirror based architecture for universal quantum computing that exploits all of the dark spins in the system as potential qubits. While this dramatically increases the number of qubits available, the composite operations required to manipulate dark-spin qubits significantly raise the error threshold for robust operation. Finally, we demonstrate that eigenmode-mediated state transfer can enable robust long-range logic between spatially separated nitrogen-vacancy registers in diamond; disorder-averaged numerics confirm that high-fidelity gates are achievable even in the presence of moderate disorder.

Burton Richter, Storage Rings, and the J/psi Particle

Science.gov Websites

[SLAC's] Technical Director, [Richter] became Director ... from 1984 through 1999. During his tenure, SLAC Limits of Quantum Electro-dynamics, DOE Technical Report, June 1959 Design Considerations for High Energy Electron -- Positron Storage Rings, DOE Technical Report, November 1966 Inclusive Yields of pi+, pi-, K

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mieno, H.; Kabe, R.; Allendorf, M. D.

Here, the first metal–organic framework exhibiting thermally activated delayed fluorescence (TADF) was developed. The zirconium-based framework (UiO-68-dpa) uses a newly designed linker composed of a terphenyl backbone, an electron-accepting carboxyl group, and an electron-donating diphenylamine and exhibits green TADF emission with a photoluminescence quantum yield of 30% and high thermal stability.

Analogues of uracil nucleosides with intrinsic fluorescence (NIF-analogues): synthesis and photophysical properties.

PubMed

Segal, Meirav; Fischer, Bilha

2012-02-28

Uridine cannot be utilized as fluorescent probe due to its extremely low quantum yield. For improving the uracil fluorescence characteristics we extended the natural chromophore at the C5 position by coupling substituted aromatic rings directly or via an alkenyl or alkynyl linker to create fluorophores. Extension of the uracil base was achieved by treating 5-I-uridine with the appropriate boronic acid under the Suzuki coupling conditions. Analogues containing an alkynyl linker were obtained from 5-I-uridine and the suitable boronic acid in a Sonogashira coupling reaction. The uracil fluorescent analogues proposed here were designed to satisfy the following requirements: a minimal chemical modification at a position not involved in base-pairing, resulting in relatively long absorption and emission wavelengths and high quantum yield. 5-((4-Methoxy-phenyl)-trans-vinyl)-2'-deoxy-uridine, 6b, was found to be a promising fluorescent probe. Probe 6b exhibits a quantum yield that is 3000-fold larger than that of the natural chromophore (Φ 0.12), maximum emission (478 nm) which is 170 nm red shifted as compared to uridine, and a Stokes shift of 143 nm. In addition, since probe 6b adopts the anti conformation and S sugar puckering favored by B-DNA, it makes a promising nucleoside analogue to be incorporated in an oligonucleotide probe for detection of genetic material.

Photoproduction of hydrated electrons from natural organic solutes in aquatic environments

USGS Publications Warehouse

Zepp, R.G.; Braun, A.M.; Hoigne, J.; Leenheer, J.A.

1987-01-01

Laser flash photolysis was used to investigate the transients formed on absorption of 355-nm light by dissolved organic matter (DOM) from natural water bodies and from soil. Absorption spectra and quenching studies of the transients provided confirming evidence that hydrated electrons were formed by all of the DOM that were studied. The DOM from the Suwannee River in Georgia and from the Greifensee, a Swiss lake, exhibited great variability in light-absorbing properties. Despite this high variability in absorption coefficients, the primary quantum yields for electron ejection from the Greifensee and Suwannee DOM fell in a narrow range (0.005-0.008). Steady-state irradiations (355 nm) of the DOM with 2-chloroethanol (0.02 M) present as an electron scavenger produced chloride ions with quantum yields that were about 2 orders of magnitude lower than the primary quantum yields. This result indicates that most of the photoejected electrons recombine with cations before escaping into bulk solution. Irradiations of DOM solutions under sunlight (April, latitude 34?? N) photoproduced electrons at rates falling in the range of 0.2-0.4 ??mol/[(mg of DOC) h]. These results indicate that hydrated electrons can play a significant role in the environmental photoreduction of persistent, electronegative pollutants but may be relatively unimportant in the environmental production of hydrogen peroxide. ?? 1987 American Chemical Society.

Separating strain from composition in unit cell parameter maps obtained from aberration corrected high resolution transmission electron microscopy imaging

DOE Office of Scientific and Technical Information (OSTI.GOV)

Schulz, T.; Remmele, T.; Korytov, M.

2014-01-21

Based on the evaluation of lattice parameter maps in aberration corrected high resolution transmission electron microscopy images, we propose a simple method that allows quantifying the composition and disorder of a semiconductor alloy at the unit cell scale with high accuracy. This is realized by considering, next to the out-of-plane, also the in-plane lattice parameter component allowing to separate the chemical composition from the strain field. Considering only the out-of-plane lattice parameter component not only yields large deviations from the true local alloy content but also carries the risk of identifying false ordering phenomena like formations of chains or platelets.more » Our method is demonstrated on image simulations of relaxed supercells, as well as on experimental images of an In{sub 0.20}Ga{sub 0.80}N quantum well. Principally, our approach is applicable to all epitaxially strained compounds in the form of quantum wells, free standing islands, quantum dots, or wires.« less

Highly luminescent core-shell InP/ZnX (X = S, Se) quantum dots prepared via a phosphine synthetic route.

PubMed

Mordvinova, Natalia; Vinokurov, Alexander; Kuznetsova, Tatiana; Lebedev, Oleg I; Dorofeev, Sergey

2017-01-24

Here we report a simple method for the creation of highly luminescent core-shell InP/ZnX (X = S, Se) quantum dots (QDs) on the basis of a phosphine synthetic route. In this method a Zn precursor was added to the reaction mixture at the beginning of the synthesis to form an In(Zn)P alloy structure, which promoted the formation of a ZnX shell. Core-shell InP/ZnX QDs exhibit highly intensive emission with a quantum yield over 50%. The proposed method is primarily important for practical applications. Advantages of this method compared to the widely used SILAR technique are discussed. We further demonstrate that the SILAR approach consisting of consequent addition of Zn and chalcogen precursors to pre-prepared non-doped InP colloidal nanoparticles is not quite suitable for shell growth without the addition of special activator agents or the use of very reactive precursors.

Semiconductor Quantum Dots for Biomedicial Applications

PubMed Central

Shao, Lijia; Gao, Yanfang; Yan, Feng

2011-01-01

Semiconductor quantum dots (QDs) are nanometre-scale crystals, which have unique photophysical properties, such as size-dependent optical properties, high fluorescence quantum yields, and excellent stability against photobleaching. These properties enable QDs as the promising optical labels for the biological applications, such as multiplexed analysis of immunocomplexes or DNA hybridization processes, cell sorting and tracing, in vivo imaging and diagnostics in biomedicine. Meanwhile, QDs can be used as labels for the electrochemical detection of DNA or proteins. This article reviews the synthesis and toxicity of QDs and their optical and electrochemical bioanalytical applications. Especially the application of QDs in biomedicine such as delivering, cell targeting and imaging for cancer research, and in vivo photodynamic therapy (PDT) of cancer are briefly discussed. PMID:22247690

Infrared-induced conformational isomerization and vibrational relaxation dynamics in melatonin and 5-methoxy-N-acetyl tryptophan methyl amide

NASA Astrophysics Data System (ADS)

Dian, Brian C.; Florio, Gina M.; Clarkson, Jasper R.; Longarte, Asier; Zwier, Timothy S.

2004-05-01

The conformational isomerization dynamics of melatonin and 5-methoxy N-acetyltryptophan methyl amide (5-methoxy NATMA) have been studied using the methods of IR-UV hole-filling spectroscopy and IR-induced population transfer spectroscopy. Using these techniques, single conformers of melatonin were excited via a well-defined NH stretch fundamental with an IR pump laser. This excess energy was used to drive conformational isomerization. By carrying out the infrared excitation early in a supersonic expansion, the excited molecules were re-cooled into their zero-point levels, partially re-filling the hole created in the ground state population of the excited conformer, and creating gains in population of the other conformers. These changes in population were detected using laser-induced fluorescence downstream in the expansion via an UV probe laser. The isomerization quantum yields for melatonin show some conformation specificity but no hint of vibrational mode specificity. In 5-methoxy NATMA, no isomerization was observed out of the single conformational well populated in the expansion in the absence of the infrared excitation. In order to study the dependence of the isomerization on the cooling rate, the experimental arrangement was modified so that faster cooling conditions could be studied. In this arrangement, the pump and probe lasers were overlapped in space in the high density region of the expansion, and the time dependence of the zero-point level populations of the conformers was probed following selective excitation of a single conformation. The analysis needed to extract isomerization quantum yields from the timing scans was developed and applied to the melatonin timing scans. Comparison between the frequency and time domain isomerization quantum yields under identical experimental conditions produced similar results. Under fast cooling conditions, the product quantum yields were shifted from their values under standard conditions. The results for melatonin are compared with those for N-acetyl tryptophan methyl amide.

Quantum state-resolved probing of strong-field-ionized xenon atoms using femtosecond high-order harmonic transient absorption spectroscopy.

PubMed

Loh, Zhi-Heng; Khalil, Munira; Correa, Raoul E; Santra, Robin; Buth, Christian; Leone, Stephen R

2007-04-06

Femtosecond high-order harmonic transient absorption spectroscopy is used to resolve the complete |j,m quantum state distribution of Xe+ produced by optical strong-field ionization of Xe atoms at 800 nm. Probing at the Xe N4/5 edge yields a population distribution rhoj,|m| of rho3/2,1/2ratiorho1/2,1/2ratiorho3/2,3/2=75+/-6 :12+/-3 :13+/-6%. The result is compared to a tunnel ionization calculation with the inclusion of spin-orbit coupling, revealing nonadiabatic ionization behavior. The sub-50-fs time resolution paves the way for tabletop extreme ultraviolet absorption probing of ultrafast dynamics.

Seasonal and spatial variabilities in the water chemistry of prairie pothole wetlands influence the photoproduction of reactive intermediates.

PubMed

McCabe, Andrew J; Arnold, William A

2016-07-01

The hydrology and water chemistry of prairie pothole wetlands vary spatially and temporally, on annual and decadal timescales. Pesticide contamination of wetlands arising from agricultural activities is a foremost concern. Photochemical reactions are important in the natural attenuation of pesticides and may be important in limiting ecological and human exposure. Little is known, however, about the variable influence of wetland water chemistry on indirect photochemistry. In this study, seasonal water samples were collected from seven sites throughout the prairie pothole region over three years to understand the spatiotemporal dynamics of reactive intermediate photoproduction. Samples were classified by the season in which they were collected (spring, summer, or fall) and the typical hydroperiod of the wetland surface water (temporary or semi-permanent). Under photostable conditions, steady-state concentrations and apparent quantum yields or quantum yield coefficients were measured for triplet excited states of dissolved organic matter, singlet oxygen, hydroxyl radical, and carbonate radical under simulated sunlight. Steady-state concentrations and quantum yields increased on average by 15% and 40% from spring to fall, respectively. Temporary wetlands had 40% higher steady-state concentrations of reactive intermediates than semi-permanent wetlands, but 50% lower quantum yields. Computed quantum yields for reactive intermediate formation were used to predict the indirect photochemical half-lives of seven pesticides in average temporary and semi-permanent prairie pothole wetlands. As a first approximation, the predictions agree to within two orders of magnitude of previously reported half-lives. Copyright © 2016 Elsevier Ltd. All rights reserved.

Remote state preparation through hyperentangled atomic states

NASA Astrophysics Data System (ADS)

Nawaz, Mehwish; ul-Islam, Rameez-; Ikram, Manzoor

2018-04-01

Hyperentangled states have enhanced channel capacity in quantum processing and have yielded` evident increased communication speed in quantum informatics as a consequence of excessively high information content coded over each quantum entity. In the present article, we intend to demonstrate this fact by utilizing atomic states simultaneously entangled both in internal as well as external degrees of freedom, i.e. the de Broglie motion for remote state preparation (RSP). The results clearly demonstrate that we can efficiently communicate two bit information while manipulating only a single quantum subsystem. The states are prepared and manipulated using atomic Bragg diffraction as well as Ramsey interferometry, both of which are now considered as standard, state of the art tools based on cavity quantum electrodynamics. Since atomic Bragg diffraction is a large interaction time regime and produces spatially well separated, decoherence resistant outputs, the schematics presented here for the RSP offer important perspectives on efficient detection as well as unambiguous information coding and readout. The article summarizes the experimental feasibility of the proposal, culminating with a brief discussion.

Generalized Weyl-Wigner map and Vey quantum mechanics

NASA Astrophysics Data System (ADS)

Dias, Nuno Costa; Prata, João Nuno

2001-12-01

The Weyl-Wigner map yields the entire structure of Moyal quantum mechanics directly from the standard operator formulation. The covariant generalization of Moyal theory, also known as Vey quantum mechanics, was presented in the literature many years ago. However, a derivation of the formalism directly from standard operator quantum mechanics, clarifying the relation between the two formulations, is still missing. In this article we present a covariant generalization of the Weyl order prescription and of the Weyl-Wigner map and use them to derive Vey quantum mechanics directly from the standard operator formulation. The procedure displays some interesting features: it yields all the key ingredients and provides a more straightforward interpretation of the Vey theory including a direct implementation of unitary operator transformations as phase space coordinate transformations in the Vey idiom. These features are illustrated through a simple example.

Robust and specific ratiometric biosensing using a copper-free clicked quantum dot-DNA aptamer sensor

NASA Astrophysics Data System (ADS)

Zhang, Haiyan; Feng, Guoqiang; Guo, Yuan; Zhou, Dejian

2013-10-01

We report herein the successful preparation of a compact and functional CdSe-ZnS core-shell quantum dot (QD)-DNA conjugate via highly efficient copper-free ``click chemistry'' (CFCC) between a dihydro-lipoic acid-polyethylene glycol-azide (DHLA-PEG-N3) capped QD and a cyclooctyne modified DNA. This represents an excellent balance between the requirements of high sensitivity, robustness and specificity for the QD-FRET (Förster resonance energy transfer) based sensor as confirmed by a detailed FRET analysis on the QD-DNA conjugate, yielding a relatively short donor-acceptor distance of ~5.8 nm. We show that this CFCC clicked QD-DNA conjugate is not only able to retain the native fluorescence quantum yield (QY) of the parent DHLA-PEG-N3 capped QD, but also well-suited for robust and specific biosensing; it can directly quantitate, at the pM level, both labelled and unlabelled complementary DNA probes with a good SNP (single-nucleotide polymorphism) discrimination ability in complex media, e.g. 10% human serum via target-binding induced FRET changes between the QD donor and the dye acceptor. Furthermore, this sensor has also been successfully exploited for the detection, at the pM level, of a specific protein target (thrombin) via the encoded anti-thrombin aptamer sequence in the QD-DNA conjugate.We report herein the successful preparation of a compact and functional CdSe-ZnS core-shell quantum dot (QD)-DNA conjugate via highly efficient copper-free ``click chemistry'' (CFCC) between a dihydro-lipoic acid-polyethylene glycol-azide (DHLA-PEG-N3) capped QD and a cyclooctyne modified DNA. This represents an excellent balance between the requirements of high sensitivity, robustness and specificity for the QD-FRET (Förster resonance energy transfer) based sensor as confirmed by a detailed FRET analysis on the QD-DNA conjugate, yielding a relatively short donor-acceptor distance of ~5.8 nm. We show that this CFCC clicked QD-DNA conjugate is not only able to retain the native fluorescence quantum yield (QY) of the parent DHLA-PEG-N3 capped QD, but also well-suited for robust and specific biosensing; it can directly quantitate, at the pM level, both labelled and unlabelled complementary DNA probes with a good SNP (single-nucleotide polymorphism) discrimination ability in complex media, e.g. 10% human serum via target-binding induced FRET changes between the QD donor and the dye acceptor. Furthermore, this sensor has also been successfully exploited for the detection, at the pM level, of a specific protein target (thrombin) via the encoded anti-thrombin aptamer sequence in the QD-DNA conjugate. Electronic supplementary information (ESI) available: Details on the synthesis, purification and characterisation of the DHLA-PEG600-N3, cyclooctyne-DNA, and QD-TBA20 conjugates as well as all supporting figures and tables. See DOI: 10.1039/c3nr02897f

Purcell-enhanced quantum yield from carbon nanotube excitons coupled to plasmonic nanocavities

DOE PAGES

Luo, Yue; Ahmadi, Ehsaneh D.; Shayan, Kamran; ...

2017-11-10

Single-walled carbon nanotubes (SWCNTs) are promising absorbers and emitters to enable novel photonic applications and devices but are also known to suffer from low optical quantum yields. Here we demonstrate SWCNT excitons coupled to plasmonic nanocavity arrays reaching deeply into the Purcell regime with Purcell factors (F P) up to F P = 180 (average F P = 57), Purcell-enhanced quantum yields of 62% (average 42%), and a photon emission rate of 15 MHz into the first lens. The cavity coupling is quasi-deterministic since the photophysical properties of every SWCNT are enhanced by at least one order of magnitude. Furthermore,more » the measured ultra-narrow exciton linewidth (18 ueV) reaches the radiative lifetime limit, which is promising towards generation of transform-limited single photons. Furthermore, to demonstrate utility beyond quantum light sources we show that nanocavity-coupled SWCNTs perform as single-molecule thermometers detecting plasmonically induced heat at cryogenic temperatures in a unique interplay of excitons, phonons, and plasmons at the nanoscale.« less

Application of DNA Aptamers and Quantum Dots to Lateral Flow Test Strips for Detection of Foodborne Pathogens with Improved Sensitivity versus Colloidal Gold

PubMed Central

Bruno, John G.

2014-01-01

Preliminary studies aimed at improving the sensitivity of foodborne pathogen detection via lateral flow (LF) test strips by use of high affinity DNA aptamers for capture and reporter functions when coupled to red-emitting quantum dots (Qdot 655) are reported. A variety of DNA aptamers developed against Escherichia coli, Listeria monocytogenes, and Salmonella enterica were paired in capture and reporter combinations to determine which yielded the strongest detection of their cognate bacteria using a colloidal gold screening system. Several promising sandwich combinations were identified for each of the three bacterial LF strip systems. The best E. coli aptamer-LF system was further studied and yielded a visible limit of detection (LOD) of ~3,000 E. coli 8739 and ~6,000 E. coli O157:H7 in buffer. These LODs were reduced to ~300–600 bacterial cells per test respectively by switching to a Qdot 655 aptamer-LF system. Novel aspects of these assays such as the use of high levels of detergents to avoid quantum dot agglutination and enhance migration in analytical membranes, identification of optimal analytical membrane types, UV-immobilization of capture aptamers, and novel dual biotin/digoxigenin-end labeled aptamer streptavidin-colloidal gold or -Qdot 655 conjugates plus anti-digoxigenin antibody control lines are also discussed. In general, this work provides proof-of-principle for highly sensitive aptamer-Qdot LF strip assays for rapid foodborne pathogen detection. PMID:25437803

Emergence of chiral spin liquids via quantum melting of noncoplanar magnetic orders

DOE PAGES

Hickey, Ciarán; Cincio, Lukasz; Papić, Zlatko; ...

2017-09-11

Quantum spin liquids (QSLs) are highly entangled states of quantum magnets which lie beyond the Landau paradigm of classifying phases of matter via broken symmetries. A physical route to arriving at QSLs is via frustration-induced quantum melting of ordered states such as valence bond crystals or magnetic orders. Using extensive exact diagonalization (ED) and density-matrix renormalization group (DMRG)we show studies of concrete S U ( 2 ) invariant spin models on honeycomb, triangular, and square lattices, that chiral spin liquids (CSLs) emerge as descendants of triple- Q spin crystals with tetrahedral magnetic order and a large scalar spin chirality. Suchmore » ordered-to-CSL melting transitions may yield lattice realizations of effective Chern-Simons-Higgs field theories. We provides a distinct unifying perspective on the emergence of CSLs and suggests that materials with certain noncoplanar magnetic orders might provide a good starting point to search for CSLs.« less

Nanodiamonds carrying silicon-vacancy quantum emitters with almost lifetime-limited linewidths

NASA Astrophysics Data System (ADS)

Jantzen, Uwe; Kurz, Andrea B.; Rudnicki, Daniel S.; Schäfermeier, Clemens; Jahnke, Kay D.; Andersen, Ulrik L.; Davydov, Valery A.; Agafonov, Viatcheslav N.; Kubanek, Alexander; Rogers, Lachlan J.; Jelezko, Fedor

2016-07-01

Colour centres in nanodiamonds are an important resource for applications in quantum sensing, biological imaging, and quantum optics. Here we report unprecedented narrow optical transitions for individual colour centres in nanodiamonds smaller than 200 nm. This demonstration has been achieved using the negatively charged silicon vacancy centre, which has recently received considerable attention due to its superb optical properties in bulk diamond. We have measured an ensemble of silicon-vacancy centres across numerous nanodiamonds to have an inhomogeneous distribution of 1.05 nm at 5 K. Individual spectral lines as narrower than 360 MHz were measured in photoluminescence excitation, and correcting for apparent spectral diffusion yielded an homogeneous linewidth of about 200 MHz which is close to the lifetime limit. These results indicate the high crystalline quality achieved in these nanodiamond samples, and advance the applicability of nanodiamond-hosted colour centres for quantum optics applications.

Deterministic implementation of a bright, on-demand single photon source with near-unity indistinguishability via quantum dot imaging.

PubMed

He, Yu-Ming; Liu, Jin; Maier, Sebastian; Emmerling, Monika; Gerhardt, Stefan; Davanço, Marcelo; Srinivasan, Kartik; Schneider, Christian; Höfling, Sven

2017-07-20

Deterministic techniques enabling the implementation and engineering of bright and coherent solid-state quantum light sources are key for the reliable realization of a next generation of quantum devices. Such a technology, at best, should allow one to significantly scale up the number of implemented devices within a given processing time. In this work, we discuss a possible technology platform for such a scaling procedure, relying on the application of nanoscale quantum dot imaging to the pillar microcavity architecture, which promises to combine very high photon extraction efficiency and indistinguishability. We discuss the alignment technology in detail, and present the optical characterization of a selected device which features a strongly Purcell-enhanced emission output. This device, which yields an extraction efficiency of η = (49 ± 4) %, facilitates the emission of photons with (94 ± 2.7) % indistinguishability.

Emergence of chiral spin liquids via quantum melting of noncoplanar magnetic orders

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hickey, Ciarán; Cincio, Lukasz; Papić, Zlatko

Quantum spin liquids (QSLs) are highly entangled states of quantum magnets which lie beyond the Landau paradigm of classifying phases of matter via broken symmetries. A physical route to arriving at QSLs is via frustration-induced quantum melting of ordered states such as valence bond crystals or magnetic orders. Using extensive exact diagonalization (ED) and density-matrix renormalization group (DMRG)we show studies of concrete S U ( 2 ) invariant spin models on honeycomb, triangular, and square lattices, that chiral spin liquids (CSLs) emerge as descendants of triple- Q spin crystals with tetrahedral magnetic order and a large scalar spin chirality. Suchmore » ordered-to-CSL melting transitions may yield lattice realizations of effective Chern-Simons-Higgs field theories. We provides a distinct unifying perspective on the emergence of CSLs and suggests that materials with certain noncoplanar magnetic orders might provide a good starting point to search for CSLs.« less

Quantum yield and rate constant of the singlet 1Δ g oxygen luminescence in an aqueous medium in the presence of nanoscale inhomogeneities

NASA Astrophysics Data System (ADS)

Jarnikova, E. S.; Parkhats, M. V.; Stasheuski, A. S.; Lepeshkevich, S. V.; Dzhagarov, B. M.

2017-04-01

The quantum yields and lifetimes of photosensitized luminescence of the 1Δ g state of singlet oxygen in an aquatic media with a controlled concentration of dielectric anisotropy centers (polyethylene glycol) have been measured using the methods of laser fluorometry. It is established that the quantum yield and the rate constant ( k r ) of the a 1Δ g → X 3Σ g - luminescence of 1O2 increase as the polymer concentration increases. The effect is analyzed within a general approach involving a relationship between kr and dielectric properties of the medium and is explained by the increased density of photon states and the local field factor in the space around O2( a 1Δ g ).

Cross sections and quantum yields of the 3 micron emission for Er(3+) and Ho(3+) dopants in crystalsls

NASA Astrophysics Data System (ADS)

Payne, Stephen A.; Smith, Larry K.; Krupke, William F.

1995-05-01

The lifetime, quantum yields, and branching ratios for the 2.8 micron emissions of several Er-and Ho-doped fluorides and oxides were measured. Among the fluoride crystals examined, which included LiYF4, BaY2F8, LaF3, and KY3F10, only the Ho:LiFY4 systems showed any proof of nonradiative decay. Conversely, all the oxide crystals were affected by nonradiative processes, resulting in measured quantum yields ranging from 3.6% for Er:Y3Al5O12 to 62% for Er in Gd3Sc2Ga3O12. In addition, plots of the 2.8 micron emission cross sections for seven Er- and Ho-doped crystals were presented.

Rigid biimidazole ancillary ligands as an avenue to bright deep blue cationic iridium(iii) complexes.

PubMed

Henwood, Adam F; Evariste, Sloane; Slawin, Alexandra M Z; Zysman-Colman, Eli

2014-01-01

Herein we report the synthesis and optoelectronic characterisation of three deep blue-emitting cationic iridium complexes, of the form [Ir(dFppy)(2)(N^N)]PF(6), bearing biimidazole-type N^N ancillary ligands (dFppyH = 2-(2,4-difluorophenyl)pyridine). Complex 1 contains the parent biimidazole, biim, while 2 contains a dimethylated analog, dMebiim, and 3 contains an ortho-xylyl-tethered biimidzole, o-xylbiim. We explore a strategy of tethering the biimidazole in order to rigidify the complex and increase the photoluminescent quantum yield, culminating in deep blue (λ(max): 457 nm in MeOH at 298 K) ligand-centered emission with a very high photoluminescent quantum yield of 68% and microsecond emission lifetime. Density functional theory calculations elucidate the origin of such disparate excited state kinetics across this series, especially in light of virtually identical optoelectronic properties observed for these compounds.

Use of a Novel Rover-mounted Fluorescence Imager and Fluorescent Probes to Detect Biological Material in the Atacama Desert in Daylight

NASA Technical Reports Server (NTRS)

Weinstein, S.; Pane, D.; Warren-Rhodes, K.; Cockell, C.; Ernst, L. A.; Minkley, E.; Fisher, G.; Emani, S.; Wettergreen, D. S.; Wagner, M.

2005-01-01

We have developed an imaging system, the Fluorescence Imager (FI), for detecting fluorescence signals from sparse microorganisms and biofilms during autonomous rover exploration. The fluorescence signals arise both from naturally occurring chromophores, such as chlorophyll of cyanobacteria and lichens, and from fluorescent probes applied to soil and rocks. Daylight imaging has been accomplished by a novel use of a high-powered flashlamp synchronized to a CCD camera. The fluorescent probes are cell permanent stains that have extremely low intrinsic fluorescence (quantum yields less than 0.01) and a large fluorescence enhancement (quantum yields greater than 0.4) when bound to the target. Each probe specifically targets either carbohydrates, proteins, nucleic acids or membrane lipids, the four classes of macromolecules found in terrestrial life. The intent of the probes is to interrogate the environment for surface and endolithic life forms.

Near-unity photoluminescence quantum yield in MoS.sub.2

DOEpatents

Amani, Matin; Lien, Der-Hsien; Kiriya, Daisuke; Bullock, James; Javey, Ali

2017-12-26

Two-dimensional (2D) transition-metal dichalcogenides have emerged as a promising material system for optoelectronic applications, but their primary figure-of-merit, the room-temperature photoluminescence quantum yield (QY) is extremely poor. The prototypical 2D material, MoS.sub.2 is reported to have a maximum QY of 0.6% which indicates a considerable defect density. We report on an air-stable solution-based chemical treatment by an organic superacid which uniformly enhances the photoluminescence and minority carrier lifetime of MoS.sub.2 monolayers by over two orders of magnitude. The treatment eliminates defect-mediated non-radiative recombination, thus resulting in a final QY of over 95% with a longest observed lifetime of 10.8.+-.0.6 nanoseconds. Obtaining perfect optoelectronic monolayers opens the door for highly efficient light emitting diodes, lasers, and solar cells based on 2D materials.

A quantum protective mechanism in photosynthesis

NASA Astrophysics Data System (ADS)

Marais, Adriana; Sinayskiy, Ilya; Petruccione, Francesco; van Grondelle, Rienk

2015-03-01

Since the emergence of oxygenic photosynthesis, living systems have developed protective mechanisms against reactive oxygen species. During charge separation in photosynthetic reaction centres, triplet states can react with molecular oxygen generating destructive singlet oxygen. The triplet product yield in bacteria is observed to be reduced by weak magnetic fields. Reaction centres from plants' photosystem II share many features with bacterial reaction centres, including a high-spin iron whose function has remained obscure. To explain observations that the magnetic field effect is reduced by the iron, we propose that its fast-relaxing spin plays a protective role in photosynthesis by generating an effective magnetic field. We consider a simple model of the system, derive an analytical expression for the effective magnetic field and analyse the resulting triplet yield reduction. The protective mechanism is robust for realistic parameter ranges, constituting a clear example of a quantum effect playing a macroscopic role vital for life.

A quantum protective mechanism in photosynthesis.

PubMed

Marais, Adriana; Sinayskiy, Ilya; Petruccione, Francesco; van Grondelle, Rienk

2015-03-03

Since the emergence of oxygenic photosynthesis, living systems have developed protective mechanisms against reactive oxygen species. During charge separation in photosynthetic reaction centres, triplet states can react with molecular oxygen generating destructive singlet oxygen. The triplet product yield in bacteria is observed to be reduced by weak magnetic fields. Reaction centres from plants' photosystem II share many features with bacterial reaction centres, including a high-spin iron whose function has remained obscure. To explain observations that the magnetic field effect is reduced by the iron, we propose that its fast-relaxing spin plays a protective role in photosynthesis by generating an effective magnetic field. We consider a simple model of the system, derive an analytical expression for the effective magnetic field and analyse the resulting triplet yield reduction. The protective mechanism is robust for realistic parameter ranges, constituting a clear example of a quantum effect playing a macroscopic role vital for life.

Surface Stabilized InP/GaP/ZnS Quantum Dots with Mg Ions for WLED Application.

PubMed

Park, Joong Pill; Kim, Sang-Wook

2016-05-01

One of the most highlighted cadmium-free quantum dots (QDs), InP-based QDs, have improved their optical properties. However, InP-based QDs have some practical drawbacks, for example, stability, compared with CdSe-based QDs. Poor stability of InP-based QDs yields critical problems, such as agglomeration and photoluminescence quenching in light emitting diode (LED). It has to be solved for applications and most research has focused on thick outer shells as an effective solution. We introduced magnesium cations for improving stability of InP-based QDs. We applied very small amounts of Mg cations as surface stabilizers, as a result, stability of QDs is clearly improved. Then, QD based LED chips also yield improved values including RA of 84.4, CCT of 3799 K, and luminous efficiency of 129.57 Im/W, which are highly improved data compared with our previous results.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Marseglia, L.; Saha, K.; Ajoy, A.

The practical implementation of quantum technologies such as quantum commu- nication and quantum cryptography relies on the development of indistinguishable, robust, and bright single photon sources that works at room temperature. The silicon- vacancy (SiV -) center in diamond has emerged as a possible candidate for a single photon source with all these characteristics. Unfortunately, due to the high refraction index mismatch between diamond and air, color centers in diamond show low photon out-coupling. This drawback can be overcome by fabrication of photonic structures that improve the in-coupling of excitation laser to the diamond defect as well as the out-couplingmore » emission from the color centers. An additional shortcoming is due to the random localization of native defects in the diamond sample. Here we demonstrate deterministic implantation of Si ions with high conversion effciency to single SiV -, targeted to fabricated nanowires. The co-localization of single SiV - defects with the nanostructures yields a ten times higher light coupling effciency as compared to single SiV - in the bulk. This result, with its intrinsic scalability, enables a new class of devices for integrated photonics and quantum information processing.« less

Water relation, leaf gas exchange and chlorophyll a fluorescence imaging of soybean leaves infected with Colletotrichum truncatum.

PubMed

Dias, Carla Silva; Araujo, Leonardo; Alves Chaves, Joicy Aparecida; DaMatta, Fábio M; Rodrigues, Fabrício A

2018-06-01

Considering the potential of anthracnose to decrease soybean yield and the need to gain more information regarding its effect on soybean physiology, the present study performed an in-depth analysis of the photosynthetic performance of soybean leaflets challenged with Colletotrichum truncatum by combining chlorophyll a fluorescence images with gas-exchange measurements and photosynthetic pigment pools. There were no significant differences between non-inoculated and inoculated plants in leaf water potential, apparent hydraulic conductance, net CO 2 assimilation rate, stomatal conductance to water vapor and transpiration rate. For internal CO 2 concentration, significant difference between non-inoculated and inoculated plants occurred only at 36 h after inoculation. Reductions in the values of the chlorophyll a fluorescence parameters [initial fluorescence (F 0 ), maximal fluorescence (F m ), maximal photosystem II quantum yield (F v /F m ), quantum yield of regulated energy dissipation (Y(NPQ))] and increases in effective PS II quantum yield (Y(II)), quantum yield of non-regulated energy dissipation Y(NO) and photochemical quenching coefficient (q P ) were noticed on the necrotic vein tissue in contrast to the surrounding leaf tissue. It appears that the impact of the infection by C. truncatum on the photosynthetic performance of the leaflets was minimal considering the preference of the fungus to colonize the veins. Copyright © 2018 Elsevier Masson SAS. All rights reserved.

Chlorophyll fluorescence is a rigorous, high throughput tool to analyze the impacts of genotype, species, and stress on plant and ecosystem productivity

NASA Astrophysics Data System (ADS)

Ewers, B. E.; Pleban, J. R.; Aston, T.; Beverly, D.; Speckman, H. N.; Hosseini, A.; Bretfeld, M.; Edwards, C.; Yarkhunova, Y.; Weinig, C.; Mackay, D. S.

2017-12-01

Abiotic and biotic stresses reduce plant productivity, yet high-throughput characterization of plant responses across genotypes, species and stress conditions are limited by both instrumentation and data analysis techniques. Recent developments in chlorophyll a fluorescence measurement at leaf to landscape scales could improve our predictive understanding of plants response to stressors. We analyzed the interaction of species and stress across two crop types, five gymnosperm and two angiosperm tree species from boreal and montane forests, grasses, forbs and shrubs from sagebrush steppe, and 30 tree species from seasonally wet tropical forest. We also analyzed chlorophyll fluorescence and gas exchange data from twelve Brassica rapa crop accessions and 120 recombinant inbred lines to investigate phenotypic responses to drought. These data represent more than 10,000 measurements of fluorescence and allow us to answer two questions 1) are the measurements from high-throughput, hand held and drone-mounted instruments quantitatively similar to lower throughput camera and gas exchange mounted instruments and 2) do the measurements find differences in genotypic, species and environmental stress on plants? We found through regression that the high and low throughput instruments agreed across both individual chlorophyll fluorescence components and calculated ratios and were not different from a 1:1 relationship with correlation greater than 0.9. We used hierarchical Bayesian modeling to test the second question. We found a linear relationship between the fluorescence-derived quantum yield of PSII and the quantum yield of CO2 assimilation from gas-exchange, with a slope of ca. 0.1 indicating that the efficiency of the entire photosynthetic process was about 10% of PSII across genotypes, species and drought stress. Posterior estimates of quantum yield revealed that drought-treatment, genotype and species differences were preserved when accounting for measurement uncertainty. High throughput handheld or drone-based measurements of chlorophyll fluorescence provide high quality, quantitative data that can be used to not only connect genotype to phenotype but also quantify how vastly different plant species and genotypes respond to stress and change ecosystem productivity.

Development of a New Class of Scintillating Fibres with Very Short Decay Time and High Light Yield

NASA Astrophysics Data System (ADS)

Borshchev, O.; Cavalcante, A. B. R.; Gavardi, L.; Gruber, L.; Joram, C.; Ponomarenko, S.; Shinji, O.; Surin, N.

2017-05-01

We present first studies of a new class of scintillating fibres which are characterised by very short decay times and high light yield. The fibres are based on a novel type of luminophores admixed to a polystyrene core matrix. These so-called Nanostructured Organosilicon Luminophores (NOL) have high photoluminescense quantum yield and decay times just above 1 ns. A blue and a green emitting prototype fibre with 250 μm diameter were produced and characterised in terms of attenuation length, ionisation light yield, decay time and tolerance to x-ray irradiation. The well-established Kuraray SCSF-78 and SCSF-3HF fibres were taken as references. Even though the two prototype fibres mark just an intermediate step in an ongoing development, their performance is already on a competitive level. In particular, their decay time constants are about a factor of two shorter than the fastest known fibres, which makes them promising candidates for time critical applications.

Defect induced photoluminescence in MoS2 quantum dots and effect of Eu3+/Tb3+ co-doping towards efficient white light emission

NASA Astrophysics Data System (ADS)

Haldar, Dhrubaa; Ghosh, Arnab; Bose, Saptasree; Mondal, Supriya; Ghorai, Uttam Kumar; Saha, Shyamal K.

2018-05-01

Intensive research has been carried out on optical properties of MoS2 quantum dots for versatile applications in photo catalytic, sensing and optoelectronic devices. However, white light generation from MoS2 quantum dots particularly using doping effect is relatively unexplored. Herein we report successful synthesis of Europium (Eu)/Terbium (Tb) co-doped MoS2 quantum dots to achieve white light for potential applications in optoelectronic devices. The dopant ions are introduced into the host lattice to retain the emission colors to cover the entire range of visible light of solar spectrum. Perfect white light (CIE = 0.31, 0.33) with high intensity (quantum yield = 28.29%) is achieved in these rare earth elements co-doped quantum dot system. A new peak is observed in the NIR region which is attributed to the defects present in MoS2 quantum dots. Temperature dependent study has been carried out to understand the origin of this new peak in the NIR region. It is seen that the 'S' defects in the QDs cause the appearance of this peak which shows a blue shift at higher temperature.

Long-lived and Well-resolved Mn2+ Ion Emissions in CuInS-ZnS Quantum Dots

PubMed Central

Cao, Sheng; Li, Chengming; Wang, Lin; Shang, Minghui; Wei, Guodong; Zheng, Jinju; Yang, Weiyou

2014-01-01

CuInS2 (CIS) quantum dots (QDs) have tunable photoluminescence (PL) behaviors in the visible and near infrared spectral range with markedly lower toxicity than the cadmium-based counterparts, making them very promising applications in light emitting and solar harvesting. However, there still remain material- and fabrication- related obstacles in realizing the high-performance CIS-based QDs with well-resolved Mn2+ d-d emission, long emission lifetimes as well as high efficiencies. Here, we demonstrate the growth of high-quality Mn2+-doped CuInS-ZnS (CIS-ZnS) QDs based on a multi-step hot-injection strategy. The resultant QDs exhibit a well-resolved Mn2+ d-d emission with a high PL quantum yield (QY) up to 66% and an extremely long excited state lifetime up to ~3.78 ms, which is nearly two times longer than the longest one of “green” QDs ever reported. It is promising that the synthesized Mn2+-doped CIS-ZnS QDs might open new doors for their practical applications in bioimaging and opto/electronic devices. PMID:25515207

New Molecular Design Concurrently Providing Superior Pure Blue, Thermally Activated Delayed Fluorescence and Optical Out-Coupling Efficiencies.

PubMed

Rajamalli, P; Senthilkumar, N; Huang, P-Y; Ren-Wu, C-C; Lin, H-W; Cheng, C-H

2017-08-16

Simultaneous enhancement of out-coupling efficiency, internal quantum efficiency, and color purity in thermally activated delayed fluorescence (TADF) emitters is highly desired for the practical application of these materials. We designed and synthesized two isomeric TADF emitters, 2DPyM-mDTC and 3DPyM-pDTC, based on di(pyridinyl)methanone (DPyM) cores as the new electron-accepting units and di(tert-butyl)carbazole (DTC) as the electron-donating units. 3DPyM-pDTC, which is structurally nearly planar with a very small ΔE ST , shows higher color purity, horizontal ratio, and quantum yield than 2DPyM-mDTC, which has a more flexible structure. An electroluminescence device based on 3DPyM-pDTC as the dopant emitter can reach an extremely high external quantum efficiency of 31.9% with a pure blue emission. This work also demonstrates a way to design materials with a high portion of horizontal molecular orientation to realize a highly efficient pure-blue device based on TADF emitters.

LASER APPLICATIONS AND OTHER TOPICS IN QUANTUM ELECTRONICS: Kinetics and quantum yield of photoluminescence of EuFOD3 doped into a nanoporous glass with the help of supercritical CO2

NASA Astrophysics Data System (ADS)

Bagratashvili, V. N.; Gerasimova, V. I.; Gordienko, V. M.; Tsypina, S. I.; Chutko, E. A.

2008-08-01

The kinetics of photoluminescence of a EuFOD3 metalloorganic compound doped into a nanoporous Vycor glass by the method of supercritical fluid impregnation is studied. The lifetime of luminescence of EuFOD3 molecules in pores excited by an excimer XeCl laser was 40 μs, which is considerably smaller than this lifetime (150—890 μs) in solutions. The quantum yield of luminescence of EuFOD3 was estimate as ≈4×10-4.

Effect of antimony incorporation on the density, shape, and luminescence of InAs quantum dots

NASA Astrophysics Data System (ADS)

Chen, J. F.; Chiang, C. H.; Wu, Y. H.; Chang, L.; Chi, J. Y.

2008-07-01

This work investigates the surfactant effect on exposed and buried InAs quantum dots (QDs) by incorporating Sb into the QD layers with various Sb beam equivalent pressures (BEPs). Secondary ion mass spectroscopy shows the presence of Sb in the exposed and buried QD layers with the Sb intensity in the exposed layer substantially exceeding that in the buried layer. Incorporating Sb can reduce the density of the exposed QDs by more than two orders of magnitude. However, a high Sb BEP yields a surface morphology with a regular periodic structure of ellipsoid terraces. A good room-temperature photoluminescence (PL) at ˜1600 nm from the exposed QDs is observed, suggesting that the Sb incorporation probably improves the emission efficiency by reducing the surface recombination velocity at the surface of the exposed QDs. Increasing Sb BEP causes a blueshift of the emission from the exposed QDs due to a reduction in the dot height as suggested by atomic force microscopy. Increasing Sb BEP can also blueshift the ˜1300 nm emission from the buried QDs by decreasing the dot height. However, a high Sb BEP yields a quantum well-like PL feature formed by the clustering of the buried QDs into an undulated planar layer. These results indicate a marked Sb surfactant effect that can be used to control the density, shape, and luminescence of the exposed and buried QDs.

Modeling quantum yield, emittance, and surface roughness effects from metallic photocathodes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dimitrov, D. A.; Bell, G. I.; Smedley, J.

Here, detailed measurements of momentum distributions of emitted electrons have allowed the investigation of the thermal limit of the transverse emittance from metal photocathodes. Furthermore, recent developments in material design and growth have resulted in photocathodes that can deliver high quantum efficiency and are sufficiently robust to use in high electric field gradient photoinjectors and free electron lasers. The growth process usually produces photoemissive material layers with rough surface profiles that lead to transverse accelerating fields and possible work function variations, resulting in emittance growth. To better understand the effects of temperature, density of states, and surface roughness on themore » properties of emitted electrons, we have developed realistic three-dimensional models for photocathode materials with grated surface structures. They include general modeling of electron excitation due to photon absorption, charge transport, and emission from flat and rough metallic surfaces. The models also include image charge and field enhancement effects. We report results from simulations with flat and rough surfaces to investigate how electron scattering, controlled roughness, work function variation, and field enhancement affect emission properties. Comparison of simulation results with measurements of the quantum yield and transverse emittance from flat Sb emission surfaces shows the importance of including efficient modeling of photon absorption, temperature effects, and the material density of states to achieve agreement with the experimental data.« less

Modeling quantum yield, emittance, and surface roughness effects from metallic photocathodes

DOE PAGES

Dimitrov, D. A.; Bell, G. I.; Smedley, J.; ...

2017-10-26

Here, detailed measurements of momentum distributions of emitted electrons have allowed the investigation of the thermal limit of the transverse emittance from metal photocathodes. Furthermore, recent developments in material design and growth have resulted in photocathodes that can deliver high quantum efficiency and are sufficiently robust to use in high electric field gradient photoinjectors and free electron lasers. The growth process usually produces photoemissive material layers with rough surface profiles that lead to transverse accelerating fields and possible work function variations, resulting in emittance growth. To better understand the effects of temperature, density of states, and surface roughness on themore » properties of emitted electrons, we have developed realistic three-dimensional models for photocathode materials with grated surface structures. They include general modeling of electron excitation due to photon absorption, charge transport, and emission from flat and rough metallic surfaces. The models also include image charge and field enhancement effects. We report results from simulations with flat and rough surfaces to investigate how electron scattering, controlled roughness, work function variation, and field enhancement affect emission properties. Comparison of simulation results with measurements of the quantum yield and transverse emittance from flat Sb emission surfaces shows the importance of including efficient modeling of photon absorption, temperature effects, and the material density of states to achieve agreement with the experimental data.« less

Highly luminescent colloidal nanoplates of perovskite cesium lead halide and their oriented assemblies

DOE PAGES

Bekenstein, Yehonadav; Koscher, Brent A.; Eaton, Samuel W.; ...

2015-12-15

Anisotropic colloidal quasi-two-dimensional nanoplates (NPLs) hold great promise as functional materials due to their combination of low dimensional optoelectronic properties and versatility through colloidal synthesis. Recently, lead-halide perovskites have emerged as important optoelectronic materials with excellent efficiencies in photovoltaic and light-emitting applications. Here we report the synthesis of quantum confined all inorganic cesium lead halide nanoplates in the perovskite crystal structure that are also highly luminescent (PLQY 84%). The controllable self-assembly of nanoplates either into stacked columnar phases or crystallographic-oriented thin-sheet structures is demonstrated. Furthermore, the broad accessible emission range, high native quantum yields, and ease of self-assembly make perovskitemore » NPLs an ideal platform for fundamental optoelectronic studies and the investigation of future devices.« less

Direct impact of the sustained decline in the photosystem II efficiency upon plant productivity at different developmental stages.

PubMed

Tian, Yonglan; Ungerer, Petra; Zhang, Huayong; Ruban, Alexander V

2017-05-01

The impact of chronic photoinhibition of photosystem II (PSII) on the productivity of plants remains unknown. The present study investigated the influences of persistent decline in the PSII yield on morphology and productivity of Arabidopsis plants that were exposed to lincomycin at two different developmental stages (seedling and rosette stage). The results indicated that, although retarded, the lincomycin treated plants were able to accomplish the entire growth period with only 50% of the maximum quantum yield of primary photochemistry (Fv/Fm) of the control plants. The decline in quantum yield limited the electron transport rate (ETR). The impact of lincomycin on NPQ was not significant in seedlings, but was pronounced in mature plants. The treated plants produced an above ground biomass of 50% compared to control plants. Moreover, a linear relationship was found between the above ground biomass and total rosette leaf area, and the slope was decreased due to photoinhibition. The starch accumulation was highly inhibited by lincomycin treatment. Lincomycin induced a significant decrease in seed yield with plants treated from the rosette state showing higher yield than those treated from the seedling stage. Our data suggest that the sustained decline of PSII efficiency decreases plant productivity by constraining the ETR, leaf development and starch production. Copyright © 2017 Elsevier GmbH. All rights reserved.

Photodissociation of quantum state-selected diatomic molecules yields new insight into ultracold chemistry

NASA Astrophysics Data System (ADS)

McDonald, Mickey; McGuyer, Bart H.; Lee, Chih-Hsi; Apfelbeck, Florian; Zelevinsky, Tanya

2016-05-01

When a molecule is subjected to a sufficiently energetic photon it can break apart into fragments through a process called ``photodissociation''. For over 70 years this simple chemical reaction has served as a vital experimental tool for acquiring information about molecular structure, since the character of the photodissociative transition can be inferred by measuring the 3D photofragment angular distribution (PAD). While theoretical understanding of this process has gradually evolved from classical considerations to a fully quantum approach, experiments to date have not yet revealed the full quantum nature of this process. In my talk I will describe recent experiments involving the photodissociation of ultracold, optical lattice-trapped, and fully quantum state-resolved 88Sr2 molecules. Optical absorption images of the PADs produced in these experiments reveal features which are inherently quantum mechanical in nature, such as matter-wave interference between output channels, and are sensitive to the quantum statistics of the molecular wavefunctions. The results of these experiments cannot be predicted using quasiclassical methods. Instead, we describe our results with a fully quantum mechanical model yielding new intuition about ultracold chemistry.

Transport properties of N2 gas at cryogenic temperatures. [computation of viscosity and thermal conductivity

NASA Technical Reports Server (NTRS)

Pearson, W. E.

1974-01-01

The viscosity and thermal conductivity of nitrogen gas for the temperature range 5 K - 135 K have been computed from the second Chapman-Enskog approximation. Quantum effects, which become appreciable at the lower temperatures, are included by utilizing collision integrals based on quantum theory. A Lennard-Jones (12-6) potential was assumed. The computations yield viscosities about 20 percent lower than those predicted for the high end of this temperature range by the method of corresponding states, but the agreement is excellent when the computed values are compared with existing experimental data.

Measurement of the entanglement of two superconducting qubits via state tomography.

PubMed

Steffen, Matthias; Ansmann, M; Bialczak, Radoslaw C; Katz, N; Lucero, Erik; McDermott, R; Neeley, Matthew; Weig, E M; Cleland, A N; Martinis, John M

2006-09-08

Demonstration of quantum entanglement, a key resource in quantum computation arising from a nonclassical correlation of states, requires complete measurement of all states in varying bases. By using simultaneous measurement and state tomography, we demonstrated entanglement between two solid-state qubits. Single qubit operations and capacitive coupling between two super-conducting phase qubits were used to generate a Bell-type state. Full two-qubit tomography yielded a density matrix showing an entangled state with fidelity up to 87%. Our results demonstrate a high degree of unitary control of the system, indicating that larger implementations are within reach.

Quantum leadership: the implication for Iranian nursing leaders.

PubMed

Dargahi, Hossein

2013-07-13

Quantum organizations are referred where stakeholders know how to access the infinite potential of the quantum field. Viewing healthcare organizations from perspective of quantum theory suggest new approaches into management techniques for effective and efficient delivery of healthcare services. This research is aimed to determine the quantum skills, quantum leadership characteristics and functions of Tehran University of Medical Sciences hospitals' nursing administrators. A cross-sectional, descriptive and analytical study was conducted among 25 nursing administrators of Tehran University of Medical Sciences (TUMS) hospitals, Tehran, Iran. The research tool for data collection was a self-constructed questionnaire that measured the quantum skills, quantum leadership characteristics and functions of TUMS hospitals' nursing administrators. The validity of questionnaire was confirmed by 5 management science experts and its reliability was performed by using test-retest method yielded a Cronbach's alpha coefficient of 0.90. Data were collected and analyzed by SPSS software and t-test statistical methods. The results of this research showed that all respondents had desired quantum skills (75.71±5.98), quantum leadership characteristics (82.01±6.77), and quantum leadership functions (78.57±6.28) and total quantum leadership (78.76±4.50). Also, passing management training courses of the respondents was significantly correlated with their quantum leadership. Iranian healthcare organizations require quantum leadership that provides an important resource to advance Iranian nursing leadership to the organizational excellence. We hope Iranian hospitals' nursing leaders who have quantum skills potentially, present a highly developed sense of self and the ability to improve nursing care outcomes in these hospitals.

Lead-free/rare earth-free Green-light-emitting crystal based on organic-inorganic hybrid [(C10H16N)2][MnBr4] with high emissive quantum yields and large crystal size

NASA Astrophysics Data System (ADS)

Cai, Xing-Wei; Zhao, Yu-Yuan; Li, Hong; Huang, Cui-Ping; Zhou, Zhen

2018-06-01

With the flourishing development of emitting materials, tremendous technological progress has been accomplished. However, they still face great challenges in convenient economical environmental-friendly large-scale commercial production. Herein we designed this organic-inorganic hybrid lead-free compound, an emerging class of high-efficiency emitting materials, [(C10H16N)2][MnBr4] (1), which emits intense greenish photoluminescence with a high emissive quantum yields of 72.26%, was prepared through the convenient economical solution method. What's more, compared with rare earth fluorescent materials (especially green-emitting Tb), Mn material is rich in natural resources and low commercial cost, which would possess an increasingly predominant advantage in the preparation of luminescent materials. Additionally, the exceptional thermal stability as well as the low-cost/convenient preparation process makes crystal 1 with the large size of more than 1 cm to be an ideal technologically important green-emitting material and it would open up a new route towards the commercialization process of lead-free/rare earth-free hybrid emitting materials in display and sensing.

Surface states in the photoionization of high-quality CdSe core/shell nanocrystals.

PubMed

Li, Shu; Steigerwald, Michael L; Brus, Louis E

2009-05-26

We use electric force microscopy (EFM) to study single nanocrystal photoionization in two classes of high-quality nanocrystals whose exciton luminescence quantum yields approach unity in solution. The CdSe/CdS/ZnS core/shell nanocrystals do not photoionize, while the CdSe/CdS nanocrystals do show substantial photoionization. This verifies the theoretical prediction that the ZnS shell confines the excited electron within the nanocrystal. Despite the high luminescence quantum yield, photoionization varies substantially among the CdSe/CdS nanocrystals. We have studied the nanocrystal photoionization with both UV (396 nm) and green (532 nm) light, and we have found that the magnitude of the charge due to photoionization per absorbed photon is greater for UV excitation than for green excitation. A fraction of the photoionization occurs directly via a "hot electron" process, using trap states that are either on the particle surface, within the ligand sphere, or within the silicon oxide layer. This must occur without relaxation to the thermalized, lowest-energy, emitting exciton. We discuss the occurrence of hot carrier processes that are common to photoionization, luminescence blinking, and the fast transient optical absorption that is associated with multiple exciton generation MEG studies.

Optimal nitrogen and phosphorus codoping carbon dots towards white light-emitting device

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhang, Feng; Wang, Yaling; Miao, Yanqin

Through a one-step fast microwave-assisted approach, nitrogen and phosphorus co-doped carbon dots (N,P-CDs) were synthesized using ammonium citrate (AC) as a carbon source and phosphates as additive reagent. Under the condition of an optimal reaction time of 140 s, the influence of additive with different N and P content on fluorescent performance of N,P-CDs was further explored. It was concluded that high nitrogen content and moderate phosphorus content are necessary for obtaining high quantum yield (QY) N,P-CDs, among which the TAP-CDs (CDs synthesized using ammonium phosphate as additive reagent) show high quantum yield (QY) of 62% and red-green-blue (RGB) spectral compositionmore » of 51.67%. Besides, the TAP-CDs exhibit satisfying thermal stability within 180 °C. By virtue of good optical and thermal properties of TAP-CDs, a white light-emitting device (LED) was fabricated by combining ultraviolet chip with TAP-CDs as phosphor. The white LED emits bright warm-white light with the CIE chromaticity coordinate of (0.38, 0.35) and the corresponding color temperature (CCT) of 4450 K, indicating the potential of TAP-CDs phosphor in white LED.« less

Continuous Purification of Colloidal Quantum Dots in Large-Scale Using Porous Electrodes in Flow Channel.

PubMed

Lim, Hosub; Woo, Ju Young; Lee, Doh C; Lee, Jinkee; Jeong, Sohee; Kim, Duckjong

2017-02-27

Colloidal quantum dots (QDs) afford huge potential in numerous applications owing to their excellent optical and electronic properties. After the synthesis of QDs, separating QDs from unreacted impurities in large scale is one of the biggest issues to achieve scalable and high performance optoelectronic applications. Thus far, however, continuous purification method, which is essential for mass production, has rarely been reported. In this study, we developed a new continuous purification process that is suitable to the mass production of high-quality QDs. As-synthesized QDs are driven by electrophoresis in a flow channel and captured by porous electrodes and finally separated from the unreacted impurities. Nuclear magnetic resonance and ultraviolet/visible/near-infrared absorption spectroscopic data clearly showed that the impurities were efficiently removed from QDs with the purification yield, defined as the ratio of the mass of purified QDs to that of QDs in the crude solution, up to 87%. Also, we could successfully predict the purification yield depending on purification conditions with a simple theoretical model. The proposed large-scale purification process could be an important cornerstone for the mass production and industrial use of high-quality QDs.

Continuous Purification of Colloidal Quantum Dots in Large-Scale Using Porous Electrodes in Flow Channel

NASA Astrophysics Data System (ADS)

Lim, Hosub; Woo, Ju Young; Lee, Doh Chang; Lee, Jinkee; Jeong, Sohee; Kim, Duckjong

2017-11-01

Colloidal Quantum dots (QDs) afford huge potential in numerous applications owing to their excellent optical and electronic properties. After the synthesis of QDs, separating QDs from unreacted impurities in large scale is one of the biggest issues to achieve scalable and high performance optoelectronic applications. Thus far, however, continuous purification method, which is essential for mass production, has rarely been reported. In this study, we developed a new continuous purification process that is suitable to the mass production of high-quality QDs. As-synthesized QDs are driven by electrophoresis in a flow channel and captured by porous electrodes and finally separated from the unreacted impurities. Nuclear magnetic resonance and ultraviolet/visible/near-infrared absorption spectroscopic data clearly showed that the impurities were efficiently removed from QDs with the purification yield, defined as the ratio of the mass of purified QDs to that of QDs in the crude solution, up to 87%. Also, we could successfully predict the purification yield depending on purification conditions with a simple theoretical model. The proposed large-scale purification process could be an important cornerstone for the mass production and industrial use of high-quality QDs.

Quantum yield for carbon monoxide production in the 248 nm photodissociation of carbonyl sulfide (OCS)

NASA Technical Reports Server (NTRS)

Zhao, Z.; Stickel, R. E.; Wine, P. H.

1995-01-01

Tunable diode laser absorption spectroscopy has been coupled with excimer laser flash photolysis to measure the quantum yield for CO production from 248 nm photodissociation of carbonyl sulfide (OCS) relative to the well-known quantum yield for CO production from 248 nm photolysis of phosgene (Cl2CO2). The temporal resolution of the experiments was sufficient to distinguish CO formed directly by photodissociation from that formed by subsequent S((sup 3)P(sub J)) reaction with OCS. Under the experimental conditions employed, CO formation via the fast S((sup 1)D(sub 2)) + OCS reaction was minimal. Measurements at 297K and total pressures from 4 to 100 Torr N2 + N2O show the CO yield to be greater than 0.95 and most likely unity. This result suggests that the contribution of OCS as a precursor to the lower stratospheric sulfate aerosol layer is somewhat larger than previously thought.

A semi-classical approach to the calculation of highly excited rotational energies for asymmetric-top molecules

PubMed Central

Schmiedt, Hanno; Schlemmer, Stephan; Yurchenko, Sergey N.; Yachmenev, Andrey

2017-01-01

We report a new semi-classical method to compute highly excited rotational energy levels of an asymmetric-top molecule. The method forgoes the idea of a full quantum mechanical treatment of the ro-vibrational motion of the molecule. Instead, it employs a semi-classical Green's function approach to describe the rotational motion, while retaining a quantum mechanical description of the vibrations. Similar approaches have existed for some time, but the method proposed here has two novel features. First, inspired by the path integral method, periodic orbits in the phase space and tunneling paths are naturally obtained by means of molecular symmetry analysis. Second, the rigorous variational method is employed for the first time to describe the molecular vibrations. In addition, we present a new robust approach to generating rotational energy surfaces for vibrationally excited states; this is done in a fully quantum-mechanical, variational manner. The semi-classical approach of the present work is applied to calculating the energies of very highly excited rotational states and it reduces dramatically the computing time as well as the storage and memory requirements when compared to the fullly quantum-mechanical variational approach. Test calculations for excited states of SO2 yield semi-classical energies in very good agreement with the available experimental data and the results of fully quantum-mechanical calculations. PMID:28000807

Culture expansion of adipose derived stromal cells. A closed automated Quantum Cell Expansion System compared with manual flask-based culture.

PubMed

Haack-Sørensen, Mandana; Follin, Bjarke; Juhl, Morten; Brorsen, Sonja K; Søndergaard, Rebekka H; Kastrup, Jens; Ekblond, Annette

2016-11-16

Adipose derived stromal cells (ASCs) are a rich and convenient source of cells for clinical regenerative therapeutic approaches. However, applications of ASCs often require cell expansion to reach the needed dose. In this study, cultivation of ASCs from stromal vascular fraction (SVF) over two passages in the automated and functionally closed Quantum Cell Expansion System (Quantum system) is compared with traditional manual cultivation. Stromal vascular fraction was isolated from abdominal fat, suspended in α-MEM supplemented with 10% Fetal Bovine Serum and seeded into either T75 flasks or a Quantum system that had been coated with cryoprecipitate. The cultivation of ASCs from SVF was performed in 3 ways: flask to flask; flask to Quantum system; and Quantum system to Quantum system. In all cases, quality controls were conducted for sterility, mycoplasmas, and endotoxins, in addition to the assessment of cell counts, viability, immunophenotype, and differentiation potential. The viability of ASCs passage 0 (P0) and P1 was above 96%, regardless of cultivation in flasks or Quantum system. Expression of surface markers and differentiation potential was consistent with ISCT/IFATS standards for the ASC phenotype. Sterility, mycoplasma, and endotoxin tests were consistently negative. An average of 8.0 × 10 7 SVF cells loaded into a Quantum system yielded 8.96 × 10 7 ASCs P0, while 4.5 × 10 6 SVF cells seeded per T75 flask yielded an average of 2.37 × 10 6 ASCs-less than the number of SVF cells seeded. ASCs P1 expanded in the Quantum system demonstrated a population doubling (PD) around 2.2 regardless of whether P0 was previously cultured in flasks or Quantum, while ASCs P1 in flasks only reached a PD of 1.0. Manufacturing of ASCs in a Quantum system enhances ASC expansion rate and yield significantly relative to manual processing in T-flasks, while maintaining the purity and quality essential to safe and robust cell production. Notably, the use of the Quantum system entails significantly reduced working hours and thereby costs.

Analysis of wavelength-dependent photoisomerization quantum yields in bilirubins by fitting two exciton absorption bands

NASA Astrophysics Data System (ADS)

Mazzoni, M.; Agati, G.; Troup, G. J.; Pratesi, R.

2003-09-01

The absorption spectra of bilirubins were deconvoluted by two Gaussian curves of equal width representing the exciton bands of the non-degenerate molecular system. The two bands were used to study the wavelength dependence of the (4Z, 15Z) rightarrow (4Z, 15E) configurational photoisomerization quantum yield of the bichromophoric bilirubin-IXalpha (BR-IX), the intrinsically asymmetric bile pigment associated with jaundice and the symmetrically substituted bilirubins (bilirubin-IIIalpha and mesobilirubin-XIIIalpha), when they are irradiated in aqueous solution bound to human serum albumin (HSA). The same study was performed for BR-IX in ammoniacal methanol solution (NH4OH/MeOH). The quantum yields of the configurational photoprocesses were fitted with a combination function of the two Gaussian bands normalized to the total absorption, using the proportionality coefficients and a scaling factor as parameters. The decrease of the (4Z, 15Z) rightarrow (4Z, 15E) quantum yield with increasing wavelength, which occurs for wavelengths longer than the most probable Franck-Condon transition of the molecule, did not result in a unique function of the exciton absorptions. In particular we found two ranges corresponding to different exciton interactions with different proportionality coefficients and scaling factors. The wavelength-dependent photoisomerization of bilirubins was described as an abrupt change in quantum yield as soon as the resulting excitation was strongly localized in each chromophore. The change was correlated to a variation of the interaction between the two chromophores when the short-wavelength exciton absorption became vanishingly small. With the help of the circular dichroism (CD) spectrum of BR-IX in HSA, a small band was resolved in the bilirubin absorption spectrum, delivering part of the energy required for the (4Z, 15Z) rightarrow (4Z, 15E) photoisomerization of the molecule.

Emulsion Synthesis of Size-Tunable CH3NH3PbBr3 Quantum Dots: An Alternative Route toward Efficient Light-Emitting Diodes.

PubMed

Huang, Hailong; Zhao, Fangchao; Liu, Lige; Zhang, Feng; Wu, Xian-gang; Shi, Lijie; Zou, Bingsuo; Pei, Qibing; Zhong, Haizheng

2015-12-30

We report a facile nonaqueous emulsion synthesis of colloidal halide perovskite quantum dots by controlled addition of a demulsifier into an emulsion of precursors. The size of resulting CH3NH3PbBr3 quantum dots can be tuned from 2 to 8 nm by varying the amount of demulsifier. Moreover, this emulsion synthesis also allows the purification of these quantum dots by precipitation from the colloidal solution and obtains solid-state powder which can be redissolved for thin film coating and device fabrication. The photoluminescence quantum yields of the quantum dots is generally in the range of 80-92%, and can be well-preserved after purification (∼80%). Green light-emitting diodes fabricated comprising a spin-cast layer of the colloidal CH3NH3PbBr3 quantum dots exhibited maximum current efficiency of 4.5 cd/A, power efficiency of 3.5 lm/W, and external quantum efficiency of 1.1%. This provides an alternative route toward high efficient solution-processed perovskite-based light-emitting diodes. In addition, the emulsion synthesis is versatile and can be extended for the fabrication of inorganic halide perovskite colloidal CsPbBr3 nanocrystals.

Demonstration of analyzers for multimode photonic time-bin qubits

NASA Astrophysics Data System (ADS)

Jin, Jeongwan; Agne, Sascha; Bourgoin, Jean-Philippe; Zhang, Yanbao; Lütkenhaus, Norbert; Jennewein, Thomas

2018-04-01

We demonstrate two approaches for unbalanced interferometers as time-bin qubit analyzers for quantum communication, robust against mode distortions and polarization effects as expected from free-space quantum communication systems including wavefront deformations, path fluctuations, pointing errors, and optical elements. Despite strong spatial and temporal distortions of the optical mode of a time-bin qubit, entangled with a separate polarization qubit, we verify entanglement using the Negative Partial Transpose, with the measured visibility of up to 0.85 ±0.01 . The robustness of the analyzers is further demonstrated for various angles of incidence up to 0 .2∘ . The output of the interferometers is coupled into multimode fiber yielding a high system throughput of 0.74. Therefore, these analyzers are suitable and efficient for quantum communication over multimode optical channels.

Cadmium-containing quantum dots: properties, applications, and toxicity.

PubMed

Mo, Dan; Hu, Liang; Zeng, Guangming; Chen, Guiqiu; Wan, Jia; Yu, Zhigang; Huang, Zhenzhen; He, Kai; Zhang, Chen; Cheng, Min

2017-04-01

The marriage of biology with nanomaterials has significantly accelerated advancement of biological techniques, profoundly facilitating practical applications in biomedical fields. With unique optical properties (e.g., tunable broad excitation, narrow emission spectra, robust photostability, and high quantum yield), fluorescent quantum dots (QDs) have been reasonably functionalized with controllable interfaces and extensively used as a new class of optical probe in biological researches. In this review, we summarize the recent progress in synthesis and properties of QDs. Moreover, we provide an overview of the outstanding potential of QDs for biomedical research and innovative methods of drug delivery. Specifically, the applications of QDs as novel fluorescent nanomaterials for biomedical sensing and imaging have been detailedly highlighted and discussed. In addition, recent concerns on potential toxicity of QDs are also introduced, ranging from cell researches to animal models.

Laser flash photolysis of ozone - O/1D/ quantum yields in the fall-off region 297-325 nm

NASA Technical Reports Server (NTRS)

Brock, J. C.; Watson, R. T.

1980-01-01

The wavelength dependence of the quantum yield for O(1D) production from ozone photolysis has been determined between 297.5 nm and 325 nm in order to resolve serious discrepancies among previous studies. The results of this investigation are compared to earlier work by calculating atmospheric production rate constants for O(1D). It is found that for the purpose of calculating this rate constant, there is now good agreement among three studies at 298 K. Furthermore, it appears that previous data on the temperature dependence of the O(1D) quantum yield fall-off is adequate for determining the vertical profile of the O(1D) production rate constant. Several experimental difficulties associated with using NO2(asterisk) chemiluminescence to monitor O(1D) have been identified.

Quantitative photoabsorption and fluorescence spectroscopy of benzene, naphthalene, and some derivatives at 106-295 nm

NASA Technical Reports Server (NTRS)

Suto, Masako; Wang, Xiuyan; Shan, Jun; Lee, L. C.

1992-01-01

Photoabsorption and fluorescence cross sections of benzene, (o-, m-, p-) xylenes, naphthalene, 1-methylnaphthalene, and 2-ethylnaphthalene in the gas phase are measured at 106-295 nm using synchrotron radiation as a light source. Fluorescences are observed from the photoexcitation of benzene and xylenes at 230-280 nm and from naphthalene and its derivatives at 190-295 nm. The absolute fluorescence cross section is determined by calibration with respect to the emission intensity of the NO(A-X) system, for which the fluorescence quantum yield is equal to 1. To cross-check the current calibration method, the quantum yield of the SO2(C-X) system at 220-230 nm was measured since it is about equal to 1. The current quantum-yield data are compared with previously published values measured by different methods.

Production of graphene quantum dots by ultrasound-assisted exfoliation in supercritical CO2/H2O medium.

PubMed

Gao, Hanyang; Xue, Chen; Hu, Guoxin; Zhu, Kunxu

2017-07-01

In this research, three kinds of graphene quantum dots (GQDs)-pristine graphene quantum dots (PGQDs), expanded graphene quantum dots (EGQDs) and graphene oxide quantum dots (GOQDs)-were produced from natural graphite, expanded graphite, and oxide graphite respectively in an ultrasound-assisted supercritical CO 2 (scCO 2 )/H 2 O system. The effects of aqueous solution content ratio, system pressure, and ultrasonic power on the yields of different kinds of GQDs were investigated. According to these experiment results, the combination of the intense knocking force generated from high-pressure acoustic cavitation in a scCO 2 /H 2 O system and the superior penetration ability of scCO 2 was considered to be the key to the successful exfoliation of such tiny pieces from bulk graphite. An interesting result was found that, contrary to common experience, the yield of PGQDs from natural graphite was much higher than that of GOQDs from graphite oxide. Based on the experimental analysis, the larger interlayer resistance of natural graphite, which hindered the insertion of scCO 2 molecules, and the hydrophobic property of natural graphite surface, which made the planar more susceptible to the attack of ultrasonic collapsing bubbles, were deduced to be the two main reasons for this result. The differences in characteristics among the three kinds of GQDs were also studied and compared in this research. In our opinion, this low-cost and time-saving method may provide an alternative green route for the production of various kinds of GQDs, especially PGQDs. Copyright © 2017 Elsevier B.V. All rights reserved.

Developing a diagnostic model for estimating terrestrial vegetation gross primary productivity using the photosynthetic quantum yield and Earth Observation data.

PubMed

Ogutu, Booker O; Dash, Jadunandan; Dawson, Terence P

2013-09-01

This article develops a new carbon exchange diagnostic model [i.e. Southampton CARbon Flux (SCARF) model] for estimating daily gross primary productivity (GPP). The model exploits the maximum quantum yields of two key photosynthetic pathways (i.e. C3 and C4 ) to estimate the conversion of absorbed photosynthetically active radiation into GPP. Furthermore, this is the first model to use only the fraction of photosynthetically active radiation absorbed by photosynthetic elements of the canopy (i.e. FAPARps ) rather than total canopy, to predict GPP. The GPP predicted by the SCARF model was comparable to in situ GPP measurements (R(2)  > 0.7) in most of the evaluated biomes. Overall, the SCARF model predicted high GPP in regions dominated by forests and croplands, and low GPP in shrublands and dry-grasslands across USA and Europe. The spatial distribution of GPP from the SCARF model over Europe and conterminous USA was comparable to those from the MOD17 GPP product except in regions dominated by croplands. The SCARF model GPP predictions were positively correlated (R(2)  > 0.5) to climatic and biophysical input variables indicating its sensitivity to factors controlling vegetation productivity. The new model has three advantages, first, it prescribes only two quantum yield terms rather than species specific light use efficiency terms; second, it uses only the fraction of PAR absorbed by photosynthetic elements of the canopy (FAPARps ) hence capturing the actual PAR used in photosynthesis; and third, it does not need a detailed land cover map that is a major source of uncertainty in most remote sensing based GPP models. The Sentinel satellites planned for launch in 2014 by the European Space Agency have adequate spectral channels to derive FAPARps at relatively high spatial resolution (20 m). This provides a unique opportunity to produce global GPP operationally using the Southampton CARbon Flux (SCARF) model at high spatial resolution. © 2013 John Wiley & Sons Ltd.

SU-D-BRB-05: Quantum Learning for Knowledge-Based Response-Adaptive Radiotherapy

DOE Office of Scientific and Technical Information (OSTI.GOV)

El Naqa, I; Ten, R

Purpose: There is tremendous excitement in radiotherapy about applying data-driven methods to develop personalized clinical decisions for real-time response-based adaptation. However, classical statistical learning methods lack in terms of efficiency and ability to predict outcomes under conditions of uncertainty and incomplete information. Therefore, we are investigating physics-inspired machine learning approaches by utilizing quantum principles for developing a robust framework to dynamically adapt treatments to individual patient’s characteristics and optimize outcomes. Methods: We studied 88 liver SBRT patients with 35 on non-adaptive and 53 on adaptive protocols. Adaptation was based on liver function using a split-course of 3+2 fractions with amore » month break. The radiotherapy environment was modeled as a Markov decision process (MDP) of baseline and one month into treatment states. The patient environment was modeled by a 5-variable state represented by patient’s clinical and dosimetric covariates. For comparison of classical and quantum learning methods, decision-making to adapt at one month was considered. The MDP objective was defined by the complication-free tumor control (P{sup +}=TCPx(1-NTCP)). A simple regression model represented state-action mapping. Single bit in classical MDP and a qubit of 2-superimposed states in quantum MDP represented the decision actions. Classical decision selection was done using reinforcement Q-learning and quantum searching was performed using Grover’s algorithm, which applies uniform superposition over possible states and yields quadratic speed-up. Results: Classical/quantum MDPs suggested adaptation (probability amplitude ≥0.5) 79% of the time for splitcourses and 100% for continuous-courses. However, the classical MDP had an average adaptation probability of 0.5±0.22 while the quantum algorithm reached 0.76±0.28. In cases where adaptation failed, classical MDP yielded 0.31±0.26 average amplitude while the quantum approach averaged a more optimistic 0.57±0.4, but with high phase fluctuations. Conclusion: Our results demonstrate that quantum machine learning approaches provide a feasible and promising framework for real-time and sequential clinical decision-making in adaptive radiotherapy.« less

Excited-state properties of nucleic acid components

NASA Astrophysics Data System (ADS)

Salet, C.; Bensasson, R. V.; Becker, R. S.

1981-12-01

Measurements were made of the fluorescence and phosphorescence spectra and lifetimes, and also of the absorption spectra, lifetimes, extinction coefficients, and quantum yields of the T1 lower triplet states of thymine, uracil, their N, N'-dimethyl derivatives, thymidine, thymidine monophosphate, uridine, and uridine monophosphate in various solvents at 300 °K. The influence of the solvent on the quantum yield of the T1 state of nucleic acid components is discussed.

Laboratory Measurements of Photolytic Parameters for Formaldehyde.

DTIC Science & Technology

1980-11-01

dynamic dilution methods. Compressed air stored in steel cylinders, carefully selected to contain carbon monoxide and hydrogen at mixing ratios of...in air has been investi- gated in the laboratory at two temperatures: 300 and 220 K. Quantum yields for the formation of CO and H2 were determined at...procedures in the case of pure formaldehyde gave consistent results. (b) Quantum Yields Mixtures of formaldehyde in air were photolyzed in a

Synthesis and characterization of near-infrared absorbing water soluble squaraines and study of their photodynamic effects in DLA live cells.

PubMed

Shafeekh, Kulathinte M; Soumya, Mohanannair S; Rahim, Moochikkadavath A; Abraham, Annie; Das, Suresh

2014-01-01

Here, we report the synthesis, photophysical properties and photodynamic effects in DLA live cells of three water soluble squaraine dyes, viz. bisbenzothiazolium squaraine dyes SQMI and SQDI with iodine in one and both benzothiazolium units, respectively, and an unsymmetrical squaraine dye ASQI containing iodinated benzothiazolium and aniline substituents. The diiodinated SQDI showed an anomalous trend in both fluorescence and triplet quantum yields over the monoiodinated SQMI, with SQDI showing higher fluorescence and lower triplet quantum yields compared to SQMI. Nanosecond laser flash photolysis of SQDI and SQMI indicated the formation of triplet excited states with quantum yield of 0.19 and 0.26, respectively. On photoirradiation, both the SQDI and SQMI generate singlet oxygen and it was observed that both dyes undergoing oxidation reactions with the singlet oxygen generated. ASQI which exhibited a lower triplet quantum yield of 0.06 was, however, stable and did not react with the singlet oxygen generated. In vitro cytotoxicity studies of these dyes in DLA live cells were performed using Trypan blue dye exclusion method and it reflect an order of cytotoxicity of SQDI>SQMI>ASQI. Intracellular generation of the ROS was confirmed by dichlorofluorescein assay after the in vitro PDT. © 2014 The American Society of Photobiology.

Efficiencies of induction of DNA double strand breaks in solution by photoabsorption at phosphorus and platinum.

PubMed

Maeda, Munetoshi; Kobayashi, Katsumi; Hieda, Kotaro

2004-01-01

This paper aims at determining and comparing the cross sections and quantum yields for DNA strand break induction by the Auger effect at the K-shell of phosphorus and at the LIII-shell of platinum. Using synchrotron radiation, free and Pt-bound pBR322 plasmid DNA were irradiated in solution with monochromatic X-rays, the energies of which were 2.153 and 2.147 keV, corresponding to "on" and "below" the phosphorus K-shell photoabsorption, and 11.566 and 11.542 keV for "above" and "below" the L(III)-shell photoabsorption of platinum, respectively. To suppress indirect effects by hydroxyl radicals, DMSO (1M) was used as a scavenger. The inner-shell photoabsorption of phosphorus and of platinum significantly increased the induction of DNA double strand breaks (DSB), whereas it had little effect on single strand break (SSB) induction. The quantum yields for the induction of DSB were calculated to be 0.017 and 1.13, in the case of phosphorus and platinum, respectively. CONCLSIONS: The value of the quantum yield for the DSB induction of platinum was about 66-fold larger than that for the phosphorus. These results clearly demonstrate that the quantum yield of DSB depends upon the magnitude of the Auger cascade.

Faster search by lackadaisical quantum walk

NASA Astrophysics Data System (ADS)

Wong, Thomas G.

2018-03-01

In the typical model, a discrete-time coined quantum walk searching the 2D grid for a marked vertex achieves a success probability of O(1/log N) in O(√{N log N}) steps, which with amplitude amplification yields an overall runtime of O(√{N} log N). We show that making the quantum walk lackadaisical or lazy by adding a self-loop of weight 4 / N to each vertex speeds up the search, causing the success probability to reach a constant near 1 in O(√{N log N}) steps, thus yielding an O(√{log N}) improvement over the typical, loopless algorithm. This improved runtime matches the best known quantum algorithms for this search problem. Our results are based on numerical simulations since the algorithm is not an instance of the abstract search algorithm.

Adapting BODIPYs to singlet oxygen production on silica nanoparticles.

PubMed

Epelde-Elezcano, Nerea; Prieto-Montero, Ruth; Martínez-Martínez, Virginia; Ortiz, María J; Prieto-Castañeda, Alejandro; Peña-Cabrera, Eduardo; Belmonte-Vázquez, José L; López-Arbeloa, Iñigo; Brown, Ross; Lacombe, Sylvie

2017-05-31

A modified Stöber method is used to synthesize spherical core-shell silica nanoparticles (NPs) with an external surface functionalized by amino groups and with an average size around 50 nm. Fluorescent dyes and photosensitizers of singlet oxygen were fixed, either separately or conjointly, respectively in the core or in the shell. Rhodamines were encapsulated in the core with relatively high fluorescence quantum yields (Φ fl ≥ 0.3), allowing fluorescence tracking of the particles. Various photosensitizers of singlet oxygen (PS) were covalenty coupled to the shell, allowing singlet oxygen production. The stability of NP suspensions strongly deteriorated upon grafting the PS, affecting their apparent singlet oxygen quantum yields. Agglomeration of NPs depends both on the type and on the amount of grafted photosensitizer. New, lab-made, halogenated 4,4-difluoro-4-bora-3a,4a-diaza-s-indacenes (BODIPY) grafted to the NPs achieved higher singlet oxygen quantum yields (Φ Δ ∼ 0.35-0.40) than Rose Bengal (RB) grafted NPs (Φ Δ ∼ 0.10-0.27). Finally, we combined both fluorescence and PS functions in the same NP, namely a rhodamine in the silica core and a BODIPY or RB grafted in the shell, achieving the performance Φ fl ∼ 0.10-0.20, Φ Δ ∼ 0.16-0.25 with a single excitation wavelength. Thus, proper choice of the dyes, of their concentrations inside and on the NPs and the grafting method enables fine-tuning of singlet oxygen production and fluorescence emission.

Synthesis and systematic evaluation of dark resonance energy transfer (DRET)-based library and its application in cell imaging.

PubMed

Su, Dongdong; Teoh, Chai Lean; Kang, Nam-Young; Yu, Xiaotong; Sahu, Srikanta; Chang, Young-Tae

2015-03-01

In this paper, we report a new strategy for constructing a dye library with large Stokes shifts. By coupling a dark donor with BODIPY acceptors of tunable high quantum yield, a novel dark resonance energy transfer (DRET)-based library, named BNM, has been synthesized. Upon excitation of the dark donor (BDN) at 490 nm, the absorbed energy is transferred to the acceptor (BDM) with high efficiency, which was tunable in a broad range from 557 nm to 716 nm, with a high quantum yield of up to 0.8. It is noteworthy to mention that the majority of the non-radiative energy loss of the donor was converted into the acceptor's fluorescence output with a minimum leak of donor emission. Fluorescence imaging tested in live cells showed that the BNM compounds are cell-permeable and can also be employed for live-cell imaging. This is a new library which can be excited through a dark donor allowing for strong fluorescence emission in a wide range of wavelengths. Thus, the BNM library is well suited for high-throughput screening or multiplex experiments in biological applications by using a single laser excitation source. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

A Brown Mesoporous TiO2-x /MCF Composite with an Extremely High Quantum Yield of Solar Energy Photocatalysis for H2 Evolution.

PubMed

Xing, Mingyang; Zhang, Jinlong; Qiu, Bocheng; Tian, Baozhu; Anpo, Masakazu; Che, Michel

2015-04-24

A brown mesoporous TiO2-x /MCF composite with a high fluorine dopant concentration (8.01 at%) is synthesized by a vacuum activation method. It exhibits an excellent solar absorption and a record-breaking quantum yield (Φ = 46%) and a high photon-hydrogen energy conversion efficiency (η = 34%,) for solar photocatalytic H2 production, which are all higher than that of the black hydrogen-doped TiO2 (Φ = 35%, η = 24%). The MCFs serve to improve the adsorption of F atoms onto the TiO2 /MCF composite surface, which after the formation of oxygen vacancies by vacuum activation, facilitate the abundant substitution of these vacancies with F atoms. The decrease of recombination sites induced by high-concentration F doping and the synergistic effect between lattice Ti(3+)-F and surface Ti(3+)-F are responsible for the enhanced lifetime of electrons, the observed excellent absorption of solar light, and the photocatalytic production of H2 for these catalysts. The as-prepared F-doped composite is an ideal solar light-driven photocatalyst with great potential for applications ranging from the remediation of environmental pollution to the harnessing of solar energy for H2 production. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Quantum Approach to Informatics

NASA Astrophysics Data System (ADS)

Stenholm, Stig; Suominen, Kalle-Antti

2005-08-01

An essential overview of quantum information Information, whether inscribed as a mark on a stone tablet or encoded as a magnetic domain on a hard drive, must be stored in a physical object and thus made subject to the laws of physics. Traditionally, information processing such as computation occurred in a framework governed by laws of classical physics. However, information can also be stored and processed using the states of matter described by non-classical quantum theory. Understanding this quantum information, a fundamentally different type of information, has been a major project of physicists and information theorists in recent years, and recent experimental research has started to yield promising results. Quantum Approach to Informatics fills the need for a concise introduction to this burgeoning new field, offering an intuitive approach for readers in both the physics and information science communities, as well as in related fields. Only a basic background in quantum theory is required, and the text keeps the focus on bringing this theory to bear on contemporary informatics. Instead of proofs and other highly formal structures, detailed examples present the material, making this a uniquely accessible introduction to quantum informatics. Topics covered include: * An introduction to quantum information and the qubit * Concepts and methods of quantum theory important for informatics * The application of information concepts to quantum physics * Quantum information processing and computing * Quantum gates * Error correction using quantum-based methods * Physical realizations of quantum computing circuits A helpful and economical resource for understanding this exciting new application of quantum theory to informatics, Quantum Approach to Informatics provides students and researchers in physics and information science, as well as other interested readers with some scientific background, with an essential overview of the field.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Orfield, Noah J.; McBride, James R.; Wang, Feng

Physical variations in colloidal nanostructures give rise to heterogeneity in expressed optical behavior. This correlation between nanoscale structure and function demands interrogation of both atomic structure and photophysics at the level of single nanostructures to be fully understood. In this paper, by conducting detailed analyses of fine atomic structure, chemical composition, and time-resolved single-photon photoluminescence data for the same individual nanocrystals, we reveal inhomogeneity in the quantum yields of single nonblinking “giant” CdSe/CdS core/shell quantum dots (g-QDs). We find that each g-QD possesses distinctive single exciton and biexciton quantum yields that result mainly from variations in the degree of charging,more » rather than from volume or structure inhomogeneity. We further establish that there is a very limited nonemissive “dark” fraction (<2%) among the studied g-QDs and present direct evidence that the g-QD core must lack inorganic passivation for the g-QD to be “dark”. Finally and therefore, in contrast to conventional QDs, ensemble photoluminescence quantum yield is principally defined by charging processes rather than the existence of dark g-QDs.« less

Exploring constrained quantum control landscapes

NASA Astrophysics Data System (ADS)

Moore, Katharine W.; Rabitz, Herschel

2012-10-01

The broad success of optimally controlling quantum systems with external fields has been attributed to the favorable topology of the underlying control landscape, where the landscape is the physical observable as a function of the controls. The control landscape can be shown to contain no suboptimal trapping extrema upon satisfaction of reasonable physical assumptions, but this topological analysis does not hold when significant constraints are placed on the control resources. This work employs simulations to explore the topology and features of the control landscape for pure-state population transfer with a constrained class of control fields. The fields are parameterized in terms of a set of uniformly spaced spectral frequencies, with the associated phases acting as the controls. This restricted family of fields provides a simple illustration for assessing the impact of constraints upon seeking optimal control. Optimization results reveal that the minimum number of phase controls necessary to assure a high yield in the target state has a special dependence on the number of accessible energy levels in the quantum system, revealed from an analysis of the first- and second-order variation of the yield with respect to the controls. When an insufficient number of controls and/or a weak control fluence are employed, trapping extrema and saddle points are observed on the landscape. When the control resources are sufficiently flexible, solutions producing the globally maximal yield are found to form connected "level sets" of continuously variable control fields that preserve the yield. These optimal yield level sets are found to shrink to isolated points on the top of the landscape as the control field fluence is decreased, and further reduction of the fluence turns these points into suboptimal trapping extrema on the landscape. Although constrained control fields can come in many forms beyond the cases explored here, the behavior found in this paper is illustrative of the impacts that constraints can introduce.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mthethwa, T.P.; Moloto, M.J., E-mail: mmoloto@uj.ac.za; De Vries, A.

Graphical abstract: SEM images of CdS/PMMA showing coiling as loading of CdS nanoparticles is increased. Thermal stability is increased with increase in %loading of both CdS and CdSe nanoparticles. Research highlights: {yields} TOPO-capped CdS and HDA-capped CdSe nanoparticles were synthesized and fully characterized. {yields} The nanoparticles were mixed with the polymer, PMMA using electrospinning technique using 2, 5 and 10% weight loadings. {yields} The mixture was spun to produce fibres with optical and thermal properties showing significant change and also the increase in loading causing bending or spiraling. {yields} Both TEM images for nanoparticles and SEM for fibres shows themore » morphology and sizes of the particles. -- Abstract: Electrospinning technique was used to fabricate poly(methyl methacrylate) (PMMA) fibres incorporating CdS and CdSe quantum dots (nanoparticles). Different nanoparticle loadings (2, 5 and 10 wt% with respect to PMMA) were used and the effect of the quantum dots on the properties of the fibres was studied. The optical properties of the hybrid composite fibres were investigated by photoluminescence and UV-vis spectrophotometry. Scanning electron microscopy (SEM), X-ray diffraction and FTIR spectrophotometry were also used to investigate the morphology and structure of the fibres. The optical studies showed that the size-tunable optical properties can be achieved in the polymer fibres by addition of quantum dots. SEM images showed that the morphologies of the fibres were dependent on the added amounts of quantum dots. A spiral type of morphology was observed with an increase in the concentration of CdS and CdSe nanoparticles. Less beaded structures and bigger diameter fibres were obtained at higher quantum dot concentrations. X-ray diffractometry detected the amorphous peaks of the polymer and even after the quantum dots were added and the FTIR analysis shows that there was no considerable interaction between the quantum dots and the polymer fibres at low concentration of quantum dots however at higher concentrations some interactions were observed which shows that QDs were present on the surfaces of the fibres.« less

Next-generation in vivo optical imaging with short-wave infrared quantum dots.

PubMed

Bruns, Oliver T; Bischof, Thomas S; Harris, Daniel K; Franke, Daniel; Shi, Yanxiang; Riedemann, Lars; Bartelt, Alexander; Jaworski, Frank B; Carr, Jessica A; Rowlands, Christopher J; Wilson, Mark W B; Chen, Ou; Wei, He; Hwang, Gyu Weon; Montana, Daniel M; Coropceanu, Igor; Achorn, Odin B; Kloepper, Jonas; Heeren, Joerg; So, Peter T C; Fukumura, Dai; Jensen, Klavs F; Jain, Rakesh K; Bawendi, Moungi G

2017-01-01

For in vivo imaging, the short-wavelength infrared region (SWIR; 1000-2000 nm) provides several advantages over the visible and near-infrared regions: general lack of autofluorescence, low light absorption by blood and tissue, and reduced scattering. However, the lack of versatile and functional SWIR emitters has prevented the general adoption of SWIR imaging by the biomedical research community. Here, we introduce a class of high-quality SWIR-emissive indium-arsenide-based quantum dots (QDs) that are readily modifiable for various functional imaging applications, and that exhibit narrow and size-tunable emission and a dramatically higher emission quantum yield than previously described SWIR probes. To demonstrate the unprecedented combination of deep penetration, high spatial resolution, multicolor imaging and fast-acquisition-speed afforded by the SWIR QDs, we quantified, in mice, the metabolic turnover rates of lipoproteins in several organs simultaneously and in real time as well as heartbeat and breathing rates in awake and unrestrained animals, and generated detailed three-dimensional quantitative flow maps of the mouse brain vasculature.

High-Performance CuInS 2 Quantum Dot Laminated Glass Luminescent Solar Concentrators for Windows

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bergren, Matthew R.; Makarov, Nikolay S.; Ramasamy, Karthik

Building-integrated sunlight harvesting utilizing laminated glass luminescent solar concentrators (LSCs) is proposed. By incorporating high quantum yield (>90%), NIR-emitting CuInS2/ZnS quantum dots into the polymer interlayer between two sheets of low-iron float glass, a record optical efficiency of 8.1% is demonstrated for a 10 cm x 10 cm device that transmits ~44% visible light. After completing prototypes by attaching silicon solar cells along the perimeter of the device, the electrical power conversion efficiency was certified at 2.2% with a black background and at 2.9% using a reflective substrate. This 'drop-in' LSC solution is particularly attractive because it fits within themore » existing glazing industry value chain with only modest changes to typical glazing products. Performance modeling predicts >1 GWh annual electricity production for a typical urban skyscraper in most major U.S. cities, enabling significant energy cost savings and potentially 'net-zero' buildings.« less

Detector and readout performance goals for quantum well and strained layer superlattice focal plane arrays imaging under tactical and strategic backgrounds

NASA Astrophysics Data System (ADS)

Bandara, Sumith V.

2009-11-01

Advancements in III-V semiconductor based, Quantum-well infrared photodetector (QWIP) and Type-II Strained-Layer Superlattice detector (T2SLS) technologies have yielded highly uniform, large-format long-wavelength infrared (LWIR) QWIP FPAs and high quantum efficiency (QE), small format, LWIR T2SLS FPAs. In this article, we have analyzed the QWIP and T2SLS detector level performance requirements and readout integrated circuit (ROIC) noise levels for several staring array long-wavelength infrared (LWIR) imaging applications at various background levels. As a result of lower absorption QE and less than unity photoconductive gain, QWIP FPAs are appropriate for high background tactical applications. However, if the application restricts the integration time, QWIP FPA performance may be limited by the read noise of the ROIC. Rapid progress in T2SLS detector material has already demonstrated LWIR detectors with sufficient performance for tactical applications and potential for strategic applications. However, significant research is needed to suppress surface leakage currents in order to reproduce performances at pixel levels of T2SLS FPAs.

Physiological effects of Meloidogyne incognita infection on cotton genotypes with differing levels of resistance in the greenhouse

USDA-ARS?s Scientific Manuscript database

Greenhouse tests were conducted to evaluate 1) the effect of Meloidogyne incognita infection in cotton on plant growth and physiology including the height-to-node ratio, chlorophyll content, dark adapted quantum yield of photosystem II, and leaf area, and 2) the extent to which moderate or high leve...

Highly efficient near-infrared light-emitting diodes by using type-II CdTe/CdSe core/shell quantum dots as a phosphor

NASA Astrophysics Data System (ADS)

Shen, Huaibin; Zheng, Ying; Wang, Hongzhe; Xu, Weiwei; Qian, Lei; Yang, Yixing; Titov, Alexandre; Hyvonen, Jake; Li, Lin Song

2013-11-01

In this paper, we present an innovative method for the synthesis of CdTe/CdSe type-II core/shell structure quantum dots (QDs) using ‘greener’ chemicals. The PL of CdTe/CdSe type-II core/shell structure QDs ranges from 600 to 820 nm, and the as-synthesized core/shell structures show narrow size distributions and stable and high quantum yields (50-75%). Highly efficient near-infrared light-emitting diodes (LEDs) have been demonstrated by employing the CdTe/CdSe type-II core/shell QDs as emitters. The devices fabricated based on these type-II core/shell QDs show color-saturated near-infrared emission from the QD layers, a low turn-on voltage of 1.55 V, an external quantum efficiency (EQE) of 1.59%, and a current density and maximum radiant emittance of 2.1 × 103 mA cm-2 and 17.7 mW cm-2 at 8 V it is the first report to use type-II core/shell QDs as near-infrared emitters and these results may offer a practicable platform for the realization of near-infrared QD-based light-emitting diodes, night-vision-readable displays, and friend/foe identification system.

Nanophotonic photon echo memory based on rare-earth-doped crystals

NASA Astrophysics Data System (ADS)

Zhong, Tian; Kindem, Jonathan; Miyazono, Evan; Faraon, Andrei; Caltech nano quantum optics Team

2015-03-01

Rare earth ions (REIs) are promising candidates for implementing solid-state quantum memories and quantum repeater devices. Their high spectral stability and long coherence times make REIs a good choice for integration in an on-chip quantum nano-photonic platform. We report the coupling of the 883 nm transition of Neodymium (Nd) to a Yttrium orthosilicate (YSO) photonic crystal nano-beam resonator, achieving Purcell enhanced spontaneous emission by 21 times and increased optical absorption. Photon echoes were observed in nano-beams of different doping concentrations, yielding optical coherence times T2 up to 80 μs that are comparable to unprocessed bulk samples. This indicates the remarkable coherence properties of Nd are preserved during nanofabrication, therefore opening the possibility of efficient on-chip optical quantum memories. The nano-resonator with mode volume of 1 . 6(λ / n) 3 was fabricated using focused ion beam, and a quality factor of 3200 was measured. Purcell enhanced absorption of 80% by an ensemble of ~ 1 × 106 ions in the resonator was measured, which fulfills the cavity impedance matching condition that is necessary to achieve quantum storage of photons with unity efficiency.

Aggregation-induced emission in lamellar solids of colloidal perovskite quantum wells

PubMed Central

Jagielski, Jakub; Kumar, Sudhir; Wang, Mingchao; Scullion, Declan; Lawrence, Robert; Li, Yen-Ting; Yakunin, Sergii; Tian, Tian; Kovalenko, Maksym V.; Chiu, Yu-Cheng; Santos, Elton J. G.; Lin, Shangchao; Shih, Chih-Jen

2017-01-01

The outstanding excitonic properties, including photoluminescence quantum yield (ηPL), of individual, quantum-confined semiconductor nanoparticles are often significantly quenched upon aggregation, representing the main obstacle toward scalable photonic devices. We report aggregation-induced emission phenomena in lamellar solids containing layer-controlled colloidal quantum wells (QWs) of hybrid organic-inorganic lead bromide perovskites, resulting in anomalously high solid-state ηPL of up to 94%. Upon forming the QW solids, we observe an inverse correlation between exciton lifetime and ηPL, distinct from that in typical quantum dot solid systems. Our multiscale theoretical analysis reveals that, in a lamellar solid, the collective motion of the surface organic cations is more restricted to orient along the [100] direction, thereby inducing a more direct bandgap that facilitates radiative recombination. Using the QW solids, we demonstrate ultrapure green emission by completely downconverting a blue gallium nitride light-emitting diode at room temperature, with a luminous efficacy higher than 90 lumen W−1 at 5000 cd m−2, which has never been reached in any nanomaterial assemblies by far. PMID:29282451

Non-adiabatic quantum state preparation and quantum state transport in chains of Rydberg atoms

NASA Astrophysics Data System (ADS)

Ostmann, Maike; Minář, Jiří; Marcuzzi, Matteo; Levi, Emanuele; Lesanovsky, Igor

2017-12-01

Motivated by recent progress in the experimental manipulation of cold atoms in optical lattices, we study three different protocols for non-adiabatic quantum state preparation and state transport in chains of Rydberg atoms. The protocols we discuss are based on the blockade mechanism between atoms which, when excited to a Rydberg state, interact through a van der Waals potential, and rely on single-site addressing. Specifically, we discuss protocols for efficient creation of an antiferromagnetic GHZ state, a class of matrix product states including a so-called Rydberg crystal and for the state transport of a single-qubit quantum state between two ends of a chain of atoms. We identify system parameters allowing for the operation of the protocols on timescales shorter than the lifetime of the Rydberg states while yielding high fidelity output states. We discuss the effect of positional disorder on the resulting states and comment on limitations due to other sources of noise such as radiative decay of the Rydberg states. The proposed protocols provide a testbed for benchmarking the performance of quantum information processing platforms based on Rydberg atoms.

Deterministic generation of remote entanglement with active quantum feedback

DOE PAGES

Martin, Leigh; Motzoi, Felix; Li, Hanhan; ...

2015-12-10

We develop and study protocols for deterministic remote entanglement generation using quantum feedback, without relying on an entangling Hamiltonian. In order to formulate the most effective experimentally feasible protocol, we introduce the notion of average-sense locally optimal feedback protocols, which do not require real-time quantum state estimation, a difficult component of real-time quantum feedback control. We use this notion of optimality to construct two protocols that can deterministically create maximal entanglement: a semiclassical feedback protocol for low-efficiency measurements and a quantum feedback protocol for high-efficiency measurements. The latter reduces to direct feedback in the continuous-time limit, whose dynamics can bemore » modeled by a Wiseman-Milburn feedback master equation, which yields an analytic solution in the limit of unit measurement efficiency. Our formalism can smoothly interpolate between continuous-time and discrete-time descriptions of feedback dynamics and we exploit this feature to derive a superior hybrid protocol for arbitrary nonunit measurement efficiency that switches between quantum and semiclassical protocols. Lastly, we show using simulations incorporating experimental imperfections that deterministic entanglement of remote superconducting qubits may be achieved with current technology using the continuous-time feedback protocol alone.« less

The effect of precursor on the optical properties of carbon quantum dots synthesized by hydrothermal/solvothermal method

NASA Astrophysics Data System (ADS)

Mozdbar, Afsaneh; Nouralishahi, Amideddin; Fatemi, Shohreh; Mirakhori, Ghazaleh

2018-01-01

In the recent decade, Carbon Quantum Dots (CQDs) have attracted lots of attention due to their excellent properties such as tunable photoluminescence, high chemical stability, low toxicity, and biocompatibility. Among all synthesis methods, the hydrothermal/solvothermal rout has been considered as one of the most common and simplest method. The type of precursors can affect the size of CQDs and determine their surface functional groups, the essential properties that deeply influence the optical specifications. In this work, the effect of different precursors on the final properties of carbon quantum dots is investigated. The carbon quantum dots were synthesized by hydrothermal/solvothermal rout using citric acid, thiourea, ethylamine and monoethanolamine as precursors in almost the same conditions of time and temperature. Resultant CQDs were characterized by using FTIR, UV-Visible Spectroscopy and Photoluminescence (PL) analysis. The results of UV-Vis spectroscopy showed that quantum dots synthesized from monoethanolamine have wider absorption band rather than the CQDs from other precursors and the absorption edge shifted from about 270 nm for ethylamine to about 470 nm in monoethanolamine. Furthermore, the results demonstrate that using citric acid and monoethanolamine as precursor improved production efficiency and emission quantum yield of the carbon dots.

A synchronous game for binary constraint systems

NASA Astrophysics Data System (ADS)

Kim, Se-Jin; Paulsen, Vern; Schafhauser, Christopher

2018-03-01

Recently, Slofstra proved that the set of quantum correlations is not closed. We prove that the set of synchronous quantum correlations is not closed, which implies his result, by giving an example of a synchronous game that has a perfect quantum approximate strategy but no perfect quantum strategy. We also exhibit a graph for which the quantum independence number and the quantum approximate independence number are different. We prove new characterisations of synchronous quantum approximate correlations and synchronous quantum spatial correlations. We solve the synchronous approximation problem of Dykema and the second author, which yields a new equivalence of Connes' embedding problem in terms of synchronous correlations.

Raising yield potential in wheat: increasing photosynthesis capacity and efficiency

USDA-ARS?s Scientific Manuscript database

Increasing wheat yields to help to ensure food security is a major challenge. Meeting this challenge requires a quantum improvement in the yield potential of wheat. Past increases in yield potential have largely resulted from improvements in harvest index not through increased biomass. Further large...

Correlation complementarity yields bell monogamy relations.

PubMed

Kurzyński, P; Paterek, T; Ramanathan, R; Laskowski, W; Kaszlikowski, D

2011-05-06

We present a method to derive Bell monogamy relations by connecting the complementarity principle with quantum nonlocality. The resulting monogamy relations are stronger than those obtained from the no-signaling principle alone. In many cases, they yield tight quantum bounds on the amount of violation of single and multiple qubit correlation Bell inequalities. In contrast with the two-qubit case, a rich structure of possible violation patterns is shown to exist in the multipartite scenario.

A simple and facile synthesis of MPA capped CdSe and CdSe/CdS core/shell nanoparticles

NASA Astrophysics Data System (ADS)

Sukanya, D.; Sagayaraj, P.

2015-06-01

II-VI semiconductor nanostructures, in particular, CdSe quantum dots have drawn a lot of attention because of their promising potential applications in biological tagging, photovoltaic, display devices etc. due to their excellent optical properties, high emission quantum yield, size dependent emission wavelength and high photostability. In this paper, we describe the synthesis and properties of mercaptopropionic acid capped CdSe and CdSe/CdS nanoparticles through a simple and efficient co-precipitation method followed by hydrothermal treatment. The growth process, characterization and the optical absorption as a function of wavelength for the synthesized MPA capped CdSe and CdSe/CdS nanoparticles have been determined using X-ray diffraction study (XRD), Ultraviolet-Visible spectroscopy (UV-Vis), Fourier transform infrared spectroscopy (FT-IR) and High Resolution Transmission Electron Microscopy (HRTEM).

Photochemical studies of a fluorescent chlorophyll catabolite--source of bright blue fluorescence in plant tissue and efficient sensitizer of singlet oxygen.

PubMed

Jockusch, Steffen; Turro, Nicholas J; Banala, Srinivas; Kräutler, Bernhard

2014-02-01

Fluorescent chlorophyll catabolites (FCCs) are fleeting intermediates of chlorophyll breakdown, which is seen as an enzyme controlled detoxification process of the chlorophylls in plants. However, some plants accumulate large amounts of persistent FCCs, such as in senescent leaves and in peels of yellow bananas. The photophysical properties of such a persistent FCC (Me-sFCC) were investigated in detail. FCCs absorb in the near UV spectral region and show blue fluorescence (max at 437 nm). The Me-sFCC fluorescence had a quantum yield of 0.21 (lifetime 1.6 ns). Photoexcited Me-sFCC intersystem crosses into the triplet state (quantum yield 0.6) and generates efficiently singlet oxygen (quantum yield 0.59). The efficient generation of singlet oxygen makes fluorescent chlorophyll catabolites phototoxic, but might also be useful as a (stress) signal and for defense of the plant tissue against infection by pathogens.

Short-Term Flooding Effects on Gas Exchange and Quantum Yield of Rabbiteye Blueberry (Vaccinium ashei Reade) 1

PubMed Central

Davies, Frederick S.; Flore, James A.

1986-01-01

Roots of 1.5-year-old `Woodard' rabbiteye blueberry plants (Vaccinium ashei Reade) were flooded in containers or maintained at container capacity over a 5-day period. Carbon assimilation, and stomatal and residual conductances were monitored on one fully expanded shoot/plant using an open flow gas analysis system. Quantum yield was calculated from light response curves. Carbon assimilation and quantum yield of flooded plants decreased to 64 and 41% of control values, respectively, after 1 day of flooding and continued decreasing to 38 and 27% after 4 days. Stomatal and residual conductances to CO2 also decreased after 1 day of flooding compared with those of unflooded plants with residual conductance severely limiting carbon assimilation after 4 days of flooding. Stomatal opening occurred in 75 to 90 minutes and rate of opening was unaffected by flooding. PMID:16664791

Highly Efficient Thermally Activated Delayed Fluorescence from an Excited-State Intramolecular Proton Transfer System

PubMed Central

2017-01-01

Thermally activated delayed fluorescence (TADF) materials have shown great potential for highly efficient organic light-emitting diodes (OLEDs). While the current molecular design of TADF materials primarily focuses on combining donor and acceptor units, we present a novel system based on the use of excited-state intramolecular proton transfer (ESIPT) to achieve efficient TADF without relying on the well-established donor–acceptor scheme. In an appropriately designed acridone-based compound with intramolecular hydrogen bonding, ESIPT leads to separation of the highest occupied and lowest unoccupied molecular orbitals, resulting in TADF emission with a photoluminescence quantum yield of nearly 60%. High external electroluminescence quantum efficiencies of up to 14% in OLEDs using this emitter prove that efficient triplet harvesting is possible with ESIPT-based TADF materials. This work will expand and accelerate the development of a wide variety of TADF materials for high performance OLEDs. PMID:28776019

Investigation of degradation mechanisms in composite matrices

NASA Technical Reports Server (NTRS)

Giori, C.; Yamauchi, T.

1982-01-01

Degradation mechanisms were investigated for graphite/polysulfone and graphite/epoxy laminates exposed to ultraviolet and high-energy electron radiations in vacuum up to 960 equivalent sun hours and 10 to the ninth power rads respectively. Based on GC and combined GC/MS analysis of volatile by-products evolved during irradiation, several free radical mechanisms of composite degradation were identified. The radiation resistance of different matrices was compared in terms of G values and quantum yields for gas formation. All the composite materials evaluated show high electron radiation stability and relatively low ultraviolet stability as indicated by low G values and high quantum for gas formation. Mechanical property measurements of irradiated samples did not reveal significant changes, with the possible exception of UV exposed polysulfone laminates. Hydrogen and methane were identified as the main by-products of irradiation, along with unexpectedly high levels of CO and CO2.

The Coupled Photochemistry of Ammonia and Acetylene: Applications to the Atmospheric Chemistry on Jupiter

NASA Astrophysics Data System (ADS)

Keane, Thomas Christopher

1995-01-01

The existence of hydrogen cyanide (HCN) in the highly reducing atmosphere of Jupiter was a surprising discovery (Tokunaga et al., 1981). Previous studies that tested the theoretical proposal of Kaye and Strobel (1983a) that the HCN observed on Jupiter is the result of NH _3 photolysis in the presence of C _2H_2 established that acetonitrile (CH_3CN) and acetaldazine (CH _3CH=NN=CHCH_3) are important intermediates in HCN formation (Ferris and Ishikawa, 1988). In this study the rates of formation of these compounds, and of other recently detected intermediates, have been determined in static photolysis experiments at 296 K and at temperatures which are closer to those found in the Jovian atmosphere. Experiments were also performed, using a photochemical flow reactor, that allowed for a better approximation of the mixing ratios of reactant gases (8 times 10^{ -4} for NH_3 and 1 times 10^{-5} for C_2H_2) and the process of advection in the Jovian atmosphere. An overall reaction pathway for HCN formation is proposed. Major intermediates and products found in these laboratory simulations that have not yet been observed on Jupiter are acetonitrile (CH_3CN), acetaldazine (CH_3CH=NN=CHCH _3), acetaldehyde hydrazone (CH_3 CH=NNH_2), N-ethylethylideneimine (CH_3CH=NC_2H _5), ethylamine (C_2H _5NH_2) and methylamine (CH _3NH_2). HCN is formed by the photolysis of NH_3/C _2H_2 mixtures (40:5 torr) at 296 K and at low temperature (208 K, 195 K and 180 K) with the highest quantum efficiency for HCN formation observed at 180 K. In static experiments using a high partial pressure of H_2 the quantum yield for HCN formation decreased three-fold relative to the 296 K photolyses when no H_2 was used. An additional ten-fold decrease in the quantum yield for HCN formation occurred when using the flow system. The quantum yields for acetaldazine and acetaldehyde hydrazone formation were found to vary inversely to that for HCN formation. For those static experiments which best simulate Jovian reaction conditions (H_2: NH_3 : C_2H_2 = 600: 7.5: 5 torr, 180 K) the following products and their quantum yields for formation were obtained: C_2H_4 (0.129), CH_3 CH=NN=CHCH_3 (0.079), CH _3CH=NNH_2 (0.049), C_2H_5NH_2 (0.038), CH_3NH_2 (0.003), CH_3CN (0.002), HCN (0.001) and CH_3CH=NC _2H_5 (0.001).

Room-Temperature Triple-Ligand Surface Engineering Synergistically Boosts Ink Stability, Recombination Dynamics, and Charge Injection toward EQE-11.6% Perovskite QLEDs.

PubMed

Song, Jizhong; Li, Jinhang; Xu, Leimeng; Li, Jianhai; Zhang, Fengjuan; Han, Boning; Shan, Qingsong; Zeng, Haibo

2018-06-10

Developing low-cost and high-quality quantum dots (QDs) or nanocrystals (NCs) and their corresponding efficient light-emitting diodes (LEDs) is crucial for the next-generation ultra-high-definition flexible displays. Here, there is a report on a room-temperature triple-ligand surface engineering strategy to play the synergistic role of short ligands of tetraoctylammonium bromide (TOAB), didodecyldimethylammonium bromide (DDAB), and octanoic acid (OTAc) toward "ideal" perovskite QDs with a high photoluminescence quantum yield (PLQY) of >90%, unity radiative decay in its intrinsic channel, stable ink characteristics, and effective charge injection and transportation in QD films, resulting in the highly efficient QD-based LEDs (QLEDs). Furthermore, the QD films with less nonradiative recombination centers exhibit improved PL properties with a PLQY of 61% through dopant engineering in A-site. The robustness of such properties is demonstrated by the fabrication of green electroluminescent LEDs based on CsPbBr 3 QDs with the peak external quantum efficiency (EQE) of 11.6%, and the corresponding peak internal quantum efficiency (IQE) and power efficiency are 52.2% and 44.65 lm W -1 , respectively, which are the most-efficient perovskite QLEDs with colloidal CsPbBr 3 QDs as emitters up to now. These results demonstrate that the as-obtained QD inks have a wide range application in future high-definition QD displays and high-quality lightings. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Fundamental Quantum 1/F Noise in Ultrasmall Semiconductor Devices and Their Optimal Design Principles

DTIC Science & Technology

1988-05-31

Hooge parameter. 2. 1 / f Noise of the Recombination Current Generated in the Depletion Region The quantum i/ f ...theory. There are two forms of quantum 11f noise . In the first place C~ and Cn4 p n to quantum 1 / f noise theory. This would yield Hooge parameters S...Fundamental Quantum 1 / f Noise in Ultrasmall S~ iodcrD’vesadOtm.Dsgn P in. 12. PERSONAL AUTHOR(S) Handel, Peter H. (Princioal investiaat r) 13a. TYPE

Proceedings of the Quantum Computation for Physical Modeling Workshop 2004. Held in North Falmouth, MA on 12-15 September 2004

DTIC Science & Technology

2005-10-01

late the difficulty of some basic 1-bit and n-bit quantum and classical operations in an simple unconstrained scenario. KEY WORDS: Time evolution... quantum circuit and design are presented for an optimized entangling probe attacking the BB84 Protocol of quantum key distribution (QKD) and yielding...unambiguous, at least some of the time. It follows that the BB84 (Bennett-Brassard 1984) proto- col of quantum key distribution has a vulnerability similar to

Highly luminescent silica-coated CdS/CdSe/CdS nanoparticles with strong chemical robustness and excellent thermal stability

NASA Astrophysics Data System (ADS)

Wang, Nianfang; Koh, Sungjun; Jeong, Byeong Guk; Lee, Dongkyu; Kim, Whi Dong; Park, Kyoungwon; Nam, Min Ki; Lee, Kangha; Kim, Yewon; Lee, Baek-Hee; Lee, Kangtaek; Bae, Wan Ki; Lee, Doh C.

2017-05-01

We present facile synthesis of bright CdS/CdSe/CdS@SiO2 nanoparticles with 72% of quantum yields (QYs) retaining ca 80% of the original QYs. The main innovative point is the utilization of the highly luminescent CdS/CdSe/CdS seed/spherical quantum well/shell (SQW) as silica coating seeds. The significance of inorganic semiconductor shell passivation and structure design of quantum dots (QDs) for obtaining bright QD@SiO2 is demonstrated by applying silica encapsulation via reverse microemulsion method to three kinds of QDs with different structure: CdSe core and 2 nm CdS shell (CdSe/CdS-thin); CdSe core and 6 nm CdS shell (CdSe/CdS-thick); and CdS core, CdSe intermediate shell and 5 nm CdS outer shell (CdS/CdSe/CdS-SQW). Silica encapsulation inevitably results in lower photoluminescence quantum yield (PL QY) than pristine QDs due to formation of surface defects. However, the retaining ratio of pristine QY is different in the three silica coated samples; for example, CdSe/CdS-thin/SiO2 shows the lowest retaining ratio (36%) while the retaining ratio of pristine PL QY in CdSe/CdS-thick/SiO2 and SQW/SiO2 is over 80% and SQW/SiO2 shows the highest resulting PL QY. Thick outermost CdS shell isolates the excitons from the defects at surface, making PL QY relatively insensitive to silica encapsulation. The bright SiO2-coated SQW sample shows robustness against harsh conditions, such as acid etching and thermal annealing. The high luminescence and long-term stability highlights the potential of using the SQW/SiO2 nanoparticles in bio-labeling or display applications.

Interaction of Water-Soluble CdTe Quantum Dots with Bovine Serum Albumin

PubMed Central

2011-01-01

Semiconductor nanoparticles (quantum dots) are promising fluorescent markers, but it is very little known about interaction of quantum dots with biological molecules. In this study, interaction of CdTe quantum dots coated with thioglycolic acid (TGA) with bovine serum albumin was investigated. Steady state spectroscopy, atomic force microscopy, electron microscopy and dynamic light scattering methods were used. It was explored how bovine serum albumin affects stability and spectral properties of quantum dots in aqueous media. CdTe–TGA quantum dots in aqueous solution appeared to be not stable and precipitated. Interaction with bovine serum albumin significantly enhanced stability and photoluminescence quantum yield of quantum dots and prevented quantum dots from aggregating. PMID:27502633

Bright conjugated polymer nanoparticles containing a biodegradable shell produced at high yields and with tuneable optical properties by a scalable microfluidic device.

PubMed

Abelha, T F; Phillips, T W; Bannock, J H; Nightingale, A M; Dreiss, C A; Kemal, E; Urbano, L; deMello, J C; Green, M; Dailey, L A

2017-02-02

This study compares the performance of a microfluidic technique and a conventional bulk method to manufacture conjugated polymer nanoparticles (CPNs) embedded within a biodegradable poly(ethylene glycol) methyl ether-block-poly(lactide-co-glycolide) (PEG 5K -PLGA 55K ) matrix. The influence of PEG 5K -PLGA 55K and conjugated polymers cyano-substituted poly(p-phenylene vinylene) (CN-PPV) and poly(9,9-dioctylfluorene-2,1,3-benzothiadiazole) (F8BT) on the physicochemical properties of the CPNs was also evaluated. Both techniques enabled CPN production with high end product yields (∼70-95%). However, while the bulk technique (solvent displacement) under optimal conditions generated small nanoparticles (∼70-100 nm) with similar optical properties (quantum yields ∼35%), the microfluidic approach produced larger CPNs (140-260 nm) with significantly superior quantum yields (49-55%) and tailored emission spectra. CPNs containing CN-PPV showed smaller size distributions and tuneable emission spectra compared to F8BT systems prepared under the same conditions. The presence of PEG 5K -PLGA 55K did not affect the size or optical properties of the CPNs and provided a neutral net electric charge as is often required for biomedical applications. The microfluidics flow-based device was successfully used for the continuous preparation of CPNs over a 24 hour period. On the basis of the results presented here, it can be concluded that the microfluidic device used in this study can be used to optimize the production of bright CPNs with tailored properties with good reproducibility.

New evidence for primordial action site of Fluazifop-P-butyl on Acanthospermum hispidum seedlings: From the effects on chlorophyll fluorescence characteristics and histological observation.

PubMed

Shang, Yuhong; Yang, Congjun; Liu, Zhihang; Song, Jiqing; Li, Pingliang; Li, Lingxu; Zhou, Fei; Xin, Hua; Wan, Fanghao; Matsumoto, Hiroshi; Luo, Xiaoyong

2017-10-01

Acanthospermum hispidum DC, an Asteraceae weed species, was very susceptible to fluazifop-P-butyl, but tolerant to other aryloxyphenoxypropionate herbicides, such as haloxyfop-P-methyl. However, other Asteraceae weeds including Bidens pilosa were all tolerant to fluazifop-P-butyl. Membrane lipid peroxidation by increasing the levels of reactive oxygen species (ROS) was proposed as an action mechanism of fluazifop-P-butyl in A. hispidum. To further clarify the primordial action site of fluazifop-P-butyl in this species, the effects on chlorophyll fluorescence characteristics and cytohistology of apical meristems were studied. Chlorophyll fluorescence characteristics (CFC) in sensitive A. hispidum seedlings were markedly affected by 10μM fluazifop-P-butyl, with the dark fluorescence yield (Fo), maximal fluorescence yield (Fm), maximal PS II quantum yield (Fv/Fm), effective photosystem II (PS II) quantum yield [Y(II)], and quantum yield of regulated energy dissipation [Y(NPQ)] declining, quantum yield of nonregulated energy dissipation [Y(NO)] rising, but these measures were not affected in Bidens pilosa. The effects of fluazifop-P-butyl on chlorophyll fluorescence properties were observed on the growing point before the mature leaves by about 4-6h. Haloxyfop-P-methyl, a control herbicide, had no effects on CFC of either A. hispidum or B. pilosa. In addition, damage to apical meristem cells of A. hispidum was observed at 6 HAT prior to changes in chlorophyll fluorescence parameters suggesting that the primary action site of fluazifop-P-butyl in this species is in the apical meristem and the effects on CFC may be the results of secondary action. Copyright © 2017 Elsevier Inc. All rights reserved.

Depopulation of highly excited singlet states of DNA model compounds: quantum yields of 193 and 245 nm photoproducts of pyrimidine monomers and dinucleoside monophosphates.

PubMed

Gurzadyan, G G; Görner, H

1996-02-01

Formation of uracil and orotic acid photodimers, uridine and 5'-UMP photohydrates, TpT photodimers and (6-4)photoproducts, dCpT photohydrates and (6-4)photoproducts and UpU, CpC and CpU photohydrates were studied in neutral deoxygenated aqueous solution at room temperature upon irradiation at either 193 or 254 nm. The photoproducts were identified and quantified and the contribution from photoionization to substrate decomposition, using lambda irr = 193 nm, was separated. The ratio of the quantum yields of respective stable products, eta = phi 193/phi 254, is indicative of the yield of internal conversion from the second to the first excited singlet state, S2-->S1. For the observed photodimers eta decreases from 0.94 for uracil to 0.7 for TpT and further to 0.55 for orotic acid. For the (6-4)photoproducts of TpT and dCpT eta = 0.5-0.8 and for the photohydrates in the cases of UpU, CpC, CpU and dCpT eta ranges from 0.55 to 1.

Can time-dependent density functional theory predict intersystem crossing in organic chromophores? A case study on benzo(bis)-X-diazole based donor-acceptor-donor type molecules.

PubMed

Tam, Teck Lip Dexter; Lin, Ting Ting; Chua, Ming Hui

2017-06-21

Here we utilized new diagnostic tools in time-dependent density functional theory to explain the trend of intersystem crossing in benzo(bis)-X-diazole based donor-acceptor-donor type molecules. These molecules display a wide range of fluorescence quantum yields and triplet yields, making them excellent candidates for testing the validity of these diagnostic tools. We believe that these tools are cost-effective and can be applied to structurally similar organic chromophores to predict/explain the trends of intersystem crossing, and thus fluorescence quantum yields and triplet yields without the use of complex and expensive multireference configuration interaction or multireference pertubation theory methods.

Quantum coherence effects in natural light-induced processes: cis-trans photoisomerization of model retinal under incoherent excitation.

PubMed

Tscherbul, Timur V; Brumer, Paul

2015-12-14

We present a theoretical study of quantum coherence effects in the primary cis-trans photoisomerization of retinal in rhodopsin induced by incoherent solar light. Using the partial secular Bloch-Redfield quantum master equation approach based on a two-state two-mode linear vibronic coupling model of the retinal chromophore [S. Hahn and G. Stock, J. Phys. Chem. B, 2000, 104, 1146-1149], we show that a sudden turn-on of incoherent pumping can generate substantial Fano coherences among the excited states of retinal. These coherences are the most pronounced in the regime where the matrix elements of the transition dipole moment between the ground and excited eigenstates are parallel to one another. We show that even when the transition dipole moments are perpendicular (implying the absence of light-induced Fano coherence) a small amount of excited-state coherence is still generated due to the coupling to intramolecular vibrational modes and the protein environment, causing depopulation of the excited eigenstates. The overall effect of the coherences on the steady-state population and on the photoproduct quantum yield is shown to be small; however we observe a significant transient effect on the formation of the trans photoproduct, enhancing the photoreaction quantum yield by ∼11% at 200 fs. These calculations suggest that coupling to intramolecular vibrational modes and the protein environment play an important role in photoreaction dynamics, suppressing oscillations in the quantum yield associated with Fano interference.

Bright nanowire single photon source based on SiV centers in diamond

DOE PAGES

Marseglia, L.; Saha, K.; Ajoy, A.; ...

2018-01-01

The practical implementation of quantum technologies such as quantum commu- nication and quantum cryptography relies on the development of indistinguishable, robust, and bright single photon sources that works at room temperature. The silicon- vacancy (SiV -) center in diamond has emerged as a possible candidate for a single photon source with all these characteristics. Unfortunately, due to the high refraction index mismatch between diamond and air, color centers in diamond show low photon out-coupling. This drawback can be overcome by fabrication of photonic structures that improve the in-coupling of excitation laser to the diamond defect as well as the out-couplingmore » emission from the color centers. An additional shortcoming is due to the random localization of native defects in the diamond sample. Here we demonstrate deterministic implantation of Si ions with high conversion effciency to single SiV -, targeted to fabricated nanowires. The co-localization of single SiV - defects with the nanostructures yields a ten times higher light coupling effciency as compared to single SiV - in the bulk. This result, with its intrinsic scalability, enables a new class of devices for integrated photonics and quantum information processing.« less

Quantum Yield of Cyclobutane Pyrimidine Dimer Formation Via the Triplet Channel Determined by Photosensitization.

PubMed

Liu, Lizhe; Pilles, Bert M; Gontcharov, Julia; Bucher, Dominik B; Zinth, Wolfgang

2016-01-21

UV-induced formation of the cyclobutane pyrimidine dimer (CPD) lesion is investigated by stationary and time-resolved photosensitization experiments. The photosensitizer 2'-methoxyacetophenone with high intersystem crossing efficiency and large absorption cross-section in the UV-A range was used. A diffusion controlled reaction model is presented. Time-resolved experiments confirmed the validity of the reaction model and provided information on the dynamics of the triplet sensitization process. With a series of concentration dependent stationary illumination experiments, we determined the quantum efficiency for CPD formation from the triplet state of the thymine dinucleotide TpT to be 4 ± 0.2%.

Advanced indium phosphide based monolithic integration using quantum well intermixing and MOCVD regrowth

NASA Astrophysics Data System (ADS)

Raring, James W.

The proliferation of the internet has fueled the explosive growth of telecommunications over the past three decades. As a result, the demand for communication systems providing increased bandwidth and flexibility at lower cost continues to rise. Lightwave communication systems meet these demands. The integration of multiple optoelectronic components onto a single chip could revolutionize the photonics industry. Photonic integrated circuits (PIC) provide the potential for cost reduction, decreased loss, decreased power consumption, and drastic space savings over conventional fiber optic communication systems comprised of discrete components. For optimal performance, each component within the PIC may require a unique epitaxial layer structure, band-gap energy, and/or waveguide architecture. Conventional integration methods facilitating such flexibility are increasingly complex and often result in decreased device yield, driving fabrication costs upward. It is this trade-off between performance and device yield that has hindered the scaling of photonic circuits. This dissertation presents high-functionality PICs operating at 10 and 40 Gb/s fabricated using novel integration technologies based on a robust quantum-well-intermixing (QWI) method and metal organic chemical vapor deposition (MOCVD) regrowth. We optimize the QWI process for the integration of high-performance quantum well electroabsorption modulators (QW-EAM) with sampled-grating (SG) DBR lasers to demonstrate the first widely-tunable negative chirp 10 and 40 Gb/s EAM based transmitters. Alone, QWI does not afford the integration of high-performance semiconductor optical amplifiers (SOA) and photodetectors with the transmitters. To overcome this limitation, we have developed a novel high-flexibility integration scheme combining MOCVD regrowth with QWI to merge low optical confinement factor SOAs and 40 Gb/s uni-traveling carrier (UTC) photodiodes on the same chip as the QW-EAM based transmitters. These high-saturation power receiver structures represent the state-of-the-art technologies for even discrete components. Using the novel integration technology, we present the first widely-tunable single-chip device capable of transmit and receive functionality at 40 Gb/s. This device monolithically integrates tunable lasers, EAMs, SOAs, and photodetectors with performance that rivals optimized discrete components. The high-flexibility integration scheme requires only simple blanket regrowth steps and thus breaks the performance versus yield trade-off plaguing conventional fabrication techniques employed for high-functionality PICs.

Purely organic electroluminescent material realizing 100% conversion from electricity to light

PubMed Central

Kaji, Hironori; Suzuki, Hajime; Fukushima, Tatsuya; Shizu, Katsuyuki; Suzuki, Katsuaki; Kubo, Shosei; Komino, Takeshi; Oiwa, Hajime; Suzuki, Furitsu; Wakamiya, Atsushi; Murata, Yasujiro; Adachi, Chihaya

2015-01-01

Efficient organic light-emitting diodes have been developed using emitters containing rare metals, such as platinum and iridium complexes. However, there is an urgent need to develop emitters composed of more abundant materials. Here we show a thermally activated delayed fluorescence material for organic light-emitting diodes, which realizes both approximately 100% photoluminescence quantum yield and approximately 100% up-conversion of the triplet to singlet excited state. The material contains electron-donating diphenylaminocarbazole and electron-accepting triphenyltriazine moieties. The typical trade-off between effective emission and triplet-to-singlet up-conversion is overcome by fine-tuning the highest occupied molecular orbital and lowest unoccupied molecular orbital distributions. The nearly zero singlet–triplet energy gap, smaller than the thermal energy at room temperature, results in an organic light-emitting diode with external quantum efficiency of 29.6%. An external quantum efficiency of 41.5% is obtained when using an out-coupling sheet. The external quantum efficiency is 30.7% even at a high luminance of 3,000 cd m−2. PMID:26477390

1/f Noise Inside a Faraday Cage

NASA Astrophysics Data System (ADS)

Handel, Peter H.; George, Thomas F.

2009-04-01

We show that quantum 1/f noise does not have a lower frequency limit given by the lowest free electromagnetic field mode in a Faraday cage, even in an ideal cage. Indeed, quantum 1/f noise comes from the infrared-divergent coupling of the field with the charges, in their joint nonlinear system, where the charges cause the field that reacts back on the charges, and so on. This low-frequency limitation is thus not applicable for the nonlinear system of matter and field in interaction. Indeed, this nonlinear system is governed by Newton's laws, Maxwell's equations, in general also by the diffusion equations for particles and heat, or reaction kinetics given by quantum matrix elements. Nevertheless, all the other quantities can be eliminated in principle, resulting in highly nonlinear integro-differential equations for the electromagnetic field only, which no longer yield a fundamental frequency. Alternatively, we may describe this through the presence of an infinite system of subharmonics. We show how this was proven early in the classical and quantum domains, adding new insight.

Emerging technologies for high performance infrared detectors

NASA Astrophysics Data System (ADS)

Tan, Chee Leong; Mohseni, Hooman

2018-01-01

Infrared photodetectors (IRPDs) have become important devices in various applications such as night vision, military missile tracking, medical imaging, industry defect imaging, environmental sensing, and exoplanet exploration. Mature semiconductor technologies such as mercury cadmium telluride and III-V material-based photodetectors have been dominating the industry. However, in the last few decades, significant funding and research has been focused to improve the performance of IRPDs such as lowering the fabrication cost, simplifying the fabrication processes, increasing the production yield, and increasing the operating temperature by making use of advances in nanofabrication and nanotechnology. We will first review the nanomaterial with suitable electronic and mechanical properties, such as two-dimensional material, graphene, transition metal dichalcogenides, and metal oxides. We compare these with more traditional low-dimensional material such as quantum well, quantum dot, quantum dot in well, semiconductor superlattice, nanowires, nanotube, and colloid quantum dot. We will also review the nanostructures used for enhanced light-matter interaction to boost the IRPD sensitivity. These include nanostructured antireflection coatings, optical antennas, plasmonic, and metamaterials.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Le, Quyet Van; Kim, Jong Beom; Kim, Soo Young

We have investigated the effect of reaction temperature of hot-injection method on the structural properties of CsPbX3 (X: Br, I, Cl) perovskite nanocrystals (NCs) using the small- and wide-angle X-ray scattering. It is confirmed that the size of the NCs decreased as the reaction temperature decreased, resulting stronger quantum confinement. The cubic-phase perovskite NCs were formed despite the reaction temperatures increased from 140 to 180 °C. However, monodispersive NC cubes which are required for densely packing self-assembly film were only formed at lower temperatures. From the X-ray scattering measurements, the spin-coated film from more monodispersive perovskite nanocubes synthesized at lowermore » temperatures resulted in more preferred orientation. This dense-packing perovskite film with preferred orientation yielded efficient light-emitting diode (LED) performance. Thus, the dense-packing structure of NC assemblies formed after spin-coating should be considered for high-efficient LEDs based on perovskite quantum dots in addition to quantum confinement effect of the quantum dots.« less

Distributing entanglement and single photons through an intra-city, free-space quantum channel.

PubMed

Resch, K; Lindenthal, M; Blauensteiner, B; Böhm, H; Fedrizzi, A; Kurtsiefer, C; Poppe, A; Schmitt-Manderbach, T; Taraba, M; Ursin, R; Walther, P; Weier, H; Weinfurter, H; Zeilinger, A

2005-01-10

We have distributed entangled photons directly through the atmosphere to a receiver station 7.8 km away over the city of Vienna, Austria at night. Detection of one photon from our entangled pairs constitutes a triggered single photon source from the sender. With no direct time-stable connection, the two stations found coincidence counts in the detection events by calculating the cross-correlation of locally-recorded time stamps shared over a public internet channel. For this experiment, our quantum channel was maintained for a total of 40 minutes during which time a coincidence lock found approximately 60000 coincident detection events. The polarization correlations in those events yielded a Bell parameter, S=2.27+/-0.019, which violates the CHSH-Bell inequality by 14 standard deviations. This result is promising for entanglement-based freespace quantum communication in high-density urban areas. It is also encouraging for optical quantum communication between ground stations and satellites since the length of our free-space link exceeds the atmospheric equivalent.

Temporal variability in chlorophyll fluorescence of back-reef corals in Ofu, American Samoa

USGS Publications Warehouse

Piniak, G.A.; Brown, E.K.

2009-01-01

Change in the yield of chlorophyll a fluorescence is a common indicator of thermal stress in corals. The present study reports temporal variability in quantum yield measurements for 10 coral species in Ofu, American Samoa - a place known to experience elevated and variable seawater temperatures. In winter, the zooxanthellae generally had higher dark-adapted maximum quantum yield (F v/Fm), higher light- adapted effective quantum yield (??F/F'm), and lower relative electron transport rates (rETR) than in the summer. Temporal changes appeared unrelated to the expected bleaching sensitivity of corals. All species surveyed, with the exception of Montipora grisea, demonstrated significant temporal changes in the three fluorescence parameters. Fluorescence responses were influenced by the microhabitat - temporal differences in fluorescence parameters were usually observed in the habitat with a more variable temperature regime (pool 300), while differences in Fv/Fm between species were observed only in the more environmentally stable habitat (pool 400). Such species-specific responses and microhabitat variability should be considered when attempting to determine whether observed in situ changes are normal seasonal changes or early signs of bleaching. ?? 2009 Marine Biological Laboratory.

Overcoming the sign problem at finite temperature: Quantum tensor network for the orbital eg model on an infinite square lattice

NASA Astrophysics Data System (ADS)

Czarnik, Piotr; Dziarmaga, Jacek; Oleś, Andrzej M.

2017-07-01

The variational tensor network renormalization approach to two-dimensional (2D) quantum systems at finite temperature is applied to a model suffering the notorious quantum Monte Carlo sign problem—the orbital eg model with spatially highly anisotropic orbital interactions. Coarse graining of the tensor network along the inverse temperature β yields a numerically tractable 2D tensor network representing the Gibbs state. Its bond dimension D —limiting the amount of entanglement—is a natural refinement parameter. Increasing D we obtain a converged order parameter and its linear susceptibility close to the critical point. They confirm the existence of finite order parameter below the critical temperature Tc, provide a numerically exact estimate of Tc, and give the critical exponents within 1 % of the 2D Ising universality class.

Experimental boundaries of the quantum rotor induced polarization (QRIP) in liquid state NMR.

PubMed

Icker, Maik; Fricke, Pascal; Grell, Toni; Hollenbach, Julia; Auer, Henry; Berger, Stefan

2013-12-01

The Haupt-effect is a rather seldom used hyperpolarization method. It is based on the interdependence between nuclear spin states and rotational states of nearly free rotating methyl groups having C3 symmetry. A sudden change in temperature from 4.2 K to room temperature by fast dissolution yields considerably enhanced (13)C and (1)H resonance signals. This phenomenon is now termed quantum rotor induced polarization. More than 40 substances have been studied by this approach in order to identify them as polarizable by the 'Haupt-effect in the liquid state'. Influencing factors have been analyzed systematically. It could be concluded that substances having a high tunneling frequency, which is due to a small and narrow potential barrier, are most likely to feature quantum rotor induced polarization-enhanced signals. Copyright © 2013 John Wiley & Sons, Ltd.

Scalable focused ion beam creation of nearly lifetime-limited single quantum emitters in diamond nanostructures

PubMed Central

Schröder, Tim; Trusheim, Matthew E.; Walsh, Michael; Li, Luozhou; Zheng, Jiabao; Schukraft, Marco; Sipahigil, Alp; Evans, Ruffin E.; Sukachev, Denis D.; Nguyen, Christian T.; Pacheco, Jose L.; Camacho, Ryan M.; Bielejec, Edward S.; Lukin, Mikhail D.; Englund, Dirk

2017-01-01

The controlled creation of defect centre—nanocavity systems is one of the outstanding challenges for efficiently interfacing spin quantum memories with photons for photon-based entanglement operations in a quantum network. Here we demonstrate direct, maskless creation of atom-like single silicon vacancy (SiV) centres in diamond nanostructures via focused ion beam implantation with ∼32 nm lateral precision and <50 nm positioning accuracy relative to a nanocavity. We determine the Si+ ion to SiV centre conversion yield to be ∼2.5% and observe a 10-fold conversion yield increase by additional electron irradiation. Low-temperature spectroscopy reveals inhomogeneously broadened ensemble emission linewidths of ∼51 GHz and close to lifetime-limited single-emitter transition linewidths down to 126±13 MHz corresponding to ∼1.4 times the natural linewidth. This method for the targeted generation of nearly transform-limited quantum emitters should facilitate the development of scalable solid-state quantum information processors. PMID:28548097

Scalable focused ion beam creation of nearly lifetime-limited single quantum emitters in diamond nanostructures

DOE PAGES

Schroder, Tim; Trusheim, Matthew E.; Walsh, Michael; ...

2017-05-26

The controlled creation of defect centre—nanocavity systems is one of the outstanding challenges for efficiently interfacing spin quantum memories with photons for photon-based entanglement operations in a quantum network. Here we demonstrate direct, maskless creation of atom-like single silicon vacancy (SiV) centres in diamond nanostructures via focused ion beam implantation with ~32 nm lateral precision and <50 nm positioning accuracy relative to a nanocavity. We determine the Si+ ion to SiV centre conversion yield to be ~2.5% and observe a 10-fold conversion yield increase by additional electron irradiation. Low-temperature spectroscopy reveals inhomogeneously broadened ensemble emission linewidths of ~51 GHz andmore » close to lifetime-limited single-emitter transition linewidths down to 126±13 MHz corresponding to ~1.4 times the natural linewidth. Furthermore, this method for the targeted generation of nearly transform-limited quantum emitters should facilitate the development of scalable solid-state quantum information processors.« less

Scalable focused ion beam creation of nearly lifetime-limited single quantum emitters in diamond nanostructures

DOE Office of Scientific and Technical Information (OSTI.GOV)

Schroder, Tim; Trusheim, Matthew E.; Walsh, Michael

The controlled creation of defect centre—nanocavity systems is one of the outstanding challenges for efficiently interfacing spin quantum memories with photons for photon-based entanglement operations in a quantum network. Here we demonstrate direct, maskless creation of atom-like single silicon vacancy (SiV) centres in diamond nanostructures via focused ion beam implantation with ~32 nm lateral precision and <50 nm positioning accuracy relative to a nanocavity. We determine the Si+ ion to SiV centre conversion yield to be ~2.5% and observe a 10-fold conversion yield increase by additional electron irradiation. Low-temperature spectroscopy reveals inhomogeneously broadened ensemble emission linewidths of ~51 GHz andmore » close to lifetime-limited single-emitter transition linewidths down to 126±13 MHz corresponding to ~1.4 times the natural linewidth. Furthermore, this method for the targeted generation of nearly transform-limited quantum emitters should facilitate the development of scalable solid-state quantum information processors.« less

Delta-Doping at Wafer Level for High Throughput, High Yield Fabrication of Silicon Imaging Arrays

NASA Technical Reports Server (NTRS)

Hoenk, Michael E. (Inventor); Nikzad, Shoulch (Inventor); Jones, Todd J. (Inventor); Greer, Frank (Inventor); Carver, Alexander G. (Inventor)

2014-01-01

Systems and methods for producing high quantum efficiency silicon devices. A silicon MBE has a preparation chamber that provides for cleaning silicon surfaces using an oxygen plasma to remove impurities and a gaseous (dry) NH3 + NF3 room temperature oxide removal process that leaves the silicon surface hydrogen terminated. Silicon wafers up to 8 inches in diameter have devices that can be fabricated using the cleaning procedures and MBE processing, including delta doping.

Development of mono- and di-AcO substituted BODIPYs on the boron center.

PubMed

Jiang, Xin-Dong; Zhang, Jian; Furuyama, Taniyuki; Zhao, Weili

2012-01-06

Mono- and di-AcO substituted BODIPYs (1 and 2) were synthesized from TM-BDP. The structures of 1 and 2 were supported by single crystal X-ray analysis. Both 1 and 2 possess a large absorption coefficient, high fluorescence quantum yield, and high light stability. Compound 2 has much improved water solubility which is highly desirable for biological applications. Theoretical calculation supports our observations in X-ray analysis, absorption, and cyclic voltammetry. © 2011 American Chemical Society

Density of Trap States and Auger-mediated Electron Trapping in CdTe Quantum-Dot Solids.

PubMed

Boehme, Simon C; Azpiroz, Jon Mikel; Aulin, Yaroslav V; Grozema, Ferdinand C; Vanmaekelbergh, Daniël; Siebbeles, Laurens D A; Infante, Ivan; Houtepen, Arjan J

2015-05-13

Charge trapping is an ubiquitous process in colloidal quantum-dot solids and a major limitation to the efficiency of quantum dot based devices such as solar cells, LEDs, and thermoelectrics. Although empirical approaches led to a reduction of trapping and thereby efficiency enhancements, the exact chemical nature of the trapping mechanism remains largely unidentified. In this study, we determine the density of trap states in CdTe quantum-dot solids both experimentally, using a combination of electrochemical control of the Fermi level with ultrafast transient absorption and time-resolved photoluminescence spectroscopy, and theoretically, via density functional theory calculations. We find a high density of very efficient electron traps centered ∼0.42 eV above the valence band. Electrochemical filling of these traps increases the electron lifetime and the photoluminescence quantum yield by more than an order of magnitude. The trapping rate constant for holes is an order of magnitude lower that for electrons. These observations can be explained by Auger-mediated electron trapping. From density functional theory calculations we infer that the traps are formed by dicoordinated Te atoms at the quantum dot surface. The combination of our unique experimental determination of the density of trap states with the theoretical modeling of the quantum dot surface allows us to identify the trapping mechanism and chemical reaction at play during charge trapping in these quantum dots.

Universal thermodynamics of the one-dimensional attractive Hubbard model

NASA Astrophysics Data System (ADS)

Cheng, Song; Yu, Yi-Cong; Batchelor, M. T.; Guan, Xi-Wen

2018-03-01

The one-dimensional (1D) Hubbard model, describing electrons on a lattice with an on-site repulsive interaction, provides a paradigm for the physics of quantum many-body phenomena. Here, by solving the thermodynamic Bethe ansatz equations, we study the universal thermodynamics, quantum criticality, and magnetism of the 1D attractive Hubbard model. We show that the compressibility and the susceptibility of the Fulde-Ferrell-Larkin-Ovchinnikov (FFLO)-like state obey simple additivity rules at low temperatures, indicating an existence of two free quantum fluids. The magnetic properties, such as magnetization and susceptibility, reveal three physical regions: quantum fluids at low temperatures, a non-Fermi liquid at high temperatures, and the quantum fluid to non-Fermi liquid crossover in between. The lattice interaction is seen to significantly influence the nature of the FFLO-like state in 1D. Furthermore, we show that the dimensionless Wilson ratio provides an ideal parameter to map out the various phase boundaries and to characterize the two free fluids of the FLLO-like state. The quantum scaling functions for the thermal and magnetic properties yield the same dynamic critical exponent z =2 and correlation critical exponent ν =1 /2 in the quantum critical region whenever a phase transition occurs. Our results provide a rigorous understanding of quantum criticality and free fluids of many-body systems on a 1D lattice.

Photolysis of CH{sub 3}CHO at 248 nm: Evidence of triple fragmentation from primary quantum yield of CH{sub 3} and HCO radicals and H atoms

DOE Office of Scientific and Technical Information (OSTI.GOV)

Morajkar, Pranay; Schoemaecker, Coralie; Fittschen, Christa, E-mail: christa.fittschen@univ-lille1.fr

2014-06-07

Radical quantum yields have been measured following the 248 nm photolysis of acetaldehyde, CH{sub 3}CHO. HCO radical and H atom yields have been quantified by time resolved continuous wave Cavity Ring Down Spectroscopy in the near infrared following their conversion to HO{sub 2} radicals by reaction with O{sub 2}. The CH{sub 3} radical yield has been determined using the same technique following their conversion into CH{sub 3}O{sub 2}. Absolute yields have been deduced for HCO radicals and H atoms through fitting of time resolved HO{sub 2} profiles, obtained under various O{sub 2} concentrations, to a complex model, while the CH{submore » 3} yield has been determined relative to the CH{sub 3} yield from 248 nm photolysis of CH{sub 3}I. Time resolved HO{sub 2} profiles under very low O{sub 2} concentrations suggest that another unknown HO{sub 2} forming reaction path exists in this reaction system besides the conversion of HCO radicals and H atoms by reaction with O{sub 2}. HO{sub 2} profiles can be well reproduced under a large range of experimental conditions with the following quantum yields: CH{sub 3}CHO + hν{sub 248nm} → CH{sub 3}CHO{sup *}, CH{sub 3}CHO{sup *} → CH{sub 3} + HCO ϕ{sub 1a} = 0.125 ± 0.03, CH{sub 3}CHO{sup *} → CH{sub 3} + H + CO ϕ{sub 1e} = 0.205 ± 0.04, CH{sub 3}CHO{sup *}→{sup o{sub 2}}CH{sub 3}CO + HO{sub 2} ϕ{sub 1f} = 0.07 ± 0.01. The CH{sub 3}O{sub 2} quantum yield has been determined in separate experiments as ϕ{sub CH{sub 3}} = 0.33 ± 0.03 and is in excellent agreement with the CH{sub 3} yields derived from the HO{sub 2} measurements considering that the triple fragmentation (R1e) is an important reaction path in the 248 nm photolysis of CH{sub 3}CHO. From arithmetic considerations taking into account the HO{sub 2} and CH{sub 3} measurements we deduce a remaining quantum yield for the molecular pathway: CH{sub 3}CHO{sup *} → CH{sub 4} + CO ϕ{sub 1b} = 0.6. All experiments can be consistently explained with absence of the formerly considered pathway: CH{sub 3}CHO{sup *} → CH{sub 3}CO + H ϕ{sub 1c} = 0.« less

Use of the fluorescence quantum yield for the determination of the number-average molecular weight of polymers of epicatechin with 4β→8 interflavin bonds

Treesearch

D. Cho; W.L. Mattice; L.J. Porter; Richard W. Hemingway

1989-01-01

Excitation at 280 nm produces a structureless emission band with a maximum at 321-324 nm for dilute solutions of catechin, epicatechin, and their oligomers in l,4-dioxane or water. The fluorescence quantum yield, Q, has been measured in these two solvents for five dimers, a trimer, a tetramer, a pentamer, a hexamer, and a polymer in which the monomer...

Excitation-emission spectra and fluorescence quantum yields for fresh and aged biogenic secondary organic aerosols

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lee, Hyun Ji; Laskin, Alexander; Laskin, Julia

2013-05-10

Certain biogenic secondary organic aerosols (SOA) become absorbent and fluorescent when exposed to reduced nitrogen compounds such as ammonia, amines and their salts. Fluorescent SOA may potentially be mistaken for biological particles by detection methods relying on fluorescence. This work quantifies the spectral distribution and effective quantum yields of fluorescence of SOA generated from two monoterpenes, limonene and a-pinene, and two different oxidants, ozone (O3) and hydroxyl radical (OH). The SOA was generated in a smog chamber, collected on substrates, and aged by exposure to ~100 ppb ammonia vapor in air saturated with water vapor. Absorption and excitation-emission matrix (EEM)more » spectra of aqueous extracts of aged and control SOA samples were measured, and the effective absorption coefficients and fluorescence quantum yields (~0.005 for 349 nm excitation) were determined from the data. The strongest fluorescence for the limonene-derived SOA was observed for excitation = 420+- 50 nm and emission = 475 +- 38 nm. The window of the strongest fluorescence shifted to excitation = 320 +- 25 nm and emission = 425 +- 38 nm for the a-pinene-derived SOA. Both regions overlap with the excitation-emission matrix (EEM) spectra of some of the fluorophores found in primary biological aerosols. Our study suggests that, despite the low quantum yield, the aged SOA particles should have sufficient fluorescence intensities to interfere with the fluorescence detection of common bioaerosols.« less

Excitation-emission spectra and fluorescence quantum yields for fresh and aged biogenic secondary organic aerosols.

PubMed

Lee, Hyun Ji Julie; Laskin, Alexander; Laskin, Julia; Nizkorodov, Sergey A

2013-06-04

Certain biogenic secondary organic aerosols (SOA) become absorbent and fluorescent when exposed to reduced nitrogen compounds such as ammonia, amines, and their salts. Fluorescent SOA may potentially be mistaken for biological particles by detection methods relying on fluorescence. This work quantifies the spectral distribution and effective quantum yields of fluorescence of water-soluble SOA generated from two monoterpenes, limonene and α-pinene, and two different oxidants, ozone (O3) and hydroxyl radical (OH). The SOA was generated in a smog chamber, collected on substrates, and aged by exposure to ∼100 ppb ammonia in air saturated with water vapor. Absorption and excitation-emission matrix (EEM) spectra of aqueous extracts of aged and control SOA samples were measured, and the effective absorption coefficients and fluorescence quantum yields (∼0.005 for 349 nm excitation) were determined from the data. The strongest fluorescence for the limonene-derived SOA was observed for λexcitation = 420 ± 50 nm and λemission = 475 ± 38 nm. The window of the strongest fluorescence shifted to λexcitation = 320 ± 25 nm and λemission = 425 ± 38 nm for the α-pinene-derived SOA. Both regions overlap with the EEM spectra of some of the fluorophores found in primary biological aerosols. Despite the low quantum yield, the aged SOA particles may have sufficient fluorescence intensities to interfere with the fluorescence detection of common bioaerosols.

Pyropia yezoensis can utilize CO2 in the air during moderate dehydration

NASA Astrophysics Data System (ADS)

Zhou, Wei; He, Linwen; Yang, Fang; Lin, Apeng; Zhang, Baoyu; Niu, Jianfeng; Wang, Guangce

2014-03-01

Pyropia yezoensis, an intertidal seaweed, experiences regular dehydration and rehydration with the tides. In this study, the responses of P. yezoensis to dehydration and rehydration under high and low CO2 concentrations ((600-700)×10-6 and (40-80)×10-6, named Group I and Group II respectively) were investigated. The thalli of Group I had a significantly higher effective photosystem II quantum yield than the thalli of Group II at 71% absolute water content (AWC). There was little difference between thalli morphology, total Rubisco activity and total protein content at 100% and 71% AWC, which might be the basis for the normal performance of photosynthesis during moderate dehydration. A higher effective photosystem I quantum yield was observed in the thalli subjected to a low CO2 concentration during moderate dehydration, which might be caused by the enhancement of cyclic electron flow. These results suggested that P. yezoensis can directly utilize CO2 in ambient air during moderate dehydration.

Antitumor effects evaluation of a novel porphyrin derivative in photodynamic therapy.

PubMed

Li, Jian-Wei; Wu, Zhong-Ming; Magetic, Davor; Zhang, Li-Jun; Chen, Zhi-Long

2015-12-01

In this paper, the antitumor activity of a novel porphyrin-based photosensitizer 5,10,15,20-tetrakis[(5-diethylamino)pentyl] porphyrin (TDPP) was reported in vitro and in vivo. The photophysical and cellular properties of TDPP were investigated. The singlet oxygen generation quantum yield of TDPP was detected; it showed a high singlet oxygen quantum yield of 0.52. The intracellular distribution of photosensitizer was detected with laser scanning confocal microscopy. The efficiency of TDPP-photodynamic therapy (PDT) in vitro was analyzed by 3-(4,5-dimethyl-2-thiazolyl)-2,5-diphenyl-2H-tetrazolium bromide (MTT) assay and in situ trypan blue exclusion test. Treated with a 630-nm laser, TDPP can kill cultured human esophageal cancer cell line (Eca-109) cells and reduce the growth of Eca-109 xenograft tumors significantly in BABL/c nude mice. And histopathological study was also used to confirm the antitumor effect. It has the perspective to be developed as a new antitumor drug in photodynamic therapy and deserves further investigation.

Atomic electric fields revealed by a quantum mechanical approach to electron picodiffraction.

PubMed

Müller, Knut; Krause, Florian F; Béché, Armand; Schowalter, Marco; Galioit, Vincent; Löffler, Stefan; Verbeeck, Johan; Zweck, Josef; Schattschneider, Peter; Rosenauer, Andreas

2014-12-15

By focusing electrons on probes with a diameter of 50 pm, aberration-corrected scanning transmission electron microscopy (STEM) is currently crossing the border to probing subatomic details. A major challenge is the measurement of atomic electric fields using differential phase contrast (DPC) microscopy, traditionally exploiting the concept of a field-induced shift of diffraction patterns. Here we present a simplified quantum theoretical interpretation of DPC. This enables us to calculate the momentum transferred to the STEM probe from diffracted intensities recorded on a pixel array instead of conventional segmented bright-field detectors. The methodical development yielding atomic electric field, charge and electron density is performed using simulations for binary GaN as an ideal model system. We then present a detailed experimental study of SrTiO3 yielding atomic electric fields, validated by comprehensive simulations. With this interpretation and upgraded instrumentation, STEM is capable of quantifying atomic electric fields and high-contrast imaging of light atoms.

Atomic electric fields revealed by a quantum mechanical approach to electron picodiffraction

NASA Astrophysics Data System (ADS)

Müller, Knut; Krause, Florian F.; Béché, Armand; Schowalter, Marco; Galioit, Vincent; Löffler, Stefan; Verbeeck, Johan; Zweck, Josef; Schattschneider, Peter; Rosenauer, Andreas

2014-12-01

By focusing electrons on probes with a diameter of 50 pm, aberration-corrected scanning transmission electron microscopy (STEM) is currently crossing the border to probing subatomic details. A major challenge is the measurement of atomic electric fields using differential phase contrast (DPC) microscopy, traditionally exploiting the concept of a field-induced shift of diffraction patterns. Here we present a simplified quantum theoretical interpretation of DPC. This enables us to calculate the momentum transferred to the STEM probe from diffracted intensities recorded on a pixel array instead of conventional segmented bright-field detectors. The methodical development yielding atomic electric field, charge and electron density is performed using simulations for binary GaN as an ideal model system. We then present a detailed experimental study of SrTiO3 yielding atomic electric fields, validated by comprehensive simulations. With this interpretation and upgraded instrumentation, STEM is capable of quantifying atomic electric fields and high-contrast imaging of light atoms.

Electron-Poor Thiophene 1,1-Dioxides: Synthesis, Characterization, and Application as Electron Relays in Photocatalytic Hydrogen Generation.

PubMed

Tsai, Chia-Hua; Chirdon, Danielle N; Kagalwala, Husain N; Maurer, Andrew B; Kaur, Aman; Pintauer, Tomislav; Bernhard, Stefan; Noonan, Kevin J T

2015-08-03

The synthesis and characterization of electron-poor thiophene 1,1-dioxides bearing cyanated phenyl groups are reported. The electron-accepting nature of these compounds was evaluated by cyclic voltammetry, and highly reversible and facile reductions were observed for several derivatives. Moreover, some of the reduced thiophene dioxides form colorful anions, which were investigated spectroelectrochemically. Photoluminescence spectra of the electron-deficient sulfones were measured in CH2 Cl2, and they emit in the blue-green region with significant variation in the quantum yield depending on the aryl substituents. By expanding the degree of substitution on the phenyl rings, quantum yields up to 34 % were obtained. X-ray diffraction data are reported for two of the thiophene 1,1-dioxides, and the electronic structure was probed for all synthesized derivatives through DFT calculations. The dioxides were also examined as electron relays in a photocatalytic water reduction reaction, and they showed potential to boost the efficiency. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Near-unity photoluminescence quantum yield in MoS₂.

PubMed

Amani, Matin; Lien, Der-Hsien; Kiriya, Daisuke; Xiao, Jun; Azcatl, Angelica; Noh, Jiyoung; Madhvapathy, Surabhi R; Addou, Rafik; KC, Santosh; Dubey, Madan; Cho, Kyeongjae; Wallace, Robert M; Lee, Si-Chen; He, Jr-Hau; Ager, Joel W; Zhang, Xiang; Yablonovitch, Eli; Javey, Ali

2015-11-27

Two-dimensional (2D) transition metal dichalcogenides have emerged as a promising material system for optoelectronic applications, but their primary figure of merit, the room-temperature photoluminescence quantum yield (QY), is extremely low. The prototypical 2D material molybdenum disulfide (MoS2) is reported to have a maximum QY of 0.6%, which indicates a considerable defect density. Here we report on an air-stable, solution-based chemical treatment by an organic superacid, which uniformly enhances the photoluminescence and minority carrier lifetime of MoS2 monolayers by more than two orders of magnitude. The treatment eliminates defect-mediated nonradiative recombination, thus resulting in a final QY of more than 95%, with a longest-observed lifetime of 10.8 ± 0.6 nanoseconds. Our ability to obtain optoelectronic monolayers with near-perfect properties opens the door for the development of highly efficient light-emitting diodes, lasers, and solar cells based on 2D materials. Copyright © 2015, American Association for the Advancement of Science.

Slow-Injection Growth of Seeded CdSe/CdS Nanorods with Unity Fluorescence Quantum Yield and Complete Shell to Core Energy Transfer.

PubMed

Coropceanu, Igor; Rossinelli, Aurelio; Caram, Justin R; Freyria, Francesca S; Bawendi, Moungi G

2016-03-22

A two-step process has been developed for growing the shell of CdSe/CdS core/shell nanorods. The method combines an established fast-injection-based step to create the initial elongated shell with a second slow-injection growth that allows for a systematic variation of the shell thickness while maintaining a high degree of monodispersity at the batch level and enhancing the uniformity at the single-nanorod level. The second growth step resulted in nanorods exhibiting a fluorescence quantum yield up to 100% as well as effectively complete energy transfer from the shell to the core. This improvement suggests that the second step is associated with a strong suppression of the nonradiative channels operating both before and after the thermalization of the exciton. This hypothesis is supported by the suppression of a defect band, ubiquitous to CdSe-based nanocrystals after the second growth.

Atomic electric fields revealed by a quantum mechanical approach to electron picodiffraction

PubMed Central

Müller, Knut; Krause, Florian F.; Béché, Armand; Schowalter, Marco; Galioit, Vincent; Löffler, Stefan; Verbeeck, Johan; Zweck, Josef; Schattschneider, Peter; Rosenauer, Andreas

2014-01-01

By focusing electrons on probes with a diameter of 50 pm, aberration-corrected scanning transmission electron microscopy (STEM) is currently crossing the border to probing subatomic details. A major challenge is the measurement of atomic electric fields using differential phase contrast (DPC) microscopy, traditionally exploiting the concept of a field-induced shift of diffraction patterns. Here we present a simplified quantum theoretical interpretation of DPC. This enables us to calculate the momentum transferred to the STEM probe from diffracted intensities recorded on a pixel array instead of conventional segmented bright-field detectors. The methodical development yielding atomic electric field, charge and electron density is performed using simulations for binary GaN as an ideal model system. We then present a detailed experimental study of SrTiO3 yielding atomic electric fields, validated by comprehensive simulations. With this interpretation and upgraded instrumentation, STEM is capable of quantifying atomic electric fields and high-contrast imaging of light atoms. PMID:25501385

SU-E-T-191: First Principle Calculation of Quantum Yield in Photodynamic Therapy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Abolfath, R; Guo, F; Chen, Z

Purpose: We present a first-principle method to calculate the spin transfer efficiency in oxygen induced by any photon fields especially in MeV energy range. The optical pumping is mediated through photosensitizers, e.g., porphyrin and/or ensemble of quantum dots. Methods: Under normal conditions, oxygen molecules are in the relatively non-reactive triplet state. In the presence of certain photosensitizer compounds such as porphyrins, electromagnetic radiation of specific wavelengths can excite oxygen to highly reactive singlet state. With selective uptake of photosensitizers by certain malignant cells, photon irradiation of phosensitized tumors can lead to selective killing of cancer cells. This is the basismore » of photodynamic therapy (PDT). Despite several attempts, PDT has not been clinically successful except in limited superficial cancers. Many parameters such as photon energy, conjugation with quantum dots etc. can be potentially combined with PDT in order to extend the role of PDT in cancer management. The key quantity for this optimization is the spin transfer efficiency in oxygen by any photon field. The first principle calculation model presented here, is an attempt to fill this need. We employ stochastic density matrix description of the quantum jumps and the rate equation methods in quantum optics based on Markov/Poisson processes and calculate time evolution of the population of the optically pumped singlet oxygen. Results: The results demonstrate the feasibility of our model in showing the dependence of the optical yield in generating spin-singlet oxygen on the experimental conditions. The adjustable variables can be tuned to maximize the population of the singlet oxygen hence the efficacy of the photodynamic therapy. Conclusion: The present model can be employed to fit and analyze the experimental data and possibly to assist researchers in optimizing the experimental conditions in photodynamic therapy.« less

Circularly Polarized Luminescence in Enantiopure Europium and Terbium Complexes with Modular, All-Oxygen Donor Ligands

PubMed Central

Seitz, Michael; Do, King; Ingram, Andrew J.; Moore, Evan G.; Muller, Gilles; Raymond, Kenneth N.

2009-01-01

Abstract: Circulaly polarized luminescence from terbium(III) complexed and excited by chiral antenna ligands gives strong emission The modular synthesis of three new octadentate, enantiopure ligands are reported - one with the bidentate chelating unit 2-hydroxyisophthalamide (IAM) and two with 1-hydroxy-2-pyridinone (1,2-HOPO) units. A new design principle is introduced for the chiral, non-racemic hexamines which constitute the central backbones for the presented class of ligands. The terbium(III) complex of the IAM ligand, as well as the europium(III) complexes of the 1,2-HOPO ligands are synthesized and characterized by various techniques (NMR, UV, CD, luminescence spectroscopy). All species exhibit excellent stability and moderate to high luminescence efficiency (quantum yields ΦEu = 0.05–0.08 and ΦTb = 0.30–0.57) in aqueous solution at physiological pH. Special focus is put onto the properties of the complexes in regard to circularly polarized luminescence (CPL). The maximum luminescence dissymmetry factors (glum) in aqueous solution are high with |glum|max = 0.08 – 0.40. Together with the very favorable general properties (good stability, high quantum yields, long lifetimes), the presented lanthanide complexes can be considered as good candidates for analytical probes based on CPL in biologically relevant environments. PMID:19639983

Photochemical processes on Titan: Irradiation of mixtures of gases that simulate Titan's atmosphere

NASA Astrophysics Data System (ADS)

Tran, Buu N.; Joseph, Jeffrey C.; Force, Michael; Briggs, Robert G.; Vuitton, Veronique; Ferris, James P.

2005-09-01

Photochemical reaction pathways in Titan's atmosphere were investigated by irradiation of the individual components and the mixture containing nitrogen, methane, hydrogen, acetylene, ethylene, and cyanoacetylene. The quantum yields for the loss of the reactants and the formation of products were determined. Photolysis of ethylene yields mainly saturated compounds (ethane, propane, and butane) while photolysis of acetylene yields the same saturated compounds as well as ethylene and diacetylene. Irradiation of cyanoacetylene yields mainly hydrogen cyanide and small amounts of acetonitrile. When an amount of methane corresponding to its mixing ratio on Titan was added to these mixtures the quantum yields for the loss of reactants decreased and the quantum yields for hydrocarbon formation increased indicative of a hydrogen atom abstraction from methane by the photochemically generated radicals. GC/MS analysis of the products formed by irradiation of mixtures of all these gases generated over 120 compounds which were mainly aliphatic hydrocarbons containing double and triple bonds along with much smaller amounts of aromatic compounds like benzene, toluene and phenylacetylene. The reaction pathways were investigated by the use of 13C acetylene in these gas mixtures. No polycyclic aromatic compounds were detected. Vapor pressures of these compounds under conditions present in Titan's atmosphere were calculated. The low molecular weight compounds likely to be present in the atmosphere and aerosols of Titan as a result of photochemical processes are proposed.

Near infrared emission of TbAG:Ce3+,Yb3+ phosphor for solar cell applications

NASA Astrophysics Data System (ADS)

Meshram, N. D.; Yadav, P. J.; Pathak, A. A.; Joshi, C. P.; Moharil, S. V.

2016-05-01

Luminescent materials doped with rare earth ions are used for many devices such as optical amplifiers in telecommunication, phosphors for white light emitting diodes (LEDs), displays, and so on. Recently, they also have attracted a great interest for photovoltaic applications to improve solar cell efficiency by modifying solar spectrum. Crystal silicon (c-Si) solar cells most effectively convert photons of energy close to the semiconductor band gap. The mis-match between the incident solar spectrum and the spectral response of solar cells is one of the main reasons to limit the cell efficiency. The efficiency limit of the c-Si has been estimated to be 29% by Shockley and Queisser. However, this limit is estimated to be improved up to 38.4% by modifying the solar spectrum by a quantum cutting (down converting) phosphor which converts one photon of high energy into two photons of lower energy. The phenomenon such as the quantum cutting or the down conversion of rare earth ions have been investigated since Dexter reported the possibility of a luminescent quantum yield greater than unity in 1957. In the past, the quantum cutting from a vacuum ultraviolet photon to visible photons for Pr3+, Gd3+,Gd3+-Eu3+, and Er3+-Tb3+ had been studied. Recently, a new quantum cutting phenomenon from visible photon shorter than 500 nm to two infrared photons for Tb3+-Yb3+, Pr3+-Yb3+, and Tm3+-Yb3+ has been reported. The Yb3+ ion is suitable as an acceptor and emitter because luminescent quantum efficiency of Yb3+ is close to 100% and the energy of the only excited level of Yb3+ (1.2 eV) is roughly in accordance with the band gap of Si (1.1 eV). In addition, the Ce3+-doped Tb3Al5O12 (TbAG), used as a phosphor for white LED, has broad absorption bands in the range of 300-500 nm due to strong ligand field and high luminescent quantum efficiency. Therefore, the Ce3+ ions in the TbAG can be suitable as an excellent sensitizing donor for down conversion materials of Si solar cells. In this paper, Ce3+ -Yb3+-codoped TbAG ceramics were prepared and the energy transfer (ET) including down conversion mechanism in Ce3+ - Yb3+ codoped TbAG ceramics have been evaluated by the photoluminescence (PL), the photoluminescence excitation (PLE), the lifetime and the quantum yield (QY), which was measured directly using an integrating sphere.

Does photodissociation of molecular oxygen from myoglobin and hemoglobin yield singlet oxygen?

PubMed

Lepeshkevich, Sergei V; Stasheuski, Alexander S; Parkhats, Marina V; Galievsky, Victor A; Dzhagarov, Boris M

2013-03-05

Time-resolved luminescence measurements in the near-infrared region indicate that photodissociation of molecular oxygen from myoglobin and hemoglobin does not produce detectable quantities of singlet oxygen. A simple and highly sensitive method of luminescence quantification is developed and used to determine the upper limit for the quantum yield of singlet oxygen production. The proposed method was preliminarily evaluated using model data sets and confirmed with experimental data for aqueous solutions of 5,10,15,20-tetrakis(4-N-methylpyridyl) porphyrin. A general procedure for error estimation is suggested. The method is shown to provide a determination of the integral luminescence intensity in a wide range of values even for kinetics with extremely low signal-to-noise ratio. The present experimental data do not deny the possibility of singlet oxygen generation during the photodissociation of molecular oxygen from myoglobin and hemoglobin. However, the photodissociation is not efficient to yield singlet oxygen escaped from the proteins into the surrounding medium. The upper limits for the quantum yields of singlet oxygen production in the surrounding medium after the photodissociation for oxyhemoglobin and oxymyoglobin do not exceed 3.4×10(-3) and 2.3×10(-3), respectively. On the average, no more than one molecule of singlet oxygen from every hundred photodissociated oxygen molecules can succeed in escaping from the protein matrix. Copyright © 2013 Elsevier B.V. All rights reserved.

High performance of PbSe/PbS core/shell quantum dot heterojunction solar cells: short circuit current enhancement without the loss of open circuit voltage by shell thickness control.

PubMed

Choi, Hyekyoung; Song, Jung Hoon; Jang, Jihoon; Mai, Xuan Dung; Kim, Sungwoo; Jeong, Sohee

2015-11-07

We fabricated heterojunction solar cells with PbSe/PbS core shell quantum dots and studied the precisely controlled PbS shell thickness dependency in terms of optical properties, electronic structure, and solar cell performances. When the PbS shell thickness increases, the short circuit current density (JSC) increases from 6.4 to 11.8 mA cm(-2) and the fill factor (FF) enhances from 30 to 49% while the open circuit voltage (VOC) remains unchanged at 0.46 V even with the decreased effective band gap. We found that the Fermi level and the valence band maximum level remain unchanged in both the PbSe core and PbSe/PbS core/shell with a less than 1 nm thick PbS shell as probed via ultraviolet photoelectron spectroscopy (UPS). The PbS shell reduces their surface trap density as confirmed by relative quantum yield measurements. Consequently, PbS shell formation on the PbSe core mitigates the trade-off relationship between the open circuit voltage and the short circuit current density. Finally, under the optimized conditions, the PbSe core with a 0.9 nm thick shell yielded a power conversion efficiency of 6.5% under AM 1.5.

Improving the efficiency of water splitting in dye-sensitized solar cells by using a biomimetic electron transfer mediator

PubMed Central

Zhao, Yixin; Swierk, John R.; Megiatto, Jackson D.; Sherman, Benjamin; Youngblood, W. Justin; Qin, Dongdong; Lentz, Deanna M.; Moore, Ana L.; Moore, Thomas A.; Gust, Devens; Mallouk, Thomas E.

2012-01-01

Photoelectrochemical water splitting directly converts solar energy to chemical energy stored in hydrogen, a high energy density fuel. Although water splitting using semiconductor photoelectrodes has been studied for more than 40 years, it has only recently been demonstrated using dye-sensitized electrodes. The quantum yield for water splitting in these dye-based systems has, so far, been very low because the charge recombination reaction is faster than the catalytic four-electron oxidation of water to oxygen. We show here that the quantum yield is more than doubled by incorporating an electron transfer mediator that is mimetic of the tyrosine-histidine mediator in Photosystem II. The mediator molecule is covalently bound to the water oxidation catalyst, a colloidal iridium oxide particle, and is coadsorbed onto a porous titanium dioxide electrode with a Ruthenium polypyridyl sensitizer. As in the natural photosynthetic system, this molecule mediates electron transfer between a relatively slow metal oxide catalyst that oxidizes water on the millisecond timescale and a dye molecule that is oxidized in a fast light-induced electron transfer reaction. The presence of the mediator molecule in the system results in photoelectrochemical water splitting with an internal quantum efficiency of approximately 2.3% using blue light. PMID:22547794

Heterodiazocines: Synthesis and Photochromic Properties, Trans to Cis Switching within the Bio-optical Window.

PubMed

Hammerich, Melanie; Schütt, Christian; Stähler, Cosima; Lentes, Pascal; Röhricht, Fynn; Höppner, Ronja; Herges, Rainer

2016-10-04

Diazocines, bridged azobenzenes, exhibit superior photophysical properties compared to parent azobenzenes such as high switching efficiencies, quantum yields, and particularly switching wavelengths in the visible range. Synthesis, however, proceeds with low yields, and derivatives are difficult to prepare. We now present two heterodiazocines which are easier to synthesize, and the general procedures should also provide facile access to derivatives. Moreover, both compounds can be switched with light in the far-red (650 nm). Accessibility and photophysical properties make them ideal candidates for applications such as photoswitchable drugs and functional materials.

Bifurcation-based adiabatic quantum computation with a nonlinear oscillator network.

PubMed

Goto, Hayato

2016-02-22

The dynamics of nonlinear systems qualitatively change depending on their parameters, which is called bifurcation. A quantum-mechanical nonlinear oscillator can yield a quantum superposition of two oscillation states, known as a Schrödinger cat state, via quantum adiabatic evolution through its bifurcation point. Here we propose a quantum computer comprising such quantum nonlinear oscillators, instead of quantum bits, to solve hard combinatorial optimization problems. The nonlinear oscillator network finds optimal solutions via quantum adiabatic evolution, where nonlinear terms are increased slowly, in contrast to conventional adiabatic quantum computation or quantum annealing, where quantum fluctuation terms are decreased slowly. As a result of numerical simulations, it is concluded that quantum superposition and quantum fluctuation work effectively to find optimal solutions. It is also notable that the present computer is analogous to neural computers, which are also networks of nonlinear components. Thus, the present scheme will open new possibilities for quantum computation, nonlinear science, and artificial intelligence.

Bifurcation-based adiabatic quantum computation with a nonlinear oscillator network

NASA Astrophysics Data System (ADS)

Goto, Hayato

2016-02-01

The dynamics of nonlinear systems qualitatively change depending on their parameters, which is called bifurcation. A quantum-mechanical nonlinear oscillator can yield a quantum superposition of two oscillation states, known as a Schrödinger cat state, via quantum adiabatic evolution through its bifurcation point. Here we propose a quantum computer comprising such quantum nonlinear oscillators, instead of quantum bits, to solve hard combinatorial optimization problems. The nonlinear oscillator network finds optimal solutions via quantum adiabatic evolution, where nonlinear terms are increased slowly, in contrast to conventional adiabatic quantum computation or quantum annealing, where quantum fluctuation terms are decreased slowly. As a result of numerical simulations, it is concluded that quantum superposition and quantum fluctuation work effectively to find optimal solutions. It is also notable that the present computer is analogous to neural computers, which are also networks of nonlinear components. Thus, the present scheme will open new possibilities for quantum computation, nonlinear science, and artificial intelligence.

Ramsey-type spectroscopy in the XUV spectral region

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pirri, A.; European Laboratory for Nonlinear Spectroscopy, Via N. Carrara 1, I-50019 Sesto Fiorentino; Sali, E.

2010-02-02

We report an experimental and theoretical investigation of Ramsey-type spectroscopy with high-order harmonic generation applied to autoionizing states of Krypton. The ionization yield, detected by an ion-mass spectrometer, shows the characteristic quantum interference pattern. The behaviour of the fringe contrast was interpreted on the basis of a simple analytic model, which reproduces the experimental data without any free parameter.

Thermally activated delayed fluorescence of a Zr-based metal–organic framework

DOE PAGES

Mieno, H.; Kabe, R.; Allendorf, M. D.; ...

2017-12-22

Here, the first metal–organic framework exhibiting thermally activated delayed fluorescence (TADF) was developed. The zirconium-based framework (UiO-68-dpa) uses a newly designed linker composed of a terphenyl backbone, an electron-accepting carboxyl group, and an electron-donating diphenylamine and exhibits green TADF emission with a photoluminescence quantum yield of 30% and high thermal stability.

Facile Preparation of Light Emitting Organic Metal Halide Crystals with Near-Unity Quantum Efficiency

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhou, Chenkun; Worku, Michael; Neu, Jennifer

Here, we report the synthesis and characterization of (Ph 4P) 2SbCl 5, a novel ionically bonded organic metal halide hybrid with a zero-dimensional (0D) structure at the molecular level. By cocrystallization of tetraphenylphosphonium (Ph 4P +) and antimony (Sb 3+) chloride salts, (Ph 4P) 2SbCl 5 bulk single crystals can be prepared in high yield, which exhibit a highly efficient broadband red emission peaked at 648 nm with a photoluminescence quantum efficiency (PLQE) of around 87%. Density functional theory (DFT) calculations reveal the origin of emission as phosphorescence from the excitons localized at SbCl 5 2– with strong excited-state structuralmore » distortion. Interestingly, (Ph 4P) 2SbCl 5 bulk crystals with a PLQE of around 100% can be prepared via a rapid crystal growth process within minutes, followed by a spontaneous structural transformation. It was found that the rapid growth process yielded a yellow emitting kinetically favored metastable product containing solvent molecules, which turned into the red emitting thermodynamically stable product slowly at room temperature or quickly upon thermal treatment.« less

Facile Preparation of Light Emitting Organic Metal Halide Crystals with Near-Unity Quantum Efficiency

DOE PAGES

Zhou, Chenkun; Worku, Michael; Neu, Jennifer; ...

2018-03-12

Here, we report the synthesis and characterization of (Ph 4P) 2SbCl 5, a novel ionically bonded organic metal halide hybrid with a zero-dimensional (0D) structure at the molecular level. By cocrystallization of tetraphenylphosphonium (Ph 4P +) and antimony (Sb 3+) chloride salts, (Ph 4P) 2SbCl 5 bulk single crystals can be prepared in high yield, which exhibit a highly efficient broadband red emission peaked at 648 nm with a photoluminescence quantum efficiency (PLQE) of around 87%. Density functional theory (DFT) calculations reveal the origin of emission as phosphorescence from the excitons localized at SbCl 5 2– with strong excited-state structuralmore » distortion. Interestingly, (Ph 4P) 2SbCl 5 bulk crystals with a PLQE of around 100% can be prepared via a rapid crystal growth process within minutes, followed by a spontaneous structural transformation. It was found that the rapid growth process yielded a yellow emitting kinetically favored metastable product containing solvent molecules, which turned into the red emitting thermodynamically stable product slowly at room temperature or quickly upon thermal treatment.« less

Molecular processes in a high temperature shock layer

NASA Technical Reports Server (NTRS)

Guberman, S. L.

1984-01-01

Models of the shock layer encountered by an Aeroassisted Orbital Transfer Vehicle require as input accurate cross sections and rate constants for the atomic and molecular processes that characterize the shock radiation. From the estimated atomic and molecular densities in the shock layer and the expected residence time of 1 m/s, it can be expected that electron-ion collision processes will be important in the shock model. Electron capture by molecular ions followed by dissociation, e.g., O2(+) + e(-) yields 0 + 0, can be expected to be of major importance since these processes are known to have high rates (e.g., 10 to the -7th power cu/cm/sec) at room temperature. However, there have been no experimental measurements of dissociative recombination (DR) at temperatures ( 12000K) that are expected to characterize the shock layer. Indeed, even at room temperature, it is often difficult to perform experiments that determine the dependence of the translational energy and quantum yields of the product atoms on the electronic and vibrational state of the reactant molecular ions. Presented are ab initio quantum chemical studies of DR for molecular ions that are likely to be important in the atmospheric shock layer.

Spectroscopic and laser characterization of emerald. Final report, April 1983-April 1986

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lai, S.T.; Chai, B.H.

1986-08-01

The spectroscopic characteristics and laser properties of emerald were investigated. The laser measurements showed that the emerald-laser tuning range was 720-842 nm and exhibited a high gain and high efficiency in the 760-790 nm range. Under a crystal growth development program, the laser loss was reduced from 11%/cm to 0.4%/cm. The limiting factor in the laser efficiency is the excited-state absorption (ESA). The ESA was measured by two methods: a laser-pumped single-pass gain method, which is generally applicable to all tunable laser materials, and a laser-pumped laser method. A 76% laser quantum yield was obtained in high-optical-quality emerald. The maximummore » yield is estimated to be 83%, based on the ESA measurements.« less

Can we Predict Quantum Yields Using Excited State Density Functional Theory for New Families of Fluorescent Dyes?

NASA Astrophysics Data System (ADS)

Kohn, Alexander W.; Lin, Zhou; Shepherd, James J.; Van Voorhis, Troy

2016-06-01

For a fluorescent dye, the quantum yield characterizes the efficiency of energy transfer from the absorbed light to the emitted fluorescence. In the screening among potential families of dyes, those with higher quantum yields are expected to have more advantages. From the perspective of theoreticians, an efficient prediction of the quantum yield using a universal excited state electronic structure theory is in demand but still challenging. The most representative examples for such excited state theory include time-dependent density functional theory (TDDFT) and restricted open-shell Kohn-Sham (ROKS). In the present study, we explore the possibility of predicting the quantum yields for conventional and new families of organic dyes using a combination of TDDFT and ROKS. We focus on radiative (kr) and nonradiative (knr) rates for the decay of the first singlet excited state (S_1) into the ground state (S_0) in accordance with Kasha's rule. M. Kasha, Discuss. Faraday Soc., 9, 14 (1950). For each dye compound, kr is calculated with the S_1-S_0 energy gap and transition dipole moment obtained using ROKS and TDDFT respectively at the relaxed S_1 geometry. Our predicted kr agrees well with the experimental value, so long as the order of energy levels is correctly predicted. Evaluation of knr is less straightforward as multiple processes are involved. Our study focuses on the S_1-T_1 intersystem crossing (ISC) and the S_1-S_0 internal conversion (IC): we investigate the properties that allow us to model the knr value using a Marcus-like expression, such as the Stokes shift, the reorganization energy, and the S_1-T_1 and S_1-S_0 energy gaps. Taking these factors into consideration, we compare our results with those obtained using the actual Marcus theory and provide explanation for discrepancy. T. Kowalczyk, T. Tsuchimochi, L. Top, P.-T. Chen, and T. Van Voorhis, J. Chem. Phys., 138, 164101 (2013). M. Kasha, Discuss. Faraday Soc., 9, 14 (1950).

Effects of surface and interface traps on exciton and multi-exciton dynamics in core/shell quantum dots

NASA Astrophysics Data System (ADS)

Bozio, Renato; Righetto, Marcello; Minotto, Alessandro

2017-08-01

Exciton interactions and dynamics are the most important factors determining the exceptional photophysical properties of semiconductor quantum dots (QDs). In particular, best performances have been obtained for ingeniously engineered core/shell QDs. We have studied two factors entering in the exciton decay dynamics with adverse effects for the luminescence efficiency: exciton trapping at surface and interface traps, and non-radiative Auger recombination in QDs carrying either net charges or multiple excitons. In this work, we present a detailed study into the optical absorption, fluorescence dynamics and quantum yield, as well as ultrafast transient absorption properties of CdSe/CdS, CdSe/Cd0.5Zn0.5S, and CdSe/ZnS QDs as a function of shell thickness. It turns out that de-trapping processes play a pivotal role in determining steady state emission properties. By studying the excitation dependent photoluminescence quantum yields (PLQY) in different CdSe/CdxZn1-xS (x = 0, 0.5, 1) QDs, we demonstrate the different role played by hot and cold carrier trapping rates in determining fluorescence quantum yields. Finally, the use of global analysis allows us untangling the complex ultrafast transient absorption signals. Smoothing of interface potential, together with effective surface passivation, appear to be crucial factors in slowing down both Auger-based and exciton trapping recombination processes.

Phototransformation of anthraquinone-2-sulphonate in aqueous solution.

PubMed

Bedini, Andrea; De Laurentiis, Elisa; Sur, Babita; Maurino, Valter; Minero, Claudio; Brigante, Marcello; Mailhot, Gilles; Vione, Davide

2012-09-01

Anthraquinone-2-sulphonate (AQ2S) is a triplet sensitiser that has recently been used to model the photoreactivity of chromophoric dissolved organic matter (CDOM). We show that the photolysis quantum yield of AQ2S under UVA irradiation varies from (3.4 ± 0.2) × 10(-3) at μM AQ2S levels to (1.8 ± 0.1) × 10(-2) at 3 mM AQ2S (μ±σ). This trend is consistent with a combination of direct phototransformation and transformation sensitised by a photogenerated reactive species. In both cases a transient water adduct of AQ2S would be involved. Depending on the initial quinone concentration, the adduct could undergo transformation, give back ground-state AQ2S or react with it. The prevalence of the latter process at high AQ2S concentration would account for the increased values of the photolysis quantum yield. When using AQ2S as a triplet sensitiser, one should not exceed an initial concentration of 0.1 mM. Under the latter conditions the sensitised process is negligible compared to the direct photolysis, providing a simpler system to be studied, and the photolysis quantum yield is independent of the initial AQ2S concentration. This paper also shows, by adoption of density functional theory calculations, that the triplet state of AQ2S has most of the spin density localised on C[double bond, length as m-dash]O, analogous to other photoactive quinones, which accounts for the oxidising character of the triplet state that tends to be reduced to a semiquinone radical.

Photophysical properties gallium octacarboxy phthalocyanines conjugated to CdSe@ZnS quantum dots.

PubMed

Tshangana, Charmaine; Nyokong, Tebello

2015-01-01

L-Glutathione (GSH) capped core CdSe (2.3 nm) and core shell CdSe@ZnS quantum dots (QDs) (3.0 nm and 3.5 nm) were coordinated to gallium octacarboxy phthalocyanine (ClGaPc(COOH)8) to form ClGaPc(COOH)8-QDs conjugates. An efficient transfer of energy from the QDs to the Pcs was demonstrated through Förster resonance energy transfer (FRET), the FRET efficiencies in all cases was above 50%. The photophysical parameters (triplet state and fluorescence quantum yields and lifetimes) were also determined for the conjugates. There was a decrease in the fluorescence lifetimes of ClGaPc(COOH)8 in the presence of all the QDs, due to the heavy atom effect. The triplet quantum yields increased in the conjugates. The lifetimes also became longer for the conjugates compared to Pc alone. Copyright © 2015 Elsevier B.V. All rights reserved.

Near-unity quantum yields from chloride treated CdTe colloidal quantum dots

DOE PAGES

Page, Robert C.; Espinobarro-Velazquez, Daniel; Leontiadou, Marina A.; ...

2014-10-27

Colloidal quantum dots (CQDs) are promising materials for novel light sources and solar energy conversion. However, trap states associated with the CQD surface can produce non-radiative charge recombination that significantly reduces device performance. Here a facile post-synthetic treatment of CdTe CQDs is demonstrated that uses chloride ions to achieve near-complete suppression of surface trapping, resulting in an increase of photoluminescence (PL) quantum yield (QY) from ca. 5% to up to 97.2 ± 2.5%. The effect of the treatment is characterised by absorption and PL spectroscopy, PL decay, scanning transmission electron microscopy, X-ray diffraction and X-ray photoelectron spectroscopy. We find thismore » process also dramatically improves the air-stability of the CQDs: before treatment the PL is largely quenched after 1 hour of air-exposure, whilst the treated samples showed a PL QY of nearly 50% after more than 12 hours.« less

Masked red-emitting carbopyronine dyes with photosensitive 2-diazo-1-indanone caging group.

PubMed

Kolmakov, Kirill; Wurm, Christian; Sednev, Maksim V; Bossi, Mariano L; Belov, Vladimir N; Hell, Stefan W

2012-03-01

Caged near-IR emitting fluorescent dyes are in high demand in optical microscopy but up to now were unavailable. We discovered that the combination of a carbopyronine dye core and a photosensitive 2-diazo-1-indanone residue leads to masked near-IR emitting fluorescent dyes. Illumination of these caged dyes with either UV or visible light (λ < 420 nm) efficiently generates fluorescent compounds with absorption and emission at 635 nm and 660 nm, respectively. A high-yielding synthetic route with attractive possibilities for further dye design is described in detail. Good photostability, high contrast, and a large fluorescence quantum yield after uncaging are the most important features of the new compounds for non-invasive imaging in high-resolution optical microscopy. For use in immunolabelling the caged dyes were decorated with a (hydrophilic) linker and an (activated) carboxyl group.

Quantum walk on a chimera graph

NASA Astrophysics Data System (ADS)

Xu, Shu; Sun, Xiangxiang; Wu, Jizhou; Zhang, Wei-Wei; Arshed, Nigum; Sanders, Barry C.

2018-05-01

We analyse a continuous-time quantum walk on a chimera graph, which is a graph of choice for designing quantum annealers, and we discover beautiful quantum walk features such as localization that starkly distinguishes classical from quantum behaviour. Motivated by technological thrusts, we study continuous-time quantum walk on enhanced variants of the chimera graph and on diminished chimera graph with a random removal of vertices. We explain the quantum walk by constructing a generating set for a suitable subgroup of graph isomorphisms and corresponding symmetry operators that commute with the quantum walk Hamiltonian; the Hamiltonian and these symmetry operators provide a complete set of labels for the spectrum and the stationary states. Our quantum walk characterization of the chimera graph and its variants yields valuable insights into graphs used for designing quantum-annealers.

Final Progress Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Josef Michl

2011-10-31

In this project we have established guidelines for the design on organic chromophores suitable for producing high triplet yields via singlet fission. We have proven their utility by identifying a chromophore of a structural class that had never been examined for singlet fission before, 1,3-diphenylisobenzofuran, and demonstrating in two independent ways that a thin layer of this material produces a triplet yield of 200% within experimental error. We have also designed a second chromophore of a very different type, again of a structural class that had not been examined for singlet fission before, and found that in a thin layermore » it produces a 70% triplet yield. Finally, we have enhanced the theoretical understanding of the quantum mechanical nature of the singlet fission process.« less

A Facile Methodology for Engineering the Morphology of CsPbX3 Perovskite Nanocrystals under Ambient Condition

NASA Astrophysics Data System (ADS)

Seth, Sudipta; Samanta, Anunay

2016-11-01

A facile and highly reproducible room temperature, open atmosphere synthesis of cesium lead halide perovskite nanocrystals of six different morphologies is reported just by varying the solvent, ligand and reaction time. Sequential evolution of the quantum dots, nanoplates and nanobars in one medium and nanocubes, nanorods and nanowires in another medium is demonstrated. These perovskite nanoparticles are shown to be of excellent crystalline quality with high fluorescence quantum yield. A mechanism of the formation of nanoparticles of different shapes and sizes is proposed. Considering the key role of morphology in nanotechnology, this simple method of fabrication of a wide range of high quality nanocrystals of different shapes and sizes of all-inorganic lead halide perovskites, whose potential is already demonstrated in light emitting and photovoltaic applications, is likely to help widening the scope and utility of these materials in optoelectronic devices.

Improved scintillation detector performance via a method of enhanced layered coatings

DOE PAGES

Wakeford, Daniel Tyler; Tornga, Shawn Robert; Adams, Jillian Cathleen; ...

2016-11-16

Increasing demand for better detection performance with a simultaneous reduction in size, weight and power consumption has motivated the use of compact semiconductors as photo-converters for many gamma-ray and neutron scintillators. The spectral response of devices such as silicon avalanche photodiodes (APDs) is poorly matched to many common high-performance scintillators. We have developed a generalized analytical method that utilizes an optical reference database to match scintillator luminescence to the excitation spectrum of high quantum efficiency semiconductor detectors. This is accomplished by the fabrication and application of a series of high quantum yield, short fluorescence lifetime, wavelengthshifting coatings. Furthermore, we showmore » here a 22% increase in photoelectron collection and a 10% improvement in energy resolution when applying a layered coating to an APD-coupled, cerium-doped, yttrium oxyorthosilicate (YSO:Ce) scintillator. Wavelength-shifted radioluminescence emission and rise time analysis are also discussed.« less

Convenient determination of luminescence quantum yield using a combined electronic absorption and emission spectrometer

DOE Office of Scientific and Technical Information (OSTI.GOV)

Prakash, John; Mishra, Ashok Kumar

2016-01-15

It is possible to measure luminescence quantum yield in a facile way, by designing an optical spectrometer capable of obtaining electronic absorption as well as luminescence spectra, with a setup that uses the same light source and detector for both the spectral measurements. Employment of a single light source and single detector enables use of the same correction factor profile for spectral corrections. A suitable instrumental scaling factor is used for adjusting spectral losses.

Production of NO2 from Photolysis of Peroxyacetyl Nitrate

NASA Technical Reports Server (NTRS)

Mazely, Troy L.; Friedl, Randall R.; Sander, Stanley P.

1965-01-01

Peroxyacetyl nitrate (PAN) vapor was photolyzed at 248 nm, and the NO2 photoproduct was detected by laser-induced fluorescence. The quantum yield for the production of NO2 from PAN photolysis was determined by comparison to HNO3 photolysis data taken under identical experimental conditions. The average of data collected over a range of total pressures, precursor concentrations, and buffer gases was 0.83 +/- 0.09 for the NO2 quantum yield, where the statistical uncertainty is 2 standard deviations.

Wakimoto realization of drinfeld current for the elliptic quantum algebra U{sub q,p}( widehat(sl{sub 3}) )

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kojima, T., E-mail: kojima@math.cst.nihon-u.ac.j

2010-02-15

We study a free field realization of the elliptic quantum algebra U{sub q,p}( widehat(sl{sub 3}) ) for arbitrary level k. We give the free field realization of elliptic analog of Drinfeld current associated with U{sub q,p}( widehat(sl{sub 3}) ) for arbitrary level k. In the limit p {yields} 0, q {yields} 1 our realization reproduces Wakimoto realization for the affine Lie algebra ( widehat(sl{sub 3}) ) .

Spatial and temporal distribution of singlet oxygen in Lake Superior.

PubMed

Peterson, Britt M; McNally, Ann M; Cory, Rose M; Thoemke, John D; Cotner, James B; McNeill, Kristopher

2012-07-03

A multiyear field study was undertaken on Lake Superior to investigate singlet oxygen ((1)O(2)) photoproduction. Specifically, trends within the lake were examined, along with an assessment of whether correlations existed between chromophoric dissolved organic matter (CDOM) characteristics and (1)O(2) production rates and quantum yields. Quantum yield values were determined and used to estimate noontime surface (1)O(2) steady-state concentrations ([(1)O(2)](ss)). Samples were subdivided into three categories based on their absorbance properties (a300): riverine, river-impacted, or open lake sites. Using calculated surface [(1)O(2)](ss), photochemical half-lives under continuous summer sunlight were calculated for cimetidine, a pharmaceutical whose reaction with (1)O(2) has been established, to be on the order of hours, days, and a week for the riverine, river-impacted, and open lake waters, respectively. Of the CDOM properties investigated, it was found that dissolved organic carbon (DOC) and a300 were the best parameters for predicting production rates of [(1)O(2)](ss). For example, given the correlations found, one could predict [(1)O(2)](ss) within a factor of 4 using a300 alone. Changes in the quantum efficiency of (1)O(2) production upon dilution of river water samples with lake water samples demonstrated that the CDOM found in the open lake is not simply diluted riverine organic matter. The open lake pool was characterized by low absorption coefficient, low fluorescence, and low DOC, but more highly efficient (1)O(2) production and predominates the Lake Superior system spatially. This study establishes that parameters that reflect the quantity of CDOM (e.g., a300 and DOC) correlate with (1)O(2) production rates, while parameters that characterize the absorbance spectrum (e.g., spectral slope coefficient and E2:E3) correlate with (1)O(2) production quantum yields.

Near-infrared emission from mesoporous crystalline germanium

NASA Astrophysics Data System (ADS)

Boucherif, Abderraouf; Korinek, Andreas; Aimez, Vincent; Arès, Richard

2014-10-01

Mesoporous crystalline germanium was fabricated by bipolar electrochemical etching of Ge wafer in HF-based electrolyte. It yields uniform mesoporous germanium layers composed of high density of crystallites with an average size 5-7 nm. Subsequent extended chemical etching allows tuning of crystallites size while preserving the same chemical composition. This highly controllable nanostructure exhibits photoluminescence emission above the bulk Ge bandgap, in the near-infrared range (1095-1360nm) with strong evidence of quantum confinement within the crystallites.

A near-infrared fluorescent probe based on BODIPY derivative with high quantum yield for selective detection of exogenous and endogenous cysteine in biological samples.

PubMed

Li, Song-Jiao; Fu, Ya-Jun; Li, Chun-Yan; Li, Yong-Fei; Yi, Lan-Hua; Ou-Yang, Juan

2017-11-22

Cysteine (Cys) is involved in cellular growth and Cys deficiency is related with many diseases. So far, a number of fluorescent probes have been constructed for the detection of Cys successfully. However, the probes are difficult to discriminate Cys from Hcy and the emission wavelength of the probes is in ultraviolet or visible range. Herein, a NIR fluorescent probe named NIR-BODIPY-Ac is synthesized and used to detect Cys. The emission wavelength of the probe is at 708 nm that belongs to near-infrared (NIR) region by attaching indolium to BODIPY core, which is suitable for bioimaging in vivo. Moreover, the probe exhibits high fluorescence quantum yield (Φ = 0.51) after the addition of Cys and high sensitivity toward Cys with 81-fold fluorescence enhancement. The linear range of the probe for Cys covers from 0.2 to 30 μM with a detection limit of 0.05 μM. Furthermore, the probe shows high selectivity towards Cys owing to the fact that there is more fast reaction rate between the probe and Cys than that of Hcy. In particular, the NIR fluorescent probe is applied for the detection of exogenous and endogenous Cys in biological samples such as cell, tissue and mouse with satisfactory results. Copyright © 2017 Elsevier B.V. All rights reserved.

Hybrid Molecule-Nanocrystal Photon Upconversion Across the Visible and Near-Infrared

DTIC Science & Technology

2015-07-10

applications in solar energy, biological imaging , and data storage. In this Letter, CdSe and PbSe semiconductor nanocrystals are combined with molecular...Goldschmidt, J. C. Absolute Upconversion Quantum Yield of β-NaYF4 Doped with Er3+ and External Quantum Efficiency of Upconverter Solar Cell Devices...C. Peak External Photocurrent Quantum Efficiency Exceeding 100% via MEG in a Quantum Dot Solar Cell . Science 2011, 334, 1530−1533. (37) Choi, J.-H

Measurement of Quantum Yield, Quantum Requirement, and Energetic Efficiency of the O2-Evolving System of Photosynthesis by a Simple Dye Reaction

NASA Astrophysics Data System (ADS)

Ros Barcelò, A.; Zapata, J. M.

1996-11-01

Photosynthesis is the conversion of absorbed radiant energy from sunlight into various forms of chemical energy by the chloroplasts of higher green plants. The overall process of photosynthesis consists of the oxidation of water (with the release of O2 as a product) and the reduction of CO2 to form carbohydrates. In the test tube electrons produced by the photolytic cleavage of H2) may be deviated from their true acceptor by inserting a suitable dye in the electron chain; i.e.; 2,6-dichlorophenol indophenol (DCPIP) (E'o = + 0.217 V), which is blue in the oxidized quinone form and which becomes colorless when reduced to the phenolic form. This dye-electrom acceptor also has the advantage that it accepts electroms directly from the quinone (Qa) electron-acceptor of the photosystem II< the reaction center associated with the O2-evolving (or water-slplitting) system. Based in the bleaching of DCPIP by illuminated spinach leaf chloroplasts, a classroom laboratory protocol has been developed to determine the quantum yield (QY = micromol O2 s-1 / micromol photons s-1, the quantum requirement (1/QY) and the energetic efficiency (f = chemical energy stored / light energy supplied) of the O2-evolving system of photosynthesis. Although values for the quantum yield, the quantum requirement and the energetic efficiency calculated in the classroom laboratory differ widely from those expected theoretically, these calculations are useful for illustrating the transformation of light energy into chemical energy by the chloroplasts of green plants.

One-step instant synthesis of protein-conjugated quantum dots at room temperature.

PubMed

He, Xuewen; Gao, Li; Ma, Nan

2013-10-02

We present a new general facile strategy for the preparation of protein-functionalized QDs in a single step at ambient conditions. We demonstrated that highly luminescent red to near-infrared (NIR) protein-functionalized QDs could be synthesized at room temperature in one second through a one-pot reaction that proceeds in aqueous solution. Herein protein-functionalized QDs were successfully constructed for a variety of proteins with a wide range of molecular weights and isoelectric points. The as-prepared protein-conjugated QDs exhibited high quantum yield, high photostabiliy and colloidal stability, and high functionalization efficiency. Importantly, the proteins attached to the QDs maintain their biological activities and are capable of catalyzing reactions and biotargeting. In particular, the as-prepared transferrin-QDs could be used to label cancer cells with high specificity. Moreover, we demonstrated that this synthetic strategy could be extended to prepare QDs functionalized with folic acids and peptides, which were also successfully applied to cancer cell imaging.

Effects of solar radiation on the Patagonian macroalga Enteromorpha linza (L.) J. Agardh-Chlorophyceae.

PubMed

Häder, D P; Lebert, M; Helbling, E W

2001-09-01

The photosynthetic performance of Enteromorpha linza (L.) J. Agardh-Chlorophyceae was determined with a portable PAM instrument in situ and under seminatural radiation conditions in Patagonia, Argentina. Solar radiation was measured in parallel with a three-channel radiometer, ELDONET (Real Time Computer, Möhrendorf, Germany), in three wavelength ranges, UV-B (280-315 nm), UV-A (315-400 nm), and PAR (400-700 nm). The effective photosynthetic quantum yield decreased after 15-min exposure to solar radiation when the thalli were kept in a fixed position but recovered in the subsequent shade conditions within several hours. A 30-min exposure of free floating thalli, however, caused less photoinhibition. The photosynthetic quantum yield of E. linza was also followed over whole days under clear sky, partly cloudy and rainy conditions in a large reservoir of water (free floating thalli) and in situ (thalli growing in rock pools). Most of the observed effect was due to visible radiation; however, the UV wavelength range, and especially UV-B, caused a significant reduction of the photosynthetic quantum yield. Fluence rate response curves indicated that the species is a typical shade plant which showed non-photochemical quenching at intermediate and higher irradiances. This is a surprising result since these algae are found in the upper eulittoral where they are exposed to high irradiances. Obviously they utilize light only during periods of low irradiances (morning, evening, high tide) while they shut down the electron transport chain during intensive exposure. Fast induction and relaxation kinetics have been measured in these algae for the first time and indicated a rapid adaptation of the photosynthetic capacity to the changing light conditions as well as a fast decrease of PS II fluorescence upon exposure to solar radiation. There was a strong bleaching of chlorophyll due to exposure to solar radiation but less drastic bleaching of carotenoids.

`Quantum Mechanics' and `Scientific Explanation' An Explanatory Strategy Aiming at Providing `Understanding'

NASA Astrophysics Data System (ADS)

Hadzidaki, Pandora

2008-01-01

Empirical studies persistently indicate that the usual explanatory strategies used in quantum mechanics (QM) instruction fail, in general, to yield understanding. In this study, we propose an instructional intervention, which: (a) incorporates into its subject matter a critical comparison of QM scientific content with the fundamental epistemological and ontological commitments of the prominent philosophical theories of explanation, a weak form of which we meet in QM teaching; (b) illuminates the reasons of their failure in the quantum domain; and (c) implements an explanatory strategy highly inspired by the epistemological pathways through which, during the birth-process of QM, science has gradually reached understanding. This strategy, an inherent element of which is the meta-cognitive and meta-scientific thinking, aims at leading learners not only to an essential understanding of QM worldview, but to a deep insight into the ‘Nature of Science’ as well.

Absorption, autoionization, and predissociation in molecular hydrogen: High-resolution spectroscopy and multichannel quantum defect theory.

PubMed

Sommavilla, M; Merkt, F; Mezei, J Zs; Jungen, Ch

2016-02-28

Absorption and photoionization spectra of H2 have been recorded at a resolution of 0.09 and 0.04 cm(-1), respectively, between 125,600 cm(-1) and 126,000 cm(-1). The observed Rydberg states belong to series (n = 10 - 14) converging on the first vibrationally excited level of the X (2)Σ(g)(+) state of H2(+), and of lower members of series converging on higher vibrational levels. The observed resonances are characterized by the competition between autoionization, predissociation, and fluorescence. The unprecedented resolution of the present experimental data leads to a full characterization of the predissociation/autoionization profiles of many resonances that had not been resolved previously. Multichannel quantum defect theory is used to predict the line positions, widths, shapes, and intensities of the observed spectra and is found to yield quantitative agreement using previously determined quantum defect functions as the unique set of input parameters.

Quantum dots in imaging, drug delivery and sensor applications

PubMed Central

Matea, Cristian T; Mocan, Teodora; Tabaran, Flaviu; Pop, Teodora; Mosteanu, Ofelia; Puia, Cosmin; Iancu, Cornel; Mocan, Lucian

2017-01-01

Quantum dots (QDs), also known as nanoscale semiconductor crystals, are nanoparticles with unique optical and electronic properties such as bright and intensive fluorescence. Since most conventional organic label dyes do not offer the near-infrared (>650 nm) emission possibility, QDs, with their tunable optical properties, have gained a lot of interest. They possess characteristics such as good chemical and photo-stability, high quantum yield and size-tunable light emission. Different types of QDs can be excited with the same light wavelength, and their narrow emission bands can be detected simultaneously for multiple assays. There is an increasing interest in the development of nano-theranostics platforms for simultaneous sensing, imaging and therapy. QDs have great potential for such applications, with notable results already published in the fields of sensors, drug delivery and biomedical imaging. This review summarizes the latest developments available in literature regarding the use of QDs for medical applications. PMID:28814860

Quantum dots in imaging, drug delivery and sensor applications.

PubMed

Matea, Cristian T; Mocan, Teodora; Tabaran, Flaviu; Pop, Teodora; Mosteanu, Ofelia; Puia, Cosmin; Iancu, Cornel; Mocan, Lucian

2017-01-01

Quantum dots (QDs), also known as nanoscale semiconductor crystals, are nanoparticles with unique optical and electronic properties such as bright and intensive fluorescence. Since most conventional organic label dyes do not offer the near-infrared (>650 nm) emission possibility, QDs, with their tunable optical properties, have gained a lot of interest. They possess characteristics such as good chemical and photo-stability, high quantum yield and size-tunable light emission. Different types of QDs can be excited with the same light wavelength, and their narrow emission bands can be detected simultaneously for multiple assays. There is an increasing interest in the development of nano-theranostics platforms for simultaneous sensing, imaging and therapy. QDs have great potential for such applications, with notable results already published in the fields of sensors, drug delivery and biomedical imaging. This review summarizes the latest developments available in literature regarding the use of QDs for medical applications.

High-order noise filtering in nontrivial quantum logic gates.

PubMed

Green, Todd; Uys, Hermann; Biercuk, Michael J

2012-07-13

Treating the effects of a time-dependent classical dephasing environment during quantum logic operations poses a theoretical challenge, as the application of noncommuting control operations gives rise to both dephasing and depolarization errors that must be accounted for in order to understand total average error rates. We develop a treatment based on effective Hamiltonian theory that allows us to efficiently model the effect of classical noise on nontrivial single-bit quantum logic operations composed of arbitrary control sequences. We present a general method to calculate the ensemble-averaged entanglement fidelity to arbitrary order in terms of noise filter functions, and provide explicit expressions to fourth order in the noise strength. In the weak noise limit we derive explicit filter functions for a broad class of piecewise-constant control sequences, and use them to study the performance of dynamically corrected gates, yielding good agreement with brute-force numerics.

A Study of Complex Deep Learning Networks on High Performance, Neuromorphic, and Quantum Computers

DOE Office of Scientific and Technical Information (OSTI.GOV)

Potok, Thomas E; Schuman, Catherine D; Young, Steven R

Current Deep Learning models use highly optimized convolutional neural networks (CNN) trained on large graphical processing units (GPU)-based computers with a fairly simple layered network topology, i.e., highly connected layers, without intra-layer connections. Complex topologies have been proposed, but are intractable to train on current systems. Building the topologies of the deep learning network requires hand tuning, and implementing the network in hardware is expensive in both cost and power. In this paper, we evaluate deep learning models using three different computing architectures to address these problems: quantum computing to train complex topologies, high performance computing (HPC) to automatically determinemore » network topology, and neuromorphic computing for a low-power hardware implementation. Due to input size limitations of current quantum computers we use the MNIST dataset for our evaluation. The results show the possibility of using the three architectures in tandem to explore complex deep learning networks that are untrainable using a von Neumann architecture. We show that a quantum computer can find high quality values of intra-layer connections and weights, while yielding a tractable time result as the complexity of the network increases; a high performance computer can find optimal layer-based topologies; and a neuromorphic computer can represent the complex topology and weights derived from the other architectures in low power memristive hardware. This represents a new capability that is not feasible with current von Neumann architecture. It potentially enables the ability to solve very complicated problems unsolvable with current computing technologies.« less

Homeotropic alignment and Förster resonance energy transfer: The way to a brighter luminescent solar concentrator

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tummeltshammer, Clemens; Taylor, Alaric; Kenyon, Anthony J.

2014-11-07

We investigate homeotropically aligned fluorophores and Förster resonance energy transfer (FRET) for luminescent solar concentrators using Monte-Carlo ray tracing. The homeotropic alignment strongly improves the trapping efficiency, while FRET circumvents the low absorption at homeotropic alignment by separating the absorption and emission processes. We predict that this design doped with two organic dye molecules can yield a 82.9% optical efficiency improvement compared to a single, arbitrarily oriented dye molecule. We also show that quantum dots are prime candidates for absorption/donor fluorophores due to their wide absorption band. The potentially strong re-absorption and low quantum yield of quantum dots is notmore » a hindrance for this design.« less

Water catalysis and anticatalysis in photochemical reactions: observation of a delayed threshold effect in the reaction quantum yield.

PubMed

Kramer, Zeb C; Takahashi, Kaito; Skodje, Rex T

2010-11-03

The possible catalysis of photochemical reactions by water molecules is considered. Using theoretical simulations, we investigate the HF-elimination reaction of fluoromethanol in small water clusters initiated by the overtone excitation of the hydroxyl group. The reaction occurs in competition with the process of water evaporation that dissipates the excitation and quenches the reaction. Although the transition state barrier is stabilized by over 20 kcal/mol through hydrogen bonding with water, the quantum yield versus energy shows a pronounced delayed threshold that effectively eliminates the catalytic effect. It is concluded that the quantum chemistry calculations of barrier lowering are not sufficient to infer water catalysis in some photochemical reactions, which instead require dynamical modeling.

Templated self-assembly of quantum dots from aqueous solution using protein scaffolds

NASA Astrophysics Data System (ADS)

Szuchmacher Blum, Amy; Soto, Carissa M.; Wilson, Charmaine D.; Whitley, Jessica L.; Moore, Martin H.; Sapsford, Kim E.; Lin, Tianwei; Chatterji, Anju; Johnson, John E.; Ratna, Banahalli R.

2006-10-01

Short, histidine-containing peptides can be conjugated to lysine-containing protein scaffolds to controllably attach quantum dots (QDs) to the scaffold, allowing for generic attachment of quantum dots to any protein without the use of specially engineered domains. This technique was used to bind quantum dots from aqueous solution to both chicken IgG and cowpea mosaic virus (CPMV), a 30 nm viral particle. These quantum dot protein assemblies were studied in detail. The IgG QD complexes were shown to retain binding specificity to their antigen after modification. The CPMV QD complexes have a local concentration of quantum dots greater than 3000 nmol ml-1, and show a 15% increase in fluorescence quantum yield over free quantum dots in solution.

Quantum dots and nanoparticles for photodynamic and radiation therapies of cancer

PubMed Central

Juzenas, Petras; Chen, Wei; Sun, Ya-Ping; Coelho, Manuel Alvaro Neto; Generalov, Roman; Generalova, Natalia; Christensen, Ingeborg Lie

2009-01-01

Semiconductor quantum dots and nanoparticles composed of metals, lipids or polymers have emerged with promising applications for early detection and therapy of cancer. Quantum dots with unique optical properties are commonly composed of cadmium contained semiconductors. Cadmium is potentially hazardous, and toxicity of such quantum dots to living cells, and humans, is not yet systematically investigated. Therefore, search for less toxic materials with similar targeting and optical properties is of further interest. Whereas, the investigation of luminescence nanoparticles as light sources for cancer therapy is very interesting. Despite advances in neurosurgery and radiotherapy the prognosis for patients with malignant gliomas has changed little for the last decades. Cancer treatment requires high accuracy in delivering ionizing radiation to reduce toxicity to surrounding tissues. Recently some research has been focused in developing photosensitizing quantum dots for production of radicals upon absorption of visible light. In spite of the fact that visible light is safe, this approach is suitable to treat only superficial tumours. Ionizing radiation (X-rays and gamma rays) penetrate much deeper thus offering a big advantage in treating patients with tumours in internal organs. Such concept of using quantum dots and nanoparticles to yield electrons and radicals in photodynamic and radiation therapies as well their combination is reviewed in this article. PMID:18840487

Bifunctional Diaminoterephthalate Fluorescent Dye as Probe for Cross-Linking Proteins.

PubMed

Wallisch, Melanie; Sulmann, Stefan; Koch, Karl-Wilhelm; Christoffers, Jens

2017-05-11

Diaminoterephthalates are fluorescent dyes and define scaffolds, which can be orthogonally functionalized at their two carboxylate residues with functional residues bearing task specific reactive groups. The synthesis of monofunctionalized dyes with thiol groups for surface binding, an azide for click chemistry, and a biotinoylated congener for streptavidin binding is reported. Two bifunctionalized dyes were prepared: One with an azide for click chemistry and a biotin for streptavidin binding, the other with a maleimide for reaction with thiol and a cyclooctyne moiety for ligation with copper-free click chemistry. In general, the compounds are red to orange, fluorescent materials with an absorption at about 450 nm and an emission at 560 nm with quantum yields between 2-41 %. Of particular interest is the maleimide-functionalized compound, which shows low fluorescence quantum yield (2 %) by itself. After addition of a thiol, the fluorescence is "turned on"; quantum yield 41 %. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Filip, Radim; Marek, Petr; Fiurasek, Jaromir

We analyze a reversibility of optimal Gaussian 1{yields}2 quantum cloning of a coherent state using only local operations on the clones and classical communication between them and propose a feasible experimental test of this feature. Performing Bell-type homodyne measurement on one clone and anticlone, an arbitrary unknown input state (not only a coherent state) can be restored in the other clone by applying appropriate local unitary displacement operation. We generalize this concept to a partial reversal of the cloning using only local operations and classical communication (LOCC) and we show that this procedure converts the symmetric cloner to an asymmetricmore » cloner. Further, we discuss a distributed LOCC reversal in optimal 1{yields}M Gaussian cloning of coherent states which transforms it to optimal 1{yields}M{sup '} cloning for M{sup '}

Calculated quantum yield of photosynthesis of phytoplankton in the Marine Light-Mixed Layers (59 deg N, 21 deg W)

NASA Technical Reports Server (NTRS)

Carder, K. L.; Lee, Z. P.; Marra, John; Steward, R. G.; Perry, M. J.

1995-01-01

The quantum yield of photosynthesis (mol C/mol photons) was calculated at six depths for the waters of the Marine Light-Mixed Layer (MLML) cruise of May 1991. As there were photosynthetically available radiation (PAR) but no spectral irradiance measurements for the primary production incubations, three ways are presented here for the calculation of the absorbed photons (AP) by phytoplankton for the purpose of calculating phi. The first is based on a simple, nonspectral model; the second is based on a nonlinear regression using measured PAR values with depth; and the third is derived through remote sensing measurements. We show that the results of phi calculated using the nonlinear regreesion method and those using remote sensing are in good agreement with each other, and are consistent with the reported values of other studies. In deep waters, however, the simple nonspectral model may cause quantum yield values much higher than theoretically possible.

Photosensitized electron transport across lipid vesicle walls: Enhancement of quantum yield by ionophores and transmembrane potentials

PubMed Central

Laane, Colja; Ford, William E.; Otvos, John W.; Calvin, Melvin

1981-01-01

The photosensitized reduction of heptylviologen in the bulk aqueous phase of phosphatidylcholine vesicles containing EDTA inside and a membrane-bound tris(2,2′-bipyridine)ruthenium(2+) derivative is enhanced by a factor of 6.5 by the addition of valinomycin in the presence of K+. A 3-fold stimulation by gramicidin and carbonyl cyanide m-chlorophenylhydrazone is observed. The results suggest that, under these conditions, the rate of photoinduced electron transfer across vesicle walls in the absence of ion carriers is limited by cotransport of cations. The rate of electron transfer across vesicle walls could be influenced further by generating transmembrane potentials with K+ gradients in the presence of valinomycin. When vesicles are made with transmembrane potentials, interior more negative, the quantum yield of heptylviologen reduction is doubled, and, conversely, when vesicles are made with transmembrane potentials, interior more positive, the quantum yield is decreased and approaches the value found in the absence of valinomycin. PMID:16593002

Determination of apparent quantum yield spectra of DMS photo-degradation in an in situ iron-induced Northeast Pacific Ocean bloom

NASA Astrophysics Data System (ADS)

Bouillon, René-Christian; Miller, William L.

2004-03-01

The wavelength dependence of the photochemical removal efficiency for DMS was studied for samples from an iron-induced bloom in the Northeastern Pacific Ocean. In July 2002, a 64 km2 patch of ocean was iron-fertilized near Ocean Station Papa (50°12'N 144°45'W). Only small changes in pseudo-first-order apparent quantum yield (AQY*DMS(λ)) were observed outside the iron-patch. However, inside the patch, AQY*DMS(λ) decreased considerably over the two weeks following the initial iron injection. A positive strong correlation was found between pseudo-first-order apparent quantum yield determined at 330 nm (AQY*DMS(330 nm)) and NO3- concentrations. We propose that NO3--photolysis has a substantial influence on DMS photo-degradation rates in oceanic waters. This finding demonstrates that in addition to control DMS production, marine phytoplankton could indirectly influence the DMS photochemical loss rate via its control on NO3- distribution.

[Optical and spectral parameters in Ce3+ -doped gadolinium gallium aluminum garnet glass-ceramics].

PubMed

Gong, Hua; Zhao, Xin; Yu, Xiao-bo; Setsuhisa, Tanabe; Lin, Hai

2010-01-01

The crystalline phases of Ce3+ -doped gadolinium gallium aluminum garnet (GGAG) glass-ceramics were investigated by X-ray diffraction, and the fluorescence spectra were recorded under the pumping of blue light-emitting diode (LED) using an integrating sphere of 10-inch in diameter, which connected to a CCD detector. The spectral power distribution of the glass-ceramics was obtained from the measured spectra first, and then the quantum yield was derived based on the photon distribution. The quantum yield of Ce3+ emission in GGAG glass-ceramics is 29.2%, meanwhile, the color coordinates and the correlated color temperature (CCT) of combined white light were proved to be x = 0.319, y = 0.349 and 6086 K, respectively. Although the quantum yield is a little smaller than the value in Ce3+ -doped YAG glass-ceramics, the CCT of the combined white light is much smaller than that in the latter. The optical behavior of GGAG glass-ceramics provides new vision for developing comfortable LED lighting devices.

Electron-Deficient Near-Infrared Pt(II) and Pd(II) Benzoporphyrins with Dual Phosphorescence and Unusually Efficient Thermally Activated Delayed Fluorescence: First Demonstration of Simultaneous Oxygen and Temperature Sensing with a Single Emitter.

PubMed

Zach, Peter W; Freunberger, Stefan A; Klimant, Ingo; Borisov, Sergey M

2017-11-01

We report a family of Pt and Pd benzoporphyrin dyes with versatile photophysical properties and easy access from cheap and abundant chemicals. Attaching 4 or 8 alkylsulfone groups onto a meso-tetraphenyltetrabenzoporphyrin (TPTBP) macrocylcle renders the dyes highly soluble in organic solvents, photostable, and electron-deficient with the redox potential raised up to 0.65 V versus the parent porphyrin. The new dyes intensively absorb in the blue (Soret band, 440-480 nm) and in the red (Q-band, 620-650 nm) parts of the electromagnetic spectrum and show bright phosphorescence at room-temperature in the NIR with quantum yields up to 30% in solution. The small singlet-triplet energy gap yields unusually efficient thermally activated delayed fluorescence (TADF) at elevated temperatures in solution and in polymeric matrices with quantum yields as high as 27% at 120 °C, which is remarkable for benzoporphyrins. Apart from oxygen sensing, these properties enable unprecedented simultaneous, self-referenced oxygen and temperature sensing with a single indicator dye: whereas oxygen can be determined either via the decay time of phosphorescence or TADF, the temperature is accessed via the ratio of the two emissions. Moreover, the dyes are efficient sensitizers for triplet-triplet annihilation (TTA)-based upconversion making possible longer sensitization wavelength than the conventional benzoporphyrin complexes. The Pt-octa-sulfone dye also features interesting semireversible transformation in basic media, which generates new NIR absorbing species.

Fractional quantum Hall effect at Landau level filling ν = 4/11

DOE PAGES

Pan, W.; Baldwin, K. W.; West, K. W.; ...

2015-01-09

In this study, we report low temperature electronic transport results on the fractional quantum Hall effect of composite fermions at Landau level filling ν = 4/11 in a very high mobility and low density sample. Measurements were carried out at temperatures down to 15mK, where an activated magnetoresistance R xx and a quantized Hall resistance R xy, within 1% of the expected value of h/(4/11)e 2, were observed. The temperature dependence of the R xx minimum at 4/11 yields an activation energy gap of ~ 7 mK. Developing Hall plateaus were also observed at the neighboring states at ν =more » 3/8 and 5/13.« less

Detecting proteins in highly autofluorescent cells using quantum dot antibody conjugates.

PubMed

Orcutt, Karen M; Ren, Shanshan; Gundersen, Kjell

2009-01-01

We have applied quantum dot (Qdot) antibody conjugates as a biomolecular probe for cellular proteins important in biogeochemical cycling in the sea. Conventional immunological methods have been hampered by the strong autofluorescence found in cyanobacteria cells. Qdot conjugates provide an ideal alternative for studies that require long-term imaging of cells such as detection of low abundance cellular antigens by fluorescence microscopy. The advantage of Qdot labeled probes over conventional immunological methods is the photostability of the probe. Phycoerythrin bleaches in cyanobacterial cells under prolonged UV or blue light excitation, which means that the semiconducting nanocrystal probe, the Qdot, can yield a strong fluorescent signal without interference from cellular pigments.

Near-optimal quantum circuit for Grover's unstructured search using a transverse field

NASA Astrophysics Data System (ADS)

Jiang, Zhang; Rieffel, Eleanor G.; Wang, Zhihui

2017-06-01

Inspired by a class of algorithms proposed by Farhi et al. (arXiv:1411.4028), namely, the quantum approximate optimization algorithm (QAOA), we present a circuit-based quantum algorithm to search for a needle in a haystack, obtaining the same quadratic speedup achieved by Grover's original algorithm. In our algorithm, the problem Hamiltonian (oracle) and a transverse field are applied alternately to the system in a periodic manner. We introduce a technique, based on spin-coherent states, to analyze the composite unitary in a single period. This composite unitary drives a closed transition between two states that have high degrees of overlap with the initial state and the target state, respectively. The transition rate in our algorithm is of order Θ (1 /√{N }) , and the overlaps are of order Θ (1 ) , yielding a nearly optimal query complexity of T ≃√{N }(π /2 √{2 }) . Our algorithm is a QAOA circuit that demonstrates a quantum advantage with a large number of iterations that is not derived from Trotterization of an adiabatic quantum optimization (AQO) algorithm. It also suggests that the analysis required to understand QAOA circuits involves a very different process from estimating the energy gap of a Hamiltonian in AQO.

White light emitting diode based on InGaN chip with core/shell quantum dots

NASA Astrophysics Data System (ADS)

Shen, Changyu; Hong, Yan; Ma, Jiandong; Ming, Jiangzhou

2009-08-01

Quantum dots have many applications in optoelectronic device such as LEDs for its many superior properties resulting from the three-dimensional confinement effect of its carrier. In this paper, single chip white light-emitting diodes (WLEDs) were fabricated by combining blue InGaN chip with luminescent colloidal quantum dots (QDs). Two kinds of QDs of core/shell CdSe /ZnS and core/shell/shell CdSe /ZnS /CdS nanocrystals were synthesized by thermal deposition using cadmium oxide and selenium as precursors in a hot lauric acid and hexadecylamine trioctylphosphine oxide hybrid. This two kinds of QDs exhibited high photoluminescence efficiency with a quantum yield more than 41%, and size-tunable emission wavelengths from 500 to 620 nm. The QDs LED mainly consists of flip luminescent InGaN chip, glass ceramic protective coating, glisten cup, QDs using as the photoluminescence material, pyroceram, gold line, electric layer, dielectric layer, silicon gel and bottom layer for welding. The WLEDs had the CIE coordinates of (0.319, 0.32). The InGaN chip white-light-emitting diodes with quantum dots as the emitting layer are potentially useful in illumination and display applications.

Hydroxyl Radical Fluorescence and Quantum Yield Following Lyman-α Photoexcitation of Water Vapor in a Room Temperature Cell and Cooled in a Supersonic Expansion.

PubMed

Young, Justin W; Booth, Ryan S; Vogelhuber, Kristen M; Stearns, Jaime A; Annesley, Christopher J

2018-06-28

Photoexcitation of water by Lyman-α (121.6 nm) induces a dissociation reaction that produces OH(A 2 Σ + ) + H. Despite this reaction being part of numerous studies, a combined understanding of the product and fluorescence yields is still lacking. Here, the rotational and vibrational distributions of OH(A) are determined from dispersed fluorescence following photoexcitation of both room-temperature and jet-cooled water vapor, for the first time in the same experiment. This work compares new data of state-resolved fluorescence with literature molecular branching ratios and brings previous studies into agreement through careful consideration of OH(A) fluorescent and predissociation lifetimes and confirms a fluorescent quantum yield of 8%. Comparison of the room-temperature and jet-cooled OH(A) populations indicate the temperature of H 2 O prior to excitation has subtle effects on the OH(A) population distribution, such as altering the rotational distribution in the ν' = 0 population and affecting the population in the ν' = 1 state. These results indicate jet-cooled water vapor may have a 1% higher fluorescence quantum yield compared to room-temperature water vapor.

Relative quantum yield of I-asterisk(2P1/2) in the tunable laser UV photodissociation of i-C3F7I and n-C3F7I - Effect of temperature and exciplex emission

NASA Technical Reports Server (NTRS)

Smedley, J. E.; Leone, S. R.

1983-01-01

Wavelength-specific relative quantum yields of metastable I from pulsed laser photodissociation of i-C3F7I and n-C3F7I in the range 265-336 nm are determined by measuring the time-resolved infrared emission from the atomic I(P-2(1/2) P-2(3/2) transition. It is shown that although this yield appears to be unity from 265 to 298 nm, it decreases dramatically at longer wavelengths. Values are also reported for the enhancement of emission from metastable I due to exciplex formation at several temperatures. The exciplex formation emission increases linearly with parent gas pressure, but decreases with increasing temperature. Absorption spectra of i- and n-C3F7I between 303 and 497 K are presented, and the effect of temperature on the quantum yields at selected wavelengths greater than 300 nm, where increasing the temperature enhances the absorption considerably, are given. The results are discussed in regard to the development of solar-pumped iodine lasers.

Experimental implementation of local adiabatic evolution algorithms by an NMR quantum information processor.

PubMed

Mitra, Avik; Ghosh, Arindam; Das, Ranabir; Patel, Apoorva; Kumar, Anil

2005-12-01

Quantum adiabatic algorithm is a method of solving computational problems by evolving the ground state of a slowly varying Hamiltonian. The technique uses evolution of the ground state of a slowly varying Hamiltonian to reach the required output state. In some cases, such as the adiabatic versions of Grover's search algorithm and Deutsch-Jozsa algorithm, applying the global adiabatic evolution yields a complexity similar to their classical algorithms. However, using the local adiabatic evolution, the algorithms given by J. Roland and N.J. Cerf for Grover's search [J. Roland, N.J. Cerf, Quantum search by local adiabatic evolution, Phys. Rev. A 65 (2002) 042308] and by Saurya Das, Randy Kobes, and Gabor Kunstatter for the Deutsch-Jozsa algorithm [S. Das, R. Kobes, G. Kunstatter, Adiabatic quantum computation and Deutsh's algorithm, Phys. Rev. A 65 (2002) 062301], yield a complexity of order N (where N=2(n) and n is the number of qubits). In this paper, we report the experimental implementation of these local adiabatic evolution algorithms on a 2-qubit quantum information processor, by Nuclear Magnetic Resonance.

Quantum dots as optical labels for ultrasensitive detection of polyphenols.

PubMed

Akshath, Uchangi Satyaprasad; Shubha, Likitha R; Bhatt, Praveena; Thakur, Munna Singh

2014-07-15

Considering the fact that polyphenols have versatile activity in-vivo, its detection and quantification is very much important for a healthy diet. Laccase enzyme can convert polyphenols to yield mono/polyquinones which can quench Quantum dots fluorescence. This phenomenon of charge transfer from quinones to QDs was exploited as optical labels to detect polyphenols. CdTe QD may undergo dipolar interaction with quinones as a result of broad spectral absorption due to multiple excitonic states resulting from quantum confinement effects. Thus, "turn-off" fluorescence method was applied for ultrasensitive detection of polyphenols by using laccase. We observed proportionate quenching of QDs fluorescence with respect to polyphenol concentration in the range of 100 µg to 1 ng/mL. Also, quenching of the photoluminescence was highly efficient and stable and could detect individual and total polyphenols with high sensitivity (LOD-1 ng/mL). Moreover, proposed method was highly efficient than any other reported methods in terms of sensitivity, specificity and selectivity. Therefore, a novel optical sensor was developed for the detection of polyphenols at a sensitive level based on the charge transfer mechanism. Copyright © 2014 Elsevier B.V. All rights reserved.

Nanostructured organosilicon luminophores and their application in highly efficient plastic scintillators

NASA Astrophysics Data System (ADS)

Ponomarenko, Sergei A.; Surin, Nikolay M.; Borshchev, Oleg V.; Luponosov, Yuriy N.; Akimov, Dmitry Y.; Alexandrov, Ivan S.; Burenkov, Alexander A.; Kovalenko, Alexey G.; Stekhanov, Viktor N.; Kleymyuk, Elena A.; Gritsenko, Oleg T.; Cherkaev, Georgiy V.; Kechek'yan, Alexander S.; Serenko, Olga A.; Muzafarov, Aziz M.

2014-10-01

Organic luminophores are widely used in various optoelectronic devices, which serve for photonics, nuclear and particle physics, quantum electronics, medical diagnostics and many other fields of science and technology. Improving their spectral-luminescent characteristics for particular technical requirements of the devices is a challenging task. Here we show a new concept to universal solution of this problem by creation of nanostructured organosilicon luminophores (NOLs), which are a particular type of dendritic molecular antennas. They combine the best properties of organic luminophores and inorganic quantum dots: high absorption cross-section, excellent photoluminescence quantum yield, fast luminescence decay time and good processability. A NOL consists of two types of covalently bonded via silicon atoms organic luminophores with efficient Förster energy transfer between them. Using NOLs in plastic scintillators, widely utilized for radiation detection and in elementary particles discoveries, led to a breakthrough in their efficiency, which combines both high light output and fast decay time. Moreover, for the first time plastic scintillators, which emit light in the desired wavelength region ranging from 370 to 700 nm, have been created. We anticipate further applications of NOLs as working elements of pulsed dye lasers in photonics, optoelectronics and as fluorescent labels in biology and medical diagnostics.

Tapping the potential of trioctylphosphine (TOP) in the realization of highly luminescent blue-emitting colloidal indium phosphide (InP) quantum dots

NASA Astrophysics Data System (ADS)

Singh, Akanksha; Chawla, Parul; Jain, Shefali; Sharma, Shailesh Narain

2017-06-01

In this work, extremely small blue emitting colloidal InP-based quantum dots (size 2-5 nm) have been synthesized using trioctylphosphine (TOP) as a source of phosphorus. The method reported here is unconventional, quite rapid ( 90 min), more viable, less expensive and relatively greener as compared to other conventional methods that employ tristrimethylsilyylphosphine(P(SiMe3)3) which is scarce, expensive, flammable, highly toxic and even banned in a few countries. Highly luminescent InP QDs having bluish-green emission (λ 490 nm) can be synthesized using this method without resorting to any post-synthesis etching to tune the emission to the blue region. Besides being the source of phosphorus and the particle size regulating agent, the efficacy of TOP is further realized during synthesis via its reduction of indium salt, which aids in the formation of indium metal and then subsequently in the development of InP QDs. The PL intensity of as-synthesized InP QDs is further enhanced by growing a shell of wide band gap material, i.e. ZnS resulting in a concurrent increment in quantum yield from 25% to 38% respectively.

Al{sub x}Ga{sub 1-x}N-based back-illuminated solar-blind photodetectors with external quantum efficiency of 89%

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cicek, E.; McClintock, R.; Cho, C. Y.

2013-11-04

We report on high performance Al{sub x}Ga{sub 1−x}N-based solar-blind ultraviolet photodetector (PD) array grown on sapphire substrate. First, high quality, crack-free AlN template layer is grown via metalorganic chemical vapor deposition. Then, we systematically optimized the device design and material doping through the growth and processing of multiple devices. After optimization, uniform and solar-blind operation is observed throughout the array; at the peak detection wavelength of 275 nm, 729 μm{sup 2} area PD showed unbiased peak external quantum efficiency and responsivity of ∼80% and ∼176 mA/W, respectively, increasing to 89% under 5 V of reverse bias. Taking the reflection loses into consideration,more » the internal quantum efficiency of these optimized PD can be estimated to be as high as ∼98%. The visible rejection ratio measured to be more than six orders of magnitude. Electrical measurements yielded a low-dark current density: <2 × 10{sup −9} A/cm{sup 2}, at 10 V of reverse bias.« less

Observable measure of quantum coherence in finite dimensional systems.

PubMed

Girolami, Davide

2014-10-24

Quantum coherence is the key resource for quantum technology, with applications in quantum optics, information processing, metrology, and cryptography. Yet, there is no universally efficient method for quantifying coherence either in theoretical or in experimental practice. I introduce a framework for measuring quantum coherence in finite dimensional systems. I define a theoretical measure which satisfies the reliability criteria established in the context of quantum resource theories. Then, I present an experimental scheme implementable with current technology which evaluates the quantum coherence of an unknown state of a d-dimensional system by performing two programmable measurements on an ancillary qubit, in place of the O(d2) direct measurements required by full state reconstruction. The result yields a benchmark for monitoring quantum effects in complex systems, e.g., certifying nonclassicality in quantum protocols and probing the quantum behavior of biological complexes.

Primary photophysical properties of moxifloxacin--a fluoroquinolone antibiotic.

PubMed

Lorenzo, Fernando; Navaratnam, Suppiah; Edge, Ruth; Allen, Norman S

2008-01-01

The photophysical properties of the fluoroquinolone antibiotic moxifloxacin (MOX) were investigated in aqueous media. MOX in water, at pH 7.4, shows two intense absorption bands at 287 and 338 nm (epsilon = 44,000 and 17,000 dm(3) mol(-1) cm(-1), respectively). The absorption and emission properties of MOX are pH-dependent, pK(a) values for the protonation equilibria of both the ground (6.1 and 9.6) and excited singlet states (6.8 and 9.1) of MOX were determined spectroscopically. MOX fluoresces weakly, the quantum yield for fluorescence emission being maximum (0.07) at pH 8. Phosphorescence from the excited triplet state in frozen ethanol solution has a quantum yield of 0.046. Laser flash photolysis and pulse radiolysis studies have been carried out to characterize the transient species of MOX in aqueous solution. On laser excitation, MOX undergoes monophotonic photoionization with a quantum yield of 0.14. This leads to the formation of a long-lived cation radical whose absorption is maximum at 470 nm (epsilon(470) = 3400 dm(3) mol(-1) cm(-1)). The photoionization process releases hydrated electron which rapidly reacts (k = 2.8 x 10(10) dm(3) mol(-1) s(-1)) with ground state MOX, yielding a long-lived anion radical with maximum absorption at 390 nm (epsilon(390) = 2400 dm(3) mol(-1) cm(-1)). The cation radical of MOX is able to oxidize protein components tryptophan and tyrosine. The bimolecular rate constants for these reactions are 2.3 x 10(8) dm(3) mol(-1) s(-1) and 1.3 x 10(8) dm(3) mol(-1) s(-1), respectively. Singlet oxygen sensitized by the MOX triplet state was also detected only in oxygen-saturated D(2)O solutions, with a quantum yield of 0.075.

Innovatively Continuous Mass Production Couette-taylor Flow: Pure Inorganic Green-Emitting Cs4PbBr6 Perovskite Microcrystal for display technology.

PubMed

Song, Young Hyun; Choi, Seung Hee; Park, Won Kyu; Yoo, Jin Sun; Kwon, Seok Bin; Kang, Bong Kyun; Park, Sang Ryul; Seo, Young Soo; Yang, Woo Seok; Yoon, Dae Ho

2018-01-31

We report for the first time the mass production of Cs 4 PbBr 6 perovskite microcrystal with a Couette-Taylor flow reactor in order to enhance the efficiency of the synthesis reaction. We obtained a pure Cs 4 PbBr 6 perovskite solid within 3 hrs that then realized a high photoluminescence quantum yield (PLQY) of 46%. Furthermore, the Cs 4 PbBr 6 perovskite microcrystal is applied with red emitting K 2 SiF 6 phosphor on a blue-emitting InGaN chip, achieving a high-performance luminescence characteristics of 9.79 lm/W, external quantum efficiency (EQE) of 2.9%, and correlated color temperature (CCT) of 2976 K; therefore, this perovskite is expected to be a promising candidate material for applications in optoelectronic devices.

Benchmarks and Reliable DFT Results for Spin Gaps of Small Ligand Fe(II) Complexes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Song, Suhwan; Kim, Min-Cheol; Sim, Eunji

2017-05-01

All-electron fixed-node diffusion Monte Carlo provides benchmark spin gaps for four Fe(II) octahedral complexes. Standard quantum chemical methods (semilocal DFT and CCSD(T)) fail badly for the energy difference between their high- and low-spin states. Density-corrected DFT is both significantly more accurate and reliable and yields a consistent prediction for the Fe-Porphyrin complex

Development of a high-voltage waveguide photodetector comprised of Schottky diodes and based on the Ge-Si structure with Ge quantum dots for portable thermophotovoltaic converters

NASA Astrophysics Data System (ADS)

Pakhanov, N. A.; Pchelyakov, O. P.; Yakimov, A. I.; Voitsekhovskii, A. V.

2017-03-01

This paper demontstrates the possibility of developing a high-voltage waveguide photodetector comprised of Schottky diodes and based on a Au/Ge — Si structure with Ge quantum dots pseudomorphic to a silicon matrix, which ensures an increase in the external quantum yield and open-circuit voltage. It is shown on this photodetector that there is a great increase and broadening in sensitivity up to λ = 2.1 μm, which coincides with the main radiation range of a black (gray) body at the emitter temperatures from 1200 to 1700 °C, practically used in thermophotovoltaic converters. This state of the ensemble of Ge quantum dots by means of molecular beam epitaxy can be obtained only under the condition of low growth temperature (250-300 °C). It is established that, below the Si absorption edge, photoresponse on the photodetectors under consideration is determined by two main mechanisms: absorption on the ensemble of Ge quantum dots and Fowler emission. It is shown by the analysis of the Raman scattering spectra on the optical photons of Ge-Si structures that the quantum efficiency of photodetectors based on them in the first case is due to the degree of nonuniform stress relaxation in the array of Ge quantum dots. The photoresponse directly associated with the Ge quantum dots is manifested on Schottky diodes with a superthin intermediate oxide layer SiO2, which eliminates the second mechanism. In further development, the proposed photodetector architecture with pseudomorphic Ge quantum dots can be used both for portable thermophotovoltaic converters and fiber-optic data transmission systems at wavelengths corresponding to basic telecommunication standards (λ = 0.85, 1.3 and 1.55, 1.3, and 1.55 μm) on the basis of silicon technologies.

Next-generation in vivo optical imaging with short-wave infrared quantum dots

PubMed Central

Bruns, Oliver T.; Bischof, Thomas S.; Harris, Daniel K.; Franke, Daniel; Shi, Yanxiang; Riedemann, Lars; Bartelt, Alexander; Jaworski, Frank B.; Carr, Jessica A.; Rowlands, Christopher J.; Wilson, Mark W.B.; Chen, Ou; Wei, He; Hwang, Gyu Weon; Montana, Daniel M.; Coropceanu, Igor; Achorn, Odin B.; Kloepper, Jonas; Heeren, Joerg; So, Peter T.C.; Fukumura, Dai; Jensen, Klavs F.; Jain, Rakesh K.; Bawendi, Moungi G.

2017-01-01

For in vivo imaging, the short-wavelength infrared region (SWIR; 1000–2000 nm) provides several advantages over the visible and near-infrared regions: general lack of autofluorescence, low light absorption by blood and tissue, and reduced scattering. However, the lack of versatile and functional SWIR emitters has prevented the general adoption of SWIR imaging by the biomedical research community. Here, we introduce a class of high-quality SWIR-emissive indium-arsenide-based quantum dots (QDs) that are readily modifiable for various functional imaging applications, and that exhibit narrow and size-tunable emission and a dramatically higher emission quantum yield than previously described SWIR probes. To demonstrate the unprecedented combination of deep penetration, high spatial resolution, multicolor imaging and fast-acquisition-speed afforded by the SWIR QDs, we quantified, in mice, the metabolic turnover rates of lipoproteins in several organs simultaneously and in real time as well as heartbeat and breathing rates in awake and unrestrained animals, and generated detailed three-dimensional quantitative flow maps of the mouse brain vasculature. PMID:29119058

Complete coherent control of silicon vacancies in diamond nanopillars containing single defect centers

DOE PAGES

Zhang, Jingyuan Linda; Lagoudakis, Konstantinos G.; Tzeng, Yan -Kai; ...

2017-10-23

Arrays of identical and individually addressable qubits lay the foundation for the creation of scalable quantum hardware such as quantum processors and repeaters. Silicon-vacancy (SiV) centers in diamond offer excellent physical properties such as low inhomogeneous broadening, fast photon emission, and a large Debye–Waller factor. The possibility for all-optical ultrafast manipulation and techniques to extend the spin coherence times makes them promising candidates for qubits. Here, we have developed arrays of nanopillars containing single (SiV) centers with high yield, and we demonstrate ultrafast all-optical complete coherent control of the excited state population of a single SiV center at the opticalmore » transition frequency. The high quality of the chemical vapor deposition (CVD) grown SiV centers provides excellent spectral stability, which allows us to coherently manipulate and quasi-resonantly read out the excited state population of individual SiV centers on picosecond timescales using ultrafast optical pulses. Furthermore, this work opens new opportunities to create a scalable on-chip diamond platform for quantum information processing and scalable nanophotonics applications.« less

Complete coherent control of silicon vacancies in diamond nanopillars containing single defect centers

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhang, Jingyuan Linda; Lagoudakis, Konstantinos G.; Tzeng, Yan -Kai

Arrays of identical and individually addressable qubits lay the foundation for the creation of scalable quantum hardware such as quantum processors and repeaters. Silicon-vacancy (SiV) centers in diamond offer excellent physical properties such as low inhomogeneous broadening, fast photon emission, and a large Debye–Waller factor. The possibility for all-optical ultrafast manipulation and techniques to extend the spin coherence times makes them promising candidates for qubits. Here, we have developed arrays of nanopillars containing single (SiV) centers with high yield, and we demonstrate ultrafast all-optical complete coherent control of the excited state population of a single SiV center at the opticalmore » transition frequency. The high quality of the chemical vapor deposition (CVD) grown SiV centers provides excellent spectral stability, which allows us to coherently manipulate and quasi-resonantly read out the excited state population of individual SiV centers on picosecond timescales using ultrafast optical pulses. Furthermore, this work opens new opportunities to create a scalable on-chip diamond platform for quantum information processing and scalable nanophotonics applications.« less

Ligand-surface interactions and surface oxidation of colloidal PbSe quantum dots revealed by thin-film positron annihilation methods

NASA Astrophysics Data System (ADS)

Shi, Wenqin; Eijt, Stephan W. H.; Suchand Sandeep, C. S.; Siebbeles, Laurens D. A.; Houtepen, Arjan J.; Kinge, Sachin; Brück, Ekkes; Barbiellini, Bernardo; Bansil, Arun

2016-02-01

Positron Two Dimensional Angular Correlation of Annihilation Radiation (2D-ACAR) measurements reveal modifications of the electronic structure and composition at the surfaces of PbSe quantum dots (QDs), deposited as thin films, produced by various ligands containing either oxygen or nitrogen atoms. In particular, the 2D-ACAR measurements on thin films of colloidal PbSe QDs capped with oleic acid ligands yield an increased intensity in the electron momentum density (EMD) at high momenta compared to PbSe quantum dots capped with oleylamine. Moreover, the EMD of PbSe QDs is strongly affected by the small ethylenediamine ligands, since these molecules lead to small distances between QDs and favor neck formation between near neighbor QDs, inducing electronic coupling between neighboring QDs. The high sensitivity to the presence of oxygen atoms at the surface can be also exploited to monitor the surface oxidation of PbSe QDs upon exposure to air. Our study clearly demonstrates that positron annihilation spectroscopy applied to thin films can probe surface transformations of colloidal semiconductor QDs embedded in functional layers.

Deep Blue Phosphorescent Organic Light-Emitting Diodes with CIEy Value of 0.11 and External Quantum Efficiency up to 22.5.

PubMed

Li, Xiaoyue; Zhang, Juanye; Zhao, Zifeng; Wang, Liding; Yang, Hannan; Chang, Qiaowen; Jiang, Nan; Liu, Zhiwei; Bian, Zuqiang; Liu, Weiping; Lu, Zhenghong; Huang, Chunhui

2018-03-01

Organic light-emitting diodes (OLEDs) based on red and green phosphorescent iridium complexes are successfully commercialized in displays and solid-state lighting. However, blue ones still remain a challenge on account of their relatively dissatisfactory Commission International de L'Eclairage (CIE) coordinates and low efficiency. After analyzing the reported blue iridium complexes in the literature, a new deep-blue-emitting iridium complex with improved photoluminescence quantum yield is designed and synthesized. By rational screening host materials showing high triplet energy level in neat film as well as the OLED architecture to balance electron and hole recombination, highly efficient deep-blue-emission OLEDs with a CIE at (0.15, 0.11) and maximum external quantum efficiency (EQE) up to 22.5% are demonstrated. Based on the transition dipole moment vector measurement with a variable-angle spectroscopic ellipsometry method, the ultrahigh EQE is assigned to a preferred horizontal dipole orientation of the iridium complex in doped film, which is beneficial for light extraction from the OLEDs. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Synthesis and formation mechanistic investigation of nitrogen-doped carbon dots with high quantum yields and yellowish-green fluorescence

NASA Astrophysics Data System (ADS)

Hou, Juan; Wang, Wei; Zhou, Tianyu; Wang, Bo; Li, Huiyu; Ding, Lan

2016-05-01

Heteroatom doped carbon dots (CDs) have received increasing attention due to their unique properties and related applications. However, previously reported CDs generally show strong emission only in the blue-light region, thus restricting their further applications. And the fundamental investigation on the preparation process is always neglected. Herein, we have developed a simple and solvent-free synthetic strategy to fabricate nitrogen-doped CDs (N-CDs) from citric acid and dicyandiamide. The as-prepared N-CDs exhibited a uniform size distribution, strong yellowish-green fluorescence emission and a high quantum yield of 73.2%. The products obtained at different formation stages were detailedly characterized by transmission electron microscopy, X-ray diffraction spectrometer, X-ray photoelectron spectroscopy and UV absorbance spectroscopy. A possible formation mechanism has thus been proposed including dehydration, polymerization and carbonization. Furthermore, the N-CDs could serve as a facile and label-free probe for the detection of iron and fluorine ions with detection limits of 50 nmol L-1 and 75 nmol L-1, respectively.Heteroatom doped carbon dots (CDs) have received increasing attention due to their unique properties and related applications. However, previously reported CDs generally show strong emission only in the blue-light region, thus restricting their further applications. And the fundamental investigation on the preparation process is always neglected. Herein, we have developed a simple and solvent-free synthetic strategy to fabricate nitrogen-doped CDs (N-CDs) from citric acid and dicyandiamide. The as-prepared N-CDs exhibited a uniform size distribution, strong yellowish-green fluorescence emission and a high quantum yield of 73.2%. The products obtained at different formation stages were detailedly characterized by transmission electron microscopy, X-ray diffraction spectrometer, X-ray photoelectron spectroscopy and UV absorbance spectroscopy. A possible formation mechanism has thus been proposed including dehydration, polymerization and carbonization. Furthermore, the N-CDs could serve as a facile and label-free probe for the detection of iron and fluorine ions with detection limits of 50 nmol L-1 and 75 nmol L-1, respectively. Electronic supplementary information (ESI) available. See DOI: 10.1039/c6nr02701f

Synthesis and spectroscopic behavior of highly luminescent Eu 3+-dibenzoylmethanate (DBM) complexes with sulfoxide ligands

NASA Astrophysics Data System (ADS)

Niyama, E.; Brito, H. F.; Cremona, M.; Teotonio, E. E. S.; Reyes, R.; Brito, G. E. S.; Felinto, M. C. F. C.

2005-09-01

In this paper the synthesis, characterization and photoluminescent behavior of the [RE(DBM) 3L 2] complexes (RE = Gd and Eu) with a variety of sulfoxide ligands; L = benzyl sulfoxide (DBSO), methyl sulfoxide (DMSO), phenyl sulfoxide (DPSO) and p-tolyl sulfoxide (PTSO) have been investigated in solid state. The emission spectra of the Eu 3+-β-diketonate complexes show characteristics narrow bands arising from the 5D 0 → 7F J ( J = 0-4) transitions, which are split according to the selection rule for C n, C nv or C s site symmetries. The experimental Judd-Ofelt intensity parameters ( Ω2 and Ω4), radiative ( Arad) and non-radiative ( Anrad) decay rates, and R02 for the europium complexes have been determined and compared. The highest value of Ω2 (61.9 × 10 -20 cm 2) was obtained to the complex with PTSO ligand, indicating that Eu 3+ ion is in the highly polarizable chemical environment. The higher values of the experimental quantum yield ( q) and emission quantum efficiency of the emitter 5D 0 level ( η) for the Eu-complexes with DMSO, DBSO and PTSO sulfoxides suggest that these complexes are promising Light Conversion Molecular Devices (LCMDs). The lower value of quantum yield ( q = 1%), for the hydrated complex [Eu(DBM) 3(H 2O)], indicates that the luminescence quenching occurs via multiphonon relaxation by coupling with the OH-oscillators from water molecule coordinated to rare earth ion. The pure red emission of the Eu-complexes has been confirmed by ( x, y) color coordinates.

A self-assembly aptasensor based on thick-shell quantum dots for sensing of ochratoxin A

NASA Astrophysics Data System (ADS)

Chu, Xianfeng; Dou, Xiaowen; Liang, Ruizheng; Li, Menghua; Kong, Weijun; Yang, Xihui; Luo, Jiaoyang; Yang, Meihua; Zhao, Ming

2016-02-01

A novel self-assembling aptasensor was fabricated by precisely attaching three phosphorothioate-modified capture aptamers onto a single thick-shell quantum dot in a controllable manner for monitoring of ochratoxin A (OTA), a poisonous contaminant widespread in foodstuffs. Herein, CdSe/CdS QDs coated in ten layer CdS shells were synthesized using a continual precursor injection method. Analysis of the prepared CdSe/CdS QDs showed a zinc-blende structure, high photoluminescence quantum yields (>80%), and a photoemission peak with a narrow full-width at half-maximum (about 29 nm), all qualities that render them as a superior choice for optical applications. By adjusting the number of phosphorothioate bases in the anchor domain, the tunable-valency aptasensor was able to self-assemble. In the sensing strategy, the thick-shell quantum dot was provided as an acceptor while OTA itself was used as a donor. In the presence of OTA, the capture aptamers drive the aptasensor function into a measurable signal through a fluorescence resonance energy transfer (FRET) system. The newly developed aptasensor had a detection limit as low as 0.5 ng mL-1, with a linear concentration in the range of 1 to 30 ng mL-1, and therefore meets the requirements for rapid, effective, and anti-interference sensors for real-world applications. Moreover, the high quality thick-shell QDs provide an ideal alternative for highly sensitive imaging and intensive illumination in the fields of biotechnology and bioengineering.A novel self-assembling aptasensor was fabricated by precisely attaching three phosphorothioate-modified capture aptamers onto a single thick-shell quantum dot in a controllable manner for monitoring of ochratoxin A (OTA), a poisonous contaminant widespread in foodstuffs. Herein, CdSe/CdS QDs coated in ten layer CdS shells were synthesized using a continual precursor injection method. Analysis of the prepared CdSe/CdS QDs showed a zinc-blende structure, high photoluminescence quantum yields (>80%), and a photoemission peak with a narrow full-width at half-maximum (about 29 nm), all qualities that render them as a superior choice for optical applications. By adjusting the number of phosphorothioate bases in the anchor domain, the tunable-valency aptasensor was able to self-assemble. In the sensing strategy, the thick-shell quantum dot was provided as an acceptor while OTA itself was used as a donor. In the presence of OTA, the capture aptamers drive the aptasensor function into a measurable signal through a fluorescence resonance energy transfer (FRET) system. The newly developed aptasensor had a detection limit as low as 0.5 ng mL-1, with a linear concentration in the range of 1 to 30 ng mL-1, and therefore meets the requirements for rapid, effective, and anti-interference sensors for real-world applications. Moreover, the high quality thick-shell QDs provide an ideal alternative for highly sensitive imaging and intensive illumination in the fields of biotechnology and bioengineering. Electronic supplementary information (ESI) available: Table S1. See DOI: 10.1039/c5nr08284f

Full spectral optical modeling of quantum-dot-converted elements for light-emitting diodes considering reabsorption and reemission effect.

PubMed

Li, Jia-Sheng; Tang, Yong; Li, Zong-Tao; Cao, Kai; Yan, Cai-Man; Ding, Xin-Rui

2018-07-20

Quantum dots (QDs) have attracted significant attention in light-emitting diode (LED) illumination and display applications, owing to their high quantum yield and unique spectral properties. However, an effective optical model of quantum-dot-converted elements (QDCEs) for (LEDs) that entirely considers the reabsorption and reemission effect is lacking. This suppresses the design of QDCE structures and further investigation of light-extraction/conversion mechanisms in QDCEs. In this paper, we proposed a full spectral optical modeling method for QDCEs packaged in LEDs, entirely considering the reabsorption and reemission effect, and its results are compared with traditional models without reabsorption or reemission. The comparisons indicate that the QDCE absorption loss of QD emission light is a major factor decreasing the radiant efficacy of LEDs, which should be considered when designing QDCE structures. According to the measurements of fabricated LEDs, only calculation results that entirely consider reabsorption and reemission show good agreement with experimental radiant efficacy, spectra, and peak wavelength at the same down-conversion efficiency. Consequently, it is highly expected that QDCE will be modeled considering the reabsorption and reemission events. This study provides a simple and effective modeling method for QDCEs, which shows great potential for their structure designs and fundamental investigations.

Full spectral optical modeling of quantum-dot-converted elements for light-emitting diodes considering reabsorption and reemission effect

NASA Astrophysics Data System (ADS)

Li, Jia-Sheng; Tang, Yong; Li, Zong-Tao; Cao, Kai; Yan, Cai-Man; Ding, Xin-Rui

2018-07-01

Quantum dots (QDs) have attracted significant attention in light-emitting diode (LED) illumination and display applications, owing to their high quantum yield and unique spectral properties. However, an effective optical model of quantum-dot-converted elements (QDCEs) for (LEDs) that entirely considers the reabsorption and reemission effect is lacking. This suppresses the design of QDCE structures and further investigation of light-extraction/conversion mechanisms in QDCEs. In this paper, we proposed a full spectral optical modeling method for QDCEs packaged in LEDs, entirely considering the reabsorption and reemission effect, and its results are compared with traditional models without reabsorption or reemission. The comparisons indicate that the QDCE absorption loss of QD emission light is a major factor decreasing the radiant efficacy of LEDs, which should be considered when designing QDCE structures. According to the measurements of fabricated LEDs, only calculation results that entirely consider reabsorption and reemission show good agreement with experimental radiant efficacy, spectra, and peak wavelength at the same down-conversion efficiency. Consequently, it is highly expected that QDCE will be modeled considering the reabsorption and reemission events. This study provides a simple and effective modeling method for QDCEs, which shows great potential for their structure designs and fundamental investigations.

Luminescent macrocyclic lanthanide complexes

DOEpatents

Raymond, Kenneth N; Corneillie, Todd M; Xu, Jide

2014-05-20

The present invention provides a novel class of macrocyclic compounds as well as complexes formed between a metal (e.g., lanthanide) ion and the compounds of the invention. Preferred complexes exhibit high stability as well as high quantum yields of lanthanide ion luminescence in aqueous media without the need for secondary activating agents. Preferred compounds incorporate hydroxy-isophthalamide moieties within their macrocyclic structure and are characterized by surprisingly low, non-specific binding to a variety of polypeptides such as antibodies and proteins as well as high kinetic stability. These characteristics distinguish them from known, open-structured ligands.

Bifurcation-based adiabatic quantum computation with a nonlinear oscillator network

PubMed Central

Goto, Hayato

2016-01-01

The dynamics of nonlinear systems qualitatively change depending on their parameters, which is called bifurcation. A quantum-mechanical nonlinear oscillator can yield a quantum superposition of two oscillation states, known as a Schrödinger cat state, via quantum adiabatic evolution through its bifurcation point. Here we propose a quantum computer comprising such quantum nonlinear oscillators, instead of quantum bits, to solve hard combinatorial optimization problems. The nonlinear oscillator network finds optimal solutions via quantum adiabatic evolution, where nonlinear terms are increased slowly, in contrast to conventional adiabatic quantum computation or quantum annealing, where quantum fluctuation terms are decreased slowly. As a result of numerical simulations, it is concluded that quantum superposition and quantum fluctuation work effectively to find optimal solutions. It is also notable that the present computer is analogous to neural computers, which are also networks of nonlinear components. Thus, the present scheme will open new possibilities for quantum computation, nonlinear science, and artificial intelligence. PMID:26899997

Quantum random access memory.

PubMed

Giovannetti, Vittorio; Lloyd, Seth; Maccone, Lorenzo

2008-04-25

A random access memory (RAM) uses n bits to randomly address N=2(n) distinct memory cells. A quantum random access memory (QRAM) uses n qubits to address any quantum superposition of N memory cells. We present an architecture that exponentially reduces the requirements for a memory call: O(logN) switches need be thrown instead of the N used in conventional (classical or quantum) RAM designs. This yields a more robust QRAM algorithm, as it in general requires entanglement among exponentially less gates, and leads to an exponential decrease in the power needed for addressing. A quantum optical implementation is presented.

Graph C ∗-algebras and Z2-quotients of quantum spheres

NASA Astrophysics Data System (ADS)

Hajac, Piotr M.; Matthes, Rainer; Szymański, Wojciech

2003-06-01

We consider two Z2-actions on the Podleś generic quantum spheres. They yield, as noncommutative quotient spaces, the Klimek-Lesmewski q-disc and the quantum real projective space, respectively. The C ∗-algebas of all these quantum spaces are described as graph C ∗-algebras. The K-groups of the thus presented C ∗-algebras are then easily determined from the general theory of graph C ∗-algebas. For the quantum real projective space, we also recall the classification of the classes of irreducible ∗-representations of its algebra and give a linear basis for this algebra.

Preparation of highly fluorescent magnetic nanoparticles for analytes-enrichment and subsequent biodetection.

PubMed

Zhang, Bingbo; Chen, Bingdi; Wang, Yilong; Guo, Fangfang; Li, Zhuoquan; Shi, Donglu

2011-01-15

Bifunctional nanoparticles with highly fluorescence and decent magnetic properties have been widely used in biomedical application. In this study, highly fluorescent magnetic nanoparticles (FMNPs) with uniform size of ca. 40 nm are prepared by encapsulation of both magnetic nanoparticles (MNPs) and shell/core quantum dots (QDs) with well-designed shell structure/compositions into silica matrix via a one-pot reverse microemulsion approach. The spectral analysis shows that the FMNPs hold high fluorescent quantum yield (QY). The QYs and saturation magnetization of the FMNPs can be regulated by varying the ratio of the encapsulated QDs to MNPs. Moreover, the surface of the FMNPs can be modified to offer chemical groups for antibody conjugation for following use in target-enrichment and subsequent fluorescent detection. The in vitro immunofluorescence assay and flow cytometric analysis indicate that the bifunctional FMNPs-antibody bioconjugates are capable of target-enrichment, magnetic separation and can also be used as alternative fluorescent probes on flow cytometry for biodetection. Copyright © 2010 Elsevier Inc. All rights reserved.

Diurnal changes of photosynthetic quantum yield in the intertidal macroalga Sargassum thunbergii under simulated tidal emersion conditions

NASA Astrophysics Data System (ADS)

Yu, Yong Qiang; Zhang, Quan Sheng; Tang, Yong Zheng; Li, Xue Meng; Liu, Hong Liang; Li, Li Xia

2013-07-01

In this study, a three-way factorial experimental design was used to investigate the diurnal changes of photosynthetic activity of the intertidal macroalga Sargassum thunbergii in response to temperature, tidal pattern and desiccation during a simulated diurnal light cycle. The maximum (Fv/Fm) and effective (ΦPSII) quantum yields of photosystem II (PSII) were estimated by chlorophyll fluorescence using a pulse amplitude modulated fluorometer. Results showed that this species exhibited sun-adapted characteristics, as evidenced by the daily variation of Fv/Fm and ΦPSII. Both yield values decreased with increasing irradiance towards noon and recovered rapidly in the afternoon suggesting a dynamic photoinhibition. The photosynthetic quantum yield of S. thunbergii thalli varied significantly with temperature, tidal pattern and desiccation. Thalli were more susceptible to light-induced damage at high temperature of 25 °C and showed complete recovery of photosynthetic activity only when exposed to 8 °C. In contrast with the mid-morning low tide period, although there was an initial increase in photosynthetic yield during emersion, thalli showed a greater degree of decline at the end of emersion and remained less able to recover when low tide occurred at mid-afternoon. Short-term air exposure of 2 h did not significantly influence the photosynthesis. However, when exposed to moderate conditions (4 h desiccation at 15 °C or 6 h desiccation at 8 °C), a significant inhibition of photosynthesis was followed by partial or complete recovery upon re-immersion in late afternoon. Only extreme conditions (4 h desiccation at 25 °C or 6 h desiccation at 15 °C or 25 °C) resulted in the complete inhibition, with little indication of recovery until the following morning, implying the occurrence of chronic PSII damage. Based on the magnitude of effect, desiccation was the predominant negative factor affecting the photosynthesis under the simulated daytime irradiance period. These results may explain the distribution pattern of this species in natural habitats, where it is generally restricted to tide pools in the intertidal zone of wave-swept rocky shores which could provide shelter from desiccation stress during low tide.

Handshake electron transfer from hydrogen Rydberg atoms incident at a series of metallic thin films

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gibbard, J. A.; Softley, T. P.

2016-06-21

Thin metallic films have a 1D quantum well along the surface normal direction, which yields particle-in-a-box style electronic quantum states. However the quantum well is not infinitely deep and the wavefunctions of these states penetrate outside the surface where the electron is bound by its own image-charge attraction. Therefore a series of discrete, vacant states reach out from the thin film into the vacuum increasing the probability of electron transfer from an external atom or molecule to the thin film, especially for the resonant case where the quantum well energy matches that of the atom. We show that “handshake” electronmore » transfer from a highly excited Rydberg atom to these thin-film states is experimentally measurable. Thicker films have a wider 1D box, changing the energetic distribution and image-state contribution to the thin film wavefunctions, resulting in more resonances. Calculations successfully predict the number of resonances and the nature of the thin-film wavefunctions for a given film thickness.« less

One-Step Synthesis of Boron Nitride Quantum Dots: Simple Chemistry Meets Delicate Nanotechnology.

PubMed

Liu, Bingping; Yan, Shihai; Song, Zhongqian; Liu, Mengli; Ji, Xuqiang; Yang, Wenrong; Liu, Jingquan

2016-12-23

Herein, a conceptually new and straightforward aqueous route is described for the synthesis of hydroxyl- and amino-functionalized boron nitride quantum dots (BNQDs) with quantum yields (QY) as high as 18.3 % by using a facile bottom-up approach, in which a mixture of boric acid and ammonia solution was hydrothermally treated in one pot at 200 °C for 12 h. The functionalized BNQDs, with excellent photoluminescence properties, could be easily dispersed in an aqueous medium and applied as fluorescent probes for the detection of ferrous (Fe 2+ ) and ferric (Fe 3+ ) ions with excellent selectivity and low detection limits. The mechanisms for the hydrothermal reaction and fluorescence quenching were also simulated by using density functional theory (DFT), which confirmed the feasibility and advantages of this strategy. It provides a scalable and eco-friendly method for preparation of BNQDs with good dispersability and could also be generalized to the synthesis of other 2D quantum dots and nanoplates. © 2016 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.