Effects of Bleaching by Nitrogen Deficiency on the Quantum Yield of Photosystem II in Synechocystis sp. PCC 6803 Revealed by Chl Fluorescence Measurements.

PubMed

Ogawa, Takako; Sonoike, Kintake

2016-03-01

Estimation of photosynthesis by Chl fluorescence measurement of cyanobacteria is always problematic due to the interference from respiratory electron transfer and from phycocyanin fluorescence. The interference from respiratory electron transfer could be avoided by the use of DCMU or background illumination by blue light, which oxidizes the plastoquinone pool that tends to be reduced by respiration. On the other hand, the precise estimation of photosynthesis in cells with a different phycobilisome content by Chl fluorescence measurement is difficult. By subtracting the basal fluorescence due to the phycobilisome and PSI, it becomes possible to estimate the precise maximum quantum yield of PSII in cyanobacteria. Estimated basal fluorescence accounted for 60% of the minimum fluorescence, resulting in a large difference between the 'apparent' yield and 'true' yield under high phycocyanin conditions. The calculated value of the 'true' maximum quantum yield of PSII was around 0.8, which was similar to the value observed in land plants. The results suggest that the cause of the apparent low yield reported in cyanobacteria is mainly ascribed to the interference from phycocyanin fluorescence. We also found that the 'true' maximum quantum yield of PSII decreased under nitrogen-deficient conditions, suggesting the impairment of the PSII reaction center, while the 'apparent' maximum quantum yield showed a marginal change under the same conditions. Due to the high contribution of phycocyanin fluorescence in cyanobacteria, it is essential to eliminate the influence of the change in phycocyanin content on Chl fluorescence measurement and to evaluate the 'true' photosynthetic condition. © The Author 2016. Published by Oxford University Press on behalf of Japanese Society of Plant Physiologists. All rights reserved. For permissions, please email: journals.permissions@oup.com.

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.

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.

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.

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

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.

Laboratory study of nitrate photolysis in Antarctic snow. I. Observed quantum yield, domain of photolysis, and secondary chemistry

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

Meusinger, Carl; Johnson, Matthew S.; Berhanu, Tesfaye A.

2014-06-28

Post-depositional processes alter nitrate concentration and nitrate isotopic composition in the top layers of snow at sites with low snow accumulation rates, such as Dome C, Antarctica. Available nitrate ice core records can provide input for studying past atmospheres and climate if such processes are understood. It has been shown that photolysis of nitrate in the snowpack plays a major role in nitrate loss and that the photolysis products have a significant influence on the local troposphere as well as on other species in the snow. Reported quantum yields for the main reaction spans orders of magnitude – apparently amore » result of whether nitrate is located at the air-ice interface or in the ice matrix – constituting the largest uncertainty in models of snowpack NO{sub x} emissions. Here, a laboratory study is presented that uses snow from Dome C and minimizes effects of desorption and recombination by flushing the snow during irradiation with UV light. A selection of UV filters allowed examination of the effects of the 200 and 305 nm absorption bands of nitrate. Nitrate concentration and photon flux were measured in the snow. The quantum yield for loss of nitrate was observed to decrease from 0.44 to 0.003 within what corresponds to days of UV exposure in Antarctica. The superposition of photolysis in two photochemical domains of nitrate in snow is proposed: one of photolabile nitrate, and one of buried nitrate. The difference lies in the ability of reaction products to escape the snow crystal, versus undergoing secondary (recombination) chemistry. Modeled NO{sub x} emissions may increase significantly above measured values due to the observed quantum yield in this study. The apparent quantum yield in the 200 nm band was found to be ∼1%, much lower than reported for aqueous chemistry. A companion paper presents an analysis of the change in isotopic composition of snowpack nitrate based on the same samples as in this study.« less

Observables, measurements and phase operators from a Bohmian perspective

NASA Technical Reports Server (NTRS)

Daumer, Martin; Goldstein, Sheldon

1993-01-01

Bohmian mechanics is a deterministic theory of point particles in motion. While avoiding all the paradoxes of nonrelativistic quantum mechanics, it yields the quantum formalism itself--especially the role of self-adjoint operators--as a macroscopic measurement formalism. As an 'application' it is shown that much of the confusion connected with the phase operator for the electromagnetic field arises from a misunderstanding of the role of operators in quantum theory.

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.

Impact of Mono-Fluorination on the Photophysics of the Flavin Chromophore.

PubMed

Reiffers, Anna; Torres Ziegenbein, Christian; Engelhardt, Alyn; Kühnemuth, Ralf; Gilch, Peter; Czekelius, Constantin

2018-03-31

Three mono-fluorinated derivatives of the flavin core system 10-methyl-isoalloxazine (MIA) were synthesized. Aqueous solutions of these compounds were characterized by steady-state and time-resolved spectroscopy. The positions for the fluorination (6, 7 and 8) were motivated by the nodal structure of the frontier orbitals of MIA. In comparison with MIA, the fluorination results in bathochromic (6F- and 7F-MIA) and hypsochromic (8F-MIA) shifts of the adiabatic excitation energy of the lowest allowed transition. Shifts of up to ~500 cm -1 were observed. These spectroscopic shifts go along with changes in fluorescence quantum yields and lifetimes. In addition, triplet yields are affected. For 7F-MIA, a 50% increase in the fluorescence quantum yield as well as a 50% decrease in triplet yield is observed rendering the compound interesting for fluorescence applications. The measured effects are discussed in terms of qualitative perturbation theory. © 2018 The American Society of Photobiology.

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

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.

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.

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

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.

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.

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.

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.

Noncommuting observables in quantum detection and estimation theory

NASA Technical Reports Server (NTRS)

Helstrom, C. W.

1972-01-01

Basing decisions and estimates on simultaneous approximate measurements of noncommuting observables in a quantum receiver is shown to be equivalent to measuring commuting projection operators on a larger Hilbert space than that of the receiver itself. The quantum-mechanical Cramer-Rao inequalities derived from right logarithmic derivatives and symmetrized logarithmic derivatives of the density operator are compared, and it is shown that the latter give superior lower bounds on the error variances of individual unbiased estimates of arrival time and carrier frequency of a coherent signal. For a suitably weighted sum of the error variances of simultaneous estimates of these, the former yield the superior lower bound under some conditions.

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.

Absolute quantum yield measurement of powder samples.

PubMed

Moreno, Luis A

2012-05-12

Measurement of fluorescence quantum yield has become an important tool in the search for new solutions in the development, evaluation, quality control and research of illumination, AV equipment, organic EL material, films, filters and fluorescent probes for bio-industry. Quantum yield is calculated as the ratio of the number of photons absorbed, to the number of photons emitted by a material. The higher the quantum yield, the better the efficiency of the fluorescent material. For the measurements featured in this video, we will use the Hitachi F-7000 fluorescence spectrophotometer equipped with the Quantum Yield measuring accessory and Report Generator program. All the information provided applies to this system. Measurement of quantum yield in powder samples is performed following these steps: 1. Generation of instrument correction factors for the excitation and emission monochromators. This is an important requirement for the correct measurement of quantum yield. It has been performed in advance for the full measurement range of the instrument and will not be shown in this video due to time limitations. 2. Measurement of integrating sphere correction factors. The purpose of this step is to take into consideration reflectivity characteristics of the integrating sphere used for the measurements. 3. Reference and Sample measurement using direct excitation and indirect excitation. 4. Quantum Yield calculation using Direct and Indirect excitation. Direct excitation is when the sample is facing directly the excitation beam, which would be the normal measurement setup. However, because we use an integrating sphere, a portion of the emitted photons resulting from the sample fluorescence are reflected by the integrating sphere and will re-excite the sample, so we need to take into consideration indirect excitation. This is accomplished by measuring the sample placed in the port facing the emission monochromator, calculating indirect quantum yield and correcting the direct quantum yield calculation. 5. Corrected quantum yield calculation. 6. Chromaticity coordinates calculation using Report Generator program. The Hitachi F-7000 Quantum Yield Measurement System offer advantages for this application, as follows: High sensitivity (S/N ratio 800 or better RMS). Signal is the Raman band of water measured under the following conditions: Ex wavelength 350 nm, band pass Ex and Em 5 nm, response 2 sec), noise is measured at the maximum of the Raman peak. High sensitivity allows measurement of samples even with low quantum yield. Using this system we have measured quantum yields as low as 0.1 for a sample of salicylic acid and as high as 0.8 for a sample of magnesium tungstate. Highly accurate measurement with a dynamic range of 6 orders of magnitude allows for measurements of both sharp scattering peaks with high intensity, as well as broad fluorescence peaks of low intensity under the same conditions. High measuring throughput and reduced light exposure to the sample, due to a high scanning speed of up to 60,000 nm/minute and automatic shutter function. Measurement of quantum yield over a wide wavelength range from 240 to 800 nm. Accurate quantum yield measurements are the result of collecting instrument spectral response and integrating sphere correction factors before measuring the sample. Large selection of calculated parameters provided by dedicated and easy to use software. During this video we will measure sodium salicylate in powder form which is known to have a quantum yield value of 0.4 to 0.5.

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.

Extending Bell's beables to encompass dissipation, decoherence, and the quantum-to-classical transition through quantum trajectories

NASA Astrophysics Data System (ADS)

Lorenzen, F.; de Ponte, M. A.; Moussa, M. H. Y.

2009-09-01

In this paper, employing the Itô stochastic Schrödinger equation, we extend Bell’s beable interpretation of quantum mechanics to encompass dissipation, decoherence, and the quantum-to-classical transition through quantum trajectories. For a particular choice of the source of stochasticity, the one leading to a dissipative Lindblad-type correction to the Hamiltonian dynamics, we find that the diffusive terms in Nelsons stochastic trajectories are naturally incorporated into Bohm’s causal dynamics, yielding a unified Bohm-Nelson theory. In particular, by analyzing the interference between quantum trajectories, we clearly identify the decoherence time, as estimated from the quantum formalism. We also observe the quantum-to-classical transition in the convergence of the infinite ensemble of quantum trajectories to their classical counterparts. Finally, we show that our extended beables circumvent the problems in Bohm’s causal dynamics regarding stationary states in quantum mechanics.

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

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.

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.

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.

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.

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.

Unity quantum yield of photogenerated charges and band-like transport in quantum-dot solids.

PubMed

Talgorn, Elise; Gao, Yunan; Aerts, Michiel; Kunneman, Lucas T; Schins, Juleon M; Savenije, T J; van Huis, Marijn A; van der Zant, Herre S J; Houtepen, Arjan J; Siebbeles, Laurens D A

2011-09-25

Solid films of colloidal quantum dots show promise in the manufacture of photodetectors and solar cells. These devices require high yields of photogenerated charges and high carrier mobilities, which are difficult to achieve in quantum-dot films owing to a strong electron-hole interaction and quantum confinement. Here, we show that the quantum yield of photogenerated charges in strongly coupled PbSe quantum-dot films is unity over a large temperature range. At high photoexcitation density, a transition takes place from hopping between localized states to band-like transport. These strongly coupled quantum-dot films have electrical properties that approach those of crystalline bulk semiconductors, while retaining the size tunability and cheap processing properties of colloidal quantum dots.

Control of Emission Color of High Quantum Yield CH3NH3PbBr3 Perovskite Quantum Dots by Precipitation Temperature.

PubMed

Huang, He; Susha, Andrei S; Kershaw, Stephen V; Hung, Tak Fu; Rogach, Andrey L

2015-09-01

Emission color controlled, high quantum yield CH 3 NH 3 PbBr 3 perovskite quantum dots are obtained by changing the temperature of a bad solvent during synthesis. The products for temperatures between 0 and 60 °C have good spectral purity with narrow emission line widths of 28-36 nm, high absolute emission quantum yields of 74% to 93%, and short radiative lifetimes of 13-27 ns.

An Analytical Quantum Model to Calculate Fluorescence Enhancement of a Molecule in Vicinity of a Sub-10 nm Metal Nanoparticle.

PubMed

Bagheri, Zahra; Massudi, Reza

2017-05-01

An analytical quantum model is used to calculate electrical permittivity of a metal nanoparticle located in an adjacent molecule. Different parameters, such as radiative and non-radiative decay rates, quantum yield, electrical field enhancement factor, and fluorescence enhancement are calculated by such a model and they are compared with those obtained by using the classical Drude model. It is observed that using an analytical quantum model presents a higher enhancement factor, up to 30%, as compared to classical model for nanoparticles smaller than 10 nm. Furthermore, the results are in better agreement with those experimentally realized.

Creating high yield water soluble luminescent graphene quantum dots via exfoliating and disintegrating carbon nanotubes and graphite flakes.

PubMed

Lin, Liangxu; Zhang, Shaowei

2012-10-21

We have developed an effective method to exfoliate and disintegrate multi-walled carbon nanotubes and graphite flakes. With this technique, high yield production of luminescent graphene quantum dots with high quantum yield and low oxidization can be achieved.

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.

Primordial non-Gaussianity and power asymmetry with quantum gravitational effects in loop quantum cosmology

NASA Astrophysics Data System (ADS)

Zhu, Tao; Wang, Anzhong; Kirsten, Klaus; Cleaver, Gerald; Sheng, Qin

2018-02-01

Loop quantum cosmology provides a resolution of the classical big bang singularity in the deep Planck era. The evolution, prior to the usual slow-roll inflation, naturally generates excited states at the onset of the slow-roll inflation. It is expected that these quantum gravitational effects could leave its fingerprints on the primordial perturbation spectrum and non-Gaussianity, and lead to some observational evidences in the cosmic microwave background. While the impact of the quantum effects on the primordial perturbation spectrum has been already studied and constrained by current data, in this paper we continue to study such effects but now on the non-Gaussianity of the primordial curvature perturbations. We present detailed and analytical calculations of the non-Gaussianity and show explicitly that the corrections due to the quantum effects are at the same magnitude of the slow-roll parameters in the observable scales and thus are well within current observational constraints. Despite this, we show that the non-Gaussianity in the squeezed limit can be enhanced at superhorizon scales and it is these effects that can yield a large statistical anisotropy on the power spectrum through the Erickcek-Kamionkowski-Carroll mechanism.

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.

Particle yields from numerical simulations

NASA Astrophysics Data System (ADS)

Homor, Marietta M.; Jakovác, Antal

2018-04-01

In this paper we use numerical field theoretical simulations to calculate particle yields. We demonstrate that in the model of local particle creation the deviation from the pure exponential distribution is natural even in equilibrium, and an approximate Tsallis-Pareto-like distribution function can be well fitted to the calculated yields, in accordance with the experimental observations. We present numerical simulations in the classical Φ4 model as well as in the SU(3) quantum Yang-Mills theory to clarify this issue.

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.

Mysteries of TOPSe revealed: insights into quantum dot nucleation.

PubMed

Evans, Christopher M; Evans, Meagan E; Krauss, Todd D

2010-08-18

We have investigated the reaction mechanism responsible for QD nucleation using optical absorption and nuclear magnetic resonance spectroscopies. For typical II-VI and IV-VI quantum dot (QD) syntheses, pure tertiary phosphine selenide sources (e.g., trioctylphosphine selenide (TOPSe)) were surprisingly found to be unreactive with metal carboxylates and incapable of yielding QDs. Rather, small quantities of secondary phosphines, which are impurities in tertiary phosphines, are entirely responsible for the nucleation of QDs; their low concentrations account for poor synthetic conversion yields. QD yields increase to nearly quantitative levels when replacing TOPSe with a stoiciometric amount of a secondary phosphine chalcogenide such as diphenylphosphine selenide. Based on our observations, we have proposed potential monomer identities, reaction pathways, and transition states and believe this mechanism to be universal to all II-VI and IV-VI QDs synthesized using phosphine based methods.

Mysteries of TOPSe Revealed: Insights into Quantum Dot Nucleation

PubMed Central

Evans, Christopher M.; Evans, Meagan E.

2010-01-01

We have investigated the reaction mechanism responsible for QD nucleation using optical absorption and nuclear magnetic resonance spectroscopies. For typical II-VI and IV-VI quantum dot (QD) syntheses, pure tertiary phosphine selenide sources (e.g. trioctylphosphine selenide (TOPSe)) were surprisingly found to be unreactive with metal carboxylates and incapable of yielding QDs. Rather, small quantities of secondary phosphines, which are impurities in tertiary phosphines, are entirely responsible for the nucleation of QDs; their low concentrations account for poor synthetic conversion yields. QD yields increase to nearly quantitative levels when replacing TOPSe with a stoiciometric amount of a secondary phosphine chalcogenide such as diphenylphosphine selenide. Based on our observations, we have proposed potential monomer identities, reaction pathways and transition states, and believe this mechanism to be universal to all II-VI and IV-VI QDs synthesized using phosphine based methods. PMID:20698646

Magneto-transport of an electron bilayer system in an undoped Si/SiGe double-quantum-well heterostructure

DOE PAGES

Laroche, Dominique; Huang, ShiHsien; Nielsen, Erik; ...

2015-04-08

We report the design, the fabrication, and the magneto-transport study of an electron bilayer system embedded in an undoped Si/SiGe double-quantum-well heterostructure. Additionally, the combined Hall densities (n Hall ) ranging from 2.6 × 10 10 cm -2 to 2.7 × 10 11 cm -2 were achieved, yielding a maximal combined Hall mobility (μ Hall ) of 7.7 × 10 5 cm 2/(V • s) at the highest density. Simultaneous electron population of both quantum wells is clearly observed through a Hall mobility drop as the Hall density is increased to n Hall > 3.3 × 10 10 cm -2,more » consistent with Schrödinger-Poisson simulations. Furthermore, the integer and fractional quantum Hall effects are observed in the device, and single-layer behavior is observed when both layers have comparable densities, either due to spontaneous interlayer coherence or to the symmetric-antisymmetric gap.« less

High quantum yield ZnO quantum dots synthesizing via an ultrasonication microreactor method.

PubMed

Yang, Weimin; Yang, Huafang; Ding, Wenhao; Zhang, Bing; Zhang, Le; Wang, Lixi; Yu, Mingxun; Zhang, Qitu

2016-11-01

Green emission ZnO quantum dots were synthesized by an ultrasonic microreactor. Ultrasonic radiation brought bubbles through ultrasonic cavitation. These bubbles built microreactor inside the microreactor. The photoluminescence properties of ZnO quantum dots synthesized with different flow rate, ultrasonic power and temperature were discussed. Flow rate, ultrasonic power and temperature would influence the type and quantity of defects in ZnO quantum dots. The sizes of ZnO quantum dots would be controlled by those conditions as well. Flow rate affected the reaction time. With the increasing of flow rate, the sizes of ZnO quantum dots decreased and the quantum yields first increased then decreased. Ultrasonic power changed the ultrasonic cavitation intensity, which affected the reaction energy and the separation of the solution. With the increasing of ultrasonic power, sizes of ZnO quantum dots first decreased then increased, while the quantum yields kept increasing. The effect of ultrasonic temperature on the photoluminescence properties of ZnO quantum dots was influenced by the flow rate. Different flow rate related to opposite changing trend. Moreover, the quantum yields of ZnO QDs synthesized by ultrasonic microreactor could reach 64.7%, which is higher than those synthesized only under ultrasonic radiation or only by microreactor. Copyright © 2016 Elsevier B.V. All rights reserved.

Mechanism for the Green Glow of the Upper Ionosphere

NASA Technical Reports Server (NTRS)

Guberman, Steven L.

1997-01-01

The generation of the green line of atomic oxygen by dissociative recombination of 02 plus occurs by the capture of an electron into a repulsive state of 02 followed by dissociation along another state of a different electronic symmetry. The two states are coupled together by mixed symmetry Rydberg states. Quantum chemical calculations give a rate coefficient at room temperature of (0.39 (+ 0.31 or -0.19)) x 10 exp -8 cubic centimeters per second. The quantum yield of excited oxygen is within the range deduced from ground, rocket, and satellite observations. The rate coefficients and yields are needed in models of the optical emission, chemistry, and energy balance of planetary ionospheres.

General Relativity without paradigm of space-time covariance, and resolution of the problem of time

NASA Astrophysics Data System (ADS)

Soo, Chopin; Yu, Hoi-Lai

2014-01-01

The framework of a theory of gravity from the quantum to the classical regime is presented. The paradigm shift from full space-time covariance to spatial diffeomorphism invariance, together with clean decomposition of the canonical structure, yield transparent physical dynamics and a resolution of the problem of time. The deep divide between quantum mechanics and conventional canonical formulations of quantum gravity is overcome with a Schrödinger equation for quantum geometrodynamics that describes evolution in intrinsic time. Unitary time development with gauge-invariant temporal ordering is also viable. All Kuchar observables become physical; and classical space-time, with direct correlation between its proper times and intrinsic time intervals, emerges from constructive interference. The framework not only yields a physical Hamiltonian for Einstein's theory, but also prompts natural extensions and improvements towards a well behaved quantum theory of gravity. It is a consistent canonical scheme to discuss Horava-Lifshitz theories with intrinsic time evolution, and of the many possible alternatives that respect 3-covariance (rather than the more restrictive 4-covariance of Einstein's theory), Horava's "detailed balance" form of the Hamiltonian constraint is essentially pinned down by this framework. Issues in quantum gravity that depend on radiative corrections and the rigorous definition and regularization of the Hamiltonian operator are not addressed in this work.

Spectroscopic investigation of alloyed quantum dot-based FRET to cresyl violet dye.

PubMed

Kotresh, M G; Adarsh, K S; Shivkumar, M A; Mulimani, B G; Savadatti, M I; Inamdar, S R

2016-05-01

Quantum dots (QDs), bright luminescent semiconductor nanoparticles, have found numerous applications ranging from optoelectronics to bioimaging. Here, we present a systematic investigation of fluorescence resonance energy transfer (FRET) from hydrophilic ternary alloyed quantum dots (CdSeS/ZnS) to cresyl violet dye with a view to explore the effect of composition of QD donors on FRET efficiency. Fluorescence emission of QD is controlled by varying the composition of QD without altering the particle size. The results show that quantum yield of the QDs increases with increase in the emission wavelength. The FRET parameters such as spectral overlap J(λ), Förster distance R0, intermolecular distance (r), rate of energy transfer k(T)(r), and transfer efficiency (E) are determined by employing both steady-state and time-resolved fluorescence spectroscopy. Additionally, dynamic quenching is noticed to occur in the present FRET system. Stern-Volmer (K(D)) and bimolecular quenching constants (k(q)) are determined from the Stern-Volmer plot. It is observed that the transfer efficiency follows a linear dependence on the spectral overlap and the quantum yield of the donor as predicted by the Förster theory upon changing the composition of the QD. Copyright © 2015 John Wiley & Sons, Ltd.

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.

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.

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.

Phytoplankton natural fluorescence variability in the Sargasso Sea

NASA Astrophysics Data System (ADS)

Westberry, T. K.; Siegel, D. A.

2003-03-01

Phytoplankton fluorescence has been used historically as a means of assessing phytoplankton biomass, rates of primary production (PP) and physiological status in laboratory, in situ, and satellite based investigations. Assumptions about the quantum yield of phytoplankton fluorescence, φf, are often overlooked and can become problematic when fluorescence based methods are applied. A time series of φf observations from the northwestern Sargasso Sea is presented with the goal of understanding the controls on fluorescence and its applicability for assessing upper ocean biological processes. Accurate estimates of φf require accounting for Raman scattering and the conversion of planar to scalar irradiance. Variability in φf occurs on both seasonal and episodic time scales. Seasonal variations show maxima in the surface layer during summer months while lower, more uniform values are found throughout the winter when deep mixing occurs. Large episodic variations in φf are observed throughout the record which dwarf seasonal changes. Predictions of depth-dependent and depth-integrated PP rates using φf and natural fluorescence fluxes are only marginally successful ( r2˜50%), although comparable with results from global bio-optical models for the Sargasso Sea. Improvements in PP predictions are hindered by weak statistical relationships with other parameters. φf is largely decoupled from the quantum yield of carbon assimilation, φc, indicating that an inverse relationship between fluorescence and photosynthesis does not exist. Consequently, variability in the quantum yield of thermal de-excitation, φh, is found to be of similar magnitude as φf on the timescales observed. These observations show that assumptions about photochemical energy flow through the phytoplankton community must be made carefully and that the fluorescence-photosynthesis relationship is not straightforward.

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.

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…

Relativistic quantum Darwinism in Dirac fermion and graphene systems

NASA Astrophysics Data System (ADS)

Ni, Xuan; Huang, Liang; Lai, Ying-Cheng; Pecora, Louis

2012-02-01

We solve the Dirac equation in two spatial dimensions in the setting of resonant tunneling, where the system consists of two symmetric cavities connected by a finite potential barrier. The shape of the cavities can be chosen to yield both regular and chaotic dynamics in the classical limit. We find that certain pointer states about classical periodic orbits can exist, which are signatures of relativistic quantum Darwinism (RQD). These localized states suppress quantum tunneling, and the effect becomes less severe as the underlying classical dynamics in the cavity is chaotic, leading to regularization of quantum tunneling. Qualitatively similar phenomena have been observed in graphene. A physical theory is developed to explain relativistic quantum Darwinism and its effects based on the spectrum of complex eigenenergies of the non-Hermitian Hamiltonian describing the open cavity system.

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.

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.

Improved photocatalytic degradation of Orange G using hybrid nanofibers

NASA Astrophysics Data System (ADS)

Ledwaba, Mpho; Masilela, Nkosiphile; Nyokong, Tebello; Antunes, Edith

2017-05-01

Functionalised electrospun polyamide-6 (PA-6) nanofibres incorporating gadolinium oxide nanoparticles conjugated to zinc tetracarboxyphenoxy phthalocyanine (ZnTCPPc) as the sensitizer were prepared for the photocatalytic degradation of Orange G. Fibres incorporating the phthalocyanine alone or a mixture of the nanoparticles and phthalocyanine were also generated. The singlet oxygen-generating ability of the sensitizer was shown to be maintained within the fibre mat, with the singlet oxygen quantum yields increasing upon incorporation of the magnetic nanoparticles. Consequently, the rate of the photodegradation of Orange G was observed to increase with an increase in singlet oxygen quantum yield. A reduction in the half-lives for the functionalised nanofibres was recorded in the presence of the magnetic nanoparticles, indicating an improvement in the efficiency of the degradation process.

A comparative photophysicochemical study of phthalocyanines encapsulated in core-shell silica nanoparticles.

PubMed

Fashina, Adedayo; Amuhaya, Edith; Nyokong, Tebello

2015-02-25

This work presents the synthesis and characterization of a new zinc phthalocyanine complex tetrasubstituted with 3-carboxyphenoxy in the peripheral position. The photophysical properties of the new complex are compared with those of phthalocyanines tetra substituted with 3-carboxyphenoxy or 4-carboxyphenoxy at non-peripheral positions. Three phthalocyanine complexes were encapsulated within silica matrix to form a core shell and the hybrid nanoparticles particles obtained were spherical and mono dispersed. When encapsulated within the silica shell nanoparticles, phthalocyanines showed improved triplet quantum yields and singlet oxygen quantum yields than surface grafted derivatives. The improvements observed could be attributed to the protection provided for the phthalocyanine complexes by the silica matrix. Copyright © 2014 Elsevier B.V. All rights reserved.

BFV approach to geometric quantization

NASA Astrophysics Data System (ADS)

Fradkin, E. S.; Linetsky, V. Ya.

1994-12-01

A gauge-invariant approach to geometric quantization is developed. It yields a complete quantum description for dynamical systems with non-trivial geometry and topology of the phase space. The method is a global version of the gauge-invariant approach to quantization of second-class constraints developed by Batalin, Fradkin and Fradkina (BFF). Physical quantum states and quantum observables are respectively described by covariantly constant sections of the Fock bundle and the bundle of hermitian operators over the phase space with a flat connection defined by the nilpotent BVF-BRST operator. Perturbative calculation of the first non-trivial quantum correction to the Poisson brackets leads to the Chevalley cocycle known in deformation quantization. Consistency conditions lead to a topological quantization condition with metaplectic anomaly.

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

Physics Meets Philosophy at the Planck Scale

NASA Astrophysics Data System (ADS)

Callender, Craig; Huggett, Nick

2001-04-01

Preface; 1. Introduction Craig Callendar and Nick Huggett; Part I. Theories of Quantum Gravity and their Philosophical Dimensions: 2. Spacetime and the philosophical challenge of quantum gravity Jeremy Butterfield and Christopher Isham; 3. Naive quantum gravity Steven Weinstein; 4. Quantum spacetime: what do we know? Carlo Rovelli; Part II. Strings: 5. Reflections on the fate of spacetime Edward Witten; 6. A philosopher looks at string theory Robert Weingard; 7. Black holes, dumb holes, and entropy William G. Unruh; Part III. Topological Quantum Field Theory: 8. Higher-dimensional algebra and Planck scale physics John C. Baez; Part IV. Quantum Gravity and the Interpretation of General Relativity: 9. On general covariance and best matching Julian B. Barbour; 10. Pre-Socratic quantum gravity Gordon Belot and John Earman; 11. The origin of the spacetime metric: Bell's 'Lorentzian Pedagogy' and its significance in general relativity Harvey R. Brown and Oliver Pooley; Part IV. Quantum Gravity and the Interpretation of Quantum Mechanics: 12. Quantum spacetime without observers: ontological clarity and the conceptual foundations of quantum gravity Sheldon Goldstein and Stefan Teufel; 13. On gravity's role in quantum state reduction Roger Penrose; 14. Why the quantum must yield to gravity Joy Christian.

Cotunneling Drag Effect in Coulomb-Coupled Quantum Dots.

PubMed

Keller, A J; Lim, J S; Sánchez, David; López, Rosa; Amasha, S; Katine, J A; Shtrikman, Hadas; Goldhaber-Gordon, D

2016-08-05

In Coulomb drag, a current flowing in one conductor can induce a voltage across an adjacent conductor via the Coulomb interaction. The mechanisms yielding drag effects are not always understood, even though drag effects are sufficiently general to be seen in many low-dimensional systems. In this Letter, we observe Coulomb drag in a Coulomb-coupled double quantum dot and, through both experimental and theoretical arguments, identify cotunneling as essential to obtaining a correct qualitative understanding of the drag behavior.

Probing structure and dynamics of DNA with 2-aminopurine: effects of local environment on fluorescence.

PubMed

Rachofsky, E L; Osman, R; Ross, J B

2001-01-30

2-Aminopurine (2AP) is an analogue of adenine that has been utilized widely as a fluorescence probe of protein-induced local conformational changes in DNA. Within a DNA strand, this fluorophore demonstrates characteristic decreases in quantum yield and emission decay lifetime that vary sensitively with base sequence, temperature, and helix conformation but that are accompanied by only small changes in emission wavelength. However, the molecular interactions that give rise to these spectroscopic changes have not been established. To develop a molecular model for interpreting the fluorescence measurements, we have investigated the effects of environmental polarity, hydrogen bonding, and the purine and pyrimidine bases of DNA on the emission energy, quantum yield, and intensity decay kinetics of 2AP in simple model systems. The effects of environmental polarity were examined in a series of solvents of varying dielectric constant, and hydrogen bonding was investigated in binary mixtures of water with 1,4-dioxane or N,N-dimethylformamide (DMF). The effects of the purine and pyrimidine bases were studied by titrating 2AP deoxyriboside (d2AP) with the nucleosides adenosine (rA), cytidine (rC), guanosine (rG), and deoxythymidine (dT), and the nucleoside triphosphates ATP and GTP in neutral aqueous solution. The nucleosides and NTPs each quench the fluorescence of d2AP by a combination of static (affecting only the quantum yield) and dynamic (affecting both the quantum yield and the lifetime, proportionately) mechanisms. The peak wavelength and shape of the emission spectrum are not altered by either of these effects. The static quenching is saturable and has half-maximal effect at approximately 20 mM nucleoside or NTP, consistent with an aromatic stacking interaction. The rate constant for dynamic quenching is near the diffusion limit for collisional interaction (k(q) approximately 2 x 10(9) M(-1) s(-1)). Neither of these effects varies significantly between the various nucleosides and NTPs studied. In contrast, hydrogen bonding with water was observed to have a negligible effect on the emission wavelength, fluorescence quantum yield, or lifetime of 2AP in either dioxane or DMF. In nonpolar solvents, the fluorescence lifetime and quantum yield decrease dramatically, accompanied by significant shifts in the emission spectrum to shorter wavelengths. However, these effects of polarity do not coincide with the observed emission wavelength-independent quenching of 2AP fluorescence in DNA. Therefore, we conclude that the fluorescence quenching of 2AP in DNA arises from base stacking and collisions with neighboring bases only but is insensitive to base-pairing or other hydrogen bonding interactions. These results implicate both structural and dynamic properties of DNA in quenching of 2AP and constitute a simple model within which the fluorescence changes induced by protein-DNA binding or other perturbations may be interpreted.

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.

[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.

Ensemble brightening and enhanced quantum yield in size-purified silicon nanocrystals

DOE PAGES

Miller, Joseph B.; Van Sickle, Austin R.; Anthony, Rebecca J.; ...

2012-07-18

Here, we report on the quantum yield, photoluminescence (PL) lifetime and ensemble photoluminescent stability of highly monodisperse plasma-synthesized silicon nanocrystals (SiNCs) prepared though density-gradient ultracentrifugation in mixed organic solvents. Improved size uniformity leads to a reduction in PL line width and the emergence of entropic order in dry nanocrystal films. We find excellent agreement with the anticipated trends of quantum confinement in nanocrystalline silicon, with a solution quantum yield that is independent of nanocrystal size for the larger fractions but decreases dramatically with size for the smaller fractions. We also find a significant PL enhancement in films assembled from themore » fractions, and we use a combination of measurement, simulation and modeling to link this ‘brightening’ to a temporally enhanced quantum yield arising from SiNC interactions in ordered ensembles of monodisperse nanocrystals. Using an appropriate excitation scheme, we exploit this enhancement to achieve photostable emission.« less

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(+).

Quantum efficiencies exceeding unity in amorphous silicon solar cells

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

Vanmaekelbergh, D.; Lagemaat, J. van de; Schropp, R.E.I.

1994-12-31

The experimental observation of internal quantum efficiencies above unity in crystalline silicon solar cells has brought up the question whether the generation of multiple electron/hole pairs has to be taken into consideration also in solar cells based on direct gap amorphous semiconductors. To study photogenerated carrier dynamics, the authors have applied Intensity Modulated Photocurrent Spectroscopy (IMPS) to hydrogenated amorphous silicon p-i-n solar cells. In the reverse voltage bias region at low illumination intensities it has been observed that the low frequency limit of the AC quantum yield Y increases significantly above unit with decreasing light intensity, indicating that more thanmore » one electron per photon is detected in the external circuit. This phenomenon can be explained by considering trapping and thermal emission of photogenerated carriers at intragap atmospheric dangling bond defect centers.« less

Field Extension of Real Values of Physical Observables in Classical Theory can Help Attain Quantum Results

NASA Astrophysics Data System (ADS)

Wang, Hai; Kumar, Asutosh; Cho, Minhyung; Wu, Junde

2018-04-01

Physical quantities are assumed to take real values, which stems from the fact that an usual measuring instrument that measures a physical observable always yields a real number. Here we consider the question of what would happen if physical observables are allowed to assume complex values. In this paper, we show that by allowing observables in the Bell inequality to take complex values, a classical physical theory can actually get the same upper bound of the Bell expression as quantum theory. Also, by extending the real field to the quaternionic field, we can puzzle out the GHZ problem using local hidden variable model. Furthermore, we try to build a new type of hidden-variable theory of a single qubit based on the result.

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.

In Search of the Perfect Photocage: Structure-Reactivity Relationships in meso-Methyl BODIPY Photoremovable Protecting Groups.

PubMed

Slanina, Tomáš; Shrestha, Pradeep; Palao, Eduardo; Kand, Dnyaneshwar; Peterson, Julie A; Dutton, Andrew S; Rubinstein, Naama; Weinstain, Roy; Winter, Arthur H; Klán, Petr

2017-10-25

A detailed investigation of the photophysical parameters and photochemical reactivity of meso-methyl BODIPY photoremovable protecting groups was accomplished through systematic variation of the leaving group (LG) and core substituents as well as substitutions at boron. Efficiencies of the LG release were evaluated using both steady-state and transient absorption spectroscopies as well as computational analyses to identify the optimal structural features. We find that the quantum yields for photorelease with this photocage are highly sensitive to substituent effects. In particular, we find that the quantum yields of photorelease are improved with derivatives with higher intersystem crossing quantum yields, which can be promoted by core heavy atoms. Moreover, release quantum yields are dramatically improved by boron alkylation, whereas alkylation in the meso-methyl position has no effect. Better LGs are released considerably more efficiently than poorer LGs. We find that these substituent effects are additive, for example, a 2,6-diiodo-B-dimethyl BODIPY photocage features quantum yields of 28% for the mediocre LG acetate and a 95% quantum yield of release for chloride. The high chemical and quantum yields combined with the outstanding absorption properties of BODIPY dyes lead to photocages with uncaging cross sections over 10 000 M -1 cm -1 , values that surpass cross sections of related photocages absorbing visible light. These new photocages, which absorb strongly near the second harmonic of an Nd:YAG laser (532 nm), hold promise for manipulating and interrogating biological and material systems with the high spatiotemporal control provided by pulsed laser irradiation, while avoiding the phototoxicity problems encountered with many UV-absorbing photocages. More generally, the insights gained from this structure-reactivity relationship may aid in the development of new highly efficient photoreactions.

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.

Near-Unity Internal Quantum Efficiency of Luminescent Silicon Nanocrystals with Ligand Passivation.

PubMed

Sangghaleh, Fatemeh; Sychugov, Ilya; Yang, Zhenyu; Veinot, Jonathan G C; Linnros, Jan

2015-07-28

Spectrally resolved photoluminescence (PL) decays were measured for samples of colloidal, ligand-passivated silicon nanocrystals. These samples have PL emission energies with peak positions in the range ∼1.4-1.8 eV and quantum yields of ∼30-70%. Their ensemble PL decays are characterized by a stretched-exponential decay with a dispersion factor of ∼0.8, which changes to an almost monoexponential character at fixed detection energies. The dispersion factors and decay rates for various detection energies were extracted from spectrally resolved curves using a mathematical approach that excluded the effect of homogeneous line width broadening. Since nonradiative recombination would introduce a random lifetime variation, leading to a stretched-exponential decay for an ensemble, we conclude that the observed monoexponential decay in size-selected ensembles signifies negligible nonradiative transitions of a similar strength to the radiative one. This conjecture is further supported as extracted decay rates agree with radiative rates reported in the literature, suggesting 100% internal quantum efficiency over a broad range of emission wavelengths. The apparent differences in the quantum yields can then be explained by a varying fraction of "dark" or blinking nanocrystals.

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.

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.

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.

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

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.

Ignorance is bliss: general and robust cancellation of decoherence via no-knowledge quantum feedback.

PubMed

Szigeti, Stuart S; Carvalho, Andre R R; Morley, James G; Hush, Michael R

2014-07-11

A "no-knowledge" measurement of an open quantum system yields no information about any system observable; it only returns noise input from the environment. Surprisingly, performing such a no-knowledge measurement can be advantageous. We prove that a system undergoing no-knowledge monitoring has reversible noise, which can be canceled by directly feeding back the measurement signal. We show how no-knowledge feedback control can be used to cancel decoherence in an arbitrary quantum system coupled to a Markovian reservoir that is being monitored. Since no-knowledge feedback does not depend on the system state or Hamiltonian, such decoherence cancellation is guaranteed to be general and robust, and can operate in conjunction with any other quantum control protocol. As an application, we show that no-knowledge feedback could be used to improve the performance of dissipative quantum computers subjected to local loss.

Optical Properties of CdSe/ZnS Nanocrystals

PubMed Central

Gaigalas, Adolfas K; DeRose, Paul; Wang, Lili; Zhang, Yu-Zhong

2014-01-01

Measurements are presented of the absorbance, fluorescence emission, fluorescence quantum yield, and fluorescence lifetime of CdSe/ZnS nanocrystals, also known as quantum dots (QDs). The study included three groups of nanocrystals whose surfaces were either passivated with organic molecules, modified further with carboxyl groups, or conjugated with CD14 mouse anti-human antibodies. The surface modifications had observable effects on the optical properties of the nanocrystals. The oscillator strength (OS) of the band edge transition was about 1.0 for the nanocrystals emitting at 565 nm, 605 nm, and 655 nm. The OS could not be determined for QDs with emission at 700 nm and 800 nm. The fluorescence lifetimes varied from 26 ns for nanocrystals emitting near 600 nm to 150 ns for nanocrystals emitting near 800 nm. The quantum yield ranged between 0.4 and 0.9 for the nanocrystals in this study. A brightness index (BI) was used to evaluate the suitability of the nanocrystal labels for flow cytometer measurements. Most QD labels are at least as bright as fluorescein for applications in flow cytometer assays with 488 nm excitation. For optimal brightness the QDs should be excited with 405 nm light. We observed a strong dependence of the QD absorbance at 250 nm on the surface modification of the QD. PMID:26601047

Combined atomic force microscopy and photoluminescence imaging to select single InAs/GaAs quantum dots for quantum photonic devices.

PubMed

Sapienza, Luca; Liu, Jin; Song, Jin Dong; Fält, Stefan; Wegscheider, Werner; Badolato, Antonio; Srinivasan, Kartik

2017-07-24

We report on a combined photoluminescence imaging and atomic force microscopy study of single, isolated self-assembled InAs quantum dots. The motivation of this work is to determine an approach that allows to assess single quantum dots as candidates for quantum nanophotonic devices. By combining optical and scanning probe characterization techniques, we find that single quantum dots often appear in the vicinity of comparatively large topographic features. Despite this, the quantum dots generally do not exhibit significant differences in their non-resonantly pumped emission spectra in comparison to quantum dots appearing in defect-free regions, and this behavior is observed across multiple wafers produced in different growth chambers. Such large surface features are nevertheless a detriment to applications in which single quantum dots are embedded within nanofabricated photonic devices: they are likely to cause large spectral shifts in the wavelength of cavity modes designed to resonantly enhance the quantum dot emission, thereby resulting in a nominally perfectly-fabricated single quantum dot device failing to behave in accordance with design. We anticipate that the approach of screening quantum dots not only based on their optical properties, but also their surrounding surface topographies, will be necessary to improve the yield of single quantum dot nanophotonic devices.

Luminescence properties of In(Zn)P alloy core/ZnS shell quantum dots

NASA Astrophysics Data System (ADS)

Thuy, Ung Thi Dieu; Reiss, Peter; Liem, Nguyen Quang

2010-11-01

Chemically synthesized InP/ZnS core/shell quantum dots (QDs) are studied using time-resolved photoluminescence spectroscopy and x-ray diffraction. Zinc stearate, which is added during the synthesis of the InP core, significantly improves the optical characteristics of the QDs. The luminescence quantum yield (QY) reaches 60%-70% and the emission is tunable from 485 to 586 nm by varying the Zn2+:In3+ molar ratio and growth temperature. The observed increased Stokes shift, luminescence decay time, and QY in the presence of Zn are rationalized by the formation of an In(Zn)P alloy structure that causes band-edge fluctuation to enhance the confinement of the excited carriers.

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

Quantum field theory of interacting dark matter and dark energy: Dark monodromies

DOE PAGES

D’Amico, Guido; Hamill, Teresa; Kaloper, Nemanja

2016-11-28

We discuss how to formulate a quantum field theory of dark energy interacting with dark matter. We show that the proposals based on the assumption that dark matter is made up of heavy particles with masses which are very sensitive to the value of dark energy are strongly constrained. Quintessence-generated long-range forces and radiative stability of the quintessence potential require that such dark matter and dark energy are completely decoupled. However, if dark energy and a fraction of dark matter are very light axions, they can have significant mixings which are radiatively stable and perfectly consistent with quantum field theory.more » Such models can naturally occur in multi-axion realizations of monodromies. The mixings yield interesting signatures which are observable and are within current cosmological limits but could be constrained further by future observations« less

Quantum field theory of interacting dark matter and dark energy: Dark monodromies

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

D’Amico, Guido; Hamill, Teresa; Kaloper, Nemanja

We discuss how to formulate a quantum field theory of dark energy interacting with dark matter. We show that the proposals based on the assumption that dark matter is made up of heavy particles with masses which are very sensitive to the value of dark energy are strongly constrained. Quintessence-generated long-range forces and radiative stability of the quintessence potential require that such dark matter and dark energy are completely decoupled. However, if dark energy and a fraction of dark matter are very light axions, they can have significant mixings which are radiatively stable and perfectly consistent with quantum field theory.more » Such models can naturally occur in multi-axion realizations of monodromies. The mixings yield interesting signatures which are observable and are within current cosmological limits but could be constrained further by future observations« less

Electro Optical Properties of Copolymer Blends: Lasing, Electroluminescence and Photophysics

DTIC Science & Technology

2006-04-15

conjugated main chain structures with high photoluminescent and electroluminescent quantum yields. The structures incorporated fluorene containing moieties...The systems studied focused on novel conjugated main chain structures with high photoluminescent and electroluminescent quantum yields. The structures...the quantum efficient fluorine group. The properties of segmented copolymers that incorporate fluorenes were compared to the homo-PPV type systems

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

A versatile method for the determination of photochemical quantum yields via online UV-Vis spectroscopy.

PubMed

Stadler, Eduard; Eibel, Anna; Fast, David; Freißmuth, Hilde; Holly, Christian; Wiech, Mathias; Moszner, Norbert; Gescheidt, Georg

2018-05-16

We have developed a simple method for determining the quantum yields of photo-induced reactions. Our setup features a fibre coupled UV-Vis spectrometer, LED irradiation sources, and a calibrated spectrophotometer for precise measurements of the LED photon flux. The initial slope in time-resolved absorbance profiles provides the quantum yield. We show the feasibility of our methodology for the kinetic analysis of photochemical reactions and quantum yield determination. The typical chemical actinometers, ferrioxalate and ortho-nitrobenzaldehyde, as well as riboflavin, a spiro-compound, phosphorus- and germanium-based photoinitiators for radical polymerizations and the frequently utilized photo-switch azobenzene serve as paradigms. The excellent agreement of our results with published data demonstrates the high potential of the proposed method as a convenient alternative to the time-consuming chemical actinometry.

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.

Optical characterization of Nd (3+):AgBr.

PubMed

Bunimovich, D; Nagli, L; Katzir, A

1997-10-20

The luminescence of silver bromide crystals, doped with neodymium, was investigated over the visible and near-infrared spectral ranges. The emission, excitation, and absorption spectra were measured over a broad temperature range. The absolute luminescence quantum yield was estimated by comparing the luminescence with that of a neodymium-doped phosphate glass, for which the manufacturer gives a value of 0.4. The Judd-Ofelt analysis was applied to both materials, and transition rates, branching ratios, and quantum efficiencies were calculated for all the observed bands. Good agreement was obtained between theory and experiment.

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.

Quantum localisation on the circle

NASA Astrophysics Data System (ADS)

Fresneda, Rodrigo; Gazeau, Jean Pierre; Noguera, Diego

2018-05-01

Covariant integral quantisation using coherent states for semi-direct product groups is implemented for the motion of a particle on the circle. In this case, the phase space is the cylinder, which is viewed as a left coset of the Euclidean group E(2). Coherent states issued from fiducial vectors are labeled by points in the cylinder and depend also on extra parameters. We carry out the corresponding quantisations of the basic classical observables, particularly the angular momentum and the 2π-periodic discontinuous angle function. We compute their corresponding lower symbols. The quantum localisation on the circle is examined through the properties of the angle operator yielded by our procedure, its spectrum and lower symbol, its commutator with the quantum angular momentum, and the resulting Heisenberg inequality. Comparison with other approaches to the long-standing question of the quantum angle is discussed.

Quantum theory as plausible reasoning applied to data obtained by robust experiments.

PubMed

De Raedt, H; Katsnelson, M I; Michielsen, K

2016-05-28

We review recent work that employs the framework of logical inference to establish a bridge between data gathered through experiments and their objective description in terms of human-made concepts. It is shown that logical inference applied to experiments for which the observed events are independent and for which the frequency distribution of these events is robust with respect to small changes of the conditions under which the experiments are carried out yields, without introducing any concept of quantum theory, the quantum theoretical description in terms of the Schrödinger or the Pauli equation, the Stern-Gerlach or Einstein-Podolsky-Rosen-Bohm experiments. The extraordinary descriptive power of quantum theory then follows from the fact that it is plausible reasoning, that is common sense, applied to reproducible and robust experimental data. © 2016 The Author(s).

The photolysis of NH3 in the presence of substituted acetylenes - A possible source of oligomers and HCN on Jupiter

NASA Technical Reports Server (NTRS)

Ferris, James P.; Jacobson, Richard R.; Guillemin, Jean C.

1992-01-01

An NMR spectral study is presently conducted of NH3 photolysis in the presence of substituted acetylenes with NMR spectra and gas chromatography. Quantum yields and percentage conversions to products are reported. It is shown that acetylenic hydrocarbons generated during methane photolysis in Jupiter's stratosphere can react with radicals formed by NH3 photolysis to yield nonvolatile, yellow-brown polymers, alkylnitriles, and in due course, HCN, as observed on Jupiter.

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.

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.

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.

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).

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.

Weak Measurement and Quantum Smoothing of a Superconducting Qubit

NASA Astrophysics Data System (ADS)

Tan, Dian

In quantum mechanics, the measurement outcome of an observable in a quantum system is intrinsically random, yielding a probability distribution. The state of the quantum system can be described by a density matrix rho(t), which depends on the information accumulated until time t, and represents our knowledge about the system. The density matrix rho(t) gives probabilities for the outcomes of measurements at time t. Further probing of the quantum system allows us to refine our prediction in hindsight. In this thesis, we experimentally examine a quantum smoothing theory in a superconducting qubit by introducing an auxiliary matrix E(t) which is conditioned on information obtained from time t to a final time T. With the complete information before and after time t, the pair of matrices [rho(t), E(t)] can be used to make smoothed predictions for the measurement outcome at time t. We apply the quantum smoothing theory in the case of continuous weak measurement unveiling the retrodicted quantum trajectories and weak values. In the case of strong projective measurement, while the density matrix rho(t) with only diagonal elements in a given basis |n〉 may be treated as a classical mixture, we demonstrate a failure of this classical mixture description in determining the smoothed probabilities for the measurement outcome at time t with both diagonal rho(t) and diagonal E(t). We study the correlations between quantum states and weak measurement signals and examine aspects of the time symmetry of continuous quantum measurement. We also extend our study of quantum smoothing theory to the case of resonance fluorescence of a superconducting qubit with homodyne measurement and observe some interesting effects such as the modification of the excited state probabilities, weak values, and evolution of the predicted and retrodicted trajectories.

Poly(vinylpyrrolidone) supported copper nanoclusters: glutathione enhanced blue photoluminescence for application in phosphor converted light emitting devices

NASA Astrophysics Data System (ADS)

Wang, Zhenguang; Susha, Andrei S.; Chen, Bingkun; Reckmeier, Claas; Tomanec, Ondrej; Zboril, Radek; Zhong, Haizheng; Rogach, Andrey L.

2016-03-01

Poly(vinylpyrrolidone) supported Cu nanoclusters were synthesized by reduction of Cu(ii) ions with ascorbic acid in water, and initially showed blue photoluminescence with a quantum yield of 8%. An enhancement of the emission quantum yield has been achieved by treatment of Cu clusters with different electron-rich ligands, with the most pronounced effect (photoluminescence quantum yield of 27%) achieved with glutathione. The bright blue emission of glutathione treated Cu NCs is fully preserved in the solid state powder, which has been combined with commercial green and red phosphors to fabricate down-conversion white light emitting diodes with a high colour rendering index of 92.Poly(vinylpyrrolidone) supported Cu nanoclusters were synthesized by reduction of Cu(ii) ions with ascorbic acid in water, and initially showed blue photoluminescence with a quantum yield of 8%. An enhancement of the emission quantum yield has been achieved by treatment of Cu clusters with different electron-rich ligands, with the most pronounced effect (photoluminescence quantum yield of 27%) achieved with glutathione. The bright blue emission of glutathione treated Cu NCs is fully preserved in the solid state powder, which has been combined with commercial green and red phosphors to fabricate down-conversion white light emitting diodes with a high colour rendering index of 92. Electronic supplementary information (ESI) available: The optical spectra of control experiments for Cu NC synthesis, optimization of the reaction conditions, and spectra for LEDs chips and blue LEDs. See DOI: 10.1039/c6nr00806b

Unbiased simulation of near-Clifford quantum circuits

DOE PAGES

Bennink, Ryan S.; Ferragut, Erik M.; Humble, Travis S.; ...

2017-06-28

Modeling and simulation are essential for predicting and verifying the behavior of fabricated quantum circuits, but existing simulation methods are either impractically costly or require an unrealistic simplification of error processes. In this paper, we present a method of simulating noisy Clifford circuits that is both accurate and practical in experimentally relevant regimes. In particular, the cost is weakly exponential in the size and the degree of non-Cliffordness of the circuit. Our approach is based on the construction of exact representations of quantum channels as quasiprobability distributions over stabilizer operations, which are then sampled, simulated, and weighted to yield unbiasedmore » statistical estimates of circuit outputs and other observables. As a demonstration of these techniques, we simulate a Steane [[7,1,3

Bounds on quantum communication via Newtonian gravity

NASA Astrophysics Data System (ADS)

Kafri, D.; Milburn, G. J.; Taylor, J. M.

2015-01-01

Newtonian gravity yields specific observable consequences, the most striking of which is the emergence of a 1/{{r}2} force. In so far as communication can arise via such interactions between distant particles, we can ask what would be expected for a theory of gravity that only allows classical communication. Many heuristic suggestions for gravity-induced decoherence have this restriction implicitly or explicitly in their construction. Here we show that communication via a 1/{{r}2} force has a minimum noise induced in the system when the communication cannot convey quantum information, in a continuous time analogue to Bell's inequalities. Our derived noise bounds provide tight constraints from current experimental results on any theory of gravity that does not allow quantum communication.

Growth patterns of self-assembled InAs quantum dots near the two-dimensional to three-dimensional transition

NASA Astrophysics Data System (ADS)

Colocci, M.; Bogani, F.; Carraresi, L.; Mattolini, R.; Bosacchi, A.; Franchi, S.; Frigeri, P.; Rosa-Clot, M.; Taddei, S.

1997-06-01

Self-assembled InAs quantum dots have been grown by molecular beam epitaxy in such a way as to obtain a continuous variation of InAs coverages across the wafer. Structured photoluminescence spectra are observed after excitation of a large number of dots; deconvolution into Gaussian components yields narrow emission bands (full width at half-maximum 20-30 meV) separated in energy by an average spacing of 30-40 meV. We ascribe the individual bands of the photoluminescence spectra after low excitation to families of dots with similar shapes and with heights differing by one monolayer, as strongly supported by numerical calculations of the fundamental electronic transitions in quantum dot structures.

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

A reductionist perspective on quantum statistical mechanics: Coarse-graining of path integrals

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

Sinitskiy, Anton V.; Voth, Gregory A., E-mail: gavoth@uchicago.edu

2015-09-07

Computational modeling of the condensed phase based on classical statistical mechanics has been rapidly developing over the last few decades and has yielded important information on various systems containing up to millions of atoms. However, if a system of interest contains important quantum effects, well-developed classical techniques cannot be used. One way of treating finite temperature quantum systems at equilibrium has been based on Feynman’s imaginary time path integral approach and the ensuing quantum-classical isomorphism. This isomorphism is exact only in the limit of infinitely many classical quasiparticles representing each physical quantum particle. In this work, we present a reductionistmore » perspective on this problem based on the emerging methodology of coarse-graining. This perspective allows for the representations of one quantum particle with only two classical-like quasiparticles and their conjugate momenta. One of these coupled quasiparticles is the centroid particle of the quantum path integral quasiparticle distribution. Only this quasiparticle feels the potential energy function. The other quasiparticle directly provides the observable averages of quantum mechanical operators. The theory offers a simplified perspective on quantum statistical mechanics, revealing its most reductionist connection to classical statistical physics. By doing so, it can facilitate a simpler representation of certain quantum effects in complex molecular environments.« less

A reductionist perspective on quantum statistical mechanics: Coarse-graining of path integrals.

PubMed

Sinitskiy, Anton V; Voth, Gregory A

2015-09-07

Computational modeling of the condensed phase based on classical statistical mechanics has been rapidly developing over the last few decades and has yielded important information on various systems containing up to millions of atoms. However, if a system of interest contains important quantum effects, well-developed classical techniques cannot be used. One way of treating finite temperature quantum systems at equilibrium has been based on Feynman's imaginary time path integral approach and the ensuing quantum-classical isomorphism. This isomorphism is exact only in the limit of infinitely many classical quasiparticles representing each physical quantum particle. In this work, we present a reductionist perspective on this problem based on the emerging methodology of coarse-graining. This perspective allows for the representations of one quantum particle with only two classical-like quasiparticles and their conjugate momenta. One of these coupled quasiparticles is the centroid particle of the quantum path integral quasiparticle distribution. Only this quasiparticle feels the potential energy function. The other quasiparticle directly provides the observable averages of quantum mechanical operators. The theory offers a simplified perspective on quantum statistical mechanics, revealing its most reductionist connection to classical statistical physics. By doing so, it can facilitate a simpler representation of certain quantum effects in complex molecular environments.

Super-Poissonian statistics of photon emission from single CdSe-CdS core-shell nanocrystals coupled to metal nanostructures.

PubMed

Park, Young-Shin; Ghosh, Yagnaseni; Chen, Yongfen; Piryatinski, Andrei; Xu, Ping; Mack, Nathan H; Wang, Hsing-Lin; Klimov, Victor I; Hollingsworth, Jennifer A; Htoon, Han

2013-03-15

We demonstrate that photon antibunching observed for individual nanocrystal quantum dots (NQDs) can be transformed into photon bunching characterized by super-Poissonian statistics when they are coupled to metal nanostructures (MNs). This observation indicates that, while the quantum yield of a biexciton (Q(2X)) is lower than that of a single exciton (Q(1X)) in freestanding NQDs, Q(2X) becomes greater than Q(1X) in NQDs coupled to MNs. This unique phenomenon is attributed to metal-induced quenching with a rate that scales more slowly with exciton multiplicity than the radiative decay rate and dominates over other nonradiative decay channels for both single excitons and biexcitons.

Photoluminescence of epoxy resin modified by carbazole and its halogen derivative at 82 K

NASA Astrophysics Data System (ADS)

Mandowska, E.; Mandowski, A.; Tsvirko, M.

2009-10-01

The spectra and relative quantum yield of fluorescence and phosphorescence were measured for 9-(2,3-epoxypropyl)carbazole (EPK) added to epoxy resin (R) (R 5EPK - 5% weight content of the carbazole group in a polymer) and its mono and dihalogen derivative (Cl and Br). The materials under study have excellent mechanical properties. At 82 K photoluminescence (PL) spectra of these materials are composed of fluorescence (FL) and phosphorescence (PH) components while at 280 K, PH component is not observed. The vibrational frequencies of fluorescence and phosphorescence for R 5EPK were determined using Gaussian deconvolution. A decrease in the fluorescence and an increase in the phosphorescence quantum efficiency were observed after chemical bonding of heavy atoms Cl and Br.

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...

Terahertz cascades from nanoparticles

NASA Astrophysics Data System (ADS)

Arnardottir, K. B.; Liew, T. C. H.

2018-05-01

In this article we propose a system capable of terahertz (THz) radiation with quantum yield above unity. The system consists of nanoparticles where the material composition varies along the radial direction of each nanoparticle in such a way that a ladder of equidistant energy levels emerges. By then exciting the highest level of this ladder we produce multiple photons of the same frequency in the THz range. We demonstrate how we can calculate a continuous material composition profile that achieves a high quantum yield and then show that a more experimentally friendly design of a multishell nanoparticle can still result in a high quantum yield.

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.

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

Nanomechanical motion measured with an imprecision below that at the standard quantum limit.

PubMed

Teufel, J D; Donner, T; Castellanos-Beltran, M A; Harlow, J W; Lehnert, K W

2009-12-01

Nanomechanical oscillators are at the heart of ultrasensitive detectors of force, mass and motion. As these detectors progress to even better sensitivity, they will encounter measurement limits imposed by the laws of quantum mechanics. If the imprecision of a measurement of the displacement of an oscillator is pushed below a scale set by the standard quantum limit, the measurement must perturb the motion of the oscillator by an amount larger than that scale. Here we show a displacement measurement with an imprecision below the standard quantum limit scale. We achieve this imprecision by measuring the motion of a nanomechanical oscillator with a nearly shot-noise limited microwave interferometer. As the interferometer is naturally operated at cryogenic temperatures, the thermal motion of the oscillator is minimized, yielding an excellent force detector with a sensitivity of 0.51 aN Hz(-1/2). This measurement is a critical step towards observing quantum behaviour in a mechanical object.

Microcanonical and resource-theoretic derivations of the thermal state of a quantum system with noncommuting charges

PubMed Central

Yunger Halpern, Nicole; Faist, Philippe; Oppenheim, Jonathan; Winter, Andreas

2016-01-01

The grand canonical ensemble lies at the core of quantum and classical statistical mechanics. A small system thermalizes to this ensemble while exchanging heat and particles with a bath. A quantum system may exchange quantities represented by operators that fail to commute. Whether such a system thermalizes and what form the thermal state has are questions about truly quantum thermodynamics. Here we investigate this thermal state from three perspectives. First, we introduce an approximate microcanonical ensemble. If this ensemble characterizes the system-and-bath composite, tracing out the bath yields the system's thermal state. This state is expected to be the equilibrium point, we argue, of typical dynamics. Finally, we define a resource-theory model for thermodynamic exchanges of noncommuting observables. Complete passivity—the inability to extract work from equilibrium states—implies the thermal state's form, too. Our work opens new avenues into equilibrium in the presence of quantum noncommutation. PMID:27384494

Why is gas phase 2-nitrophenol photolysis a potentially important source of OH radicals in the polluted atmosphere?

NASA Astrophysics Data System (ADS)

Zhu, L.

2017-12-01

2-Nitrophenol is an important component of "brown carbon" in the atmosphere. The concentration of 2-nitrophenol is higher in polluted urban areas where there are increased emissions of aromatic hydrocarbons. To assess the air quality impacts of pollutant emissions, it is important to understand the oxidant formation potential of the emitted species. Photolysis is the dominant atmospheric removal process for 2-nitrophenol. Although photodissociation dynamics studies of 2-nitrophenol have reported OH formation at photolysis wavelengths of 266 nm, 355 nm, and over the 361-390 nm range, and HONO has been observed as a product from 2-nitrophenol photolysis in an environmental chamber, the lack of quantitative absorption cross section and product quantum yield information has prevented quantitative assessment of the extent of oxidant formation from the photolysis of 2-nitrophenol in the atmosphere. My group determined the gas phase absorption cross sections of 2-nitrophenol in the 295-400 nm region by using cavity ring-down spectroscopy. The OH, HONO, and NO2 formation channels following the gas phase photolysis of 2-nitrophenol at 308 and 351 nm were investigated. Direct NO2 formation was not observed. OH and HONO were direct products from the 2-nitrophenol photolysis, and their quantum yields were obtained. The sum of the OH and the HONO quantum yields was about unity at both photolysis wavelengths. The estimated photolysis rate constant of 2-nitrophenol was about twice that of NO2. I will discuss the importance of 2-nitrophenol gas phase photolysis as a potential source of OH and HONO in regions of high anthropogenic emissions.

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.

Water-Assisted Size and Shape Control of CsPbBr3 Perovskite Nanocrystals.

PubMed

Zhang, Xiaoyu; Bai, Xue; Wu, Hua; Zhang, Xiangtong; Sun, Chun; Zhang, Yu; Zhang, Wei; Zheng, Weitao; Yu, William W; Rogach, Andrey L

2018-03-19

Lead-halide perovskites are well known to decompose rapidly when exposed to polar solvents, such as water. Contrary to this common-place observation, we have found that through introducing a suitable minor amount of water into the reaction mixture, we can synthesize stable CsPbBr 3 nanocrystals. The size and the crystallinity, and as a result the band gap tunability of the strongly emitting CsPbBr 3 nanocrystals correlate with the water content. Suitable amounts of water change the crystallization environment, inducing the formation of differently shaped perovskites, namely spherical NCs, rectangular nanoplatelets, or nanowires. Bright CsPbBr 3 nanocrystals with the photoluminescence quantum yield reaching 90 % were employed for fabrication of inverted hybrid inorganic/organic light-emitting devices, with the peak luminance of 4428 cd m -2 and external quantum yield of 1.7 %. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

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.

Kinetics of bacterial fluorescence staining with 3,3'-diethylthiacyanine.

PubMed

Thomas, Marlon S; Nuñez, Vicente; Upadhyayula, Srigokul; Zielins, Elizabeth R; Bao, Duoduo; Vasquez, Jacob M; Bahmani, Baharak; Vullev, Valentine I

2010-06-15

For more than a century, colorimetric and fluorescence staining have been the foundation of a broad range of key bioanalytical techniques. The dynamics of such staining processes, however, still remains largely unexplored. We investigated the kinetics of fluorescence staining of two gram-negative and two gram-positive species with 3,3'-diethylthiacyanine (THIA) iodide. An increase in the THIA fluorescence quantum yield, induced by the bacterial dye uptake, was the principal reason for the observed emission enhancement. The fluorescence quantum yield of THIA depended on the media viscosity and not on the media polarity, which suggested that the microenvironment of the dye molecules taken up by the cells was restrictive. The kinetics of fluorescence staining did not manifest a statistically significant dependence neither on the dye concentration, nor on the cell count. In the presence of surfactant additives, however, the fluorescence-enhancement kinetic patterns manifested species specificity with statistically significant discernibility.

Indirect absorption spectroscopy using quantum cascade lasers: mid-infrared refractometry and photothermal spectroscopy.

PubMed

Pfeifer, Marcel; Ruf, Alexander; Fischer, Peer

2013-11-04

We record vibrational spectra with two indirect schemes that depend on the real part of the index of refraction: mid-infrared refractometry and photothermal spectroscopy. In the former, a quantum cascade laser (QCL) spot is imaged to determine the angles of total internal reflection, which yields the absorption line via a beam profile analysis. In the photothermal measurements, a tunable QCL excites vibrational resonances of a molecular monolayer, which heats the surrounding medium and changes its refractive index. This is observed with a probe laser in the visible. Sub-monolayer sensitivities are demonstrated.

Photoluminescence spectroscopy and the effective mass theory of strained (In,Ga)As/GaAs heterostructures grown on (112)B GaAs substrates

NASA Technical Reports Server (NTRS)

Henderson, R. H.; Sun, D.; Towe, E.

1995-01-01

The photoluminescence characteristics of pseudomorphic In(0.19)Ga(0.81)As/GaAs quantum well structures grown on both the conventional (001) and the unconventional (112)B GaAs substrate are investigated. It is found that the emission spectra of the structures grown on the (112)B surface exhibit some spectral characteristics not observed on similar structures grown on the (001) surface. A spectral blue shift of the e yields hh1 transition with increasing optical pump intensity is observed for the quantum wells on the (112) surface. This shift is interpreted to be evidence of a strain-induced piezoelectric field. A second spectral feature located within the band gap of the In(0.19)Ga(0.81)As layer is also observed for the (112) structure; this feature is thought to be an impurity-related emission. The expected transition energies of the quantum well structures are calculated using the effective mass theory based on the 4 x 4 Luttinger valence band Hamiltonian, and related strain Hamiltonian.

The energy dependence of CO(v,J) produced from H2CO via the transition state, roaming, and triple fragmentation channels.

PubMed

Quinn, Mitchell S; Andrews, Duncan U; Nauta, Klaas; Jordan, Meredith J T; Kable, Scott H

2017-07-07

The dynamics of CO production from photolysis of H 2 CO have been explored over a 8000 cm -1 energy range (345 nm-266 nm). Two-dimensional ion imaging, which simultaneously measures the speed and angular momentum distribution of a photofragment, was used to characterise the distribution of rotational and translational energy and to quantify the branching fraction of roaming, transition state (TS), and triple fragmentation (3F) pathways. The rotational distribution for the TS channel broadens significantly with increasing energy, while the distribution is relatively constant for the roaming channel. The branching fraction from roaming is also relatively constant at 20% of the observed CO. Above the 3F threshold, roaming decreases in favour of triple fragmentation. Combining the present data with our previous study on the H-atom branching fractions and published quantum yields for radical and molecular channels, absolute quantum yields were determined for all five dissociation channels for the entire S 1 ←S 0 absorption band, covering almost 8000 cm -1 of excitation energy. The S 0 radical and TS molecular channels are the most important over this energy range. The absolute quantum yield of roaming is fairly constant ∼5% at all energies. The T 1 radical channel is important (20%-40%) between 1500 and 4000 cm -1 above the H + HCO threshold, but becomes unimportant at higher energy. Triple fragmentation increases rapidly above its threshold reaching a maximum of 5% of the total product yield at the highest energy.

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.

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.

The photolysis of chlorine in the presence of ozone, nitric acid and nitrogen dioxide

NASA Technical Reports Server (NTRS)

Stuper, W. W.

1979-01-01

The following three systems were investigated: the Cl2-O3 system, the Cl2-O2-NO system and the Cl2-NO2-M system. In the first system, the reaction between ClO and O3, the reaction between OClO and O3, and the mechanism of the Cl2-O3 system were studied. In the second system, the reaction between ClOO and NO was investigated. In the last system, the reaction between Cl and NO2 was investigated as well as the kinetics of the chemiluminescence of the Cl-NO2-O3 reaction. In the first system, Cl2 was photolyzed at 366 nm in the presence of O3 within the temperature range 254-297 K. O3 was removed with quantum yields of 5.8 + or - 0.5, 4.0 + or - 0.3, 2.9 + or - 0.3 and 1.9 + or - 0.2 at 297, 283, 273, and 252 K respectively, invariant to changes in the initial O3 or Cl2 concentration, the extent of conversion or the absorbed intensity, I sub a. The addition of nitrogen had no effect on -phi(03). The Cl2 removal quantum yields were 0.11 + or - 0.02 at 297 K for Cl2 conversions of about 30%, much higher than expected from mass balance considerations based on the initial quantum yield of 0.089 + or - 0.013 for OClO formation at 297 K. The final chlorine-containing product was Cl2O7. It was produced at least in part through the formation of OClO as an intermediate which was also observed with an initial quantum yield of phi sub i(OClO) = 2500 exp(-(3025 + or - 625)/T) independent of (O3) or I sub a.

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.

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.

Quantum theory of the far-off-resonance continuous-wave Raman laser: Heisenberg-Langevin approach

NASA Astrophysics Data System (ADS)

Roos, P. A.; Murphy, S. K.; Meng, L. S.; Carlsten, J. L.; Ralph, T. C.; White, A. G.; Brasseur, J. K.

2003-07-01

We present the quantum theory of the far-off-resonance continuous-wave Raman laser using the Heisenberg-Langevin approach. We show that the simplified quantum Langevin equations for this system are mathematically identical to those of the nondegenerate optical parametric oscillator in the time domain with the following associations: pump ↔ pump, Stokes ↔ signal, and Raman coherence ↔ idler. We derive analytical results for both the steady-state behavior and the time-dependent noise spectra, using standard linearization procedures. In the semiclassical limit, these results match with previous purely semiclassical treatments, which yield excellent agreement with experimental observations. The analytical time-dependent results predict perfect photon statistics conversion from the pump to the Stokes and nonclassical behavior under certain operational conditions.

Triplet and ground state potential energy surfaces of 1,4-diphenyl-1,3-butadiene: theory and experiment.

PubMed

Saltiel, J; Dmitrenko, O; Pillai, Z S; Klima, R; Wang, S; Wharton, T; Huang, Z-N; van de Burgt, L J; Arranz, J

2008-05-01

Relative energies of the ground state isomers of 1,4-diphenyl-1,3-butadiene (DPB) are determined from the temperature dependence of equilibrium isomer compositions obtained with the use of diphenyl diselenide as catalyst. Temperature and concentration effects on photostationary states and isomerization quantum yields with biacetyl or fluorenone as triplet sensitizers with or without the presence of O(2), lead to significant modification of the proposed DPB triplet potential energy surface. Quantum yields for ct-DPB formation from tt-DPB increase with [tt-DPB] revealing a quantum chain process in the tt --> ct direction, as had been observed for the ct --> tt direction, and suggesting an energy minimum at the (3)ct* geometry. They confirm the presence of planar and twisted isomeric triplets in equilibrium (K), with energy transfer from planar or quasi-planar geometries (quantum chain events from tt and ct triplets) and unimolecular decay (k(d)) from twisted geometries. Starting from cc-DPB, varphi(cc-->tt) increases with increasing [cc-DPB] whereas varphi(cc-->ct) is relatively insensitive to concentration changes. The concentration and temperature dependencies of the decay rate constants of DPB triplets in cyclohexane are consistent with the mechanism deduced from the photoisomerization quantum yields. The experimental DeltaH between (3)tt-DPB* and (3)tp-DPB*, 2.7 kcal mol(-1), is compared with the calculated energy difference [DFT with B3LYP/6-31+G(d,p) basis set]. Use of the calculated DeltaS = 4.04 eu between the two triplets gives k(d) = (2.4-6.4) x 10(7) s(-1), close to 1.70 x 10(7) s(-1), the value for twisted stilbene triplet decay. Experimental and calculated relative energies of DPB isomers on the ground and triplet state surfaces agree and theory is relied upon to deduce structural characteristics of the equilibrated conformers in the DPB triplet state.

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%.

Silicon Nanoparticles with Surface Nitrogen: 90% Quantum Yield with Narrow Luminescence Bandwidth and the Ligand Structure Based Energy Law.

PubMed

Li, Qi; Luo, Tian-Yi; Zhou, Meng; Abroshan, Hadi; Huang, Jingchun; Kim, Hyung J; Rosi, Nathaniel L; Shao, Zhengzhong; Jin, Rongchao

2016-09-27

Silicon nanoparticles (NPs) have been widely accepted as an alternative material for typical quantum dots and commercial organic dyes in light-emitting and bioimaging applications owing to silicon's intrinsic merits of least toxicity, low cost, and high abundance. However, to date, how to improve Si nanoparticle photoluminescence (PL) performance (such as ultrahigh quantum yield, sharp emission peak, high stability) is still a major issue. Herein, we report surface nitrogen-capped Si NPs with PL quantum yield up to 90% and narrow PL bandwidth (full width at half-maximum (fwhm) ≈ 40 nm), which can compete with commercial dyes and typical quantum dots. Comprehensive studies have been conducted to unveil the influence of particle size, structure, and amount of surface ligand on the PL of Si NPs. Especially, a general ligand-structure-based PL energy law for surface nitrogen-capped Si NPs is identified in both experimental and theoretical analyses, and the underlying PL mechanisms are further discussed.

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.

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.

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...

Cellular interaction influenced by surface modification strategies of gelatin-based nanoparticles.

PubMed

Tse, Wai Hei; Gyenis, Laszlo; Litchfield, David W; Zhang, Jin

2017-02-01

Theranostic applications of gelatin nanospheres require two major components, a method of detection and good biocompatibility. We characterized the response of UTA-6 human osteosarcoma cells to the introduction of functionalized 90 bloom-based gelatin nanospheres (158 ± 49 nm) modified with three elements in different order: (a) hybridization with cadmium-based quantum dots for optical detection, (b) bioconjugation with anti-human IgG FAB (anti-IgG) for cell targeting, with/without (c) capping with polyethylene glycol on the surface for enhanced biocompatibility. A one-pot process is developed for incorporating quantum dots and antibody with gelatin nanospheres. Path A of modifying gelatin nanospheres with quantum dots first followed by anti-IgG resulted in a significantly greater cellular viability than Path B with anti-IgG first followed by quantum dots. Capping with polyethylene glycol as the final step in modification yielded significantly opposing results with decreases in Path A and increases in Path B. Three-dimensional z-stacking fluorescent images of hybrid gelatin nanospheres with anti-IgG is observed to have an increase in cellular association. The observed results suggest the modification order for building hybrid nanospheres may have an impact on cellular response.

Photodissociation of pernitric acid (HO2NO2) at 248 nm

NASA Technical Reports Server (NTRS)

Macleod, Helene; Smith, Gregory P.; Golden, David M.

1989-01-01

The photodissociation of pernitric acid (PNA) was studied at 248 nm. The quantum yield for production of OH radicals is 34 + or - 16 percent. The yield of OH from PNA was measured relative to that of H2O2. The translational and rotational energy content of the OH photofragment from PNA was characterized. A fluorescent emission was also observed and characterized. It is attributed to electronically excited NO2 produced in the PNA photodissociation. A maximum yield of 30 percent for NO2 production was determined. The intensity of this emission, and a mass spectrometric peak at m/e = 33, were found to be useful means of characterizing the purity of the PNA sample.

Quantum Criticality and Black Holes

ScienceCinema

Sachdev, Subir [Harvard University, Cambridge, Massachusetts, United States

2017-12-09

I will describe the behavior of a variety of condensed matter systems in the vicinity of zero temperature quantum phase transitions. There is a remarkable analogy between the hydrodynamics of such systems and the quantum theory of black holes. I will show how insights from this analogy have shed light on recent experiments on the cuprate high temperature superconductors. Studies of new materials and trapped ultracold atoms are yielding new quantum phases, with novel forms of quantum entanglement. Some materials are of technological importance: e.g. high temperature superconductors. Exact solutions via black hole mapping have yielded first exact results for transport coefficients in interacting many-body systems, and were valuable in determining general structure of hydrodynamics. Theory of VBS order and Nernst effect in cuprates. Tabletop 'laboratories for the entire universe': quantum mechanics of black holes, quark-gluon plasma, neutrons stars, and big-bang physics.

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.

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

Enhanced Fluorescence Properties of Carbon Dots in Polymer Films

PubMed Central

Liu, Yamin; Wang, Ping; Shiral Fernando, K. A.; LeCroy, Gregory E.; Maimaiti, Halidan; Harruff-Miller, Barbara A.; Lewis, William K.; Bunker, Christopher E.; Hou, Zhi-Ling; Sun, Ya-Ping

2016-01-01

Carbon dots of small carbon nanoparticles surface-functionalized with 2,2′-(ethylenedioxy)bis(ethylamine) (EDA) were synthesized, and the as-synthesized sample was separated on an aqueous gel column to obtain fractions of the EDA-carbon dots with different fluorescence quantum yields. As already discussed in the literature, the variations in fluorescence performance among the fractions were attributed to the different levels and/or effectiveness of the surface functionalization-passivation in the carbon dots. These fractions, as well as carbon nanoparticles without any deliberate surface functionalization, were dispersed into poly(vinyl alcohol) (PVA) for composite films. In the PVA film matrix, the carbon dots and nanoparticles exhibited much enhanced fluorescence emissions in comparison with their corresponding aqueous solutions. The increased fluorescence quantum yields in the films were determined quantitatively by using a specifically designed and constructed film sample holder in the emission spectrometer. The observed fluorescence decays of the EDA-carbon dots in film and in solution were essentially the same, suggesting that the significant enhancement in fluorescence quantum yields from solution to film is static in nature. Mechanistic implications of the results, including a rationalization in terms of the compression effect on the surface passivation layer (similar to a soft corona) in carbon dots when embedded in the more restrictive film environment resulting in more favorable radiative recombinations of the carbon particle surface-trapped electrons and holes, and also potential technological applications of the brightly fluorescent composite films are highlighted and discussed. PMID:28133537

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 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.

Tailoring the Energy Landscape in Quasi-2D Halide Perovskites Enables Efficient Green-Light Emission.

PubMed

Quan, Li Na; Zhao, Yongbiao; García de Arquer, F Pelayo; Sabatini, Randy; Walters, Grant; Voznyy, Oleksandr; Comin, Riccardo; Li, Yiying; Fan, James Z; Tan, Hairen; Pan, Jun; Yuan, Mingjian; Bakr, Osman M; Lu, Zhenghong; Kim, Dong Ha; Sargent, Edward H

2017-06-14

Organo-metal halide perovskites are a promising platform for optoelectronic applications in view of their excellent charge-transport and bandgap tunability. However, their low photoluminescence quantum efficiencies, especially in low-excitation regimes, limit their efficiency for light emission. Consequently, perovskite light-emitting devices are operated under high injection, a regime under which the materials have so far been unstable. Here we show that, by concentrating photoexcited states into a small subpopulation of radiative domains, one can achieve a high quantum yield, even at low excitation intensities. We tailor the composition of quasi-2D perovskites to direct the energy transfer into the lowest-bandgap minority phase and to do so faster than it is lost to nonradiative centers. The new material exhibits 60% photoluminescence quantum yield at excitation intensities as low as 1.8 mW/cm 2 , yielding a ratio of quantum yield to excitation intensity of 0.3 cm 2 /mW; this represents a decrease of 2 orders of magnitude in the excitation power required to reach high efficiency compared with the best prior reports. Using this strategy, we report light-emitting diodes with external quantum efficiencies of 7.4% and a high luminescence of 8400 cd/m 2 .

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

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.

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.

Carrier multiplication detected through transient photocurrent in device-grade films of lead selenide quantum dots

DOE PAGES

Gao, Jianbo; Fidler, Andrew F.; Klimov, Victor I.

2015-09-08

In carrier multiplication, the absorption of a single photon results in two or more electron–hole pairs. Quantum dots are promising materials for implementing carrier multiplication principles in real-life technologies. So far, however, most of research in this area has focused on optical studies of solution samples with yet to be proven relevance to practical devices. We report ultra-fast electro-optical studies of device-grade films of electronically coupled quantum dots that allow us to observe multiplication directly in the photocurrent. Our studies help rationalize previous results from both optical spectroscopy and steady-state photocurrent measurements and also provide new insights into effects ofmore » electric field and ligand treatments on multiexciton yields. Importantly, we demonstrate that using appropriate chemical treatments of the films, extra charges produced by carrier multiplication can be extracted from the quantum dots before they are lost to Auger recombination and hence can contribute to photocurrent of practical devices.« less

Carrier multiplication detected through transient photocurrent in device-grade films of lead selenide quantum dots

PubMed Central

Gao, Jianbo; Fidler, Andrew F.; Klimov, Victor I.

2015-01-01

In carrier multiplication, the absorption of a single photon results in two or more electron–hole pairs. Quantum dots are promising materials for implementing carrier multiplication principles in real-life technologies. So far, however, most of research in this area has focused on optical studies of solution samples with yet to be proven relevance to practical devices. Here we report ultrafast electro-optical studies of device-grade films of electronically coupled quantum dots that allow us to observe multiplication directly in the photocurrent. Our studies help rationalize previous results from both optical spectroscopy and steady-state photocurrent measurements and also provide new insights into effects of electric field and ligand treatments on multiexciton yields. Importantly, we demonstrate that using appropriate chemical treatments of the films, extra charges produced by carrier multiplication can be extracted from the quantum dots before they are lost to Auger recombination and hence can contribute to photocurrent of practical devices. PMID:26345390

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

McNeill, Jason Douglas

Electronic states of a thin layer of material on a surface possess unique physical and chemical properties. Some of these properties arise from the reduced dimensionality of the thin layer with respect to the bulk or the properties of the electric field where two materials of differing dielectric constants meet at an interface. Other properties are related to the nature of the surface chemical bond. Here, the properties of excess electrons in thin layers of Xenon, Krypton, and alkali metals are investigated, and the bound state energies and effective masses of the excess electrons are determined using two-photon photoemission. Formore » Xenon, the dependence of bound state energy, effective mass, and lifetime on layer thickness from one to nine layers is examined. Not all quantities were measured at each coverage. The two photon photoemission spectra of thin layers of Xenon on a Ag(111) substrate exhibit a number of sharp, well-defined peaks. The binding energy of the excess electronic states of Xenon layers exhibited a pronounced dependence on coverage. A discrete energy shift was observed for each additional atomic layer. At low coverage, a series of states resembling a Rydberg series is observed. This series is similar to the image state series observed on clean metal surfaces. Deviations from image state energies can be described in terms of the dielectric constant of the overlayer material and its effect on the image potential. For thicker layers of Xe (beyond the first few atomic layers), the coverage dependence of the features begins to resemble that of quantum well states. Quantum well states are related to bulk band states. However, the finite thickness of the layer restricts the perpendicular wavevector to a discrete set of values. Therefore, the spectrum of quantum well states contains a series of peaks which correspond to the various allowed values of the perpendicular wavevector. Analysis of the quantum well spectrum yields electronic band structure information. In this case, the quantum well states examined are derived from the Xenon conduction band. Measurements of the energies as a function of coverage yield the dispersion along the axis perpendicular to the surface while angle-resolved two-photon photoemission measurements yield information about dispersion along the surface parallel. The relative importance of the image potential and the overlayer band structure also depends on the quantum number and energy of the state. Some members of the image series may have an energy which is in an energy gap of the layer material, therefore such states may tend to remain physically outside the layer and retain much of their image character even at higher coverages. This is the case for the n = 1 image state of the Xe/Ag(111) system. The energies of image states which are excluded from the layer have a complex dependence on the thickness of the layer and its dielectric constant. The population decay kinetics of excited electronic states of the layer were also determined. Lifetimes are reported for the first three excited states for 1-6 atomic layers of Xe on Ag(111). As the image states evolve into quantum well states with increasing coverage, the lifetimes undergo an oscillation which marks a change in the spatial extent of the state. For example, the n = 2 quantum well state decreases substantially at 3-5 layers as the electron probability density in the layer increases. The lifetime data are modeled by extending the two-band nearly-free-electron approximation to account for the insulating Xe layer.« less

Stringent and efficient assessment of boson-sampling devices.

PubMed

Tichy, Malte C; Mayer, Klaus; Buchleitner, Andreas; Mølmer, Klaus

2014-07-11

Boson sampling holds the potential to experimentally falsify the extended Church-Turing thesis. The computational hardness of boson sampling, however, complicates the certification that an experimental device yields correct results in the regime in which it outmatches classical computers. To certify a boson sampler, one needs to verify quantum predictions and rule out models that yield these predictions without true many-boson interference. We show that a semiclassical model for many-boson propagation reproduces coarse-grained observables that are proposed as witnesses of boson sampling. A test based on Fourier matrices is demonstrated to falsify physically plausible alternatives to coherent many-boson propagation.

Torus as phase space: Weyl quantization, dequantization, and Wigner formalism

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

Ligabò, Marilena, E-mail: marilena.ligabo@uniba.it

2016-08-15

The Weyl quantization of classical observables on the torus (as phase space) without regularity assumptions is explicitly computed. The equivalence class of symbols yielding the same Weyl operator is characterized. The Heisenberg equation for the dynamics of general quantum observables is written through the Moyal brackets on the torus and the support of the Wigner transform is characterized. Finally, a dequantization procedure is introduced that applies, for instance, to the Pauli matrices. As a result we obtain the corresponding classical symbols.

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.

The source of stratospheric NO and N2O

NASA Technical Reports Server (NTRS)

Slanger, T. G.

1984-01-01

The photodissociation of O3 was investigated as a possible sources of N2O production in the stratosphere. Photolysis was conducted at 1576 A to generate the excited O2 states that react with N2 to form N2O. At this wavelength, there is a quantum yield of two for prompt production of oygen atoms, which is a consequence of the existence of two photodissociative channels giving comparable yields. One of these channels gives O(D1) and O2(b1sigma(+)subg), with a quantum yield of 0.6, whereas the other results in fragmentation of the O3, with production of three ground state oxygen atoms. The O2(b) is generated with vibrational excitation, and there are comparable populations in levels O to 3. These observations are the first to show O2(b) production from any photodissociative process, and were made under conditions in which the kinetics of vibrationally excited O2(b) can be studied. It appears that O3 photodissociation at 1576 A is not a good system for generating the higher electronic states of O2; it is likely that better results will be obtained at 1930 A.

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.

Analytical pair correlations in ideal quantum gases: temperature-dependent bunching and antibunching.

PubMed

Bosse, J; Pathak, K N; Singh, G S

2011-10-01

The fluctuation-dissipation theorem together with the exact density response spectrum for ideal quantum gases has been utilized to yield a new expression for the static structure factor, which we use to derive exact analytical expressions for the temperature-dependent pair distribution function g(r) of the ideal gases. The plots of bosonic and fermionic g(r) display "Bose pile" and "Fermi hole" typically akin to bunching and antibunching as observed experimentally for ultracold atomic gases. The behavior of spin-scaled pair correlation for fermions is almost featureless, but bosons show a rich structure including long-range correlations near T(c). The coherent state at T=0 shows no correlation at all, just like single-mode lasers. The depicted decreasing trend in correlation with decrease in temperature for T

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.

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.

Photophysical properties of fluorescently-labeled peptoids.

PubMed

Rudat, Birgit; Birtalan, Esther; Vollrath, Sidonie B L; Fritz, Daniel; Kölmel, Dominik K; Nieger, Martin; Schepers, Ute; Müllen, Klaus; Eisler, Hans-Jürgen; Lemmer, Uli; Bräse, Stefan

2011-09-01

Fluorescently-labeled biomolecules are often utilized in biochemical or cellular experiments without further detailed spectroscopical characterization. This report is intended to narrow this gap and therefore presents the photophysical investigation of a library of 17 fluorescently-labeled molecules, namely peptoid transporters. First, one peptoid structure is labeled with seven different fluorophores and the spectroscopical properties are examined. Absorption and fluorescence maxima are almost identical for free dyes and conjugated dyes, suggesting free choice of a spectrally suitable fluorophore for different applications. Otherwise, extinction coefficients and quantum yields, and therefore the brightness of all seven dyes are strongly influenced. For the fluorophores, e.g. rhodamine B, the extent of this influence depends on the peptoid itself. This is shown by comparing different structures in the second part of this report. Especially the side chain functionalities influence the brightness. And finally, peptoids having two identical fluorescent labels are presented, which show decreased quantum yields. Possible reasons for the observed photophysical properties are discussed. Copyright © 2011 Elsevier Masson SAS. All rights reserved.

Energy-Conversion Properties of Vapor-Liquid-Solid-Grown Silicon Wire-Array Photocathodes

NASA Astrophysics Data System (ADS)

Boettcher, Shannon W.; Spurgeon, Joshua M.; Putnam, Morgan C.; Warren, Emily L.; Turner-Evans, Daniel B.; Kelzenberg, Michael D.; Maiolo, James R.; Atwater, Harry A.; Lewis, Nathan S.

2010-01-01

Silicon wire arrays, though attractive materials for use in photovoltaics and as photocathodes for hydrogen generation, have to date exhibited poor performance. Using a copper-catalyzed, vapor-liquid-solid-growth process, SiCl4 and BCl3 were used to grow ordered arrays of crystalline p-type silicon (p-Si) microwires on p+-Si(111) substrates. When these wire arrays were used as photocathodes in contact with an aqueous methyl viologen2+/+ electrolyte, energy-conversion efficiencies of up to 3% were observed for monochromatic 808-nanometer light at fluxes comparable to solar illumination, despite an external quantum yield at short circuit of only 0.2. Internal quantum yields were at least 0.7, demonstrating that the measured photocurrents were limited by light absorption in the wire arrays, which filled only 4% of the incident optical plane in our test devices. The inherent performance of these wires thus conceptually allows the development of efficient photovoltaic and photoelectrochemical energy-conversion devices based on a radial junction platform.

Energy-conversion properties of vapor-liquid-solid-grown silicon wire-array photocathodes.

PubMed

Boettcher, Shannon W; Spurgeon, Joshua M; Putnam, Morgan C; Warren, Emily L; Turner-Evans, Daniel B; Kelzenberg, Michael D; Maiolo, James R; Atwater, Harry A; Lewis, Nathan S

2010-01-08

Silicon wire arrays, though attractive materials for use in photovoltaics and as photocathodes for hydrogen generation, have to date exhibited poor performance. Using a copper-catalyzed, vapor-liquid-solid-growth process, SiCl4 and BCl3 were used to grow ordered arrays of crystalline p-type silicon (p-Si) microwires on p+-Si(111) substrates. When these wire arrays were used as photocathodes in contact with an aqueous methyl viologen(2+/+) electrolyte, energy-conversion efficiencies of up to 3% were observed for monochromatic 808-nanometer light at fluxes comparable to solar illumination, despite an external quantum yield at short circuit of only 0.2. Internal quantum yields were at least 0.7, demonstrating that the measured photocurrents were limited by light absorption in the wire arrays, which filled only 4% of the incident optical plane in our test devices. The inherent performance of these wires thus conceptually allows the development of efficient photovoltaic and photoelectrochemical energy-conversion devices based on a radial junction platform.

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.

Solvatochromic fluorescence characteristics of cinnamoyl pyrone derivatives

NASA Astrophysics Data System (ADS)

Benosmane, Nadjib; Boutemeur, Baya; Hamdi, Safouane M.; Hamdi, Maamar; Silva, Artur S. M.

2017-12-01

The solvatochromic fluorescence behavior of cinnamoyl pyrone derivatives has been studied in several polar and non-polar solvents. The fluorescence spectra of these compounds exhibit red shift from its absorption spectra and present an excellent correlation with solvent polarity. Cinnamoyl pyrones show a significant spectral shift in fluorescence emission as a function of water composition in binary aqueous solutions mixture. This change is due to the specific intermolecular hydrogen bonding of cinnamoyl pyrones with a molecules of water, due to the deactivation of the lowest excited singlet state of these compounds. The relative quantum yields are calculated. It is found that the quantum yields of the cinnamoyl pyrones vary with the change in the solvent polarity indicating the dependency of fluorescence properties on the solvent nature. It has been observed that the addition of water and pH medium can affect the fluorescence properties of cinnamoyl pyrones in ethanol. This study exhibited that due to the solvent sensitive emission, cinnamoyl pyrone derivatives are a good compound to be used as fluorescence probes.

Formation of hemoglobin photoproduct is responsible for two-photon and single photon-excited fluorescence of red blood cells

NASA Astrophysics Data System (ADS)

Shirshin, Evgeny A.; Yakimov, Boris P.; Rodionov, Sergey A.; Omelyanenko, Nikolai P.; Priezzhev, Alexander V.; Fadeev, Victor V.; Lademann, Juergen; Darvin, Maxim E.

2018-07-01

Two-photon excited fluorescence of red blood cells (RBC) has been reported to be applicable for their assessment in vitro and in vivo. The corresponding fluorescence emission was ascribed to hemoglobin (Hb), however, as Hb is essentially non-fluorescent at single-photon excitation, the mechanism of two-photon excited fluorescence of RBC remains debatable. Here we show that a fluorescent photoproduct, characterized by an ultrafast decay of excitation, is formed after irradiation of Hb with femtosecond laser pulses with ca. 8 · 10‑5 quantum yield, and that it is also fluorescent at single-photon excitation. The formation of a similar photoproduct was also shown for Hb continuous wave irradiation with blue light with ca. 10‑5 formation quantum yield. The kinetics of the Hb photoproduct formation and its spectral properties were investigated. The obtained results clarify the processes responsible for RBC fluorescence observed in two-photon microscopy experiments.

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.

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.

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.

[Effects of light intensity on growth and photosynthetic characteristics of Tulipa edulis].

PubMed

Xu, Hongjian; Zhu, Zaibiao; Guo, Qiaosheng; Wu, Zhengjun; Ma, Hongliang; Miao, Yuanyuan

2012-02-01

Present study was conducted to explore the growth and photosynthetic characteristics of Tulipa edulis under different light conditions (23%, 45%, 63%, 78%, 100% of full sunlight) and to determine the optimum light intensity for growth of T. edulis. The leaf area and biomass indicators as well as reproductive characteristics were measured. The photosynthetic basic parameters and light response curve were determined by a LI-6400XT portable photosynthesis system, and the light response curve characteristic parameters was determined. Additionally, chlorophyll fluorescence parameters were determined by assorted fluorescence leaf chamber of LI-6400XT. The lowest biomass yield was observed in the 23% and 100% of full sunlight treatments while the highest value was found under the 78% of full sunlight conditions. With the reduction of light availability, the success rate of sexual reproduction, light saturation point (LSP) and light compensation point (LCP) reduced, while apparent quantum yield (AQY) increased. 23% and 45% of full sunlight treatments led to lower photosynthesis rate (Pn) and higher apparent quantum yield (AQY) in comparison with other treatents. The highest photosynthesis rate was observed in the 78% and 100% of full sunlight treatments. In addition, 78% of full sunlight treatments led to highest Fv/Fm, Fv'/Fm', PhiPS II, ETR, and qP. T. edulis was able to adapt in a wide range of light intensity, and 78% of full sunlinght was the most suitable light condition for growth of T. edulis.

Quantum partner-dance in the 12C + 12C system yields sub-Coulomb fusion resonances

NASA Astrophysics Data System (ADS)

Diaz-Torres, Alexis; Wiescher, Michael

2014-03-01

A preliminary study of the 12C + 12C sub-Coulomb fusion reaction using the time-dependent wave-packet method is presented. The theoretical sub-Coulomb fusion resonances seem to correspond well with observations. The present method might be a more suitable tool for expanding the cross-section predictions towards lower energies than the commonly used potential-model approximation.

Specific interactions of alcohols and non-alcohols with a biologically active boronic acid derivative: a spectroscopic study.

PubMed

Geethanjali, H S; Melavanki, R M; Nagaraja, D; Patil, N R; Thipperudrappa, J; Kusanur, R A

2016-08-01

The photophysical properties of 4-fluoro-2-methoxyphenyl boronic acid (4FMPBA) are characterized using absorption and fluorescence techniques in series of non-alcohols and alcohols. The results are analyzed using different solvent polarity functions and Kamlet and Catalan's multiple regression approaches. The excited state dipole moment and change in dipole moment are calculated using both the solvatochromic shift method and Reichardt's microscopic solvent polarity parameter ETN. The ground state dipole moment is evaluated using quantum chemical calculations. It is found that general solute-solvent and hydrogen bond interactions are operative in this system. A red shift of ~ 9 nm in the emission spectra is observed with an increase in the solvent polarity, which depicts π→π(*) transitions, as well as the possibility of an intramolecular charge transfer (ICT) character in the emitting singlet state of 4FMPBA. The relative quantum yield, radiative and non-radiative decay constants are calculated in alkanes and alcohols using the single point method. It is found that the quantum yield of the molecule varies from 16.81% to 50.79% with the change in solvent polarity, indicating the dependence of fluorescence on the solvent environment. Copyright © 2015 John Wiley & Sons, Ltd. Copyright © 2015 John Wiley & Sons, Ltd.

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.

Anomalous quantum critical spin dynamics in YFe2Al10

NASA Astrophysics Data System (ADS)

Huang, K.; Tan, C.; Zhang, J.; Ding, Z.; MacLaughlin, D. E.; Bernal, O. O.; Ho, P.-C.; Baines, C.; Wu, L. S.; Aronson, M. C.; Shu, L.

2018-04-01

We report results of a muon spin relaxation (μ SR ) study of YFe2Al10 , a quasi-two-dimensional (2D) nearly ferromagnetic metal in which unconventional quantum critical behavior is observed. No static Fe2 + magnetism, with or without long-range order, is found down to 19 mK. The dynamic muon spin relaxation rate λ exhibits power-law divergences in temperature and magnetic field, the latter for fields that are too weak to affect the electronic spin dynamics directly. We attribute this to the proportionality of λ (ωμ,T ) to the dynamic structure factor S (ωμ,T ) , where ωμ≈105-107s-1 is the muon Zeeman frequency. These results suggest critical divergences of S (ωμ,T ) in both temperature and frequency. Power-law scaling and a 2D dissipative quantum XY model both yield forms for S (ω ,T ) that agree with neutron scattering data (ω ≈1012s-1 ). Extrapolation to μ SR frequencies agrees semiquantitatively with the observed temperature dependence of λ (ωμ,T ) , but predicts frequency independence for ωμ≪T , in extreme disagreement with experiment. We conclude that the quantum critical spin dynamics of YFe2Al10 is not well understood at low frequencies.

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.

Role of electron transfer in Ce{sup 3+} sensitized Yb{sup 3+} luminescence in borate glass

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

Sontakke, Atul D., E-mail: sontakke.atul.55a@st.kyoto-u.ac.jp; Katayama, Yumiko; Zhuang, Yixi

2015-01-07

In a Ce{sup 3+}-Yb{sup 3+} system, two mechanisms are proposed so far namely, the quantum cutting mechanism and the electron transfer mechanism explaining Yb{sup 3+} infrared luminescence under Ce{sup 3+} excitation. Among them, the quantum cutting mechanism, where one Ce{sup 3+} photon (ultraviolet/blue) gives rise to two Yb{sup 3+} photons (near infrared) is widely sought for because of its huge potential in enhancing the solar cell efficiency. In present study on Ce{sup 3+}-Yb{sup 3+} codoped borate glasses, Ce{sup 3+} sensitized Yb{sup 3+} luminescence at ∼1 μm have been observed on Ce{sup 3+} 5d state excitation. However, the intensity of sensitized Yb{supmore » 3+} luminescence is found to be very weak compared to the strong quenching occurred in Ce{sup 3+} luminescence in Yb{sup 3+} codoped glasses. Moreover, the absolute luminescence quantum yield also showed a decreasing trend with Yb{sup 3+} codoping in the glasses. The overall behavior of the luminescence properties and the quantum yield is strongly contradicting with the quantum cutting phenomenon. The results are attributed to the energetically favorable electron transfer interactions followed by Ce{sup 3+}-Yb{sup 3+} ⇌ Ce{sup 4+}-Yb{sup 2+} inter-valence charge transfer and successfully explained using the absolute electron binding energies of dopant ions in the studied borate glass. Finally, an attempt has been presented to generalize the electron transfer mechanism among opposite oxidation/reduction property dopant ions using the vacuum referred electron binding energy (VRBE) scheme for lanthanide series.« less

Boron difluoride dibenzoylmethane derivatives: Electronic structure and luminescence

NASA Astrophysics Data System (ADS)

Tikhonov, Sergey A.; Vovna, Vitaliy I.; Osmushko, Ivan S.; Fedorenko, Elena V.; Mirochnik, Anatoliy G.

2018-01-01

Electronic structure and optical properties of boron difluoride dibenzoylmethanate and four of its derivatives have been studied by X-ray photoelectron spectroscopy, absorption and luminescence spectroscopy and quantum chemistry (DFT, TDDFT). The relative quantum luminescence yields have been revealed to correlate with charge transfers of HOMO-LUMO transitions, energy barriers of aromatic substituents rotation and the lifetime of excited states in the investigated complexes. The bathochromic shift of intensive bands in the optical spectra has been observed to occur when the functional groups are introduced into p-positions of phenyl cycles due to destabilizing HOMO levels. Calculated energy intervals between electronic levels correlate well with XPS spectra structure of valence and core electrons.

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

Bennink, Ryan S.; Ferragut, Erik M.; Humble, Travis S.

Modeling and simulation are essential for predicting and verifying the behavior of fabricated quantum circuits, but existing simulation methods are either impractically costly or require an unrealistic simplification of error processes. In this paper, we present a method of simulating noisy Clifford circuits that is both accurate and practical in experimentally relevant regimes. In particular, the cost is weakly exponential in the size and the degree of non-Cliffordness of the circuit. Our approach is based on the construction of exact representations of quantum channels as quasiprobability distributions over stabilizer operations, which are then sampled, simulated, and weighted to yield unbiasedmore » statistical estimates of circuit outputs and other observables. As a demonstration of these techniques, we simulate a Steane [[7,1,3

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

Surface ligands affect photoinduced modulation of the quantum dots optical performance

NASA Astrophysics Data System (ADS)

Krivenkov, Victor A.; Samokhvalov, Pavel S.; Linkov, Pavel A.; Solovyeva, Daria O.; Kotkovskii, Gennadii E.; Chistyakov, Alexander A.; Nabiev, Igor

2014-05-01

Changes of optical properties of the solutions of CdSe/ZnS quantum dots (QDs) covered with the trioctylphosphine oxide (TOPO) ligands under the pulsed ultraviolet (UV) laser irradiation are observed. The fluorescence quantum yield (QY) of QDs decreases by more than an order of magnitude when the radiation dose approaches 2 × 10-15 J per particle. This process is accompanied by a blue shift of both fluorescence and the first excitonic absorption peaks. The fluorescence quenching becomes less pronounced when the overall TOPO content in the solution is increased. When ТОРО ligands are replaced with n-hexadecylamine (HDA), QY and spectral properties are not changed at the same irradiation conditions. We assume that the above changes of the optical properties are associated with photooxidation of TOPO ligands by excited QD. Such process is less probable for the HDA ligand due to its different energy structure.

Quantum learning of classical stochastic processes: The completely positive realization problem

NASA Astrophysics Data System (ADS)

Monràs, Alex; Winter, Andreas

2016-01-01

Among several tasks in Machine Learning, a specially important one is the problem of inferring the latent variables of a system and their causal relations with the observed behavior. A paradigmatic instance of this is the task of inferring the hidden Markov model underlying a given stochastic process. This is known as the positive realization problem (PRP), [L. Benvenuti and L. Farina, IEEE Trans. Autom. Control 49(5), 651-664 (2004)] and constitutes a central problem in machine learning. The PRP and its solutions have far-reaching consequences in many areas of systems and control theory, and is nowadays an important piece in the broad field of positive systems theory. We consider the scenario where the latent variables are quantum (i.e., quantum states of a finite-dimensional system) and the system dynamics is constrained only by physical transformations on the quantum system. The observable dynamics is then described by a quantum instrument, and the task is to determine which quantum instrument — if any — yields the process at hand by iterative application. We take as a starting point the theory of quasi-realizations, whence a description of the dynamics of the process is given in terms of linear maps on state vectors and probabilities are given by linear functionals on the state vectors. This description, despite its remarkable resemblance with the hidden Markov model, or the iterated quantum instrument, is however devoid of any stochastic or quantum mechanical interpretation, as said maps fail to satisfy any positivity conditions. The completely positive realization problem then consists in determining whether an equivalent quantum mechanical description of the same process exists. We generalize some key results of stochastic realization theory, and show that the problem has deep connections with operator systems theory, giving possible insight to the lifting problem in quotient operator systems. Our results have potential applications in quantum machine learning, device-independent characterization and reverse-engineering of stochastic processes and quantum processors, and more generally, of dynamical processes with quantum memory [M. Guţă, Phys. Rev. A 83(6), 062324 (2011); M. Guţă and N. Yamamoto, e-print arXiv:1303.3771(2013)].

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 ).

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.

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.

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.

Two Hymenophyllaceae species from contrasting natural environments exhibit a homoiochlorophyllous strategy in response to desiccation stress.

PubMed

Flores-Bavestrello, Alejandra; Król, Marianna; Ivanov, Alexander G; Hüner, Norman P A; García-Plazaola, José Ignacio; Corcuera, Luis J; Bravo, León A

2016-02-01

Hymenophyllaceae is a desiccation tolerant family of Pteridophytes which are poikilohydric epiphytes. Their fronds are composed by a single layer of cells and lack true mesophyll cells and stomata. Although they are associated with humid and shady environments, their vertical distribution varies along the trunk of the host plant with some species inhabiting the drier sides with a higher irradiance. The aim of this work was to compare the structure and function of the photosynthetic apparatus during desiccation and rehydration in two species, Hymenophyllum dentatum and Hymenoglossum cruentum, isolated from a contrasting vertical distribution along the trunk of their hosts. Both species were subjected to desiccation and rehydration kinetics to analyze frond phenotypic plasticity, as well as the structure, composition and function of the photosynthetic apparatus. Minimal differences in photosynthetic pigments were observed upon dehydration. Measurements of ϕPSII (effective quantum yield of PSII), ϕNPQ (quantum yield of the regulated energy dissipation of PSII), ϕNO (quantum yield of non-regulated energy dissipation of PSII), and TL (thermoluminescence) indicate that both species convert a functional photochemical apparatus into a structure which exhibits maximum quenching capacity in the dehydrated state with minimal changes in photosynthetic pigments and polypeptide compositions. This dehydration-induced conversion in the photosynthetic apparatus is completely reversible upon rehydration. We conclude that H. dentatum and H. cruentum are homoiochlorophyllous with respect to desiccation stress and exhibited no correlation between inherent desiccation tolerance and the vertical distribution along the host tree trunk. Copyright © 2015 Elsevier GmbH. All rights reserved.

The application of signal detection theory to optics

NASA Technical Reports Server (NTRS)

Helstrom, C. W.

1971-01-01

The restoration of images focused on a photosensitive surface is treated from the standpoint of maximum likelihood estimation, taking into account the Poisson distributions of the observed data, which are the numbers of photoelectrons from various elements of the surface. A detector of an image focused on such a surface utilizes a certain linear combination of those numbers as the optimum detection statistic. Methods for calculating the false alarm and detection probabilities are proposed. It is shown that measuring noncommuting observables in an ideal quantum receiver cannot yield a lower Bayes cost than that attainable by a system measuring only commuting observables.

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.

Yields of O2(b 1 Sigma g +) from reactions of HO2. [in planetary atmospheres

NASA Technical Reports Server (NTRS)

Keyser, L. F.; Choo, K. Y.; Leu, M. T.

1985-01-01

The production of O2(b 1 Sigma g +) has been monitored for several reactions of the HO2 radical at 300 K using a discharge-flow apparatus with resonance fluorescence and chemiluminescence detection. In all cases, the resulting quantum efficiencies were found to be less than 0.03. O2(b) was observed when F atoms were added to H2O2 in the gas phase. The signal strengths of O2(b) were proportional to initial concentrations of HO2 formed by the F + H2O2 reaction. Observed /O2(b)/, /HO2/, and /OH/ vs /F/0 were analyzed using a simple three-step mechanism and a more complete computer simulation with 22 reaction steps. The results indicate that the F + HO2 reaction yields O2(b) with an efficiency of (3.6 + or - 1.4) x 10 to the -3rd. Yields from the O + OH2 reaction were less than 0.02, indicating that this reaction cannot be a major source of the O2(b) emission observed in the earth's nightglow.

Inkjet printed fluorescent nanorod layers exhibit superior optical performance over quantum dots

NASA Astrophysics Data System (ADS)

Halivni, Shira; Shemesh, Shay; Waiskopf, Nir; Vinetsky, Yelena; Magdassi, Shlomo; Banin, Uri

2015-11-01

Semiconductor nanocrystals exhibit unique fluorescence properties which are tunable in size, shape and composition. The high quantum yield and enhanced stability have led to their use in biomedical imaging and flat panel displays. Here, semiconductor nanorod based inkjet inks are presented, overcoming limitations of the commonly reported quantum dots in printing applications. Fluorescent seeded nanorods were found to be outstanding candidates for fluorescent inks, due to their low particle-particle interactions and negligible self-absorption. This is manifested by insignificant emission shifts upon printing, even in highly concentrated printed layers and by maintenance of a high fluorescence quantum yield, unlike quantum dots which exhibit fluorescence wavelength shifts and quenching effects. This behavior results from the reduced absorption/emission overlap, accompanied by low energy transfer efficiencies between the nanorods as supported by steady state and time resolved fluorescence measurements. The new seeded nanorod inks enable patterning of thin fluorescent layers, for demanding light emission applications such as signage and displays.Semiconductor nanocrystals exhibit unique fluorescence properties which are tunable in size, shape and composition. The high quantum yield and enhanced stability have led to their use in biomedical imaging and flat panel displays. Here, semiconductor nanorod based inkjet inks are presented, overcoming limitations of the commonly reported quantum dots in printing applications. Fluorescent seeded nanorods were found to be outstanding candidates for fluorescent inks, due to their low particle-particle interactions and negligible self-absorption. This is manifested by insignificant emission shifts upon printing, even in highly concentrated printed layers and by maintenance of a high fluorescence quantum yield, unlike quantum dots which exhibit fluorescence wavelength shifts and quenching effects. This behavior results from the reduced absorption/emission overlap, accompanied by low energy transfer efficiencies between the nanorods as supported by steady state and time resolved fluorescence measurements. The new seeded nanorod inks enable patterning of thin fluorescent layers, for demanding light emission applications such as signage and displays. Electronic supplementary information (ESI) available. See DOI: 10.1039/c5nr06248a

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.

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.

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.

Aqueous synthesis of high bright and tunable near-infrared AgInSe2-ZnSe quantum dots for bioimaging.

PubMed

Che, Dongchen; Zhu, Xiaoxu; Wang, Hongzhi; Duan, Yourong; Zhang, Qinghong; Li, Yaogang

2016-02-01

Efficient synthetic methods for near-infrared quantum dots with good biophysical properties as bioimaging agents are urgently required. In this work, a simple and fast synthesis of highly luminescent, near-infrared AgInSe2-ZnSe quantum dots (QDs) with tunable emissions in aqueous media is reported. This method avoids high temperature and pressure and organic solvents to directly generate water-dispersible AgInSe2-ZnSe QDs. The photoluminescence emission peak of the AgInSe2-ZnSe QDs ranged from 625 to 940nm, with quantum yields up to 31%. The AgInSe2-ZnSe QDs with high quantum yield, near-infrared and low cytotoxic could be used as good cell labels, showing great potential applications in bio-imaging. Copyright © 2015 Elsevier Inc. All rights reserved.

Laboratory observations of the photochemistry of parent molecules: A review

NASA Technical Reports Server (NTRS)

Jackson, W. M.

1976-01-01

The photochemistry of possible parent molecules of comets has been reviewed. Quantum yields for many of the primary processes are unknown. Energy partitioning among the fragments has not been extensively investigated. A few of the studies have been performed as a function of the number of collisions that the excited molecules undergo, so that possible differences that may occur in a cometary environment may be ascertained.

Photoremovable chiral auxiliary.

PubMed

Kammath, Viju Balachandran; Sebej, Peter; Slanina, Tomáš; Kříž, Zdeněk; Klán, Petr

2012-03-01

A new concept of a photoremovable chiral auxiliary (PCA), based on the chiral benzoin chromophore, is introduced. This moiety can control the asymmetric formation of a Diels-Alder adduct, and then be removed in a subsequent photochemical step in high chemical and quantum yields. Selective formation of the products at up to 96% ee was observed in the presence of a Lewis acid catalyst in the case of a 2-methoxybenzoinyl chiral auxiliary.

Solvent induced fluorescence enhancement of graphene oxide studied by ultrafast spectroscopy

NASA Astrophysics Data System (ADS)

Zhao, Litao; Chen, Jinquan; He, Xiaoxiao; Yu, Xiantong; Yan, Shujun; Zhang, Sanjun; Pan, Haifeng; Xu, Jianhua

2018-05-01

Femtosecond transient absorption (TA) spectroscopy combined with picosecond time resolved fluorescence (TRF) were used to reveal the fluorescence kinetics of graphene oxide (GO) in water, ethanol and water-ethanol mixtures. Size-independent fluorescence of GO were observed in water, and pH-dependent fluorescence spectra could be fitted well by a triple emission relaxation with peaks around 440 nm, 500 nm, and 590 nm respectively. The results indicate that polycyclic aromatic hydrocarbons (PAHs) linked by oxygen-containing functional groups dominate GO's fluorescence emission. GO's fluorescence quantum yield was measured to be 2.8% in ethanol but 1.2% in water. The three decay components fluorescence decay, as well as the transient absorption dynamics with an offset, confirmed this solvent induced fluorescence enhancement. GO's Raman spectral signals showed that GO in ethanol has a smaller average size of PAHs than that of GO in water. Therefore, besides other enhancement effects reported in literatures, we proposed that solvents could also change the size of PAHs, resulting in a photoluminescence enhancement. Our experimental data demonstrates that GO's quantum yield could be up to 2.8% in water and 8.4% in ethanol and this observation may help ones to improve GO's photoluminescence efficiency as well as its applications in solution.

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.

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 effects in energy and charge transfer in an artificial photosynthetic complex

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

Ghosh, Pulak Kumar; Smirnov, Anatoly Yu.; Nori, Franco

2011-06-28

We investigate the quantum dynamics of energy and charge transfer in a wheel-shaped artificial photosynthetic antenna-reaction center complex. This complex consists of six light-harvesting chromophores and an electron-acceptor fullerene. To describe quantum effects on a femtosecond time scale, we derive the set of exact non-Markovian equations for the Heisenberg operators of this photosynthetic complex in contact with a Gaussian heat bath. With these equations we can analyze the regime of strong system-bath interactions, where reorganization energies are of the order of the intersite exciton couplings. We show that the energy of the initially excited antenna chromophores is efficiently funneled tomore » the porphyrin-fullerene reaction center, where a charge-separated state is set up in a few picoseconds, with a quantum yield of the order of 95%. In the single-exciton regime, with one antenna chromophore being initially excited, we observe quantum beatings of energy between two resonant antenna chromophores with a decoherence time of {approx}100 fs. We also analyze the double-exciton regime, when two porphyrin molecules involved in the reaction center are initially excited. In this regime we obtain pronounced quantum oscillations of the charge on the fullerene molecule with a decoherence time of about 20 fs (at liquid nitrogen temperatures). These results show a way to directly detect quantum effects in artificial photosynthetic systems.« less

Efficient energy transfer in light-harvesting systems: Quantum-classical comparison, flux network, and robustness analysis

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

Wu Jianlan; Department of Chemistry, Massachusetts Institute of Technology, 77 Massachusetts Ave., Cambridge, Massachusetts 02139; Liu Fan

2012-11-07

Following the calculation of optimal energy transfer in thermal environment in our first paper [J. L. Wu, F. Liu, Y. Shen, J. S. Cao, and R. J. Silbey, New J. Phys. 12, 105012 (2010)], full quantum dynamics and leading-order 'classical' hopping kinetics are compared in the seven-site Fenna-Matthews-Olson (FMO) protein complex. The difference between these two dynamic descriptions is due to higher-order quantum corrections. Two thermal bath models, classical white noise (the Haken-Strobl-Reineker (HSR) model) and quantum Debye model, are considered. In the seven-site FMO model, we observe that higher-order corrections lead to negligible changes in the trapping time ormore » in energy transfer efficiency around the optimal and physiological conditions (2% in the HSR model and 0.1% in the quantum Debye model for the initial site at BChl 1). However, using the concept of integrated flux, we can identify significant differences in branching probabilities of the energy transfer network between hopping kinetics and quantum dynamics (26% in the HSR model and 32% in the quantum Debye model for the initial site at BChl 1). This observation indicates that the quantum coherence can significantly change the distribution of energy transfer pathways in the flux network with the efficiency nearly the same. The quantum-classical comparison of the average trapping time with the removal of the bottleneck site, BChl 4, demonstrates the robustness of the efficient energy transfer by the mechanism of multi-site quantum coherence. To reconcile with the latest eight-site FMO model which is also investigated in the third paper [J. Moix, J. L. Wu, P. F. Huo, D. F. Coker, and J. S. Cao, J. Phys. Chem. Lett. 2, 3045 (2011)], the quantum-classical comparison with the flux network analysis is summarized in Appendix C. The eight-site FMO model yields similar trapping time and network structure as the seven-site FMO model but leads to a more disperse distribution of energy transfer pathways.« less

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.

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.

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.

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

The photochemistry and kinetics of chlorine compounds important to stratospheric mid-latitude ozone destruction

NASA Astrophysics Data System (ADS)

Goldfarb, Leah

1997-09-01

The catalytic destruction of stratospheric ozone via chlorinated species was first proposed in the 1970's. Since that time a decline in column ozone abundance in the polar regions as well as at mid-latitudes has been observed. Much of this reduction has been attributed to the increases in anthropogenic chlorine compounds such as CFCs. This study summarizes experimental results obtained using pulsed-photolysis resonance fluorescence and pulsed- photolysis long-path absorption methods to study processes important to chlorine-catalyzed ozone destruction: the quantum yields of the products in the dissociation of ClONO2 and the reactions of free radicals with ClONO2 and ClO. The quantum yields for the production of O, Cl and ClO from ClONO2 were studied at specific laser wavelengths (193, 222, 248, and 308 nm). Cl and ClO yields were comparable at nearly all the wavelengths, expect for 193 nm, where the O atom yield was appreciable. The yields at 308 nm (a wavelength available in the stratosphere) were 0.64 ± 0.17 for Cl, 0.37 ± 0.18 for ClO and <0.05 for O. The rate coefficients of O and Cl atoms with ClONO2 were measured over a wide range of temperatures, and the NO3 product yield for the former reaction, previously unreported, was determined to be ~1. The kinetics of the reaction of O atoms with ClO were measured using a new experimental system built specifically to investigate such radical-radical reactions. A slight negative temperature dependence (E/B = -90 ± 30) was observed over the temperature range (227-363 K). From the measured Arrhenius equation the rate constant at 240 K is 4.1 × 10-11 cm3molecule-1s-1 which is in excellent agreement (l.4% greater) with the currently recommended value. This observation is significant, since this reaction is the rate limiting the dominate chlorine catalytic cycle that destroys O3 near 40 km. To analyze the implications of the kinetic and photochemical information from this work, a box model was constructed. The vertical profile of ozone concentrations and loss rates calculated by this simple model compare well with atmospheric measurements and calculations.

Universal Topological Quantum Computation from a Superconductor-Abelian Quantum Hall Heterostructure

NASA Astrophysics Data System (ADS)

Mong, Roger S. K.; Clarke, David J.; Alicea, Jason; Lindner, Netanel H.; Fendley, Paul; Nayak, Chetan; Oreg, Yuval; Stern, Ady; Berg, Erez; Shtengel, Kirill; Fisher, Matthew P. A.

2014-01-01

Non-Abelian anyons promise to reveal spectacular features of quantum mechanics that could ultimately provide the foundation for a decoherence-free quantum computer. A key breakthrough in the pursuit of these exotic particles originated from Read and Green's observation that the Moore-Read quantum Hall state and a (relatively simple) two-dimensional p+ip superconductor both support so-called Ising non-Abelian anyons. Here, we establish a similar correspondence between the Z3 Read-Rezayi quantum Hall state and a novel two-dimensional superconductor in which charge-2e Cooper pairs are built from fractionalized quasiparticles. In particular, both phases harbor Fibonacci anyons that—unlike Ising anyons—allow for universal topological quantum computation solely through braiding. Using a variant of Teo and Kane's construction of non-Abelian phases from weakly coupled chains, we provide a blueprint for such a superconductor using Abelian quantum Hall states interlaced with an array of superconducting islands. Fibonacci anyons appear as neutral deconfined particles that lead to a twofold ground-state degeneracy on a torus. In contrast to a p+ip superconductor, vortices do not yield additional particle types, yet depending on nonuniversal energetics can serve as a trap for Fibonacci anyons. These results imply that one can, in principle, combine well-understood and widely available phases of matter to realize non-Abelian anyons with universal braid statistics. Numerous future directions are discussed, including speculations on alternative realizations with fewer experimental requirements.

Dirac electrons in quantum rings

NASA Astrophysics Data System (ADS)

Gioia, L.; Zülicke, U.; Governale, M.; Winkler, R.

2018-05-01

We consider quantum rings realized in materials where the dynamics of charge carriers mimics that of two-dimensional (2D) Dirac electrons. A general theoretical description of the ring-subband structure is developed that applies to a range of currently available 2D systems, including graphene, transition-metal dichalcogenides, and narrow-gap semiconductor quantum wells. We employ the scattering-matrix approach to calculate the electronic two-terminal conductance through the ring and investigate how it is affected by Dirac-electron interference. The interplay of pseudospin chirality and hard-wall confinement is found to distinctly affect the geometric phase that is experimentally accessible in mesoscopic-conductance measurements. We derive an effective Hamiltonian for the azimuthal motion of charge carriers in the ring that yields deeper insight into the physical origin of the observed transport effects, including the unique behavior exhibited by the lowest ring subband in the normal and topological (i.e., band-inverted) regimes. Our paper provides a unified approach to characterizing confined Dirac electrons, which can be used to explore the design of valley- and spintronic devices based on quantum interference and the confinement-tunable geometric phase.

Continuous excitations of the triangular-lattice quantum spin liquid YbMgGaO 4

DOE PAGES

Paddison, Joseph A. M.; Daum, Marcus; Dun, Zhiling; ...

2016-12-05

A quantum spin liquid (QSL) is an exotic state of matter in which electrons’ spins are quantum entangled over long distances, but do not show magnetic order in the zero-temperature limit. The observation of QSL states is a central aim of experimental physics, because they host collective excitations that transcend our knowledge of quantum matter; however, examples in real materials are scarce. We report neutron-scattering experiments on YbMgGaO 4, a QSL candidate in which Yb 3+ ions with effective spin-1/2 occupy a triangular lattice. Furthermore, our measurements reveal a continuum of magnetic excitations—the essential experimental hallmark of a QSL7—at verymore » low temperature (0.06 K). The origin of this peculiar excitation spectrum is a crucial question, because isotropic nearest-neighbour interactions do not yield a QSL ground state on the triangular lattice. In using measurements the field-polarized state, we identify antiferromagnetic next-nearest-neighbour interactions spin-space anisotropies and chemical disorder between the magnetic layers as key ingredients in YbMgGaO 4.« less

Controlled synthesis of AlN/GaN multiple quantum well nanowire structures and their optical properties.

PubMed

Qian, Fang; Brewster, Megan; Lim, Sung K; Ling, Yichuan; Greene, Christopher; Laboutin, Oleg; Johnson, Jerry W; Gradečak, Silvija; Cao, Yu; Li, Yat

2012-06-13

We report the controlled synthesis of AlN/GaN multi-quantum well (MQW) radial nanowire heterostructures by metal-organic chemical vapor deposition. The structure consists of a single-crystal GaN nanowire core and an epitaxially grown (AlN/GaN)(m) (m = 3, 13) MQW shell. Optical excitation of individual MQW nanowires yielded strong, blue-shifted photoluminescence in the range 340-360 nm, with respect to the GaN near band-edge emission at 368.8 nm. Cathodoluminescence analysis on the cross-sectional MQW nanowire samples showed that the blue-shifted ultraviolet luminescence originated from the GaN quantum wells, while the defect-associated yellow luminescence was emitted from the GaN core. Computational simulation provided a quantitative analysis of the mini-band energies in the AlN/GaN superlattices and suggested the observed blue-shifted emission corresponds to the interband transitions between the second subbands of GaN, as a result of quantum confinement and strain effect in these AlN/GaN MQW nanowire structures.

Terahertz response in the quantum-Hall-effect regime of a quantum-well-based charge-sensitive infrared phototransistor

NASA Astrophysics Data System (ADS)

Nakagawa, Daisuke; Takizawa, Kazuhiro; Ikushima, Kenji; Kim, Sunmi; Patrashin, Mikhail; Hosako, Iwao; Komiyama, Susumu

2018-04-01

The characteristics of a charge-sensitive infrared phototransistor (CSIP) based on a GaAs/AlGaAs multiple quantum-well (QW) structure are studied under a magnetic field. In the CSIP, the upper QWs serve as a floating gate that is charged by photoexcitation. The photoinduced charges are detected using the resistance of the lowest QW conducting channel. The conducting channel exhibits the integer quantum Hall effect (QHE) in a perpendicular high magnetic field, yielding the magnetic field dependence of the terahertz (THz) response ΔR. We found two different features of ΔR. One is that ΔR switches sign across the QHE plateau, which is explained simply by an increased electron density in the conducting channel. The other feature is observed as an enhanced positive ΔR when a potential barrier is formed in the conducting channel. The latter mechanism can be interpreted as the promotion of edge/bulk scattering due to photoinduced charges. These findings suggest ways to enhance the THz response by using magnetic fields and potential barriers.

Towards cosmological dynamics from loop quantum gravity

NASA Astrophysics Data System (ADS)

Li, Bao-Fei; Singh, Parampreet; Wang, Anzhong

2018-04-01

We present a systematic study of the cosmological dynamics resulting from an effective Hamiltonian, recently derived in loop quantum gravity using Thiemann's regularization and earlier obtained in loop quantum cosmology (LQC) by keeping the Lorentzian term explicit in the Hamiltonian constraint. We show that quantum geometric effects result in higher than quadratic corrections in energy density in comparison to LQC, causing a nonsingular bounce. Dynamics can be described by the Hamilton or Friedmann-Raychaudhuri equations, but the map between the two descriptions is not one to one. A careful analysis resolves the tension on symmetric versus asymmetric bounce in this model, showing that the bounce must be asymmetric and symmetric bounce is physically inconsistent, in contrast to the standard LQC. In addition, the current observations only allow a scenario where the prebounce branch is asymptotically de Sitter, similar to a quantization of the Schwarzschild interior in LQC, and the postbounce branch yields the classical general relativity. For a quadratic potential, we find that a slow-roll inflation generically happens after the bounce, which is quite similar to what happens in LQC.

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.

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

Stimulation of Cysteine-Coated CdSe/ZnS Quantum Dot Luminescence by meso-Tetrakis (p-sulfonato-phenyl) Porphyrin

NASA Astrophysics Data System (ADS)

Parra, Gustavo G.; Ferreira, Lucimara P.; Gonçalves, Pablo J.; Sizova, Svetlana V.; Oleinikov, Vladimir A.; Morozov, Vladimir N.; Kuzmin, Vladimir A.; Borissevitch, Iouri E.

2018-02-01

Interaction between porphyrins and quantum dots (QD) via energy and/or charge transfer is usually accompanied by reduction of the QD luminescence intensity and lifetime. However, for CdSe/ZnS-Cys QD water solutions, kept at 276 K during 3 months (aged QD), the significant increase in the luminescence intensity at the addition of meso-tetrakis (p-sulfonato-phenyl) porphyrin (TPPS4) has been observed in this study. Aggregation of QD during the storage provokes reduction in the quantum yield and lifetime of their luminescence. Using steady-state and time-resolved fluorescence techniques, we demonstrated that TPPS4 stimulated disaggregation of aged CdSe/ZnS-Cys QD in aqueous solutions, increasing the quantum yield of their luminescence, which finally reached that of the fresh-prepared QD. Disaggregation takes place due to increase in electrostatic repulsion between QD at their binding with negatively charged porphyrin molecules. Binding of just four porphyrin molecules per single QD was sufficient for total QD disaggregation. The analysis of QD luminescence decay curves demonstrated that disaggregation stronger affected the luminescence related with the electron-hole annihilation in the QD shell. The obtained results demonstrate the way to repair aged QD by adding of some molecules or ions to the solutions, stimulating QD disaggregation and restoring their luminescence characteristics, which could be important for QD biomedical applications, such as bioimaging and fluorescence diagnostics. On the other hand, the disaggregation is important for QD applications in biology and medicine since it reduces the size of the particles facilitating their internalization into living cells across the cell membrane.

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.

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.

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.

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.

A classical phase r-centroid approach to molecular wave packet dynamics illustrating the danger of using an incomplete set of initial states for thermal averaging

NASA Astrophysics Data System (ADS)

Hansson, Tony

1999-08-01

An inexpensive semiclassical method to simulate time-resolved pump-probe spectroscopy on molecular wave packets is applied to NaK molecules at high temperature. The method builds on the introduction of classical phase factors related to the r-centroids for vibronic transitions and assumes instantaneous laser-molecule interaction. All observed quantum mechanical features are reproduced - for short times where experimental data are available even quantitatively. Furthermore, it is shown that fully quantum dynamical molecular wave packet calculations on molecules at elevated temperatures, which do not include all rovibrational states, must be regarded with caution, as they easily might yield even qualitatively incorrect results.

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

Chen, S. L., E-mail: shuch@ist.hokudai.ac.jp; Takayama, J.; Murayama, A.

Power-dependent time-resolved optical spin orientation measurements were performed on In{sub 0.1}Ga{sub 0.9}As quantum well (QW) and In{sub 0.5}Ga{sub 0.5}As quantum dot (QD) tunnel-coupled structures with an 8-nm-thick GaAs barrier. A fast transient increase of electron spin polarization was observed at the QW ground state after circular-polarized pulse excitation. The temporal maximum of polarization increased with increasing pumping fluence owing to enhanced spin blocking in the QDs, yielding a highest amplification of 174% with respect to the initial spin polarization. Further elevation of the laser power gradually quenched the polarization dynamics, which was induced by saturated spin filling of both themore » QDs and the QW phase spaces.« less

Determination of the D{sup 0}{yields}K{sup -}{pi}{sup +}{pi}{sup 0} and D{sup 0}{yields}K{sup -}{pi}{sup +}{pi}{sup +}{pi}{sup -} coherence factors and average strong-phase differences using quantum-correlated measurements

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

Lowrey, N.; Mehrabyan, S.; Selen, M.

The first measurements of the coherence factors (R{sub K{pi}}{sub {pi}{sup 0}} and R{sub K3{pi}}) and the average strong-phase differences ({delta}{sub D}{sup K{pi}}{sup {pi}{sup 0}} and {delta}{sub D}{sup K3{pi}}) for D{sup 0}{yields}K{sup -}{pi}{sup +}{pi}{sup 0} and D{sup 0}{yields}K{sup -}{pi}{sup +}{pi}{sup +}{pi}{sup -} are presented. These parameters can be used to improve the determination of the unitarity triangle angle {gamma} in B{sup -}{yields}DK{sup -} decays, where D is a D{sup 0} or D{sup 0} meson decaying to the same final state. The measurements are made using quantum-correlated, fully reconstructed D{sup 0}D{sup 0} pairs produced in e{sup +}e{sup -} collisions at the {psi}(3770)more » resonance. The measured values are: R{sub K{pi}}{sub {pi}{sup 0}}=0.84{+-}0.07, {delta}{sub D}{sup K{pi}}{sup {pi}{sup 0}}=(227{sub -17}{sup +14}) deg., R{sub K3{pi}}=0.33{sub -0.23}{sup +0.20}, and {delta}{sub D}{sup K3{pi}}=(114{sub -23}{sup +26}) deg. These results indicate significant coherence in the decay D{sup 0}{yields}K{sup -}{pi}{sup +}{pi}{sup 0}, whereas lower coherence is observed in the decay D{sup 0}{yields}K{sup -}{pi}{sup +}{pi}{sup +}{pi}{sup -}. The analysis also results in a small improvement in the knowledge of other D-meson parameters, in particular, the strong-phase difference for D{sup 0}{yields}K{sup -}{pi}{sup +}, {delta}{sub D}{sup K{pi}}, and the mixing parameter y.« less

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

Ti-Catalyzed Hydroamination for the Synthesis of Amine-Containing π-Conjugated Materials.

PubMed

Hao, Han; Thompson, Kyle A; Hudson, Zachary M; Schafer, Laurel L

2018-04-11

A series of conjugated enamines were prepared by Ti catalyzed anti-Markovnikov hydroamination. The synthetic route is efficient with yields of up to 94 % and the 100 % atom efficiency of the reaction means that these products are easily isolated and purified. Due to the extended conjugated system, the enamine tautomers were observed exclusively in both solid and solution phases, as determined by X-ray crystallography and NMR spectroscopy. These new conjugated molecules, with N incorporated into the backbone, show interesting photophysical properties including photo-luminescent quantum yields of up to 0.26. Notably, through the incorporation of B to give a donor-acceptor π-conjugated system, a redshift of approximately 100 nm is observed for the emission maximum along with the anticipated solvatochromic shifts. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

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.

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

Generating Converged Accurate Free Energy Surfaces for Chemical Reactions with a Force-Matched Semiempirical Model.

PubMed

Kroonblawd, Matthew P; Pietrucci, Fabio; Saitta, Antonino Marco; Goldman, Nir

2018-04-10

We demonstrate the capability of creating robust density functional tight binding (DFTB) models for chemical reactivity in prebiotic mixtures through force matching to short time scale quantum free energy estimates. Molecular dynamics using density functional theory (DFT) is a highly accurate approach to generate free energy surfaces for chemical reactions, but the extreme computational cost often limits the time scales and range of thermodynamic states that can feasibly be studied. In contrast, DFTB is a semiempirical quantum method that affords up to a thousandfold reduction in cost and can recover DFT-level accuracy. Here, we show that a force-matched DFTB model for aqueous glycine condensation reactions yields free energy surfaces that are consistent with experimental observations of reaction energetics. Convergence analysis reveals that multiple nanoseconds of combined trajectory are needed to reach a steady-fluctuating free energy estimate for glycine condensation. Predictive accuracy of force-matched DFTB is demonstrated by direct comparison to DFT, with the two approaches yielding surfaces with large regions that differ by only a few kcal mol -1 .

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.

Generating Converged Accurate Free Energy Surfaces for Chemical Reactions with a Force-Matched Semiempirical Model

DOE PAGES

Kroonblawd, Matthew P.; Pietrucci, Fabio; Saitta, Antonino Marco; ...

2018-03-15

Here, we demonstrate the capability of creating robust density functional tight binding (DFTB) models for chemical reactivity in prebiotic mixtures through force matching to short time scale quantum free energy estimates. Molecular dynamics using density functional theory (DFT) is a highly accurate approach to generate free energy surfaces for chemical reactions, but the extreme computational cost often limits the time scales and range of thermodynamic states that can feasibly be studied. In contrast, DFTB is a semiempirical quantum method that affords up to a thousandfold reduction in cost and can recover DFT-level accuracy. Here, we show that a force-matched DFTBmore » model for aqueous glycine condensation reactions yields free energy surfaces that are consistent with experimental observations of reaction energetics. Convergence analysis reveals that multiple nanoseconds of combined trajectory are needed to reach a steady-fluctuating free energy estimate for glycine condensation. Predictive accuracy of force-matched DFTB is demonstrated by direct comparison to DFT, with the two approaches yielding surfaces with large regions that differ by only a few kcal mol –1.« less

Generating Converged Accurate Free Energy Surfaces for Chemical Reactions with a Force-Matched Semiempirical Model

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

Kroonblawd, Matthew P.; Pietrucci, Fabio; Saitta, Antonino Marco

Here, we demonstrate the capability of creating robust density functional tight binding (DFTB) models for chemical reactivity in prebiotic mixtures through force matching to short time scale quantum free energy estimates. Molecular dynamics using density functional theory (DFT) is a highly accurate approach to generate free energy surfaces for chemical reactions, but the extreme computational cost often limits the time scales and range of thermodynamic states that can feasibly be studied. In contrast, DFTB is a semiempirical quantum method that affords up to a thousandfold reduction in cost and can recover DFT-level accuracy. Here, we show that a force-matched DFTBmore » model for aqueous glycine condensation reactions yields free energy surfaces that are consistent with experimental observations of reaction energetics. Convergence analysis reveals that multiple nanoseconds of combined trajectory are needed to reach a steady-fluctuating free energy estimate for glycine condensation. Predictive accuracy of force-matched DFTB is demonstrated by direct comparison to DFT, with the two approaches yielding surfaces with large regions that differ by only a few kcal mol –1.« less

Systematic investigations on fused π-system compounds of seven benzene rings prepared by photocyclization of diphenanthrylethenes.

PubMed

Fujino, Shota; Yamaji, Minoru; Okamoto, Hideki; Mutai, Toshiki; Yoshikawa, Isao; Houjou, Hirohiko; Tani, Fumito

2017-06-14

We studied the photoproducts of 1-(n-phenanthryl)-2-(m-phenanthryl)ethenes (nEm; n, m = 1, 3 and 9) for understanding photocyclization patterns based on NMR spectroscopy. The crystal structures of the photoproducts were analyzed by X-ray crystallography, and the photophysical features of the photocyclized molecules were investigated based on emission and transient absorption measurements. Phenanthrene derivatives substituted at the 1- and 3-positions were prepared for synthesizing nEm by photocyclization of stilbene derivatives. We obtained four types of primary photoproducts (n@m) from the corresponding nEm. Two of them were found to have racemic molecular structures in the single crystal determined by X-ray crystallography. Besides the primary photoproducts, two types of secondary photoproducts (n@mPP) were isolated. Fluorescence quantum yields and lifetimes of the obtained photoproducts were determined in solution whereas the definite fluorescence quantum yields were obtained in the powder. Observation of the triplet-triplet absorption spectra in solution by laser photolysis techniques showed that intersystem crossing to the triplet state competes with the fluorescence process.

Organic photochemical storage of solar energy. Progress report, February 1, 1979-January 31, 1980

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

Jones, G. II

1980-02-01

Study of valence isomerization of organic compounds has focused on two mechanisms of photosensitization involving either electron donor-acceptor interaction or energy transfer. The quenching of fluorescent sensitizers by isomerizable substrates results in the formation of excited complexes. These sensitizer-substrate pairs are highly polarized, leading to changes in bond order for the substrates. For several substrates such as quadricyclene, hexamethyldewarbenzene, and a nonbornadiene derivative, this perturbation results in efficient valence isomerization. Isomerization observed on irradiation of charge transfer complexes of isomerizable substrates is consistent with a similar exciplex - template mechanism. The energy transfer mechanism of photosensitization has been studied bymore » measuring the temperature dependence of quantum yield for isomerization of dimethyl norbornadiene-2,3-dicarboxylate sensitized by benzanthrone. From temperature and quencher concentration profiles quenching constants have been obtained which are consistent with an endoergic triplet energy transfer mechanism. The thermal upconversion of the low energy triplet of benzanthrone results in a threefold increase in isomerization quantum yield over a 90/sup 0/ temperature range.« less

Signatures of Induced Superconductivity in NbTi Contacted InAs Quantum Wells

NASA Astrophysics Data System (ADS)

McFadden, Anthony; Shabani, Javad; Shojaei, Borzoyeh; Lee, Joon Sue; Palmstrøm, Chris

We have studied electrical transport through InAs quantum wells grown by MBE with unannealed superconducting NbTi contacts deposited ex-situ and patterned by optical photolithography. Characterization of the InAs 2DEG's without superconducting contacts yields typical mobilities greater than 100,000 cm2/Vs at a density of 4e11 cm-2. NbTi-InAs-NbTi (SNS) and NbTi-InAs (SN) devices with dimensions greater than 1 µm are fabricated using optical lithography. Although the dimensions of the fabricated SNS devices are too large to observe a supercurrent, signatures of superconductivity induced in the InAs are present. We observe two superconducting critical temperatures: one of the NbTi leads (Tc~8K), and a second (Tc <4.5K) attributed to superconductivity induced in the InAs channel. dI/dV vs V spectroscopy on SNS junctions below the second critical temperature shows a conductance maximum at zero applied voltage while conductance minima appear at finite bias voltage which is attributed to the presence of an induced superconducting gap in the InAs quantum well. This work has been supported by Microsoft research.

Thermodynamics and proton activities of protic ionic liquids with quantum cluster equilibrium theory

NASA Astrophysics Data System (ADS)

Ingenmey, Johannes; von Domaros, Michael; Perlt, Eva; Verevkin, Sergey P.; Kirchner, Barbara

2018-05-01

We applied the binary Quantum Cluster Equilibrium (bQCE) method to a number of alkylammonium-based protic ionic liquids in order to predict boiling points, vaporization enthalpies, and proton activities. The theory combines statistical thermodynamics of van-der-Waals-type clusters with ab initio quantum chemistry and yields the partition functions (and associated thermodynamic potentials) of binary mixtures over a wide range of thermodynamic phase points. Unlike conventional cluster approaches that are limited to the prediction of thermodynamic properties, dissociation reactions can be effortlessly included into the bQCE formalism, giving access to ionicities, as well. The method is open to quantum chemical methods at any level of theory, but combination with low-cost composite density functional theory methods and the proposed systematic approach to generate cluster sets provides a computationally inexpensive and mostly parameter-free way to predict such properties at good-to-excellent accuracy. Boiling points can be predicted within an accuracy of 50 K, reaching excellent accuracy for ethylammonium nitrate. Vaporization enthalpies are predicted within an accuracy of 20 kJ mol-1 and can be systematically interpreted on a molecular level. We present the first theoretical approach to predict proton activities in protic ionic liquids, with results fitting well into the experimentally observed correlation. Furthermore, enthalpies of vaporization were measured experimentally for some alkylammonium nitrates and an excellent linear correlation with vaporization enthalpies of their respective parent amines is observed.

Supersymmetric preons and the standard model

NASA Astrophysics Data System (ADS)

Raitio, Risto

2018-06-01

The experimental fact that standard model superpartners have not been observed compels one to consider an alternative implementation for supersymmetry. The basic supermultiplet proposed here consists of a photon and a charged spin 1/2 preon field, and their superpartners. These fields are shown to yield the standard model fermions, Higgs fields and gauge symmetries. Supersymmetry is defined for unbound preons only. Quantum group SLq (2) representations are introduced to classify topologically scalars, preons, quarks and leptons.

Suppressing recombination in polymer photovoltaic devices via energy-level cascades.

PubMed

Tan, Zhi-Kuang; Johnson, Kerr; Vaynzof, Yana; Bakulin, Artem A; Chua, Lay-Lay; Ho, Peter K H; Friend, Richard H

2013-08-14

An energy cascading structure is designed in a polymer photovoltaic device to suppress recombination and improve quantum yields. By the insertion of a thin polymer interlayer with intermediate energy levels, electrons and holes can effectively shuttle away from each other while being spatially separated from recombination. An increase in open-circuit voltage and short-circuit current are observed in modified devices. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

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.

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.

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

Ultrafast studies of organometallic photochemistry: The mechanism of carbon-hydrogen bond activation in solution

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

Bromberg, S.E.

1998-05-01

When certain organometallic compounds are photoexcited in room temperature alkane solution, they are able to break or activate the C-H bonds of the solvent. Understanding this potentially practical reaction requires a detailed knowledge of the entire reaction mechanism. Because of the dynamic nature of chemical reactions, time-resolved spectroscopy is commonly employed to follow the important events that take place as reactants are converted to products. For the organometallic reactions examined here, the electronic/structural characteristics of the chemical systems along with the time scales for the key steps in the reaction make ultrafast UV/Vis and IR spectroscopy along with nanosecond Step-Scanmore » FTIR spectroscopy the ideal techniques to use for this study. An initial study of the photophysics of (non-activating) model metal carbonyls centering on the photodissociation of M(CO){sub 6} (M = Cr, W, Mo) was carried out in alkane solutions using ultrafast IR spectroscopy. Next, picosecond UV/vis studies of the C-H bond activation reaction of Cp{sup *}M(CO){sub 2} (M = Rh, Ir), conducted in room temperature alkane solution, are described in an effort to investigate the origin of the low quantum yield for bond cleavage ({approximately}1%). To monitor the chemistry that takes place in the reaction after CO is lost, a system with higher quantum yield is required. The reaction of Tp{sup *}Rh(CO){sub 2} (Tp{sup *} = HB-Pz{sub 3}{sup *}, Pz{sup *} = 3,5-dimethylpyrazolyl) in alkanes has a quantum yield of {approximately}30%, making time resolved spectroscopic measurements possible. From ultrafast IR experiments, two subsequently formed intermediates were observed. The nature of these intermediates are discussed and the first comprehensive reaction mechanism for a photochemical C-H activating organometallic complex is presented.« less

Experimental realization of non-Abelian non-adiabatic geometric gates.

PubMed

Abdumalikov, A A; Fink, J M; Juliusson, K; Pechal, M; Berger, S; Wallraff, A; Filipp, S

2013-04-25

The geometric aspects of quantum mechanics are emphasized most prominently by the concept of geometric phases, which are acquired whenever a quantum system evolves along a path in Hilbert space, that is, the space of quantum states of the system. The geometric phase is determined only by the shape of this path and is, in its simplest form, a real number. However, if the system has degenerate energy levels, then matrix-valued geometric state transformations, known as non-Abelian holonomies--the effect of which depends on the order of two consecutive paths--can be obtained. They are important, for example, for the creation of synthetic gauge fields in cold atomic gases or the description of non-Abelian anyon statistics. Moreover, there are proposals to exploit non-Abelian holonomic gates for the purposes of noise-resilient quantum computation. In contrast to Abelian geometric operations, non-Abelian ones have been observed only in nuclear quadrupole resonance experiments with a large number of spins, and without full characterization of the geometric process and its non-commutative nature. Here we realize non-Abelian non-adiabatic holonomic quantum operations on a single, superconducting, artificial three-level atom by applying a well-controlled, two-tone microwave drive. Using quantum process tomography, we determine fidelities of the resulting non-commuting gates that exceed 95 per cent. We show that two different quantum gates, originating from two distinct paths in Hilbert space, yield non-equivalent transformations when applied in different orders. This provides evidence for the non-Abelian character of the implemented holonomic quantum operations. In combination with a non-trivial two-quantum-bit gate, our method suggests a way to universal holonomic quantum computing.

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

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

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 learning of classical stochastic processes: The completely positive realization problem

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

Monràs, Alex; Centre for Quantum Technologies, National University of Singapore, 3 Science Drive 2, Singapore 117543; Winter, Andreas

2016-01-15

Among several tasks in Machine Learning, a specially important one is the problem of inferring the latent variables of a system and their causal relations with the observed behavior. A paradigmatic instance of this is the task of inferring the hidden Markov model underlying a given stochastic process. This is known as the positive realization problem (PRP), [L. Benvenuti and L. Farina, IEEE Trans. Autom. Control 49(5), 651–664 (2004)] and constitutes a central problem in machine learning. The PRP and its solutions have far-reaching consequences in many areas of systems and control theory, and is nowadays an important piece inmore » the broad field of positive systems theory. We consider the scenario where the latent variables are quantum (i.e., quantum states of a finite-dimensional system) and the system dynamics is constrained only by physical transformations on the quantum system. The observable dynamics is then described by a quantum instrument, and the task is to determine which quantum instrument — if any — yields the process at hand by iterative application. We take as a starting point the theory of quasi-realizations, whence a description of the dynamics of the process is given in terms of linear maps on state vectors and probabilities are given by linear functionals on the state vectors. This description, despite its remarkable resemblance with the hidden Markov model, or the iterated quantum instrument, is however devoid of any stochastic or quantum mechanical interpretation, as said maps fail to satisfy any positivity conditions. The completely positive realization problem then consists in determining whether an equivalent quantum mechanical description of the same process exists. We generalize some key results of stochastic realization theory, and show that the problem has deep connections with operator systems theory, giving possible insight to the lifting problem in quotient operator systems. Our results have potential applications in quantum machine learning, device-independent characterization and reverse-engineering of stochastic processes and quantum processors, and more generally, of dynamical processes with quantum memory [M. Guţă, Phys. Rev. A 83(6), 062324 (2011); M. Guţă and N. Yamamoto, e-print http://arxiv.org/abs/1303.3771 (2013)].« less

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 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.

Quantum efficiency measurements of eROSITA pnCCDs

NASA Astrophysics Data System (ADS)

Ebermayer, Stefanie; Andritschke, Robert; Elbs, Johannes; Meidinger, Norbert; Strüder, Lothar; Hartmann, Robert; Gottwald, Alexander; Krumrey, Michael; Scholze, Frank

2010-07-01

For the eROSITA X-ray telescope, which is planned to be launched in 2012, detectors were developed and fabricated at the MPI Semiconductor Laboratory. The fully depleted, back-illuminated pnCCDs have an ultrathin pn-junction to improve the low-energy X-ray response function and quantum efficiency. The device thickness of 450 μm is fully sensitive to X-ray photons yielding high quantum efficiency of more than 90% at photon energies of 10 keV. An on-chip filter is deposited on top of the entrance window to suppress visible and UV light which would interfere with the X-ray observations. The pnCCD type developed for the eROSITA telescope was characterized in terms of quantum efficiency and spectral response function. The described measurements were performed in 2009 at the synchrotron radiation sources BESSY II and MLS as cooperation between the MPI Semiconductor Laboratory and the Physikalisch-Technische Bundesanstalt (PTB). Quantum efficiency measurements over a wide range of photon energies from 3 eV to 11 keV as well as spectral response measurements are presented. For X-ray energies from 3 keV to 10 keV the quantum efficiency of the CCD including on-chip filter is shown to be above 90% with an attenuation of visible light of more than five orders of magnitude. A detector response model is described and compared to the measurements.

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.

Enhanced carrier multiplication in engineered quasi-type-II quantum dots

PubMed Central

Cirloganu, Claudiu M.; Padilha, Lazaro A.; Lin, Qianglu; Makarov, Nikolay S.; Velizhanin, Kirill A.; Luo, Hongmei; Robel, Istvan; Pietryga, Jeffrey M.; Klimov, Victor I.

2014-01-01

One process limiting the performance of solar cells is rapid cooling (thermalization) of hot carriers generated by higher-energy solar photons. In principle, the thermalization losses can be reduced by converting the kinetic energy of energetic carriers into additional electron-hole pairs via carrier multiplication (CM). While being inefficient in bulk semiconductors this process is enhanced in quantum dots, although not sufficiently high to considerably boost the power output of practical devices. Here we demonstrate that thick-shell PbSe/CdSe nanostructures can show almost a fourfold increase in the CM yield over conventional PbSe quantum dots, accompanied by a considerable reduction of the CM threshold. These structures enhance a valence-band CM channel due to effective capture of energetic holes into long-lived shell-localized states. The attainment of the regime of slowed cooling responsible for CM enhancement is indicated by the development of shell-related emission in the visible observed simultaneously with infrared emission from the core. PMID:24938462

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...

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

PubMed

Sutter-Fella, Carolin M; Li, Yanbo; Amani, Matin; Ager, Joel W; Toma, Francesca M; Yablonovitch, Eli; Sharp, Ian D; Javey, Ali

2016-01-13

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 CH3NH3PbI3-xBrx 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 dynamic 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 ≤ Eg ≤ 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.

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.

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.

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.

Generalized Galilean transformations and the measurement problem in the entropic dynamics approach to quantum theory

NASA Astrophysics Data System (ADS)

Johnson, David T.

Quantum mechanics is an extremely successful and accurate physical theory, yet since its inception, it has been afflicted with numerous conceptual difficulties. The primary subject of this thesis is the theory of entropic quantum dynamics (EQD), which seeks to avoid these conceptual problems by interpreting quantum theory from an informational perspective. We begin by reviewing Cox's work in describing probability theory as a means of rationally and consistently quantifying uncertainties. We then discuss how probabilities can be updated according to either Bayes' theorem or the extended method of maximum entropy (ME). After that discussion, we review the work of Caticha and Giffin that shows that Bayes' theorem is a special case of ME. This important result demonstrates that the ME method is the general method for updating probabilities. We then review some motivating difficulties in quantum mechanics before discussing Caticha's work in deriving quantum theory from the approach of entropic dynamics, which concludes our review. After entropic dynamics is introduced, we develop the concepts of symmetries and transformations from an informational perspective. The primary result is the formulation of a symmetry condition that any transformation must satisfy in order to qualify as a symmetry in EQD. We then proceed to apply this condition to the extended Galilean transformation. This transformation is of interest as it exhibits features of both special and general relativity. The transformation yields a gravitational potential that arises from an equivalence of information. We conclude the thesis with a discussion of the measurement problem in quantum mechanics. We discuss the difficulties that arise in the standard quantum mechanical approach to measurement before developing our theory of entropic measurement. In entropic dynamics, position is the only observable. We show how a theory built on this one observable can account for the multitude of measurements present in quantum theory. Furthermore, we show that the Born rule need not be postulated, but can be derived in EQD. Finally, we show how the wave function can be updated by the ME method as the phase is constructed purely in terms of probabilities.

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.

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.

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.

Reducing the photo-bleaching effect of a new europium complex embedded in styrene butadiene copolymer

NASA Astrophysics Data System (ADS)

Jiménez, G. Lesly; Reyes-Rodríguez, J. L.; Padilla, Isela; Alarcón-Flores, G.; Falcony, C.

2018-02-01

A highly luminescent europium complex obtained with two different ligands, succinimide (SI) and 2-thenoyltrifluoroacetone (TTA) , was synthetized with different TTA concentrations. The photoluminescence (PL) emission from these materials corresponds to the characteristic inter-electronic energy level transitions of the Eu3+ ions. However, the excitation spectrum is strongly dependent on the presence of TTA, having an optimum response when 0.75 mmol of this compound is added to the EuL3(H2O)3 complex. The quantum yield obtained by these powders were around 72 % ± 1.7 % indicating an optimum sensitization of these complex. The EuL3 TTA complex with the best PL properties was embedded in a styrene butadiene copolymer (SBC) film, produced by the drop casting method, obtaining similar PL behavior at different concentrations, the highest intensity was observed at 1.2% (w/v) of EuL3 TTA complex and the quantum yield of these composite films was 60.5 % ± 2 % . These films were exposed to continuous UV irradiation and after 141 h no photo-bleaching effect was observed in contrast with the EuL3 TTA complex that exhibited a noticeable photoluminescence intensity degradation at much shorter exposure times. Both the Eu-complexes and the composite films were characterized by FT-IR, XRD, SEM and fluorescence spectroscopy.

Triplet-State Dissolved Organic Matter Quantum Yields and Lifetimes from Direct Observation of Aromatic Amine Oxidation.

PubMed

Schmitt, Markus; Erickson, Paul R; McNeill, Kristopher

2017-11-21

Excited triplet state chromophoric dissolved organic matter ( 3 CDOM*) is a short-lived mixture of excited-state species that plays important roles in aquatic photochemical processes. Unlike the study of the triplet states of well-defined molecules, which are amenable to transient absorbance spectroscopy, the study of 3 CDOM* is hampered by it being a complex mixture and its low average intersystem crossing quantum yield (Φ ISC ). This study is an alternative approach to investigating 3 CDOM* using transient absorption laser spectroscopy. The radical cation of N,N,N',N'-tetramethyl-p-phenylenediamine (TMPD), formed through oxidation by 3 CDOM*, was directly observable by transient absorption spectroscopy and was used to probe basic photophysical properties of 3 CDOM*. Quenching and control experiments verified that TMPD •+ was formed from 3 CDOM* under anoxic conditions. Model triplet sensitizers with a wide range of excited triplet state reduction potentials and CDOM oxidized TMPD at near diffusion-controlled rates. This gives support to the idea that a large cross-section of 3 CDOM* moieties are able to oxidize TMPD and that the complex mixture of 3 CDOM* can be simplified to a single signal. Using the TMPD •+ transient, the natural triplet lifetime and Φ ISC for different DOM isolates and natural waters were quantified; values ranged from 12 to 26 μs and 4.1-7.8%, respectively.

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.

Top quark polarization and T-odd spin correlations as tools for testing (non) Standard Model predictions

NASA Astrophysics Data System (ADS)

Bernreuther, W.; Ma, J. P.; Schroeder, T.

In this paper a number of T-odd spin-momentum correlations are defined for t and t-bar quarks and directly measurable correlations involving the momenta of the charged leptons and/or b jets from t and t-bar decay are identified. It concentrates on observables which can be classified as being even under a CP symmetry transformation in the case of e(sup +)e(sup -) yields tt-bar X or pp-bar yields tt-bar X (unpolarized or transversely polarized beams). These correlations project onto absorptive parts of the scattering matrix which are induced by CP-conserving interactions. In order to estimate the effects of the Standard Model interactions the Quantum Chromodynamics and Higgs boson contributions were calculated to a number of these observables. Several of them are considered to be useful tools for a detailed study of the tt-bar system at future hadron colliders.

Photophysical properties of blue – emitting silicon nanoparticles

PubMed Central

Portolés, Manuel J. Llansola; Nieto, Felipe Rodriguez; Soria, Delia B.; Amalvy, Javier I.; Peruzzo, Pablo J.; Mártire, Daniel O.; Kotler, Mónica; Holub, Oliver; Gonzalez, Mónica C.

2012-01-01

Silicon nanoparticles with strong blue photoluminescence were synthesized by electrochemical etching of silicon wafers and ultrasonically removed under N2 atmosphere in organic solvents to produce colloids. Thermal treatment leads to the formation of colloidal Si particles of 3 ± 1 nm diameter, which upon excitation with 340 – 380 nm light exhibited room temperature luminescence in the range from 400 to 500 nm. The emission and the one- and two-photon excitation spectra of the particles are not sensitive to surface functionalization with methyl 2-methylprop-2-enoate. However, the derivatized particles show higher emission quantum yields in air-saturated suspensions (44%) than the underivatized particles (27%), as well as higher stability of its dispersions. FTIR and XPS spectra indicate a significant surface oxidation of the particles. The Si:O:C ratio at the surface of the derivatized particles estimated from XPS is Si3O6(C5O2Hy)1, with y = 7 - 8. Vibronic spacing is observed in both the emission and excitation spectra. The information obtained from one-photon excitation experiments (emission and excitation spectra, photoluminescence quantum yields, luminescence decay lifetimes and anisotropy correlation lifetimes), as well as from two-photon excitation fluorescence correlation spectroscopy (brightness and diffusion coefficients) and TEM indicate that the blue-emitting particles are monodisperse and ball-shaped. Particle size clearly determines the emission and excitation spectral region, as expected from quantum confinement, but the presence and extent of Si-O species on the silicon networks seem crucial for determining the spectrum features and intensity of emission. The nanoparticles could hold great potential as quantum dots for applications as luminescence sensors in biology and environmental science. PMID:22866180

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).

Detectivity enhancement in quantum well infrared photodetectors utilizing a photonic crystal slab resonator.

PubMed

Kalchmair, S; Gansch, R; Ahn, S I; Andrews, A M; Detz, H; Zederbauer, T; Mujagić, E; Reininger, P; Lasser, G; Schrenk, W; Strasser, G

2012-02-27

We characterize the performance of a quantum well infrared photodetector (QWIP), which is fabricated as a photonic crystal slab (PCS) resonator. The strongest resonance of the PCS is designed to coincide with the absorption peak frequency at 7.6 µm of the QWIP. To accurately characterize the detector performance, it is illuminated by using single mode mid-infrared lasers. The strong resonant absorption enhancement yields a detectivity increase of up to 20 times. This enhancement is a combined effect of increased responsivity and noise current reduction. With increasing temperature, we observe a red shift of the PCS-QWIP resonance peak of -0.055 cm(-1)/K. We attribute this effect to a refractive index change and present a model based on the revised plane wave method.

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.

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.

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

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

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.

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.

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}) ) .

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.

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

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

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

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.

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.

Surface defect assisted broad spectra emission from CdSe quantum dots for white LED application

NASA Astrophysics Data System (ADS)

Samuel, Boni; Mathew, S.; Anand, V. R.; Correya, Adrine Antony; Nampoori, V. P. N.; Mujeeb, A.

2018-02-01

This paper reports, broadband photoluminescence from CdSe quantum dots (QDs) under the excitation of 403 nm using fluorimeter and 403 nm CW laser excitation. The broad spectrum obtained from the colloidal quantum dots was ranges from 450 nm to 800 nm. The broadness of the spectra was attributed to the merging of band edge and defect driven emissions from the QDs. Six different sizes of particles were prepared via kinetic growth method by using CdO and elemental Se as sources of Cd and Se respectively. The particle sizes were measured from TEM images. The size dependent effect on broad emission was also studied and the defect state emission was found to be predominant in very small QDs. The defect driven emission was also observed to be redshifted, similar to the band edge emission, due to quantum confinement effect. The emission corresponding to different laser power was also studied and a linear relation was obtained. In order to study the colour characteristics of the emission, CIE chromaticity coordinate, CRI and CCT of the prepared samples were measured. It is observed that, these values were tunable by the addition of suitable intensity of blue light from the excitation source to yield white light of various colour temperatures. The broad photoluminescence spectrum of the QDs, were compared with that of a commercially available white LED. It was found that the prepared QDs are good alternatives for the phosphor in phosphor converted white LEDs, to provide good spectral tunability.

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

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.

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.

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

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.

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

[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.

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.

Cadmium telluride quantum dots induce apoptosis in human breast cancer cell lines.

PubMed

Naderi, Saeed; Zare, Hakimeh; Taghavinia, Nima; Irajizad, Azam; Aghaei, Mahmoud; Panjehpour, Mojtaba

2018-05-01

Semiconductor quantum dots (QDs), especially those containing cadmium, have undergone marked improvements and are now widely used nanomaterials in applicable biological fields. However, great concerns exist regarding their toxicity in biomedical applications. Because of the lack of sufficient data regarding the toxicity mechanism of QDs, this study aimed to evaluate the cytotoxicity of three types of QDs: CdTe QDs, high yield CdTe QDs, and CdTe/CdS core/shell QDs on two human breast cancer cell lines MDA-MB468 and MCF-7. The breast cancer cells were treated with different concentrations of QDs, and cell viability was evaluated via MTT assay. Hoechst staining was applied for observation of morphological changes due to apoptosis. Apoptotic DNA fragmentation was visualized by the agarose gel electrophoresis assay. Flow cytometric annexin V/propidium iodide (PI) measurement was used for apoptosis detection. A significant decrease in cell viability was observed after QDs treatment ( p < 0.05). Apoptotic bodies and chromatin condensation was observed by Hoechst staining. DNA fragmentation assay demonstrated a DNA ladder profile in the exposed cells and also annexin V/PI flow cytometry confirmed apoptosis in a dose-dependent manner. Our results revealed that CdTe, high yield CdTe, and CdTe/CdS core/shell QDs induce apoptosis in breast cancer cell lines in a dose-dependent manner. This study would help realizing the underlying cytotoxicity mechanism, at least partly, of CdTe QDs and may provide information for the development of nanotoxicology and safe use of biological applications of QDs.

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.

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.

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

De Raedt, Hans; Katsnelson, Mikhail I.; Donker, Hylke C.

It is shown that the Pauli equation and the concept of spin naturally emerge from logical inference applied to experiments on a charged particle under the conditions that (i) space is homogeneous (ii) the observed events are logically independent, and (iii) the observed frequency distributions are robust with respect to small changes in the conditions under which the experiment is carried out. The derivation does not take recourse to concepts of quantum theory and is based on the same principles which have already been shown to lead to e.g. the Schrödinger equation and the probability distributions of pairs of particles inmore » the singlet or triplet state. Application to Stern–Gerlach experiments with chargeless, magnetic particles, provides additional support for the thesis that quantum theory follows from logical inference applied to a well-defined class of experiments. - Highlights: • The Pauli equation is obtained through logical inference applied to robust experiments on a charged particle. • The concept of spin appears as an inference resulting from the treatment of two-valued data. • The same reasoning yields the quantum theoretical description of neutral magnetic particles. • Logical inference provides a framework to establish a bridge between objective knowledge gathered through experiments and their description in terms of concepts.« less

Dissociation energy and photochemistry of NO[sub 3

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

Davis, H.F.; Kim, Bongsoo; Johnston, H.S.

1993-03-11

The photodissociation of NO[sub 3] was studied using the method of molecular beam photofragmentation translational spectroscopy. The existence of two photodissociation channels was confirmed under collision-free conditions. At excitation energies below D[sub 0](O-NO[sub 2]) for internally cold NO[sub 3], the authors observe a large quantum yield (0.70 [+-] 0.10 at 588 nm) for a concerted three-center rearrangement resulting in NO([sup 2][Pi]) + O[sub 2]([sup 3][Sigma][sub g][sup [minus

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

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

Calva-Tellez, E.

The angular distributions of the process e/sup +/e/sup -/ yields e/sup +/e/sup / measured by the Bologna-CERN-Frascati group at the electron-positron colliding-beam facility Adonc are analyzed in terms of standard quantum 3/ including soft-and hard-photon emission. An analytical expression is given for the cross section of the process e/sup +/e/sup -/ yields e/sup +/e gamma for hard photons. Detailed numerical r esults for that specific experimental setup are obtained by a Monte Carlo progrm. It is found that this bremsstrahlung process is responsible for the noncollinear and noncoplanar events observed at Frasscati. Therefore, these data, together with the present calculation,more » provide a test of QED for this particular physical situation involving high energies and large momentum transfers. (auth)« less

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

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.

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.

The influence of the quantum dot/polymethylmethacrylate composite preparation method on the stability of its optical properties under laser radiation

NASA Astrophysics Data System (ADS)

Zvaigzne, M. A.; Martynov, I. L.; Krivenkov, V. A.; Samokhvalov, P. S.; Nabiev, I. R.

2017-01-01

Photoluminescent semiconductor nanocrystals, quantum dots (QDs), are nowadays one of the most promising materials for developing a new generation of fluorescent labels, new types of light-emitting devices and displays, flexible electronic components, and solar panels. In many areas the use of QDs is associated with an intense optical excitation, which, in the case of a prolonged exposure, often leads to changes in their optical characteristics. In the present work we examined how the method of preparation of quantum dot/polymethylmethacrylate (QD/PMMA) composite influenced the stability of the optical properties of QD inside the polymer matrix under irradiation by different laser harmonics in the UV (355 nm) and visible (532 nm) spectral regions. The composites were synthesized by spin-coating and radical polymerization methods. Experiments with the samples obtained by spin-coating showed that the properties of the QD/PMMA films remain almost constant at values of the radiation dose below 10 fJ per particle. Irradiating the composites prepared by the radical polymerization method, we observed a monotonic increase in the luminescence quantum yield (QY) accompanied by an increase in the luminescence decay time regardless of the wavelength of the incident radiation. We assume that the observed difference in the optical properties of the samples under exposure to laser radiation is associated with the processes occurring during radical polymerization, in particular, with charge transfer from the radical particles inside QDs. The results of this study are important for understanding photophysical properties of composites on the basis of QDs, as well as for selection of the type of polymer and the composite synthesis method with quantum dots that would allow one to avoid the degradation of their luminescence.

Time-Resolved Photoluminescence Spectroscopy Of The Carrier Dynamics In GaAs/AlxGa1-xAs Quantum Wells

NASA Astrophysics Data System (ADS)

Polland, Hans J.; Kuhl, Jurgen; Gobel, Ernst O.

1988-08-01

Picosecond photoluminescence experiments at low temperature (6K) have been employed to study the trapping dynamics of photoexcited carriers in GaAs/AlGaAs single quantum wells for different shapes of the AlxGai_xAs confinement layers. We have obtained the following results by analyzing the spectral and temporal distribution of the photoluminescence after picosecond pulse excitation: Trapping efficiency is ==, 40% for a standard ungraded cladding layer (A10.3G1.7As with constant band gap and 5nm thick wells) but increases to ,-, 60% and 100% for samp es with a spatially parabolic or linear band gap profile of the confinement layers, respectively. Trapping times are appreciably shorter than the luminescence risetime which is between 60ps to 100ps. Thus carrier trapping does not impose severe limitations on the modulation speed of single quantum well devices up to frequencies in the order of 10GHz. Similar results are obtained for a well with a width of 1.2nm. Inhomogeneities in the carrier trapping mechanism due to well width fluctuations are not observed in our samples. In the second part we describe the photoluminescence properties of GaAs/A1,Gai_x As quantum wells (x=0.3) under the influence of electric fields perpendicular to the layers. We observe a drastic red shift and a concomitant strong increase of the electron-hole recombination lifetime for well widths > lOnm due to the quantum-confined Stark effect. At high fields (50-100kV/cm) field ionization due to tunneling leads to a decrease of both the photoluminescence yield and decay time, in accordance with a simple WKB theory

Photochemical synthesis and photophysical properties of coumarins bearing extended polyaromatic rings studied by emission and transient absorption measurements.

PubMed

Yamaji, Minoru; Hakoda, Yuma; Okamoto, Hideki; Tani, Fumito

2017-04-12

We prepared a variety of coumarin derivatives having expanded π-electron systems along the direction crossing the C 3 -C 4 bond of the coumarin skeleton via a photochemical cyclization process and investigated their photophysical features as a function of the number (n) of the added benzene rings based on emission and transient absorption measurements. Upon increasing n, the fluorescence quantum yields of the π-extended coumarins increased. Expanding the π-electron system on the C 3 -C 4 bond of the coumarin skeleton was found to be efficient for increasing the fluorescence ability more than that on the C 7 -C 8 bond. Introducing the methoxy group at the 7-position was also efficient for enhancing the fluorescence quantum yield and rate of the expanded coumarins. The non-radiative process from the fluorescence state was not substantially influenced by the expanded π-electron system. The competitive process with the fluorescence was found to be intersystem crossing to the triplet state based on the observations of the triplet-triplet absorption. The effects of the expanded π-electron systems on the fluorescence ability were investigated with the aid of TD-DFT calculations.

Watching the Real-time Evolution of a Laser Modified Atom Using Attosecond Pulses

NASA Astrophysics Data System (ADS)

Shivaram, Niranjan; Timmers, Henry; Tong, Xiao-Min; Sandhu, Arvinder

2011-10-01

In the presence of even moderately strong laser fields, atomic states are heavily modified and develop rich structure. Such a laser dressed atom can be described using the Floquet theory in which the laser dressed states called Floquet states are composed of different Fourier components. In this work we use XUV attosecond pulses to excite a He atom from its ground state to near-infrared (NIR) laser dressed Floquet states, which are ionized by the dressing laser field. Quantum interferences between Fourier components of these Floquet states lead to oscillations in He ion yield as a function of time-delay between the XUV and NIR pulses. From the ion yield signal we measure the quantum phase difference between transition matrix elements to two different Fourier components as a function of both time-delay (instantaneous NIR intensity) and NIR pulse peak intensity. These measurements along with information from time-dependent Schrodinger equation simulations enable us to observe the real-time evolution of the laser modified atom as the dominant Floquet state mediating the ionization changes from the 5p Floquet state to the 2p Floquet state with increasing NIR intensity.

Discrimination and quantification of autofluorescence spectra of human lung cells

NASA Astrophysics Data System (ADS)

Rahmani, Mahya; Khani, Mohammad Mehdi; Khazaei Koohpar, Zeinab; Molik, Paria

2016-10-01

To study laser-induced autofluorescence spectroscopy of the human lung cell line, we evaluated the native fluorescence properties of cancer QU-DB and normal MRC-5 human lung cells during continuous exposure to 405 nm laser light. Two emission bands centered at ~470 nm and ~560 nm were observed. These peaks are most likely attributable to mitochondrial fluorescent reduced nicotinamide adenine dinucleotide and riboflavin fluorophores, respectively. This article highlights lung cell autofluorescence characterization and signal discrimination by collective investigation of different spectral features. The absolute intensity, the spectral shape factor or redox ratio, the full width of half-maximum and the full width of quarter maximum was evaluated. Moreover, the intensity ratio, the area under the peak and the area ratio as a contrast factor for normal and cancerous cells were also calculated. Among all these features it seems that the contrast factor precisely and significantly discriminates the spectral differences of normal and cancerous lung cells. On the other hand, the relative quantum yield for both cell types were found by comparing the quantum yield of an unknown compound with known fluorescein sodium as a reference solution.

Ultrafast primary processes of an iron-(III) azido complex in solution induced with 266 nm light.

PubMed

Vennekate, Hendrik; Schwarzer, Dirk; Torres-Alacan, Joel; Krahe, Oliver; Filippou, Alexander C; Neese, Frank; Vöhringer, Peter

2012-05-14

The ultrafast photo-induced primary processes of the iron-(III) azido complex, [Fe(III)N(3)(cyclam-acetato)] PF(6) (1), in acetonitrile solution at room temperature were studied using femtosecond spectroscopy with ultraviolet (UV) excitation and mid-infrared (MIR) detection. Following the absorption of a 266 nm photon, the complex undergoes an internal conversion back to the electronic doublet ground state at a time scale below 2 ps. Subsequently, the electronic ground state vibrationally cools with a characteristic time constant of 13 ps. A homolytic bond cleavage was also observed by the appearance of ground state azide radicals, which were identified by their asymmetric stretching vibration at 1659 cm(-1). The azide radical recombines in a geminate fashion with the iron containing fragment within 20 ps. The cage escape leading to well separated fragments after homolytic Fe-N bond breakage was found to occur with a quantum yield of 35%. Finally, non-geminate recombination at nanosecond time scales was seen to further reduce the photolytic quantum yield to below 20% at a wavelength of 266 nm. This journal is © the Owner Societies 2012

Interest rates in quantum finance: the Wilson expansion and Hamiltonian.

PubMed

Baaquie, Belal E

2009-10-01

Interest rate instruments form a major component of the capital markets. The Libor market model (LMM) is the finance industry standard interest rate model for both Libor and Euribor, which are the most important interest rates. The quantum finance formulation of the Libor market model is given in this paper and leads to a key generalization: all the Libors, for different future times, are imperfectly correlated. A key difference between a forward interest rate model and the LMM lies in the fact that the LMM is calibrated directly from the observed market interest rates. The short distance Wilson expansion [Phys. Rev. 179, 1499 (1969)] of a Gaussian quantum field is shown to provide the generalization of Ito calculus; in particular, the Wilson expansion of the Gaussian quantum field A(t,x) driving the Libors yields a derivation of the Libor drift term that incorporates imperfect correlations of the different Libors. The logarithm of Libor phi(t,x) is defined and provides an efficient and compact representation of the quantum field theory of the Libor market model. The Lagrangian and Feynman path integrals of the Libor market model of interest rates are obtained, as well as a derivation given by its Hamiltonian. The Hamiltonian formulation of the martingale condition provides an exact solution for the nonlinear drift of the Libor market model. The quantum finance formulation of the LMM is shown to reduce to the industry standard Bruce-Gatarek-Musiela-Jamshidian model when the forward interest rates are taken to be exactly correlated.

Water deficit in field-grown Gossypium hirsutum primarily limits net photosynthesis by decreasing stomatal conductance, increasing photorespiration, and increasing the ratio of dark respiration to gross photosynthesis.

PubMed

Chastain, Daryl R; Snider, John L; Collins, Guy D; Perry, Calvin D; Whitaker, Jared; Byrd, Seth A

2014-11-01

Much effort has been expended to improve irrigation efficiency and drought tolerance of agronomic crops; however, a clear understanding of the physiological mechanisms that interact to decrease source strength and drive yield loss has not been attained. To elucidate the underlying mechanisms contributing to inhibition of net carbon assimilation under drought stress, three cultivars of Gossypium hirsutum were grown in the field under contrasting irrigation regimes during the 2012 and 2013 growing season near Camilla, Georgia, USA. Physiological measurements were conducted on three sample dates during each growing season (providing a broad range of plant water status) and included, predawn and midday leaf water potential (ΨPD and ΨMD), gross and net photosynthesis, dark respiration, photorespiration, and chlorophyll a fluorescence. End-of-season lint yield was also determined. ΨPD ranged from -0.31 to -0.95MPa, and ΨMD ranged from -1.02 to -2.67MPa, depending upon irrigation regime and sample date. G. hirsutum responded to water deficit by decreasing stomatal conductance, increasing photorespiration, and increasing the ratio of dark respiration to gross photosynthesis, thereby limiting PN and decreasing lint yield (lint yield declines observed during the 2012 growing season only). Conversely, even extreme water deficit, causing a 54% decline in PN, did not negatively affect actual quantum yield, maximum quantum yield, or photosynthetic electron transport. It is concluded that PN is primarily limited in drought-stressed G. hirsutum by decreased stomatal conductance, along with increases in respiratory and photorespiratory carbon losses, not inhibition or down-regulation of electron transport through photosystem II. It is further concluded that ΨPD is a reliable indicator of drought stress and the need for irrigation in field-grown cotton. Copyright © 2014 Elsevier GmbH. All rights reserved.

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.

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.

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

Liu, Xiu-Li, E-mail: usually.158@163.com; Hubei Key Laboratory of Tumor Biological Behaviors and Hubei Cancer Clinical Study Center, No 169 Donghu Road, Wuchang District, Wuhan 430071; Peng, Chun-Wei, E-mail: pqc278@163.com

Highlights: {yields} HER2 level is closely related to the biologic behaviors of breast cancer cells. {yields} A new method to simultaneously image HER2 and type IV collagen was established. {yields} HER2 status and type IV collagen degradation predict breast cancer invasion. {yields} The complex interactions between tumor and its environment were revealed. -- Abstract: It has been well recognized that human epidermal growth factor receptor 2 (HER2) level in breast cancer (BC) is closely related to the malignant biologic behaviors of the tumor, including invasion and metastasis. Yet, there has been a lack of directly observable evidence to support suchmore » notion. Here we report a quantum dots (QDs)-based double-color imaging technique to simultaneously show the HER2 level on BC cells and the type IV collagen in the tumor matrix. In benign breast tumor, the type IV collagen was intact. With the increasing of HER2 expression level, there has been a progressive decrease in type IV collagen around the cancer nest. At HER2 (3+) expression level, there has virtually been a total destruction of type IV collagen. Moreover, HER2 (3+) BC cells also show direct invasion into the blood vessels. This novel imaging method provides direct observable evidence to support the theory that the HER2 expression level is directly related to BC invasion.« less

What limits photosynthetic energy conversion efficiency in nature? Lessons from the oceans.

PubMed

Falkowski, Paul G; Lin, Hanzhi; Gorbunov, Maxim Y

2017-09-26

Constraining photosynthetic energy conversion efficiency in nature is challenging. In principle, two yield measurements must be made simultaneously: photochemistry, fluorescence and/or thermal dissipation. We constructed two different, extremely sensitive and precise active fluorometers: one measures the quantum yield of photochemistry from changes in variable fluorescence, the other measures fluorescence lifetimes in the picosecond time domain. By deploying the pair of instruments on eight transoceanic cruises over six years, we obtained over 200 000 measurements of fluorescence yields and lifetimes from surface waters in five ocean basins. Our results revealed that the average quantum yield of photochemistry was approximately 0.35 while the average quantum yield of fluorescence was approximately 0.07. Thus, closure on the energy budget suggests that, on average, approximately 58% of the photons absorbed by phytoplankton in the world oceans are dissipated as heat. This extraordinary inefficiency is associated with the paucity of nutrients in the upper ocean, especially dissolved inorganic nitrogen and iron. Our results strongly suggest that, in nature, most of the time, most of the phytoplankton community operates at approximately half of its maximal photosynthetic energy conversion efficiency because nutrients limit the synthesis or function of essential components in the photosynthetic apparatus.This article is part of the themed issue 'Enhancing photosynthesis in crop plants: targets for improvement'. © 2017 The Author(s).

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

Dynamical basis sets for algebraic variational calculations in quantum-mechanical scattering theory

NASA Technical Reports Server (NTRS)

Sun, Yan; Kouri, Donald J.; Truhlar, Donald G.; Schwenke, David W.

1990-01-01

New basis sets are proposed for linear algebraic variational calculations of transition amplitudes in quantum-mechanical scattering problems. These basis sets are hybrids of those that yield the Kohn variational principle (KVP) and those that yield the generalized Newton variational principle (GNVP) when substituted in Schlessinger's stationary expression for the T operator. Trial calculations show that efficiencies almost as great as that of the GNVP and much greater than the KVP can be obtained, even for basis sets with the majority of the members independent of energy.

Photodynamic activity of pyropheophorbide methyl ester and pyropheophorbide a in dimethylformamide solution.

PubMed

Al-Omari, Saleh; Ali, Ahmad

2009-03-01

Comparative spectroscopic study including the photosensitizers of pyropheophorbide methyl ester (PPME) and pyropheophorbide a (PPa) was performed to study their photodynamic activity. The investigated photosensitizers in a homogeneous system of dimethylformamide (DMF) are not photostable upon irradiation. The photobleaching efficiency of PPa is higher than that of PPME. Combining these results with the data obtained by measuring the singlet oxygen quantum yield and the hydroxyl group generation, it was revealed that the photobleaching efficiency could be correlated with the singlet oxygen quantum yield and the hydroxyl group production of the photosensitizer.

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.

Tunable UV Laser Photolysis of NF2: Quantum Yield for NF(a1 delta) Production.

DTIC Science & Technology

1988-05-25

UV Laser Photolysis of NF2: Quantum Yield for NF(a A) Production ’v0 LR. F. HEIDNER, H . HELVAJIAN , 4and J. B. KOFFEND Aerophysics Laboratory...experiments, the chemistry of NF2 with various hydrocarbons has been studied. It has also been shown that the addition-elimination reaction between H and NF2...COMPLI R LEN SP, 3 ,HAND L BE AM~ H O [ I , , i 1 CAIHOC IAM COOLED GaAs CAPACITANCE PHOTOTUIBE MANOMETER _ LENS /’~ ~L + . ANMEE _.... BANDPASS FILTER

Loop-quantum-gravity vertex amplitude.

PubMed

Engle, Jonathan; Pereira, Roberto; Rovelli, Carlo

2007-10-19

Spin foam models are hoped to provide the dynamics of loop-quantum gravity. However, the most popular of these, the Barrett-Crane model, does not have the good boundary state space and there are indications that it fails to yield good low-energy n-point functions. We present an alternative dynamics that can be derived as a quantization of a Regge discretization of Euclidean general relativity, where second class constraints are imposed weakly. Its state space matches the SO(3) loop gravity one and it yields an SO(4)-covariant vertex amplitude for Euclidean loop gravity.

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

Damtie, Fikeraddis A., E-mail: Fikeraddis.Damtie@teorfys.lu.se; Wacker, Andreas, E-mail: Andreas.Wacker@fysik.lu.se; Karki, Khadga J., E-mail: Khadga.Karki@chemphys.lu.se

Multiple exciton generation (MEG) is a process in which more than one electron hole pair is generated per absorbed photon. It allows us to increase the efficiency of solar energy harvesting. Experimental studies have shown the multiple exciton generation yield of 1.2 in isolated colloidal quantum dots. However real photoelectric devices require the extraction of electron hole pairs to electric contacts. We provide a systematic study of the corresponding quantum coherent processes including extraction and injection and show that a proper design of extraction and injection rates enhances the yield significantly up to values around 1.6.

Measures of disturbance and incompatibility for quantum measurements

NASA Astrophysics Data System (ADS)

Mandayam, Prabha; Srinivas, M. D.

2014-06-01

We propose a class of incompatibility measures for quantum observables based on quantifying the effect of a measurement of one observable on the statistics of the outcomes of another. Specifically, for a pair of observables A and B with purely discrete spectra, we compare the following two probability distributions: one resulting from a measurement of A followed by a measurement of B on a given state and the other obtained from a measurement of B alone on the same state. We show that maximizing the distance between these two distributions over all states yields a valid measure of the incompatibility of observables A and B, which is zero if and only if they commute and is strictly greater than zero (and less than or equal to one) otherwise. For finite-dimensional systems, we obtain a tight upper bound on the incompatibility of any pair of observables and show that the bound is attained when the observables are totally nondegenerate and associated with mutually unbiased bases. In the process, we also establish an important relation between the incompatibility of a pair of observables and the maximal disturbances due to their measurements. Finally, we indicate how these measures of incompatibility and disturbance can be extended to the more general class of nonprojective measurements. In particular, we obtain a nontrivial upper bound on the incompatibility of one Lüders instrument with another.

Loop Quantum Gravity.

PubMed

Rovelli, Carlo

2008-01-01

The problem of describing the quantum behavior of gravity, and thus understanding quantum spacetime , is still open. Loop quantum gravity is a well-developed approach to this problem. It is a mathematically well-defined background-independent quantization of general relativity, with its conventional matter couplings. Today research in loop quantum gravity forms a vast area, ranging from mathematical foundations to physical applications. Among the most significant results obtained so far are: (i) The computation of the spectra of geometrical quantities such as area and volume, which yield tentative quantitative predictions for Planck-scale physics. (ii) A physical picture of the microstructure of quantum spacetime, characterized by Planck-scale discreteness. Discreteness emerges as a standard quantum effect from the discrete spectra, and provides a mathematical realization of Wheeler's "spacetime foam" intuition. (iii) Control of spacetime singularities, such as those in the interior of black holes and the cosmological one. This, in particular, has opened up the possibility of a theoretical investigation into the very early universe and the spacetime regions beyond the Big Bang. (iv) A derivation of the Bekenstein-Hawking black-hole entropy. (v) Low-energy calculations, yielding n -point functions well defined in a background-independent context. The theory is at the roots of, or strictly related to, a number of formalisms that have been developed for describing background-independent quantum field theory, such as spin foams, group field theory, causal spin networks, and others. I give here a general overview of ideas, techniques, results and open problems of this candidate theory of quantum gravity, and a guide to the relevant literature.

Bidentate Ligand-Passivated CsPbI3 Perovskite Nanocrystals for Stable Near-Unity Photoluminescence Quantum Yield and Efficient Red Light-Emitting Diodes.

PubMed

Pan, Jun; Shang, Yuequn; Yin, Jun; De Bastiani, Michele; Peng, Wei; Dursun, Ibrahim; Sinatra, Lutfan; El-Zohry, Ahmed M; Hedhili, Mohamed N; Emwas, Abdul-Hamid; Mohammed, Omar F; Ning, Zhijun; Bakr, Osman M

2018-01-17

Although halide perovskite nanocrystals (NCs) are promising materials for optoelectronic devices, they suffer severely from chemical and phase instabilities. Moreover, the common capping ligands like oleic acid and oleylamine that encapsulate the NCs will form an insulating layer, precluding their utility in optoelectronic devices. To overcome these limitations, we develop a postsynthesis passivation process for CsPbI 3 NCs by using a bidentate ligand, namely 2,2'-iminodibenzoic acid. Our passivated NCs exhibit narrow red photoluminescence with exceptional quantum yield (close to unity) and substantially improved stability. The passivated NCs enabled us to realize red light-emitting diodes (LEDs) with 5.02% external quantum efficiency and 748 cd/m 2 luminance, surpassing by far LEDs made from the nonpassivated NCs.

Faithful nonclassicality indicators and extremal quantum correlations in two-qubit states

NASA Astrophysics Data System (ADS)

Girolami, Davide; Paternostro, Mauro; Adesso, Gerardo

2011-09-01

The state disturbance induced by locally measuring a quantum system yields a signature of nonclassical correlations beyond entanglement. Here, we present a detailed study of such correlations for two-qubit mixed states. To overcome the asymmetry of quantum discord and the unfaithfulness of measurement-induced disturbance (severely overestimating quantum correlations), we propose an ameliorated measurement-induced disturbance as nonclassicality indicator, optimized over joint local measurements, and we derive its closed expression for relevant two-qubit states. We study its analytical relation with discord, and characterize the maximally quantum-correlated mixed states, that simultaneously extremize both quantifiers at given von Neumann entropy: among all two-qubit states, these states possess the most robust quantum correlations against noise.

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.

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.

The effect of annulation of benzene rings on the photophysics and electronic structure of tetraazachlorin molecules

NASA Astrophysics Data System (ADS)

Pershukevich, P. P.; Volkovich, D. I.; Gladkov, L. L.; Dudkin, S. V.; Kuzmitsky, V. A.; Makarova, E. A.; Solovyev, K. N.

2017-10-01

The photophysics and electronic structure of tribenzotetraazachlorins (H2, Zn, and Mg), which are novel analogues of phtalocyanines, have been studied experimentally and theoretically. At 293 K, the electronic absorption, fluorescence, and fluorescence excitation spectra are recorded and the fluorescence quantum yield and lifetime, as well as the quantum yield of singlet oxygen generation, are measured; at 77 K, the fluorescence, fluorescence excitation, and fluorescence polarization spectra are recorded and the fluorescence lifetime values are measured. The dependences of the absorption spectra and photophysical parameters on the structure variation are analyzed in detail. Quantum-chemical calculations of the electronic structure and absorption spectra of tribenzotetraazachlorins (H2, Mg) are performed using the INDO/Sm method (modified INDO/S method) based on molecular-geometry optimization by the DFT PBE/TZVP method. The results of quantum-chemical calculations of the electronic absorption spectra are in very good agreement with the experimental data for the transitions to two lower electronic states.

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.

A study of Kapton degradation under simulated shuttle environment

NASA Technical Reports Server (NTRS)

Eck, T. G.; Hoffman, R. W.

1986-01-01

A system was developed which employs a source of low energy oxygen ion to simulate the shuttle low Earth orbit environment. This source, together with diagnostic tools including surface analysis ans mass spectroscopic capability, was used to measure the dependence of ion energy of the oxygen induced CO signals from pyrolytic graphite and Kapton. For graphite the CO signal was examined at energies ranging form 4.5 to 465 eV and for Kapton from 4.5 to 188 eV. While the relative quantum yields inferred from the data are reasonably precise, there are large uncertainties in the absolute yields because of the assumptions necessary to covert the measured signal strengths to quantum yields. These assumptions are discussed in detail.

Phase transfer of 1- and 2-dimensional Cd-based nanocrystals

NASA Astrophysics Data System (ADS)

Kodanek, Torben; Banbela, Hadeel M.; Naskar, Suraj; Adel, Patrick; Bigall, Nadja C.; Dorfs, Dirk

2015-11-01

In this work, luminescent CdSe@CdS dot-in-rod nanocrystals, CdSe@CdS/ZnS nanorods as well as CdSe-CdS core-crown nanoplatelets were transferred into aqueous phase via ligand exchange reactions. For this purpose, bifunctional thiol-based ligands were employed, namely mercaptoacetic acid (MAA), 3-mercaptopropionic acid (MPA), 11-mercaptoundecanoic acid (MUA) as well as 2-(dimethylamino)ethanthiol (DMAET). Systematic investigations by means of photoluminescence quantum yield measurements as well as photoluminescence decay measurements have shown that the luminescence properties of the transferred nanostructures are affected by hole traps (induced by the thiol ligands themselves) as well as by spatial insulation and passivation against the environment. The influence of the tips of the nanorods on the luminescence is, however, insignificant. Accordingly, different ligands yield optimum results for different nanoparticle samples, mainly depending on the inorganic passivation of the respective samples. In case of CdSe@CdS nanorods, the highest emission intensities have been obtained by using short-chain ligands for the transfer preserving more than 50% of the pristine quantum yield of the hydrophobic nanorods. As opposed to this, the best possible quantum efficiency for the CdSe@CdS/ZnS nanorods has been achieved via MUA. The gained knowledge could be applied to transfer for the first time 2-dimensional CdSe-CdS core-crown nanoplatelets into water while preserving significant photoluminescence (up to 12% quantum efficiency).In this work, luminescent CdSe@CdS dot-in-rod nanocrystals, CdSe@CdS/ZnS nanorods as well as CdSe-CdS core-crown nanoplatelets were transferred into aqueous phase via ligand exchange reactions. For this purpose, bifunctional thiol-based ligands were employed, namely mercaptoacetic acid (MAA), 3-mercaptopropionic acid (MPA), 11-mercaptoundecanoic acid (MUA) as well as 2-(dimethylamino)ethanthiol (DMAET). Systematic investigations by means of photoluminescence quantum yield measurements as well as photoluminescence decay measurements have shown that the luminescence properties of the transferred nanostructures are affected by hole traps (induced by the thiol ligands themselves) as well as by spatial insulation and passivation against the environment. The influence of the tips of the nanorods on the luminescence is, however, insignificant. Accordingly, different ligands yield optimum results for different nanoparticle samples, mainly depending on the inorganic passivation of the respective samples. In case of CdSe@CdS nanorods, the highest emission intensities have been obtained by using short-chain ligands for the transfer preserving more than 50% of the pristine quantum yield of the hydrophobic nanorods. As opposed to this, the best possible quantum efficiency for the CdSe@CdS/ZnS nanorods has been achieved via MUA. The gained knowledge could be applied to transfer for the first time 2-dimensional CdSe-CdS core-crown nanoplatelets into water while preserving significant photoluminescence (up to 12% quantum efficiency). Electronic supplementary information (ESI) available: Further TEM images, further extinction spectra, particle size distribution and discussion about optical properties of the hydrophobic nanostructures. See DOI: 10.1039/c5nr06221g

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.

Rational Design of Emissive NIR-Absorbing Chromophores: Rh(III) Porphyrin-Aza-BODIPY Conjugates with Orthogonal Metal-Carbon Bonds.

PubMed

Zhou, Jinfeng; Gai, Lizhi; Zhou, Zhikuan; Yang, Wu; Mack, John; Xu, Kejing; Zhao, Jianzhang; Zhao, Yue; Qiu, Hailin; Chan, Kin Shing; Shen, Zhen

2016-09-05

The facile synthesis of Group 9 Rh(III) porphyrin-aza-BODIPY conjugates that are linked through an orthogonal Rh-C(aryl) bond is reported. The conjugates combine the advantages of the near-IR (NIR) absorption and intense fluorescence of aza-BODIPY dyes with the long-lived triplet states of transition metal rhodium porphyrins. Only one emission peak centered at about 720 nm is observed, irrespective of the excitation wavelength, demonstrating that the conjugates act as unique molecules rather than as dyads. The generation of a locally excited (LE) state with intramolecular charge-transfer (ICT) character has been demonstrated by solvatochromic effects in the photophysical properties, singlet oxygen quantum yields in polar solvents, and by the results of density functional theory (DFT) calculations. In nonpolar solvents, the Rh(III) conjugates exhibit strong aza-BODIPY-centered fluorescence at around 720 nm (ΦF =17-34 %), and negligible singlet oxygen generation. In polar solvents, enhancements of the singlet-oxygen quantum yield (ΦΔ =19-27 %, λex =690 nm) have been observed. Nanosecond pulsed time-resolved absorption spectroscopy confirms that relatively long-lived triplet excited states are formed. The synthetic methodology outlined herein provides a useful strategy for the assembly of functional materials that are highly desirable for a wide range of applications in material science and biomedical fields. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Assessment of filtration efficiency and physiological responses of selected plant species to indoor air pollutants (toluene and 2-ethylhexanol) under chamber conditions.

PubMed

Hörmann, Vanessa; Brenske, Klaus-Reinhard; Ulrichs, Christian

2018-01-01

Three common plant species (Dieffenbachia maculata, Spathiphyllum wallisii, and Asparagus densiflorus) were tested against their capacity to remove the air pollutants toluene (20.0 mg m -3 ) and 2-ethylhexanol (14.6 mg m -3 ) under light or under dark in chamber experiments of 48-h duration. Results revealed only limited pollutant filtration capabilities and indicate that aerial plant parts of the tested species are only of limited value for indoor air quality improvement. The removal rate constant ranged for toluene from 3.4 to 5.7 L h -1  m -2 leaf area with no significant differences between plant species or light conditions (light/dark). The values for 2-ethylhexanol were somewhat lower, fluctuating around 2 L h -1  m -2 leaf area for all plant species tested, whereas differences between light and dark were observed for two of the three species. In addition to pollutant removal, CO 2 fixation/respiration and transpiration as well as quantum yield were evaluated. These physiological characteristics seem to have no major impact on the VOC removal rate constant. Exposure to toluene or 2-ethylhexanol revealed no or only minor effects on D. maculata and S. wallisii. In contrast, a decrease in quantum yield and CO 2 fixation was observed for A. densiflorus when exposed to 2-ethylhexanol or toluene under light, indicating phytotoxic effects in this species.

A comparative study of the spectral, fluorometric properties and photostability of natural curcumin, iron- and boron- complexed curcumin

NASA Astrophysics Data System (ADS)

Mohammed, Fatima; Rashid-Doubell, Fiza; Cassidy, Seamas; Henari, Fryad

2017-08-01

Curcumin is a yellow phenolic compound with a wide range of reported biological effects. However, two main obstacles hinder the use of curcumin therapeutically, namely its poor bioavailability and photostability. We have synthesized two curcumin complexes, the first a boron curcumin complex (B-Cur2) and the second an iron (Fe-Cur3) complex of curcumin. Both derivatives showed high fluorescence efficiency (quantum yield) and greater photostability in solution. The improved photostability could be attributed to the coordination structures and the removal of β-diketone group from curcumin. The fluorescence and ultra violet/visible absorption spectra of curcumin, B-Cur2 and Fe-Cur3 all have a similar spectral pattern when dissolved in the same organic solvent. However, a shift towards a lower wavelength was observed when moving from polar to non-polar solvents, possibly due to differences in solvent polarity. A plot of Stokes' shift vs the orientation polarity parameter (Δf) or vs the solvent polarity parameter (ET 30) showed an improved correlation between the solvent polarity parameter than with the orientation polarity parameter and indicating that the red shift observed could be due to hydrogen-bonding between the solvent molecules. A similar association was obtained when Stokes' shift was replaced by maximum synchronous fluorescence. Both B-Cur2 and Fe-Cur3 had larger quantum yields than curcumin, suggesting they may be good candidates for medical imaging and in vitro studies.

Effect of Ligand Exchange on the Photoluminescence Properties of Cu-Doped Zn-In-Se Quantum Dots

NASA Astrophysics Data System (ADS)

Dong, Xiaofei; Xu, Jianping; Yang, Hui; Zhang, Xiaosong; Mo, Zhaojun; Shi, Shaobo; Li, Lan; Yin, Shougen

2018-04-01

The surface-bound ligands of a semiconductor nanocrystal can affect its electron transition behavior. We investigate the photoluminescence (PL) properties of Cu-doped Zn-In-Se quantum dots (QDs) through the exchange of oleylamine with 6-mercaptohexanol (MCH). Fourier transform infrared and 1H nuclear magnetic resonance spectroscopies, and mass spectrometry reveal that the short-chain MCH molecules are bound to the QD surface. The emission peaks remain unchanged after ligand exchange, and the PL quantum yield is reduced from 49% to 38%. The effects of particle size and defect type on the change in PL behavior upon ligand substitution are excluded through high-resolution transmission electron microscopy, UV-Vis absorption, and PL spectroscopies. The origin of the decreased PL intensity is associated with increased ligand density and the stronger ligand electron-donating abilities of MCH-capped QDs that induce an increase in the nonradiative transition probability. A lower PL quenching transition temperature is observed for MCH-capped QDs and is associated with increasing electron-acoustic phonon coupling due to the lower melting temperature of MCH.

Study on the structural, optical, and electrical properties of the yellow light-emitting diode grown on free-standing (0001) GaN substrate

NASA Astrophysics Data System (ADS)

Deng, Gaoqiang; Zhang, Yuantao; Yu, Ye; Yan, Long; Li, Pengchong; Han, Xu; Chen, Liang; Zhao, Degang; Du, Guotong

2018-04-01

In this paper, GaN-based yellow light-emitting diodes (LEDs) were homoepitaxially grown on free-standing (0001) GaN substrates by metal-organic chemical vapor deposition. X-ray diffraction (XRD), photoluminescence (PL), and electroluminescence (EL) measurements were conducted to investigate the structural, optical, and electrical properties of the yellow LED. The XRD measurement results showed that the InGaN/GaN multiple quantum wells (MQWs) in the LED structure have good periodicity because the distinct MQWs related higher order satellite peaks can be clearly observed from the profile of 2θ-ω XRD scan. The low temperature (10 K) and room temperature PL measurement results yield an internal quantum efficiency of 16% for the yellow LED. The EL spectra of the yellow LED present well Gaussian distribution with relatively low linewidth (47-55 nm), indicating the homogeneous In-content in the InGaN quantum well layers in the yellow LED structure. It is believed that this work will aid in the future development of GaN on GaN LEDs with long emission wavelength.

1300 nm wavelength InAs quantum dot photodetector grown on silicon.

PubMed

Sandall, Ian; Ng, Jo Shien; David, John P R; Tan, Chee Hing; Wang, Ting; Liu, Huiyun

2012-05-07

The optical and electrical properties of InAs quantum dots epitaxially grown on a silicon substrate have been investigated to evaluate their potential as both photodiodes and avalanche photodiodes (APDs) operating at a wavelength of 1300 nm. A peak responsivity of 5 mA/W was observed at 1280 nm, with an absorption tail extending beyond 1300 nm, while the dark currents were two orders of magnitude lower than those reported for Ge on Si photodiodes. The diodes exhibited avalanche breakdown at 22 V reverse bias which is probably dominated by impact ionisation occurring in the GaAs and AlGaAs barrier layers. A red shift in the absorption peak of 61.2 meV was measured when the reverse bias was increased from 0 to 22 V, which we attributed to the quantum confined stark effect. This shift also leads to an increase in the responsivity at a fixed wavelength as the bias is increased, yielding a maximum increase in responsivity by a factor of 140 at the wavelength of 1365 nm, illustrating the potential for such a structure to be used as an optical modulator.

Cl2O photochemistry: ultraviolet/vis absorption spectrum temperature dependence and O(3P) quantum yield at 193 and 248 nm.

PubMed

Papanastasiou, Dimitrios K; Feierabend, Karl J; Burkholder, James B

2011-05-28

The photochemistry of Cl(2)O (dichlorine monoxide) was studied using measurements of its UV/vis absorption spectrum temperature dependence and the O((3)P) atom quantum yield, Φ(Cl(2)O)(O)(λ), in its photolysis at 193 and 248 nm. The Cl(2)O UV/vis absorption spectrum was measured over the temperature range 201-296 K between 200 and 500 nm using diode array spectroscopy. Cl(2)O absorption cross sections, σ(Cl(2)O)(λ,T), at temperatures <296 K were determined relative to its well established room temperature values. A wavelength and temperature dependent parameterization of the Cl(2)O spectrum using the sum of six Gaussian functions, which empirically represent transitions from the ground (1)A(1) electronic state to excited states, is presented. The Gaussian functions are found to correlate well with published theoretically calculated vertical excitation energies. O((3)P) quantum yields in the photolysis of Cl(2)O at 193 and 248 nm were measured using pulsed laser photolysis combined with atomic resonance fluorescence detection of O((3)P) atoms. O((3)P) quantum yields were measured to be 0.85 ± 0.15 for 193 nm photolysis at 296 K and 0.20 ± 0.03 at 248 nm, which was also found to be independent of temperature (220-352 K) and pressure (17 and 28 Torr, N(2)). The quoted uncertainties are at the 2σ (95% confidence) level and include estimated systematic errors. ClO radical temporal profiles obtained following the photolysis of Cl(2)O at 248 nm, as reported previously in Feierabend et al. [J. Phys. Chem. A 114, 12052, (2010)], were interpreted to establish a <5% upper-limit for the O + Cl(2) photodissociation channel, which indicates that O((3)P) is primarily formed in the three-body, O + 2Cl, photodissociation channel at 248 nm. The analysis also indirectly provided a Cl atom quantum yield of 1.2 ± 0.1 at 248 nm. The results from this work are compared with previous studies where possible. © 2011 American Institute of Physics

Terahertz quantum cascade laser as local oscillator in a heterodyne receiver.

PubMed

Hübers, Heinz-Wilhelm; Pavlov, S; Semenov, A; Köhler, R; Mahler, L; Tredicucci, A; Beere, H; Ritchie, D; Linfield, E

2005-07-25

Terahertz quantum cascade lasers have been investigated with respect to their performance as a local oscillator in a heterodyne receiver. The beam profile has been measured and transformed in to a close to Gaussian profile resulting in a good matching between the field patterns of the quantum cascade laser and the antenna of a superconducting hot electron bolometric mixer. Noise temperature measurements with the hot electron bolometer and a 2.5 THz quantum cascade laser yielded the same result as with a gas laser as local oscillator.

Divide and conquer approach to quantum Hamiltonian simulation

NASA Astrophysics Data System (ADS)

Hadfield, Stuart; Papageorgiou, Anargyros

2018-04-01

We show a divide and conquer approach for simulating quantum mechanical systems on quantum computers. We can obtain fast simulation algorithms using Hamiltonian structure. Considering a sum of Hamiltonians we split them into groups, simulate each group separately, and combine the partial results. Simulation is customized to take advantage of the properties of each group, and hence yield refined bounds to the overall simulation cost. We illustrate our results using the electronic structure problem of quantum chemistry, where we obtain significantly improved cost estimates under very mild assumptions.

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.

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 confinement effects across two-dimensional planes in MoS{sub 2} quantum dots

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

Gan, Z. X.; Liu, L. Z.; Wu, H. Y.

2015-06-08

The low quantum yield (∼10{sup −5}) has restricted practical use of photoluminescence (PL) from MoS{sub 2} composed of a few layers, but the quantum confinement effects across two-dimensional planes are believed to be able to boost the PL intensity. In this work, PL from 2 to 9 nm MoS{sub 2} quantum dots (QDs) is excluded from the solvent and the absorption and PL spectra are shown to be consistent with the size distribution. PL from MoS{sub 2} QDs is also found to be sensitive to aggregation due to the size effect.

Quantum non-Gaussianity and quantification of nonclassicality

NASA Astrophysics Data System (ADS)

Kühn, B.; Vogel, W.

2018-05-01

The algebraic quantification of nonclassicality, which naturally arises from the quantum superposition principle, is related to properties of regular nonclassicality quasiprobabilities. The latter are obtained by non-Gaussian filtering of the Glauber-Sudarshan P function. They yield lower bounds for the degree of nonclassicality. We also derive bounds for convex combinations of Gaussian states for certifying quantum non-Gaussianity directly from the experimentally accessible nonclassicality quasiprobabilities. Other quantum-state representations, such as s -parametrized quasiprobabilities, insufficiently indicate or even fail to directly uncover detailed information on the properties of quantum states. As an example, our approach is applied to multi-photon-added squeezed vacuum states.

Experimental demonstration of a quantum annealing algorithm for the traveling salesman problem in a nuclear-magnetic-resonance quantum simulator

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

Chen Hongwei; High Magnetic Field Laboratory, Hefei Institutes of Physical Science, Chinese Academy of Sciences, Hefei 230031; Kong Xi

The method of quantum annealing (QA) is a promising way for solving many optimization problems in both classical and quantum information theory. The main advantage of this approach, compared with the gate model, is the robustness of the operations against errors originated from both external controls and the environment. In this work, we succeed in demonstrating experimentally an application of the method of QA to a simplified version of the traveling salesman problem by simulating the corresponding Schroedinger evolution with a NMR quantum simulator. The experimental results unambiguously yielded the optimal traveling route, in good agreement with the theoretical prediction.

Decoherence and dissipation for a quantum system coupled to a local environment

NASA Technical Reports Server (NTRS)

Gallis, Michael R.

1994-01-01

Decoherence and dissipation in quantum systems has been studied extensively in the context of Quantum Brownian Motion. Effective decoherence in coarse grained quantum systems has been a central issue in recent efforts by Zurek and by Hartle and Gell-Mann to address the Quantum Measurement Problem. Although these models can yield very general classical phenomenology, they are incapable of reproducing relevant characteristics expected of a local environment on a quantum system, such as the characteristic dependence of decoherence on environment spatial correlations. I discuss the characteristics of Quantum Brownian Motion in a local environment by examining aspects of first principle calculations and by the construction of phenomenological models. Effective quantum Langevin equations and master equations are presented in a variety of representations. Comparisons are made with standard results such as the Caldeira-Leggett master equation.

Deterministic generation of multiparticle entanglement by quantum Zeno dynamics.

PubMed

Barontini, Giovanni; Hohmann, Leander; Haas, Florian; Estève, Jérôme; Reichel, Jakob

2015-09-18

Multiparticle entangled quantum states, a key resource in quantum-enhanced metrology and computing, are usually generated by coherent operations exclusively. However, unusual forms of quantum dynamics can be obtained when environment coupling is used as part of the state generation. In this work, we used quantum Zeno dynamics (QZD), based on nondestructive measurement with an optical microcavity, to deterministically generate different multiparticle entangled states in an ensemble of 36 qubit atoms in less than 5 microseconds. We characterized the resulting states by performing quantum tomography, yielding a time-resolved account of the entanglement generation. In addition, we studied the dependence of quantum states on measurement strength and quantified the depth of entanglement. Our results show that QZD is a versatile tool for fast and deterministic entanglement generation in quantum engineering applications. Copyright © 2015, American Association for the Advancement of Science.

Quantum information processing in the radical-pair mechanism: Haberkorn's theory violates the Ozawa entropy bound

NASA Astrophysics Data System (ADS)

Mouloudakis, K.; Kominis, I. K.

2017-02-01

Radical-ion-pair reactions, central for understanding the avian magnetic compass and spin transport in photosynthetic reaction centers, were recently shown to be a fruitful paradigm of the new synthesis of quantum information science with biological processes. We show here that the master equation so far constituting the theoretical foundation of spin chemistry violates fundamental bounds for the entropy of quantum systems, in particular the Ozawa bound. In contrast, a recently developed theory based on quantum measurements, quantum coherence measures, and quantum retrodiction, thus exemplifying the paradigm of quantum biology, satisfies the Ozawa bound as well as the Lanford-Robinson bound on information extraction. By considering Groenewold's information, the quantum information extracted during the reaction, we reproduce the known and unravel other magnetic-field effects not conveyed by reaction yields.

Anomalous negative magnetoresistance of two-dimensional electrons

NASA Astrophysics Data System (ADS)

Kanter, Jesse; Vitkalov, Sergey; Bykov, A. A.

2018-05-01

Effects of temperature T (6-18 K) and variable in situ static disorder on dissipative resistance of two-dimensional electrons are investigated in GaAs quantum wells placed in a perpendicular magnetic-field B⊥. Quantum contributions to the magnetoresistance, leading to quantum positive magnetoresistance (QPMR), are separated by application of an in-plane magnetic field. QPMR decreases considerably with both the temperature and the static disorder and is in good quantitative agreement with theory. The remaining resistance R decreases with the magnetic field exhibiting an anomalous polynomial dependence on B⊥:[R (B⊥) -R (0 ) ] =A (T ,τq) B⊥η where the power is η ≈1.5 ±0.1 in a broad range of temperatures and disorder. The disorder is characterized by electron quantum lifetime τq. The scaling factor A (T ,τq) ˜[κ(τq) +β (τq) T2] -1 depends significantly on both τq and T where the first term κ ˜τq-1/2 decreases with τq. The second term is proportional to the square of the temperature and diverges with increasing static disorder. Above a critical disorder the anomalous magnetoresistance is absent, and only a positive magnetoresistance, exhibiting no distinct polynomial behavior with the magnetic field, is observed. The presented model accounts memory effects and yields η = 3/2.

Quantum interference in laser-induced nonsequential double ionization

NASA Astrophysics Data System (ADS)

Quan, Wei; Hao, XiaoLei; Wang, YanLan; Chen, YongJu; Yu, ShaoGang; Xu, SongPo; Xiao, ZhiLei; Sun, RenPing; Lai, XuanYang; Hu, ShiLin; Liu, MingQing; Shu, Zheng; Wang, XiaoDong; Li, WeiDong; Becker, Wilhelm; Liu, XiaoJun; Chen, Jing

2017-09-01

Quantum interference plays an important role in various intense-laser-driven atomic phenomena, e.g., above-threshold ionization and high-order-harmonic generation, and provides a useful tool in ultrafast imaging of atomic and molecular structure and dynamics. However, it has eluded observation in nonsequential double ionization (NSDI), which serves as an ideal prototype to study electron-electron correlation. Thus far, NSDI usually could be well understood from a semiclassical perspective, where all quantum aspects have been ignored after the first electron has tunneled. Here we perform coincidence measurements for NSDI of xenon subject to laser pulses at 2400 nm. It is found that the intensity dependence of the asymmetry parameter between the yields in the second and fourth quadrants and those in the first and third quadrants of the electron-momentum-correlation distributions exhibits a peculiar fast oscillatory structure, which is beyond the scope of the semiclassical picture. Our theoretical analysis indicates that this oscillation can be attributed to interference between the contributions of different excited states in the recollision-excitation-with-subsequent-ionization channel. Our work demonstrates the significant role of quantum interference in NSDI and may create an additional pathway towards manipulation and imaging of the ultrafast atomic and molecular dynamics in intense laser fields.

Optical and Photophysical Investigation of (2E)-1-(2,5-Dimethylfuran-3-Yl)-3-(9-Ethyl-9H-Carbazol-3-Yl)Prop-2-en-1-One (DEPO) by Spectrofluorometer in Organized Medium.

PubMed

Asiri, Abdullah M; Al-Dies, Al-Anood M; Khan, Salman A

2017-07-01

(2E)-1-(2,5-dimethylfuran-3-yl)-3-(9-ethyl-9H-carbazol-3-yl)prop-2-en-1-one (DEPO) was prepared by the reaction of 9-ethyl-9H-carbazole-3-carbaldehyde with 1-(2,5-dimethylfuran-3-yl)ethanone under microwave irradiation. The structure of DEPO was established experimentally by EI-MS, FT-IR, 1 H and 13 C NMR spectral studies. Electronic absorption and emission spectra of DEPO were studied in different solvents on the basis of polarities, and the obtain data were used to determine the solvatochromic properties such as extinction coefficient, oscillator strength, transition dipole moment, stokes shift, fluorescence quantum yield and photochemical quantum yield. Photochemical quantum yield (Φ c ) of DEPO dye was determined in different solvent. The dye comparatively photostable in DMSO but undergoes photodecomposition in chloro methane solvents. The DEPO dye may be use as probe or quencher to determine critical micelle concentration (CMC) of cetyltri methyl ammonium bromide (CTAB) and sodium dodecyl sulfate (SDS).

Synthesis, quantitative structure-property relationship study of novel fluorescence active 2-pyrazolines and application.

PubMed

Girgis, Adel S; Basta, Altaf H; El-Saied, Houssni; Mohamed, Mohamed A; Bedair, Ahmad H; Salim, Ahmad S

2018-03-01

A variety of fluorescence-active fluorinated pyrazolines 13-33 was synthesized in good yields through cyclocondensation reaction of propenones 1-9 with aryl hydrazines 10-12 . Some of the synthesized compounds provided promising fluorescence properties with quantum yield ( Φ ) higher than that of quinine sulfate (standard reference). Quantitative structure-property relationship studies were undertaken supporting the exhibited fluorescence properties and estimating the parameters governing properties. Five synthesized fluorescence-active pyrazolines ( 13 , 15 , 18 , 19 and 23 ) with variable Φ were selected for treating two types of paper sheets (Fabriano and Bible paper). These investigated fluorescence compounds, especially compounds 19 and 23 , provide improvements in strength properties of paper sheets. Based on the observed performance they can be used as markers in security documents.

Synthesis, quantitative structure–property relationship study of novel fluorescence active 2-pyrazolines and application

PubMed Central

Girgis, Adel S.; El-Saied, Houssni; Mohamed, Mohamed A.; Bedair, Ahmad H.; Salim, Ahmad S.

2018-01-01

A variety of fluorescence-active fluorinated pyrazolines 13–33 was synthesized in good yields through cyclocondensation reaction of propenones 1–9 with aryl hydrazines 10–12. Some of the synthesized compounds provided promising fluorescence properties with quantum yield (Φ) higher than that of quinine sulfate (standard reference). Quantitative structure–property relationship studies were undertaken supporting the exhibited fluorescence properties and estimating the parameters governing properties. Five synthesized fluorescence-active pyrazolines (13, 15, 18, 19 and 23) with variable Φ were selected for treating two types of paper sheets (Fabriano and Bible paper). These investigated fluorescence compounds, especially compounds 19 and 23, provide improvements in strength properties of paper sheets. Based on the observed performance they can be used as markers in security documents. PMID:29657796

Synthesis, quantitative structure-property relationship study of novel fluorescence active 2-pyrazolines and application

NASA Astrophysics Data System (ADS)

Girgis, Adel S.; Basta, Altaf H.; El-Saied, Houssni; Mohamed, Mohamed A.; Bedair, Ahmad H.; Salim, Ahmad S.

2018-03-01

A variety of fluorescence-active fluorinated pyrazolines 13-33 was synthesized in good yields through cyclocondensation reaction of propenones 1-9 with aryl hydrazines 10-12. Some of the synthesized compounds provided promising fluorescence properties with quantum yield (Φ) higher than that of quinine sulfate (standard reference). Quantitative structure-property relationship studies were undertaken supporting the exhibited fluorescence properties and estimating the parameters governing properties. Five synthesized fluorescence-active pyrazolines (13, 15, 18, 19 and 23) with variable Φ were selected for treating two types of paper sheets (Fabriano and Bible paper). These investigated fluorescence compounds, especially compounds 19 and 23, provide improvements in strength properties of paper sheets. Based on the observed performance they can be used as markers in security documents.

Factors Affecting the Production of Aromatic Immonium Ions in MALDI 157 nm Photodissociation Studies

NASA Astrophysics Data System (ADS)

DeGraan-Weber, Nick; Ashley, Daniel C.; Keijzer, Karlijn; Baik, Mu-Hyun; Reilly, James P.

2016-05-01

Immonium ions are commonly observed in the high energy fragmentation of peptide ions. In a MALDI-TOF/TOF mass spectrometer, singly charged peptides photofragmented with 157 nm VUV light yield a copious abundance of immonium ions, especially those from aromatic residues. However, their intensities may vary from one peptide to another. In this work, the effect of varying amino acid position, peptide length, and peptide composition on immonium ion yield is investigated. Internal immonium ions are found to have the strongest intensity, whereas immonium ions arising from C-terminal residues are the weakest. Peptide length and competition among residues also strongly influence the immonium ion production. Quantum calculations provide insights about immonium ion structures and the fragment ion conformations that promote or inhibit immonium ion formation.

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.

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.

Photophysics and catalysis of porphyrinoids

NASA Astrophysics Data System (ADS)

Aggarwal, Amit

Organic nanoparticles (ONP) of metalloporphyrins can be versatile catalysts for the selective oxidation of alkenes and other hydrocarbons. Herein, we report the catalytic activity of ONP of 5,10,15,20-tetrakis-[4-(1'H,1'H,2'H,2'H-heptadecafluorodecane-1-thiol)-2,3,5,6-tetrafluorophenyl] porphyrinato iron(III), Fe(III)TPPF84, and 5,10,15,20-tetakis-(2,3,4,5,6-pentafluorophenyl) porphyrinato manganese(III), Mn(III)TPPF20, for cyclohexene oxidation using molecular oxygen as an oxidant in water under ambient conditions. Sequential dipping of indium-tin-oxide electrodes into solutions of tetra cationic porphyrins and tetra anionic polyoxometalates results in the controlled formation of nm thick films. The potential applications of these robust films on electrodes range from catalysts to sensors. This chapter focuses on the electrochemistry of the multilayered films where it is found that the oxidation and reduction potentials of each species remain largely the same as found in solution. Photophysical properties of Porphyrinoids bearing four rigid hydrogen bonding motifs on the meso positions, self-assembled into a cofacial cage with four complementary bis(decyl)melamine units in dry solvents are presented here. Self-assembly was investigated by NMR spectroscopy, dynamic light scattering, and atomic force microscopy. The phototphysical properties of the cage formation involve the measurement of their absorption and emission spectra and the fluorescence life time in dry THF. The hydrocarbon chains on the bis(decyl)melamine mediate the formation of nanofilms on surfaces as the solvent slowly evaporates. A systematic study of the photophysical properties of a series of porphyrinoids is presented. The role of the location of a heavy atom in shunting the excited state from the singlet to the triplet manifolds is compared for three cases. It is well known that Pt(II) metalloporphyrins do not fluoresce. For meso pyridyl porphyrins, the fluorescence quantum yield decreases as the number of coordinatively attached Pt(II) complexes increase from 0-4, but the tetracoordinated species retains about 30% of the fluorescence. Covalently attaching a heavy metal complex e.g. Pt(II) complex to the macrocycle by an organometalic bond at the peripheral meso position causes greater than a 20-fold decrease in fluorescence quantum yield and may enhance some internal conversion to the ground state. For comparison, the fluorescence quantum yield decreases somewhat as the number of pyridyl groups on the meso positions increase 0-4. We also evaluate the photophysical properties of a series of porphyrins with nitro groups on the beta pyrrole position and on the meso phenyl group, which also quenches the fluorescence. These studies bear on the use of metal ions to enhance the photophysical properties of these dyes as photodynamic therapeutics and for supramolecular systems, while the nitrated macrocycles have potential application in non linear optics. The photophysical properties of non-hydrolysable tetra- thioglycosylated conjugates of chlorin (CGlc4), isobacteriochlorin (IGlc4) and bacteriochlorin (BGlc4) and core F20 platforms are reported here. These studies involve the measurement of absorption and emission spectra, fluorescence quantum yield, singlet oxygen quantum yield, and singlet state life time in three different solvents: phosphate buffer saline (PBS), ethanol, and ethylacetate. Compared to the porphyrin in PBS, CGlc4 has a markedly greater absorbance of red light near 650 nm and a 6-fold increase in fluorescence quantum yield; whereas IGlc4 has broad Q bands and a 12-fold increase in fluorescence quantum yield. Since IGlc4 CGlc4 very slowly bleach, these properties may enable their use as fluorescent tags to track biological processes. BGlc4 has a similar fluorescence quantum yield to PGlc4, (<10%), but the lowest energy absorption/emission peaks of BGlc4 are considerably red shifted to near 730 nm with a nearly 50-fold greater absorbance, which may allow this conjugate to be an effective PDT agent. (Abstract shortened by UMI.)

1,3-Diphenylisobenzofuran: a Model Chromophore for Singlet Fission

DOE PAGES

Johnson, Justin C.; Michl, Josef

2017-09-11

In this review we first provide an introductory description of the singlet fission phenomenon and then describe the ground and electronically excited states of the parent 1,3-diphenylisobenzofuran chromophore (1) and about a dozen of its derivatives. A discussion of singlet fission in thin polycrystalline layers of these materials follows. The highest quantum yield of triplet formation by singlet fission, 200% at 80 K, is found in one of the two known crystal modification of the parent. In the other modification and in many derivatives, excimer formation competes successfully and triplet yields are low. A description of solution photophysics of covalentmore » dimers is described in the next section. Triplet yields are very low, but interesting phenomena are uncovered. One is an observation of a separated-charges (charge-transfer) intermediate in highly polar solvents. The other is an observation of excitation isomerism in both singlet and triplet states, where in one isomer the excitation is delocalized over both halves of the covalent dimer, whereas in the other it is localized on one of the halves. Finally, in the last section we present the operation of a simple device illustrating the use of triplets generated by singlet fission for charge separation.« less

Quantum-capacity-approaching codes for the detected-jump channel

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

Grassl, Markus; Wei Zhaohui; Ji Zhengfeng

2010-12-15

The quantum-channel capacity gives the ultimate limit for the rate at which quantum data can be reliably transmitted through a noisy quantum channel. Degradable quantum channels are among the few channels whose quantum capacities are known. Given the quantum capacity of a degradable channel, it remains challenging to find a practical coding scheme which approaches capacity. Here we discuss code designs for the detected-jump channel, a degradable channel with practical relevance describing the physics of spontaneous decay of atoms with detected photon emission. We show that this channel can be used to simulate a binary classical channel with both erasuresmore » and bit flips. The capacity of the simulated classical channel gives a lower bound on the quantum capacity of the detected-jump channel. When the jump probability is small, it almost equals the quantum capacity. Hence using a classical capacity-approaching code for the simulated classical channel yields a quantum code which approaches the quantum capacity of the detected-jump channel.« less

Design and Synthesis of Antiblinking and Antibleaching Quantum Dots in Multiple Colors via Wave Function Confinement.

PubMed

Cao, Hujia; Ma, Junliang; Huang, Lin; Qin, Haiyan; Meng, Renyang; Li, Yang; Peng, Xiaogang

2016-12-07

Single-molecular spectroscopy reveals that photoluminescence (PL) of a single quantum dot blinks, randomly switching between bright and dim/dark states under constant photoexcitation, and quantum dots photobleach readily. These facts cast great doubts on potential applications of these promising emitters. After ∼20 years of efforts, synthesis of nonblinking quantum dots is still challenging, with nonblinking quantum dots only available in red-emitting window. Here we report synthesis of nonblinking quantum dots covering most part of the visible window using a new synthetic strategy, i.e., confining the excited-state wave functions of the core/shell quantum dots within the core quantum dot and its inner shells (≤ ∼5 monolayers). For the red-emitting ones, the new synthetic strategy yields nonblinking quantum dots with small sizes (∼8 nm in diameter) and improved nonblinking properties. These new nonblinking quantum dots are found to be antibleaching. Results further imply that the PL blinking and photobleaching of quantum dots are likely related to each other.

Unified field theory from the classical wave equation: Preliminary application to atomic and nuclear structure

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

Múnera, Héctor A., E-mail: hmunera@hotmail.com; Retired professor, Department of Physics, Universidad Nacional de Colombia, Bogotá, Colombia, South America

2016-07-07

It is postulated that there exists a fundamental energy-like fluid, which occupies the flat three-dimensional Euclidean space that contains our universe, and obeys the two basic laws of classical physics: conservation of linear momentum, and conservation of total energy; the fluid is described by the classical wave equation (CWE), which was Schrödinger’s first candidate to develop his quantum theory. Novel solutions for the CWE discovered twenty years ago are nonharmonic, inherently quantized, and universal in the sense of scale invariance, thus leading to quantization at all scales of the universe, from galactic clusters to the sub-quark world, and yielding amore » unified Lorentz-invariant quantum theory ab initio. Quingal solutions are isomorphic under both neo-Galilean and Lorentz transformations, and exhibit nother remarkable property: intrinsic unstability for large values of ℓ (a quantum number), thus limiting the size of each system at a given scale. Unstability and scale-invariance together lead to nested structures observed in our solar system; unstability may explain the small number of rows in the chemical periodic table, and nuclear unstability of nuclides beyond lead and bismuth. Quingal functions lend mathematical basis for Boscovich’s unified force (which is compatible with many pieces of evidence collected over the past century), and also yield a simple geometrical solution for the classical three-body problem, which is a useful model for electronic orbits in simple diatomic molecules. A testable prediction for the helicoidal-type force is suggested.« less

Photoactive high explosives: linear and nonlinear photochemistry of petrin tetrazine chloride.

PubMed

Greenfield, Margo T; McGrane, Shawn D; Bolme, Cindy A; Bjorgaard, Josiah A; Nelson, Tammie R; Tretiak, Sergei; Scharff, R Jason

2015-05-21

Pentaerythritol tetranitrate (PETN), a high explosive, initiates with traditional shock and thermal mechanisms. In this study, the tetrazine-substituted derivative of PETN, pentaerythritol trinitrate chlorotetrazine (PetrinTzCl), is being investigated for a photochemical initiation mechanism that could allow control over the chemistry contributing to decomposition leading to initiation. PetrinTzCl exhibits a photochemical quantum yield (QYPC) at 532 nm not evident with PETN. Using static spectroscopic methods, we observe energy absorption on the tetrazine (Tz) ring that results in photodissociation yielding N2, Cl-CN, and Petrin-CN as the major photoproducts. The QYPC was enhanced with increasing irradiation intensity. Experiment and theoretical calculations imply this excitation mechanism follows sequential photon absorption. Dynamic simulations demonstrate that the relaxation mechanism leading to the observed photochemistry in PetrinTzCl is due to vibrational excitation during internal conversion. PetrinTzCl's single photon stability and intensity dependence suggest this material could be stable in ambient lighting, yet possible to initiate with short-pulsed lasers.

Unravelling the Electronic State of NO2 Product in Ultrafast Photodissociation of Nitromethane.

PubMed

Adachi, Shunsuke; Kohguchi, Hiroshi; Suzuki, Toshinori

2018-01-18

The primary photochemical reaction of nitromethane (NM) after ππ* excitation is known to be C-N bond cleavage (CH 3 NO 2 + hν → CH 3 + NO 2 ). On the other hand, NO 2 can be formed in both the ground and excited states, and identification of the electronic state of the NO 2 product has been a central subject in the experimental and theoretical studies. Here we present time-resolved photoelectron spectroscopy using vacuum-ultraviolet probe pulses to observe all transient electronic states of NM and the reaction products. The result indicates that ultrafast internal conversion occurs down to S 1 and S 0 within 24 fs, and the dissociation proceeds on the S 1 surface (τ diss ≲ 50 fs), leading to comparable product yields of NO 2 (A) and NO 2 (X). The overall dissociation quantum yield within our observation time window (<2 ps) is estimated to be 0.29.

Uncertainty relation for non-Hamiltonian quantum systems

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

Tarasov, Vasily E.

2013-01-15

General forms of uncertainty relations for quantum observables of non-Hamiltonian quantum systems are considered. Special cases of uncertainty relations are discussed. The uncertainty relations for non-Hamiltonian quantum systems are considered in the Schroedinger-Robertson form since it allows us to take into account Lie-Jordan algebra of quantum observables. In uncertainty relations, the time dependence of quantum observables and the properties of this dependence are discussed. We take into account that a time evolution of observables of a non-Hamiltonian quantum system is not an endomorphism with respect to Lie, Jordan, and associative multiplications.

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.

A molecular-field approximation for quantum crystals. Ph.D. Thesis; [considering ground state properties

NASA Technical Reports Server (NTRS)

Danilowicz, R.

1973-01-01

Ground-state properties of quantum crystals have received considerable attention from both theorists and experimentalists. The theoretical results have varied widely with the Monte Carlo calculations being the most successful. The molecular field approximation yields ground-state properties which agree closely with the Monte Carlo results. This approach evaluates the dynamical behavior of each pair of molecules in the molecular field of the other N-2 molecules. In addition to predicting ground-state properties that agree well with experiment, this approach yields data on the relative importance of interactions of different nearest neighbor pairs.

Optical study of HgCdTe infrared photodetectors using internal photoemission spectroscopy

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

Lao, Yan-Feng; Unil Perera, A. G., E-mail: uperera@gsu.edu; Wijewarnasuriya, Priyalal S.

2014-03-31

We report a study of internal photoemission spectroscopy (IPE) applied to a n-type Hg{sub 1−x}Cd{sub x}Te/Hg{sub 1−y}Cd{sub y}Te heterojunction. An exponential line-shape of the absorption tail in HgCdTe is identified by IPE fittings of the near-threshold quantum yield spectra. The reduction of quantum yield (at higher photon energy) below the fitting value is explained as a result of carrier-phonon scatterings. In addition, the obtained bias independence of the IPE threshold indicates a negligible electron barrier at the heterojunction interface.

pHP-Tethered N-Acyl Carbamate: A Photocage for Nicotinamide.

PubMed

Salahi, Farbod; Purohit, Vatsal; Ferraudi, Guillermo; Stauffacher, Cynthia; Wiest, Olaf; Helquist, Paul

2018-05-04

The synthesis of a new photocaged nicotinamide having an N-acyl carbamate linker and a p-hydroxyphenacyl (pHP) chromophore is described. The photophysical and photochemical studies showed an absorption maximum at λ = 330 nm and a quantum yield for release of 11% that are dependent upon both pH and solvent. While the acyl carbamate releases nicotinamide efficiently, a simpler amide linker was inert to photocleavage. This photocaged nicotinamide has significant advantages with respect to quantum yield, absorbance wavelength, rate of release, and solubility that make it the first practical example of a photocaged amide.

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.

Dilepton production from hot hadronic matter in nonequilibrium

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

Schenke, B.; Greiner, C.

2006-03-15

The influence of time-dependent medium modifications of low-mass vector mesons on dilepton production is investigated within a nonequilibrium quantum field-theoretical description on the basis of the Kadanoff-Baym equations. Time scales for the adaption of the spectral properties to changing self-energies are given, and, under use of a model for the fireball evolution, nonequilibrium dilepton yields from the decay of {rho} and {omega} mesons are calculated. In a comparison of these yields, those from calculations that assume instantaneous (Markovian) adaption to the changing-medium quantum-mechanical memory effects turn out to be important.

Do genotypic differences in thermotolerance plasticity correspond with water-induced differences in yield and photosynthetic stability for field-grown upland cotton?

USDA-ARS?s Scientific Manuscript database

To determine if cultivar differences in thermotolerance plasticity of photosystem II promote yield or photosynthetic stability when variability in both parameters is water-induced, the temperature response of maximum quantum yield of photosystem II (Fv/Fm) was evaluated for two cotton cultivars (FM ...

Revisiting the quantum Szilard engine with fully quantum considerations

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

Li, Hai; School of Information and Electronics Engineering, Shandong Institute of Business and Technology, Yantai 264000; Zou, Jian, E-mail: zoujian@bit.edu.cn

2012-12-15

By considering level shifting during the insertion process we revisit the quantum Szilard engine (QSZE) with fully quantum consideration. We derive the general expressions of the heat absorbed from thermal bath and the total work done to the environment by the system in a cycle with two different cyclic strategies. We find that only the quantum information contributes to the absorbed heat, and the classical information acts like a feedback controller and has no direct effect on the absorbed heat. This is the first demonstration of the different effects of quantum information and classical information for extracting heat from themore » bath in the QSZE. Moreover, when the well width L{yields}{infinity} or the temperature of the bath T{yields}{infinity} the QSZE reduces to the classical Szilard engine (CSZE), and the total work satisfies the relation W{sub tot}=k{sub B}Tln2 as obtained by Sang Wook Kim et al. [S.W. Kim, T. Sagawa, S. De Liberato, M. Ueda, Phys. Rev. Lett. 106 (2011) 070401] for one particle case. - Highlights: Black-Right-Pointing-Pointer For the first time analyze the QSZE by considering energy level shifts. Black-Right-Pointing-Pointer Find different roles played by classical and quantum information in the QSZE. Black-Right-Pointing-Pointer The amount of work extracted depends on the cyclic strategies of the QSZE. Black-Right-Pointing-Pointer Verify that the QSZE will reduce to the CSZE in the classical limits.« less

Non-Abelian fermionization and fractional quantum Hall transitions

NASA Astrophysics Data System (ADS)

Hui, Aaron; Mulligan, Michael; Kim, Eun-Ah

2018-02-01

There has been a recent surge of interest in dualities relating theories of Chern-Simons gauge fields coupled to either bosons or fermions within the condensed matter community, particularly in the context of topological insulators and the half-filled Landau level. Here, we study the application of one such duality to the long-standing problem of quantum Hall interplateaux transitions. The key motivating experimental observations are the anomalously large value of the correlation length exponent ν ≈2.3 and that ν is observed to be superuniversal, i.e., the same in the vicinity of distinct critical points [Sondhi et al., Rev. Mod. Phys. 69, 315 (1997), 10.1103/RevModPhys.69.315]. Duality motivates effective descriptions for a fractional quantum Hall plateau transition involving a Chern-Simons field with U (Nc) gauge group coupled to Nf=1 fermion. We study one class of theories in a controlled limit where Nf≫Nc and calculate ν to leading nontrivial order in the absence of disorder. Although these theories do not yield an anomalously large exponent ν within the large Nf≫Nc expansion, they do offer a new parameter space of theories that is apparently different from prior works involving Abelian Chern-Simons gauge fields [Wen and Wu, Phys. Rev. Lett. 70, 1501 (1993), 10.1103/PhysRevLett.70.1501; Chen et al., Phys. Rev. B 48, 13749 (1993), 10.1103/PhysRevB.48.13749].

Comparison of the iterated equation of motion approach and the density matrix formalism for the quantum Rabi model

NASA Astrophysics Data System (ADS)

Kalthoff, Mona; Keim, Frederik; Krull, Holger; Uhrig, Götz S.

2017-05-01

The density matrix formalism and the equation of motion approach are two semi-analytical methods that can be used to compute the non-equilibrium dynamics of correlated systems. While for a bilinear Hamiltonian both formalisms yield the exact result, for any non-bilinear Hamiltonian a truncation is necessary. Due to the fact that the commonly used truncation schemes differ for these two methods, the accuracy of the obtained results depends significantly on the chosen approach. In this paper, both formalisms are applied to the quantum Rabi model. This allows us to compare the approximate results and the exact dynamics of the system and enables us to discuss the accuracy of the approximations as well as the advantages and the disadvantages of both methods. It is shown to which extent the results fulfill physical requirements for the observables and which properties of the methods lead to unphysical results.

Quantum chemistry-assisted synthesis route development

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

Hori, Kenji; Sumimoto, Michinori; Murafuji, Toshihiro

2015-12-31

We have been investigating “quantum chemistry-assisted synthesis route development” using in silico screenings and applied the method to several targets. Another example was conducted to develop synthesis routes for a urea derivative, namely 1-(4-(trifluoromethyl)-2-oxo-2H-chromen-7-yl)urea. While five synthesis routes were examined, only three routes passed the second in silico screening. Among them, the reaction of 7-amino-4-(trifluoromethyl)-2H-chromen-2-one and O-methyl carbamate with BF{sub 3} as an additive was ranked as the first choice for synthetic work. We were able to experimentally obtain the target compound even though its yield was as low as 21 %. The theoretical result was thus consistent with thatmore » observed. The summary of transition state data base (TSDB) is also provided. TSDB is the key to reducing time of in silico screenings.« less

Photosynthesis in chlorolichens: the influence of the habitat light regime.

PubMed

Piccotto, Massimo; Tretiach, Mauro

2010-11-01

The hypothesis that CO(2) gas exchange and chlorophyll a fluorescence (ChlaF) of lichens vary according to the light regimes of their original habitat, as observed in vascular plants, was tested by analysing the photosynthetic performance of 12 populations of seven dorsoventral, foliose lichens collected from open, south-exposed rocks to densely shaded forests. Light response curves were induced at optimum thallus water content and ChlaF emission curves at the species-specific photon flux at which the quantum yield of CO(2) assimilation is the highest and is saturating the photosynthetic process. Photosynthetic pigments were quantified in crude extracts. The results confirm that the maximum rate of gross photosynthesis is correlated with the chlorophyll content of lichens, which is influenced by light as well as by nitrogen availability. Like leaves, shade tolerant lichens emit more ChlaF than sun-loving ones, whereas the photosynthetic quantum conversion is higher in the latter.

Probing Nonrelativistic QCD Factorization in Polarized J/ψ Photoproduction at Next-to-Leading Order

NASA Astrophysics Data System (ADS)

Butenschoen, Mathias; Kniehl, Bernd A.

2011-12-01

We analyze the polarization observables of J/ψ photoproduction at next-to-leading order within the factorization formalism of nonrelativistic quantum chromodynamics (NRQCD). This is a complete next-to-leading-order study of heavy-quarkonium polarization including the full relativistic corrections due to the intermediate S0[8]1, S1[8]3, and PJ[8]3 color-octet states closing a gap in the worldwide endeavor to test NRQCD factorization at the quantum level. We present theoretical predictions in the helicity, target, and Collins-Soper frames of DESY HERA, evaluated using the color-octet long-distance matrix elements previously extracted through a global fit to experimental data of unpolarized J/ψ production, and confront them with recent measurements by the H1 and ZEUS Collaborations. We find the overall agreement to be satisfactory but the case for NRQCD to be not as strong as for the J/ψ yield.

Leveraging Nanocavity Harmonics for Control of Optical Processes in 2D Semiconductors

DOE PAGES

Akselrod, Gleb M.; Ming, Tian; Argyropoulos, Christos; ...

2015-04-07

Optical cavities with multiple tunable resonances have the potential to provide unique electromagnetic environments at two or more distinct wavelengths–critical for control of optical processes such as nonlinear generation, entangled photon generation, or photoluminescence (PL) enhancement. Here, we show a plasmonic nanocavity based on a nanopatch antenna design that has two tunable resonant modes in the visible spectrum separated by 350 nm and with line widths of ~60 nm. The importance of utilizing two resonances simultaneously is demonstrated by integrating monolayer MoS 2, a two-dimensional semiconductor, into the colloidally synthesized nanocavities. Here, we observe a 2000-fold enhancement in the PLmore » intensity of MoS 2– which has intrinsically low absorption and small quantum yield–at room temperature, enabled by the combination of tailored absorption enhancement at the first harmonic and PL quantum-yield enhancement at the fundamental resonance.« less

Emission efficiency limit of Si nanocrystals

PubMed Central

Limpens, Rens; Luxembourg, Stefan L.; Weeber, Arthur W.; Gregorkiewicz, Tom

2016-01-01

One of the important obstacles on the way to application of Si nanocrystals for development of practical devices is their typically low emissivity. In this study we explore the limits of external quantum yield of photoluminescence of solid-state dispersions of Si nanocrystals in SiO2. By making use of a low-temperature hydrogen passivation treatment we demonstrate a maximum emission quantum efficiency of approximately 35%. This is the highest value ever reported for this type of material. By cross-correlating PL lifetime with EQE values, we obtain a comprehensive understanding of the efficiency limiting processes induced by Pb-defects. We establish that the observed record efficiency corresponds to an interface density of Pb-centers of 1.3 × 1012 cm12, which is 2 orders of magnitude higher than for the best Si/SiO2 interface. This result implies that Si nanocrystals with up to 100% emission efficiency are feasible. PMID:26786062

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.

Realization of a Cascaded Quantum System: Heralded Absorption of a Single Photon Qubit by a Single-Electron Charged Quantum Dot.

PubMed

Delteil, Aymeric; Sun, Zhe; Fält, Stefan; Imamoğlu, Atac

2017-04-28

Photonic losses pose a major limitation for the implementation of a quantum state transfer between nodes of a quantum network. A measurement that heralds a successful transfer without revealing any information about the qubit may alleviate this limitation. Here, we demonstrate the heralded absorption of a single photonic qubit, generated by a single neutral quantum dot, by a single-electron charged quantum dot that is located 5 m away. The transfer of quantum information to the spin degree of freedom takes place upon the emission of a photon; for a properly chosen or prepared quantum dot, the detection of this photon yields no information about the qubit. We show that this process can be combined with local operations optically performed on the destination node by measuring classical correlations between the absorbed photon color and the final state of the electron spin. Our work suggests alternative avenues for the realization of quantum information protocols based on cascaded quantum systems.

Quantum and classical noise in practical quantum-cryptography systems based on polarization-entangled photons

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

Castelletto, S.; Degiovanni, I.P.; Rastello, M.L.

2003-02-01

Quantum-cryptography key distribution (QCKD) experiments have been recently reported using polarization-entangled photons. However, in any practical realization, quantum systems suffer from either unwanted or induced interactions with the environment and the quantum measurement system, showing up as quantum and, ultimately, statistical noise. In this paper, we investigate how an ideal polarization entanglement in spontaneous parametric down-conversion (SPDC) suffers quantum noise in its practical implementation as a secure quantum system, yielding errors in the transmitted bit sequence. Since all SPDC-based QCKD schemes rely on the measurement of coincidence to assert the bit transmission between the two parties, we bundle up themore » overall quantum and statistical noise in an exhaustive model to calculate the accidental coincidences. This model predicts the quantum-bit error rate and the sifted key and allows comparisons between different security criteria of the hitherto proposed QCKD protocols, resulting in an objective assessment of performances and advantages of different systems.« less

MARY spectroscopy in the presence of coordination compound Zn(hfac) 2(PPO) 2

NASA Astrophysics Data System (ADS)

Sergey, N. V.; Burdukov, A. B.; Pervukhina, N. V.; Kuibida, L. V.; Pozdnyakov, I. P.; Stass, D. V.

2011-02-01

MARY spectroscopy is finding increasing use in the studies of transient organic radical ions and their reactions. Extending this technique to organometallic species will broaden the class of potential target compounds and can help answer important mechanistic questions in organometallic and spin chemistry. We probed this approach using a tailored Zn(hfac)2(PPO)2 complex. The synthesized complex has quantum yield and fluorescence lifetime (n-decane solution) φ ∼0.8 and τ ∼1.3 ns, respectively. For this type of complex it is the first observation of MARY spectra different from those of free ligand, thus implying participation of the complex in the development of the observed signal.

Quantum walled Brauer algebra: commuting families, Baxterization, and representations

NASA Astrophysics Data System (ADS)

Semikhatov, A. M.; Tipunin, I. Yu

2017-02-01

For the quantum walled Brauer algebra, we construct its Specht modules and (for generic parameters of the algebra) seminormal modules. The latter construction yields the spectrum of a commuting family of Jucys-Murphy elements. We also propose a Baxterization prescription; it involves representing the quantum walled Brauer algebra in terms of morphisms in a braided monoidal category and introducing parameters into these morphisms, which allows constructing a ‘universal transfer matrix’ that generates commuting elements of the algebra.

New and Better Near-Infrared Detectors for JWST Near Infrared Spectrograph

NASA Technical Reports Server (NTRS)

Rauscher, Bernard J.; Mott, D. Brent; Wen, Yiting; Linder, Don; Greenhouse, Matthew A.; Hill, Robert J.

2014-01-01

ESA and NASA recently selected two 5 m cutoff Teledyne H2RG sensor chip assemblies (SCA) for flight on the James Webb Space Telescope (JWST) Near Infrared Spectrograph (NIRSpec). These HgCdTe SCAs incorporate Teledynes improved barrier layer design that eliminates the degradation that affected earlier JWST H2RGs(Rauscher et al. 2012a). The better indium barrier, together with other design changes, has improved the performance and reliability of JWSTs SCAs. In this article, we describe the measured performance characteristics that most directly affect scientific observations including read noise, total noise, dark current, quantum efficiency (QE), and image persistence. As part of measuring QE, we measured the quantum yield as a function of photon energy,, and found that it exceeds unity for photon energies E (2.65.2) Eg, where Eg is the HgCdTe bandgap energy. This corresponds to. 2 m for NIRSpecs 5 m cutoff HgCdTe. Our measurements agree well with a previous measurement by McCullough et al. (2008) for. 1.3. For 1.3, we find a slower increase in with photon energy than McCullough et al. did. However, and as McCullough et al. note, their two state model of the yield process is not valid for large 1.

Augmented Quantum Yield of a 2D Monolayer Photodetector by Surface Plasmon Coupling.

PubMed

Bang, Seungho; Duong, Ngoc Thanh; Lee, Jubok; Cho, Yoo Hyun; Oh, Hye Min; Kim, Hyun; Yun, Seok Joon; Park, Chulho; Kwon, Min-Ki; Kim, Ja-Yeon; Kim, Jeongyong; Jeong, Mun Seok

2018-04-11

Monolayer (1L) transition metal dichalcogenides (TMDCs) are promising materials for nanoscale optoelectronic devices because of their direct band gap and wide absorption range (ultraviolet to infrared). However, 1L-TMDCs cannot be easily utilized for practical optoelectronic device applications (e.g., photodetectors, solar cells, and light-emitting diodes) because of their extremely low optical quantum yields (QYs). In this investigation, a high-gain 1L-MoS 2 photodetector was successfully realized, based on the surface plasmon (SP) of the Ag nanowire (NW) network. Through systematic optical characterization of the hybrid structure consisting of a 1L-MoS 2 and the Ag NW network, it was determined that a strong SP and strain relaxation effect influenced a greatly enhanced optical QY. The photoluminescence (PL) emission was drastically increased by a factor of 560, and the main peak was shifted to the neutral exciton of 1L-MoS 2 . Consequently, the overall photocurrent of the hybrid 1L-MoS 2 photodetector was observed to be 250 times better than that of the pristine 1L-MoS 2 photodetector. In addition, the photoresponsivity and photodetectivity of the hybrid photodetector were effectively improved by a factor of ∼1000. This study provides a new approach for realizing highly efficient optoelectronic devices based on TMDCs.

Large transient nonproton ion movements in purple membrane suspensions are abolished by solubilization in Triton X-100.

PubMed Central

Marinetti, T; Mauzerall, D

1986-01-01

Light-induced release/uptake of both protons and other ions cause transient changes in conductivity in suspensions of purple membrane (PM) fragments (Marinetti, Tim, and David Mauzerall, 1983, Proc. Natl. Acad. Sci. USA, 80:178-180). We find that the release/uptake of nonproton ions with quantum yield greater than 1 is observed at most pHs and ionic strengths. Only at both low pH and low ionic strength is the conductivity transient mostly due to protons. Our hypothesis is that during the photocycle, changes occur in the PM's dense surface charge distribution that result in changes in the number of counterions bound or condensed at the membrane surface. To test this, the PM structure was perturbed with the nonionic detergent Triton X-100. Immediately after addition, Triton does not abolish the nonproton ion movements; in fact at low detergent concentrations (0.02% vol/vol) the signal amplitudes increased considerably. However, when PM is completely solubilized into monomers in Triton, the conductivity transients are due to protons alone, though at lower quantum yield compared with native PM. These results suggest that changes in the surface charge distribution in native PM's photocycle could contribute to proton transfer between the aqueous phase and bR itself. PMID:3019444

Analysis of doxorubicin distribution in MCF-7 cells treated with drug-loaded nanoparticles by combination of two fluorescence-based techniques, confocal spectral imaging and capillary electrophoresis.

PubMed

Gautier, Juliette; Munnier, Emilie; Soucé, Martin; Chourpa, Igor; Douziech Eyrolles, Laurence

2015-05-01

The intracellular distribution of the antiancer drug doxorubicin (DOX) was followed qualitatively by fluorescence confocal spectral imaging (FCSI) and quantitatively by capillary electrophoresis (CE). FCSI permits the localization of the major fluorescent species in cell compartments, with spectral shifts indicating the polarity of the respective environment. However, distinction between drug and metabolites by FCSI is difficult due to their similar fluorochromes, and direct quantification of their fluorescence is complicated by quantum yield variation between different subcellular environments. On the other hand, capillary electrophoresis with fluorescence detection (CE-LIF) is a quantitative method capable of separating doxorubicin and its metabolites. In this paper, we propose a method for determining drug and metabolite concentration in enriched nuclear and cytosolic fractions of cancer cells by CE-LIF, and we compare these data with those of FCSI. Significant differences in the subcellular distribution of DOX are observed between the drug administered as a molecular solution or as a suspension of drug-loaded iron oxide nanoparticles coated with polyethylene glycol. Comparative analysis of the CE-LIF vs FCSI data may lead to a tentative calibration of this latter method in terms of DOX fluorescence quantum yields in the nucleus and more or less polar regions of the cytosol.

Efficient Carrier-to-Exciton Conversion in Field Emission Tunnel Diodes Based on MIS-Type van der Waals Heterostack.

PubMed

Wang, Shunfeng; Wang, Junyong; Zhao, Weijie; Giustiniano, Francesco; Chu, Leiqiang; Verzhbitskiy, Ivan; Zhou Yong, Justin; Eda, Goki

2017-08-09

We report on efficient carrier-to-exciton conversion and planar electroluminescence from tunnel diodes based on a metal-insulator-semiconductor (MIS) van der Waals heterostack consisting of few-layer graphene (FLG), hexagonal boron nitride (hBN), and monolayer tungsten disulfide (WS 2 ). These devices exhibit excitonic electroluminescence with extremely low threshold current density of a few pA·μm -2 , which is several orders of magnitude lower compared to the previously reported values for the best planar EL devices. Using a reference dye, we estimate the EL quantum efficiency to be ∼1% at low current density limit, which is of the same order of magnitude as photoluminescence quantum yield at the equivalent excitation rate. Our observations reveal that the efficiency of our devices is not limited by carrier-to-exciton conversion efficiency but by the inherent exciton-to-photon yield of the material. The device characteristics indicate that the light emission is triggered by injection of hot minority carriers (holes) to n-doped WS 2 by Fowler-Nordheim tunneling and that hBN serves as an efficient hole-transport and electron-blocking layer. Our findings offer insight into the intelligent design of van der Waals heterostructures and avenues for realizing efficient excitonic devices.

CDOM Sources and Photobleaching Control Quantum Yields for Oceanic DMS Photolysis.

PubMed

Galí, Martí; Kieber, David J; Romera-Castillo, Cristina; Kinsey, Joanna D; Devred, Emmanuel; Pérez, Gonzalo L; Westby, George R; Marrasé, Cèlia; Babin, Marcel; Levasseur, Maurice; Duarte, Carlos M; Agustí, Susana; Simó, Rafel

2016-12-20

Photolysis is a major removal pathway for the biogenic gas dimethylsulfide (DMS) in the surface ocean. Here we tested the hypothesis that apparent quantum yields (AQY) for DMS photolysis varied according to the quantity and quality of its photosensitizers, chiefly chromophoric dissolved organic matter (CDOM) and nitrate. AQY compiled from the literature and unpublished studies ranged across 3 orders of magnitude at the 330 nm reference wavelength. The smallest AQY(330) were observed in coastal waters receiving major riverine inputs of terrestrial CDOM (0.06-0.5 m 3 (mol quanta) -1 ). In open-ocean waters, AQY(330) generally ranged between 1 and 10 m 3 (mol quanta) -1 . The largest AQY(330), up to 34 m 3 (mol quanta) -1 ), were seen in the Southern Ocean potentially associated with upwelling. Despite the large AQY variability, daily photolysis rate constants at the sea surface spanned a smaller range (0.04-3.7 d -1 ), mainly because of the inverse relationship between CDOM absorption and AQY. Comparison of AQY(330) with CDOM spectral signatures suggests there is an interplay between CDOM origin (terrestrial versus marine) and photobleaching that controls variations in AQYs, with a secondary role for nitrate. Our results can be used for regional or large-scale assessment of DMS photolysis rates in future studies.

Photochemical attenuation of N-nitrosodimethylamine (NDMA) and other nitrosamines in surface water.

PubMed

Plumlee, Megan H; Reinhard, Martin

2007-09-01

The aqueous photolysis of seven alkyl nitrosamines was studied by irradiation in a solar simulator. Nitrosamines included N-nitrosodimethylamine (NDMA), N-nitrosomethylethylamine (NMEA), N-nitrosodiethylamine (NDEA), N-nitrosodi-n-propylamine (NDPA), N-nitrosodi-n-butylamine (NDBA), N-nitrosopiperidine (NPip), and N-nitrosopyrrolidine (NPyr). Direct photolysis at irradiations of 765 W/m2, representing Southern California midsummer, midday sun, resulted in half-lives of 16 min for NDMA and 12-15 min for the other nitrosamines. The quantum yield for NDMA was determined to be phi = 0.41 and phi = 0.43-0.61 for the other nitrosamines. Quantified products of NDMA photolysis included methylamine, dimethylamine, nitrite, nitrate, and formate, with nitrogen and carbon balances exceeding 98 and 79%, respectively. Indirect photolysis of nitrosamines in surface water was not observed; increasing dissolved organic carbon (DOC) slowed the NDMA photolysis rate because of light screening. Removal of NDMA measured in tertiary treated effluent flowing in a shallow, sunlit engineered channel agreed with photolysis rates predicted based on the measured quantum yield and system parameters. Because biodegradation is relatively slow, aquatic photolysis of NDMA is generally expected to be more significant even at relatively low levels of solar irradiation (t(1/2) = 8-38 h at 244-855 W/m2, 51 degrees N latitude, 1 m depth).

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.

Vibrational photochemistry of porphine imbedded in a n-hexane-d sub 14 Shpol'skii matrix

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

Butenhoff, T.J.; Chuck, R.S.; Limbach, H.H.

The near-infrared-induced tautomerization of free-base porphine incorporated in a n-hexane-d{sub 14} matrix is reported. Porphine occupies two sites in a n-hexane-d{sub 14} matrix as opposed to one site in a n-hexane matrix. Two spectroscopically distinct tautomers, differing by a 90{degree} rotation of the NH bond axes within the molecular plane, exist for each site. Nernst glower irradiation on the NH stretch fundamental does not induce tautomerization, but irradiation in the regions 4,000 < {nu} < 5,100 cm{sup {minus}1} and 5,630 < {nu} < 7,700 cm{sup {minus}1} does induce tautomerization. Narrow-band (8 cm{sup {minus}1} fwhm) laser irradiation studies in the NHmore » symmetric plus antisymmetric stretch combination band region (6,300 < {nu} < 6,600 cm{sup {minus}1}) show that the near-infrared-induced tautomerization occurs at select wavelengths. Tautomer conversion in absence of site conversion is strong evidence that the observed photochemistry is due to absorption of light by porphine and not by hexane. The estimated quantum yield is roughly 5 {times} 10{sup {minus}4} for 6,530-cm{sup {minus}1} irradiation; this is 1-3 orders of magnitude larger than the quantum yield expected from RRKM theory.« less

Quantum communication complexity using the quantum Zeno effect

NASA Astrophysics Data System (ADS)

Tavakoli, Armin; Anwer, Hammad; Hameedi, Alley; Bourennane, Mohamed

2015-07-01

The quantum Zeno effect (QZE) is the phenomenon in which the unitary evolution of a quantum state is suppressed, e.g., due to frequent measurements. Here, we investigate the use of the QZE in a class of communication complexity problems (CCPs). Quantum entanglement is known to solve certain CCPs beyond classical constraints. However, recent developments have yielded CCPs for which superclassical results can be obtained using only communication of a single d -level quantum state (qudit) as a resource. In the class of CCPs considered here, we show quantum reduction of complexity in three ways: using (i) entanglement and the QZE, (ii) a single qudit and the QZE, and (iii) a single qudit. We have performed a proof of concept experimental demonstrations of three party CCP protocol based on single-qubit communication with and without QZE.

Time-bin entangled photons from a quantum dot

PubMed Central

Jayakumar, Harishankar; Predojević, Ana; Kauten, Thomas; Huber, Tobias; Solomon, Glenn S.; Weihs, Gregor

2014-01-01

Long distance quantum communication is one of the prime goals in the field of quantum information science. With information encoded in the quantum state of photons, existing telecommunication fibre networks can be effectively used as a transport medium. To achieve this goal, a source of robust entangled single photon pairs is required. Here, we report the realization of a source of time-bin entangled photon pairs utilizing the biexciton-exciton cascade in a III/V self-assembled quantum dot. We analyse the generated photon pairs by an inherently phase-stable interferometry technique, facilitating uninterrupted long integration times. We confirm the entanglement by performing quantum state tomography of the emitted photons, which yields a fidelity of 0.69(3) and a concurrence of 0.41(6) for our realization of time-energy entanglement from a single quantum emitter. PMID:24968024

Time-bin entangled photons from a quantum dot.

PubMed

Jayakumar, Harishankar; Predojević, Ana; Kauten, Thomas; Huber, Tobias; Solomon, Glenn S; Weihs, Gregor

2014-06-26

Long-distance quantum communication is one of the prime goals in the field of quantum information science. With information encoded in the quantum state of photons, existing telecommunication fibre networks can be effectively used as a transport medium. To achieve this goal, a source of robust entangled single-photon pairs is required. Here we report the realization of a source of time-bin entangled photon pairs utilizing the biexciton-exciton cascade in a III/V self-assembled quantum dot. We analyse the generated photon pairs by an inherently phase-stable interferometry technique, facilitating uninterrupted long integration times. We confirm the entanglement by performing quantum state tomography of the emitted photons, which yields a fidelity of 0.69(3) and a concurrence of 0.41(6) for our realization of time-energy entanglement from a single quantum emitter.

Quantum versus classical dynamics in the optical centrifuge

NASA Astrophysics Data System (ADS)

Armon, Tsafrir; Friedland, Lazar

2017-09-01

The interplay between classical and quantum-mechanical evolution in the optical centrifuge (OC) is discussed. The analysis is based on the quantum-mechanical formalism starting from either the ground state or a thermal ensemble. Two resonant mechanisms are identified, i.e., the classical autoresonance and the quantum-mechanical ladder climbing, yielding different dynamics and rotational excitation efficiencies. The rotating-wave approximation is used to analyze the two resonant regimes in the associated dimensionless two-parameter space and calculate the OC excitation efficiency. The results show good agreement between numerical simulations and theory and are relevant to existing experimental setups.

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.

Multi-functional quantum router using hybrid opto-electromechanics

NASA Astrophysics Data System (ADS)

Ma, Peng-Cheng; Yan, Lei-Lei; Chen, Gui-Bin; Li, Xiao-Wei; Liu, Shu-Jing; Zhan, You-Bang

2018-03-01

Quantum routers engineered with multiple frequency bands play a key role in quantum networks. We propose an experimentally accessible scheme for a multi-functional quantum router, using photon-phonon conversion in a hybrid opto-electromechanical system. Our proposed device functions as a bidirectional, tunable multi-channel quantum router, and demonstrates the possibility to route single optical photons bidirectionally and simultaneously to three different output ports, by adjusting the microwave power. Further, the device also behaves as an interswitching unit for microwave and optical photons, yielding probabilistic routing of microwave (optical) signals to optical (microwave) outports. With respect to potential application, we verify the insignificant influence from vacuum and thermal noises in the performance of the router under cryogenic conditions.

One-pot and ultrafast synthesis of nitrogen and phosphorus co-doped carbon dots possessing bright dual wavelength fluorescence emission

NASA Astrophysics Data System (ADS)

Sun, Xiangcheng; Brückner, Christian; Lei, Yu

2015-10-01

Very brief microwave heating of aniline, ethylene diamine, and phosphoric acid in water at ambient pressure generated nitrogen and phosphorus co-doped carbon dots (N,P-CDs) that exhibit bright dual blue (centred at 450 nm; 51% quantum yield) and green (centred at 510 nm, 38% quantum yield) fluorescence emission bands. The N,P-CDs were characterized using TEM, XRD, XPS, IR, UV-vis, and fluorescence spectroscopy, demonstrating their partially crystalline carbon, partially amorphous structures, and the incorporation of O, N, and P into the carbogenic scaffold. The N,P-CDs demonstrated excitation-dependent and nearly pH-independent emission properties. The unique dual emission properties lay the foundation for the use of N,P-CDs in ratiometric sensing applications.Very brief microwave heating of aniline, ethylene diamine, and phosphoric acid in water at ambient pressure generated nitrogen and phosphorus co-doped carbon dots (N,P-CDs) that exhibit bright dual blue (centred at 450 nm; 51% quantum yield) and green (centred at 510 nm, 38% quantum yield) fluorescence emission bands. The N,P-CDs were characterized using TEM, XRD, XPS, IR, UV-vis, and fluorescence spectroscopy, demonstrating their partially crystalline carbon, partially amorphous structures, and the incorporation of O, N, and P into the carbogenic scaffold. The N,P-CDs demonstrated excitation-dependent and nearly pH-independent emission properties. The unique dual emission properties lay the foundation for the use of N,P-CDs in ratiometric sensing applications. Electronic supplementary information (ESI) available: Detailed experimental section, XRD, FTIR, explosive sensing and the applications results. See DOI: 10.1039/c5nr05549k

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.

Photochemical properties of squarylium cyanine dyes.

PubMed

Ferreira, D P; Conceição, D S; Ferreira, V R A; Graça, V C; Santos, P F; Vieira Ferreira, L F

2013-11-01

This study presents several new squarylium dyes derived from benzothiazole and benzoselenazole with several structural variations, namely the nature of the heteroaromatic ring and the length of the N,N'-dialkyl groups. Before being investigated in connection with their effect on living cells and/or tissues, these novel compounds were characterized, namely with respect to the determination of their main photophysical parameters. Therefore, a study of the ground state absorption, fluorescence emission (quantum yields and lifetimes) and singlet oxygen generation quantum yields was performed for all the compounds synthesized in order to evaluate their efficiency as photosensitizers. An increase of the alkyl chain length from ethyl to hexyl did not produce a clear change in the fluorescence quantum yields, showing no influence on the photoisomerization process. Heavy atom inclusion (Se instead of S) enhanced the singlet oxygen generation efficiency and decreased the intensity of the fluorescence emission. The external heavy atom effect (I(-) as a counterion instead of CF3SO3(-)) produced a significant increase in the singlet oxygen formation quantum yield (about 20%). Transient absorption studies in aerated and oxygen free samples revealed that the photoisomerization process, which could compete with the triplet state formation for all dyes in solution, is a negligible pathway for the excited state deactivation, in accordance with the rigidity introduced by the squaric ring into the polymethine chain of the dye, both in chloroform and ethanol. However, in the case of the chloroform solution a new transient was detected in air equilibrated solutions, resulting from a reaction of the excited squarylium dye in the singlet state with CHCl3˙, and assigned to the radical cation (SQ(+)˙) of the dye.

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.

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.

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.

An insight into non-emissive excited states in conjugated polymers

NASA Astrophysics Data System (ADS)

Hu, Zhongjian; Willard, Adam P.; Ono, Robert J.; Bielawski, Christopher W.; Rossky, Peter J.; vanden Bout, David A.

2015-09-01

Conjugated polymers in the solid state usually exhibit low fluorescence quantum yields, which limit their applications in many areas such as light-emitting diodes. Despite considerable research efforts, the underlying mechanism still remains controversial and elusive. Here, the nature and properties of excited states in the archetypal polythiophene are investigated via aggregates suspended in solvents with different dielectric constants (ε). In relatively polar solvents (ε>~ 3), the aggregates exhibit a low fluorescence quantum yield (QY) of 2-5%, similar to bulk films, however, in relatively nonpolar solvents (ε<~ 3) they demonstrate much higher fluorescence QY up to 20-30%. A series of mixed quantum-classical atomistic simulations illustrate that dielectric induced stabilization of nonradiative charge-transfer (CT) type states can lead to similar drastic reduction in fluorescence QY as seen experimentally. Fluorescence lifetime measurement reveals that the CT-type states exist as a competitive channel of the formation of emissive exciton-type states.

Near-threshold harmonics from a femtosecond enhancement cavity-based EUV source: effects of multiple quantum pathways on spatial profile and yield.

PubMed

Hammond, T J; Mills, Arthur K; Jones, David J

2011-12-05

We investigate the photon flux and far-field spatial profiles for near-threshold harmonics produced with a 66 MHz femtosecond enhancement cavity-based EUV source operating in the tight-focus regime. The effects of multiple quantum pathways in the far-field spatial profile and harmonic yield show a strong dependence on gas jet dynamics, particularly nozzle diameter and position. This simple system, consisting of only a 700 mW Ti:Sapphire oscillator and an enhancement cavity produces harmonics up to 20 eV with an estimated 30-100 μW of power (intracavity) and > 1μW (measured) of power spectrally-resolved and out-coupled from the cavity. While this power is already suitable for applications, a quantum mechanical model of the system indicates substantial improvements should be possible with technical upgrades.

Achieving Optimal Quantum Acceleration of Frequency Estimation Using Adaptive Coherent Control.

PubMed

Naghiloo, M; Jordan, A N; Murch, K W

2017-11-03

Precision measurements of frequency are critical to accurate time keeping and are fundamentally limited by quantum measurement uncertainties. While for time-independent quantum Hamiltonians the uncertainty of any parameter scales at best as 1/T, where T is the duration of the experiment, recent theoretical works have predicted that explicitly time-dependent Hamiltonians can yield a 1/T^{2} scaling of the uncertainty for an oscillation frequency. This quantum acceleration in precision requires coherent control, which is generally adaptive. We experimentally realize this quantum improvement in frequency sensitivity with superconducting circuits, using a single transmon qubit. With optimal control pulses, the theoretically ideal frequency precision scaling is reached for times shorter than the decoherence time. This result demonstrates a fundamental quantum advantage for frequency estimation.

Coined quantum walks on weighted graphs

NASA Astrophysics Data System (ADS)

Wong, Thomas G.

2017-11-01

We define a discrete-time, coined quantum walk on weighted graphs that is inspired by Szegedy’s quantum walk. Using this, we prove that many lackadaisical quantum walks, where each vertex has l integer self-loops, can be generalized to a quantum walk where each vertex has a single self-loop of real-valued weight l. We apply this real-valued lackadaisical quantum walk to two problems. First, we analyze it on the line or one-dimensional lattice, showing that it is exactly equivalent to a continuous deformation of the three-state Grover walk with faster ballistic dispersion. Second, we generalize Grover’s algorithm, or search on the complete graph, to have a weighted self-loop at each vertex, yielding an improved success probability when l < 3 + 2\\sqrt{2} ≈ 5.828 .

Quantum plasmonic sensing

DOE PAGES

Fan, Wenjiang; Lawrie, Benjamin J.; Pooser, Raphael C.

2015-11-04

Surface plasmon resonance (SPR) sensors can reach the quantum noise limit of the optical readout field in various configurations. We demonstrate that two-mode intensity squeezed states produce a further enhancement in sensitivity compared with a classical optical readout when the quantum noise is used to transduce an SPR sensor signal in the Kretschmann configuration. The quantum noise reduction between the twin beams when incident at an angle away from the plasmonic resonance, combined with quantum noise resulting from quantum anticorrelations when on resonance, results in an effective SPR-mediated modulation that yields a measured sensitivity 5 dB better than that withmore » a classical optical readout in this configuration. Furthermore, the theoretical potential of this technique points to resolving particle concentrations with more accuracy than is possible via classical approaches to optical transduction.« less

Biosynthesis of fluorescent CdS nanocrystals with semiconductor properties: Comparison of microbial and plant production systems.

PubMed

Al-Shalabi, Zahwa; Doran, Pauline M

2016-04-10

This study investigated fission yeast (Schizosaccharomyces pombe) and hairy roots of tomato (Solanum lycopersicum) as in vitro production vehicles for biological synthesis of CdS quantum dots. Cd added during the mid-growth phase of the cultures was detoxified within the biomass into inorganic sulphide-containing complexes with the quantum confinement properties of semiconductor nanocrystals. Significant differences were found between the two host systems in terms of nanoparticle production kinetics, yield and quality. The much slower growth rate of hairy roots compared with yeast is a disadvantage for commercial scaled-up production. Nanoparticle extraction from the biomass was less effective for the roots: 19% of the Cd present in the hairy roots was recovered after extraction compared with 34% for the yeast. The overall yield of CdS quantum dots was also lower for the roots: relative to the amount of Cd taken up into the biomass, 8.5% was recovered in yeast gel filtration fractions exhibiting quantum dot properties whereas the result for hairy roots was only 0.99%. Yeast-produced CdS crystallites were somewhat smaller with diameters of approximately 2-6 nm compared with those of 4-10nm obtained from the roots. The average ratio of inorganic sulphide to Cd for the purified and size-fractionated particles was 0.44 for the yeast and 1.6 for the hairy roots. Despite the limitations associated with hairy roots in terms of culture kinetics and product yield, this system produced CdS nanoparticles with enhanced photostability and 3.7-13-fold higher fluorescence quantum efficiency compared with those generated by yeast. This work demonstrates that the choice of cellular host can have a significant effect on nanoparticle functional properties as well as on the bioprocessing aspects of biological quantum dot synthesis. Copyright © 2016 Elsevier B.V. All rights reserved.

Aryl-modified graphene quantum dots with enhanced photoluminescence and improved pH tolerance

NASA Astrophysics Data System (ADS)

Luo, Peihui; Ji, Zhe; Li, Chun; Shi, Gaoquan

2013-07-01

Chemical modification is an important technique to modulate the chemical and optical properties of graphene quantum dots (GQDs). In this paper, we report a versatile diazonium chemistry method to graft aryl groups including phenyl, 4-carboxyphenyl, 4-sulfophenyl and 5-sulfonaphthyl to GQDs via Gomberg-Bachmann reaction. The aryl-modified GQDs are nanocrystals with lateral dimensions in the range of 2-4 nm and an average thickness lower than 1 nm. Upon chemical modification with aryl groups, the photoluminescence (PL) bands of GQDs were tuned in the range of 418 and 447 nm, and their fluorescence quantum yields (QYs) were increased for up to about 6 times. Furthermore, the aryl-modified GQDs exhibited stable PL (both intensity and peak position) in a wide pH window of 1-11. The mechanism of improving the PL properties of GQDs by aryl-modification was also discussed.Chemical modification is an important technique to modulate the chemical and optical properties of graphene quantum dots (GQDs). In this paper, we report a versatile diazonium chemistry method to graft aryl groups including phenyl, 4-carboxyphenyl, 4-sulfophenyl and 5-sulfonaphthyl to GQDs via Gomberg-Bachmann reaction. The aryl-modified GQDs are nanocrystals with lateral dimensions in the range of 2-4 nm and an average thickness lower than 1 nm. Upon chemical modification with aryl groups, the photoluminescence (PL) bands of GQDs were tuned in the range of 418 and 447 nm, and their fluorescence quantum yields (QYs) were increased for up to about 6 times. Furthermore, the aryl-modified GQDs exhibited stable PL (both intensity and peak position) in a wide pH window of 1-11. The mechanism of improving the PL properties of GQDs by aryl-modification was also discussed. Electronic supplementary information (ESI) available: Fluorescence quantum yield measurements, estimation of grafting ratio, TEM images, FTIR spectra, PL spectra and zeta potentials. See DOI: 10.1039/c3nr02156d

Principle of minimal work fluctuations.

PubMed

Xiao, Gaoyang; Gong, Jiangbin

2015-08-01

Understanding and manipulating work fluctuations in microscale and nanoscale systems are of both fundamental and practical interest. For example, in considering the Jarzynski equality 〈e-βW〉=e-βΔF, a change in the fluctuations of e-βW may impact how rapidly the statistical average of e-βW converges towards the theoretical value e-βΔF, where W is the work, β is the inverse temperature, and ΔF is the free energy difference between two equilibrium states. Motivated by our previous study aiming at the suppression of work fluctuations, here we obtain a principle of minimal work fluctuations. In brief, adiabatic processes as treated in quantum and classical adiabatic theorems yield the minimal fluctuations in e-βW. In the quantum domain, if a system initially prepared at thermal equilibrium is subjected to a work protocol but isolated from a bath during the time evolution, then a quantum adiabatic process without energy level crossing (or an assisted adiabatic process reaching the same final states as in a conventional adiabatic process) yields the minimal fluctuations in e-βW, where W is the quantum work defined by two energy measurements at the beginning and at the end of the process. In the classical domain where the classical work protocol is realizable by an adiabatic process, then the classical adiabatic process also yields the minimal fluctuations in e-βW. Numerical experiments based on a Landau-Zener process confirm our theory in the quantum domain, and our theory in the classical domain explains our previous numerical findings regarding the suppression of classical work fluctuations [G. Y. Xiao and J. B. Gong, Phys. Rev. E 90, 052132 (2014)].

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.

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.

Utilizing Molecular Dynamics ' Multipotent Methodologies to Measure Microscopic Motions of DNA Molecules: A Magniloquent Manuscript On DNA's Means and Mannerisms

NASA Astrophysics Data System (ADS)

Kingsland, Addie

DNA is an amazing molecule which is the basic template for all genetics. It is the primary molecule for storing biological information, and has many applications in nanotechnology. Double-stranded DNA may contain mismatched base pairs beyond the Watson-Crick pairs guanine-cytosine and adenine-thymine. To date, no one has found a physical property of base pair mismatches which describes the behavior of naturally occurring mismatch repair enzymes. Many materials properties of DNA are also unknown, for instance, when pulling DNA in different configurations, different energy differences are observed with no obvious reason why. DNA mismatches also affect their local environment, for instance changing the quantum yield of nearby azobenzene moieties. We utilize molecular dynamics computer simulations to study the structure and dynamics for both matched and mismatched base pairs, within both biological and materials contexts, and in both equilibrium and biased dynamics. We show that mismatched pairs shift further in the plane normal to the DNA strand and are more likely to exhibit non-canonical structures, including the e-motif. Base pair mismatches alter their local environment, affecting the trans- to cis- photoisomerization quantum yield of azobenzene, as well as increasing the likelihood of observing the e-motif. We also show that by using simulated data, we can give new insights on theoretical models to calculate the energetics of pulling DNA strands apart. These results, all relatively inexpensive on modern computer hardware, can help guide the design of DNA-based nanotechnologies, as well as give new insights into the functioning of mismatch repair systems in cancer prevention.

Effect of sequential isoproturon pulse exposure on Scenedesmus vacuolatus.

PubMed

Vallotton, Nathalie; Eggen, Rik Ilda Lambertus; Chèvre, Nathalie

2009-04-01

Aquatic organisms are typically exposed to fluctuating concentrations of herbicides in streams. To assess the effects on algae of repeated peak exposure to the herbicide isoproturon, we subjected the alga Scenedesmus vacuolatus to two sequential pulse exposure scenarios. Effects on growth and on the inhibition of the effective quantum yield of photosystem II (PSII) were measured. In the first scenario, algae were exposed to short, 5-h pulses at high isoproturon concentrations (400 and 1000 microg/l), each followed by a recovery period of 18 h, while the second scenario consisted of 22.5-h pulses at lower concentrations (60 and 120 microg/l), alternating with short recovery periods (1.5 h). In addition, any changes in the sensitivity of the algae to isoproturon following sequential pulses were examined by determining the growth rate-EC(50) prior to and following exposure. In both exposure scenarios, we found that algal growth and its effective quantum yield were systematically inhibited during the exposures and that these effects were reversible. Sequential pulses to isoproturon could be considered a sequence of independent events. Nevertheless, a consequence of inhibited growth during the repeated exposures is the cumulative decrease in biomass production. Furthermore, in the second scenario, when the sequence of long pulses began to approach a scenario of continuous exposure, a slight increase in the tolerance of the algae to isoproturon was observed. These findings indicated that sequential pulses do affect algae during each pulse exposure, even if algae recover between the exposures. These observations could support an improved risk assessment of fluctuating exposures to reversibly acting herbicides.

Enhanced salt-induced antioxidative responses involve a contribution of polyamine biosynthesis in grapevine plants.

PubMed

Ikbal, Fatima Ezzohra; Hernández, José Antonio; Barba-Espín, Gregorio; Koussa, Tayeb; Aziz, Aziz; Faize, Mohamed; Diaz-Vivancos, Pedro

2014-06-15

The possible involvement of polyamines in the salt stress adaptation was investigated in grapevine (Vitis vinifera L.) plantlets focusing on photosynthesis and oxidative metabolism. Salt stress resulted in the deterioration of plant growth and photosynthesis, and treatment of plantlets with methylglyoxal-bis(guanylhydrazone) (MGBG), a S-adenosylmethionine decarboxylase (SAMDC) inhibitor, enhanced the salt stress effect. A decrease in PSII quantum yield (Fv/Fm), effective PSII quantum yield (Y(II)) and coefficient of photochemical quenching (qP) as well as increases in non-photochemical quenching (NPQ) and its coefficient (qN) was observed by these treatments. Salt and/or MGBG treatments also triggered an increase in lipid peroxidation and reactive oxygen species (ROS) accumulation as well as an increase of superoxide dismutase (SOD) and peroxidase (POX) activities, but not ascorbate peroxidase (APX) activity. Salt stress also resulted in an accumulation of oxidized ascorbate (DHA) and a decrease in reduced glutathione. MGBG alone or in combination with salt stress increased monodehydroascorbate reductase (MDHAR), SOD and POX activities and surprisingly no accumulation of DHA was noticed following treatment with MGBG. These salt-induced responses correlated with the maintaining of high level of free and conjugated spermidine and spermine, whereas a reduction of agmatine and putrescine levels was observed, which seemed to be amplified by the MGBG treatment. These results suggest that maintaining polyamine biosynthesis through the enhanced SAMDC activity in grapevine leaf tissues under salt stress conditions could contribute to the enhanced ROS scavenging activity and a protection of photosynthetic apparatus from oxidative damages. Copyright © 2014 Elsevier GmbH. All rights reserved.

Efficient hybrid-symbolic methods for quantum mechanical calculations

NASA Astrophysics Data System (ADS)

Scott, T. C.; Zhang, Wenxing

2015-06-01

We present hybrid symbolic-numerical tools to generate optimized numerical code for rapid prototyping and fast numerical computation starting from a computer algebra system (CAS) and tailored to any given quantum mechanical problem. Although a major focus concerns the quantum chemistry methods of H. Nakatsuji which has yielded successful and very accurate eigensolutions for small atoms and molecules, the tools are general and may be applied to any basis set calculation with a variational principle applied to its linear and non-linear parameters.

Orbital Picture of Ionization and Its Breakdown in Nanoarrays of Quantum Dots

NASA Astrophysics Data System (ADS)

Bâldea, Ioan; Cederbaum, Lorenz S.

2002-09-01

We present exact numerical results indicating that ionization could be a useful tool to study electron correlations in artificial molecules and nanoarrays of metallic quantum dots. For nanorings consisting of Ag quantum dots of the type already fabricated, we demonstrate that the molecular orbital picture breaks down even for lowest energy ionization processes, in contrast to ordinary molecules. Our ionization results yield a transition point between localization and delocalization regimes in good agreement with various experimental data.

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.

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.

Camphor-mediated synthesis of carbon nanoparticles, graphitic shell encapsulated carbon nanocubes and carbon dots for bioimaging

PubMed Central

Oza, Goldie; Ravichandran, M.; Merupo, Victor-Ishrayelu; Shinde, Sachin; Mewada, Ashmi; Ramirez, Jose Tapia; Velumani, S.; Sharon, Madhuri; Sharon, Maheshwar

2016-01-01

A green method for an efficient synthesis of water-soluble carbon nanoparticles (CNPs), graphitic shell encapsulated carbon nanocubes (CNCs), Carbon dots (CDs) using Camphor (Cinnamomum camphora) is demonstrated. Here, we describe a competent molecular fusion and fission route for step-wise synthesis of CDs. Camphor on acidification and carbonization forms CNPs, which on alkaline hydrolysis form CNCs that are encapsulated by thick graphitic layers and on further reduction by sodium borohydride yielded CDs. Though excitation wavelength dependent photoluminescence is observed in all the three carbon nanostructures, CDs possess enhanced photoluminescent properties due to more defective carbonaceous structures. The surface hydroxyl and carboxyl functional groups make them water soluble in nature. They possess excellent photostability, higher quantum yield, increased absorption, decreased cytotoxicity and hence can be utilized as a proficient bio imaging agent. PMID:26905737

Camphor-mediated synthesis of carbon nanoparticles, graphitic shell encapsulated carbon nanocubes and carbon dots for bioimaging

NASA Astrophysics Data System (ADS)

Oza, Goldie; Ravichandran, M.; Merupo, Victor-Ishrayelu; Shinde, Sachin; Mewada, Ashmi; Ramirez, Jose Tapia; Velumani, S.; Sharon, Madhuri; Sharon, Maheshwar

2016-02-01

A green method for an efficient synthesis of water-soluble carbon nanoparticles (CNPs), graphitic shell encapsulated carbon nanocubes (CNCs), Carbon dots (CDs) using Camphor (Cinnamomum camphora) is demonstrated. Here, we describe a competent molecular fusion and fission route for step-wise synthesis of CDs. Camphor on acidification and carbonization forms CNPs, which on alkaline hydrolysis form CNCs that are encapsulated by thick graphitic layers and on further reduction by sodium borohydride yielded CDs. Though excitation wavelength dependent photoluminescence is observed in all the three carbon nanostructures, CDs possess enhanced photoluminescent properties due to more defective carbonaceous structures. The surface hydroxyl and carboxyl functional groups make them water soluble in nature. They possess excellent photostability, higher quantum yield, increased absorption, decreased cytotoxicity and hence can be utilized as a proficient bio imaging agent.

Fluorescence enhancement by Au nanostructures: nanoshells and nanorods.

PubMed

Bardhan, Rizia; Grady, Nathaniel K; Cole, Joseph R; Joshi, Amit; Halas, Naomi J

2009-03-24

Metallic nanoparticles influence the quantum yield and lifetime of adjacent fluorophores in a manner dependent on the properties of the nanostructure. Here we directly compare the fluorescence enhancement of the near-infrared fluorophore IR800 by Au nanoshells (NSs) and Au nanorods (NRs), where human serum albumin (HSA) serves as a spacer layer between the nanoparticle and the fluorophore. Our measurements reveal that the quantum yield of IR800 is enhanced from approximately 7% as an isolated fluorophore to 86% in a NSs-HSA-IR800 complex and 74% in a NRs-HSA-IR800 complex. This dramatic increase in fluorescence shows tremendous potential for contrast enhancement in fluorescence-based bioimaging.

The Chameleonic Nature of Platinum(II) Imidazopyridine Complexes.

PubMed

Pinter, Piermaria; Pittkowski, Rebecca; Soellner, Johannes; Strassner, Thomas

2017-10-12

The synthesis and characterization of cyclometalated C^C* platinum(II) complexes with unique photophysical properties, aggregation induced enhancement of the quantum yields with a simultaneous decrease of phosphorescence lifetimes, is reported. Additionally, a change of emission color is induced by variation of the excitation wavelength. The aggregation behavior of these complexes is controlled by the steric demand of the substituents. The photophysical properties of these complexes are investigated through emission-excitation matrix analysis (EEM). The monomeric complexes are excellent room temperature phosphorescent blue emitters with emission maxima below 470 nm and quantum yields of up to 93 %. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Interaction of light with dye-doped calcium phosphate nanoparticles

NASA Astrophysics Data System (ADS)

Russin, Timothy John

In this work we present work on a novel amorphous calcium phosphate nanoparticle system for use in bioimaging and drug delivery applications. The system, by virtue of its synthesis, can be made to encapsulate and protect any number of molecules that are not suitable for biological applications on their own; for example, medication that is poorly soluble in aqueous solution can be encapsulated for delivery, or fragile optical molecules can be encapsulated to protect them from the local environment. We have encapsulated the near-infrared dye indocyanine green, which has beneficial properties for optical imaging (low biotoxicity, absorption and emission at a minimum of tissue absorption). There are two original works presented in this thesis. The first describes the measurement of the quantum yield of the indocyanine green-doped nanoparticles, as well as the development of a theoretical method to extract the molecular quantum yield of a fluorophore encapsulated in a dielectric sphere from effective quantum yield measurements of nanoparticle dispersions in solution. The second work is an application of diffuse scattering theory to the problem of light propagation in biological tissue; specifically, the limits on penetration depth for photodynamic therapy and bioimaging.

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.

The influence of the Tbeta level upon fluorescence and laser properties of aromatic compounds.

PubMed

Nijegorodov, N; Winkoun, D P; Nkoma, J S

2004-07-01

The fluorescence and laser properties of seven specially chosen aromatic compounds are studied at 293 degrees C. The quantum yield of fluorescence, gamma, decay times, tauf, of the deaerated and non-deaerated solutions are measured. The oscillator strength, fe, fluorescence rate constants, kf, natural lifetimes, tauT0, and intersystem crossing rate constants, kST, are calculated. Some laser parameters are calculated or measured experimentally. It is found that the position of the Tbeta level plays an important role in the fluorescence and laser properties of aromatic compounds. If the Tbeta level is situated below the Sp level, it decreases the quantum yield of fluorescence and the decay time and increases the threshold of laser action. If, due to some structural changes of a molecule, the Tbeta level is situated higher than the Sp level, then the quantum yield of fluorescence and the decay times are increasing and the threshold of laser action is decreasing. Such influence of the position of the Tbeta level upon fluorescence and laser properties of aromatic compound is explained by the fact that the Sp level mixes with the Tbeta level more readily than with other taupipi* levels.

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.

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

Vignat, C.; Bercher, J.-F.

The family of Tsallis entropies was introduced by Tsallis in 1988. The Shannon entropy belongs to this family as the limit case q{yields}1. The canonical distributions in R{sup n} that maximize this entropy under a covariance constraint are easily derived as Student-t (q<1) and Student-r (q>1) multivariate distributions. A nice geometrical result about these Student-r distributions is that they are marginal of uniform distributions on a sphere of larger dimension d with the relationship p = n+2+(2/q-1). As q{yields}1, we recover the famous Poincare's observation according to which a Gaussian vector can be viewed as the projection of a vectormore » uniformly distributed on the infinite dimensional sphere. A related property in the case q<1 is also available. Often associated to Renyi-Tsallis entropies is the notion of escort distributions. We provide here a geometric interpretation of these distributions. Another result concerns a universal system in physics, the harmonic oscillator: in the usual quantum context, the waveform of the n-th state of the harmonic oscillator is a Gaussian waveform multiplied by the degree n Hermite polynomial. We show, starting from recent results by Carinena et al., that the quantum harmonic oscillator on spaces with constant curvature is described by maximal Tsallis entropy waveforms multiplied by the extended Hermite polynomials derived from this measure. This gives a neat interpretation of the non-extensive parameter q in terms of the curvature of the space the oscillator evolves on; as q{yields}1, the curvature of the space goes to 0 and we recover the classical harmonic oscillator in R{sup 3}.« less

Solvatochromism in highly luminescent environmental friendly carbon quantum dots for sensing applications: Conversion of bio-waste into bio-asset

NASA Astrophysics Data System (ADS)

Pramanik, A.; Biswas, S.; Kumbhakar, P.

2018-02-01

Recently studies on synthesis and fluorescence based sensing in biocompatible carbon quantum dots (CQDs) have become a widely spoken topic of research due to the several advantageous properties of CQDs in compared to semiconductor quantum dots. In this work, we have reported the rarely reported solvatochromism along-with a high photoluminescence (PL) quantum yield (PLQY) of 22%. Samples have been synthesized by using a simple process of hydrothermal carbonization of a naturally occurring bio-waste i.e. Aegle marmelos leaves powder. The linear absorption and PL emission characteristics of CQDs have been studied in different solvent environments to explore the origin of the observed excitation dependent PL emissions characteristics of the sample. The interesting solvatochromic PL (SPL) behavior of CQDs are observed at an excitation wavelength of 325 nm by dispersing them in different polar protic and aprotic solvents, which suggest their possible applications as a replacement of solvatochromic dye molecules for sensing applications. Different polarity functions and molecular-microscopic solvent polarity parameter (ETN) are used to calculate the change in dipole moment (Δδ) of the solute-solvent system and the origin of SPL in CQDs has been explained. The SPL behavior of CQDs has been utilized for fluorescence sensing of organic liquids (Ethanol and Tetrahydrofuran) in water. Whereas, the photo-induced electron transfer mediated quenching in PL of aqueous dispersion of CQDs has led to development of ;turn off; fluorescence Fe3 + ion sensor with a detection limit of 0.12 μM. Therefore, this work may open a new avenue of conversion of a bio-waste into a fluorescent bio-asset.

Hole Transfer from Low Band Gap Quantum Dots to Conjugated Polymers in Organic/Inorganic Hybrid Photovoltaics.

PubMed

Colbert, Adam E; Janke, Eric M; Hsieh, Stephen T; Subramaniyan, Selvam; Schlenker, Cody W; Jenekhe, Samson A; Ginger, David S

2013-01-17

We use photoinduced absorption (PIA) spectroscopy to investigate pathways for photocurrent generation in hybrid organic/inorganic quantum dot bulk heterojunction solar cells. We study blends of the conjugated polymer poly(2,3-bis(2-(hexyldecyl)quinoxaline-5,8-diyl-alt-N-(2-hexyldecyl)dithieno[3,2-b:2',3'-d]pyrrole) (PDTPQx-HD) with PbS quantum dots and find that positively charged polarons are formed on the conjugated polymer following selective photoexcitation of the PbS quantum dots. This result provides a direct spectroscopic fingerprint demonstrating that photoinduced hole transfer occurs from the photoexcited quantum dots to the host polymer. We compute the relative yields of long-lived holes following photoexcitation of both the polymer and quantum dot phases and estimate that more long-lived polarons are produced per photon absorbed by the polymer phase than by the quantum dot phase.

Noninformative prior in the quantum statistical model of pure states

NASA Astrophysics Data System (ADS)

Tanaka, Fuyuhiko

2012-06-01

In the present paper, we consider a suitable definition of a noninformative prior on the quantum statistical model of pure states. While the full pure-states model is invariant under unitary rotation and admits the Haar measure, restricted models, which we often see in quantum channel estimation and quantum process tomography, have less symmetry and no compelling rationale for any choice. We adopt a game-theoretic approach that is applicable to classical Bayesian statistics and yields a noninformative prior for a general class of probability distributions. We define the quantum detection game and show that there exist noninformative priors for a general class of a pure-states model. Theoretically, it gives one of the ways that we represent ignorance on the given quantum system with partial information. Practically, our method proposes a default distribution on the model in order to use the Bayesian technique in the quantum-state tomography with a small sample.

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.

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.

Identifying a cooperative control mechanism between an applied field and the environment of open quantum systems

NASA Astrophysics Data System (ADS)

Gao, Fang; Rey-de-Castro, Roberto; Wang, Yaoxiong; Rabitz, Herschel; Shuang, Feng

2016-05-01

Many systems under control with an applied field also interact with the surrounding environment. Understanding the control mechanisms has remained a challenge, especially the role played by the interaction between the field and the environment. In order to address this need, here we expand the scope of the Hamiltonian-encoding and observable-decoding (HE-OD) technique. HE-OD was originally introduced as a theoretical and experimental tool for revealing the mechanism induced by control fields in closed quantum systems. The results of open-system HE-OD analysis presented here provide quantitative mechanistic insights into the roles played by a Markovian environment. Two model open quantum systems are considered for illustration. In these systems, transitions are induced by either an applied field linked to a dipole operator or Lindblad operators coupled to the system. For modest control yields, the HE-OD results clearly show distinct cooperation between the dynamics induced by the optimal field and the environment. Although the HE-OD methodology introduced here is considered in simulations, it has an analogous direct experimental formulation, which we suggest may be applied to open systems in the laboratory to reveal mechanistic insights.

Preparation of carbon quantum dots based high photostability luminescent membranes.

PubMed

Zhao, Jinxing; Liu, Cui; Li, Yunchuan; Liang, Jiyuan; Liu, Jiyan; Qian, Tonghui; Ding, Jianjun; Cao, Yuan-Cheng

2017-06-01

Urethane acrylate (UA) was used to prepare carbon quantum dots (C-dots) luminescent membranes and the resultants were examined with FT-IR, mechanical strength, scanning electron microscope (SEM) and quantum yields (QYs). FT-IR results showed the polyurethane acrylate (PUA) prepolymer -C = C-vibration at 1101 cm -1 disappeared but there was strong vibration at1687cm -1 which was contributed from the-C = O groups in cross-linking PUA. Mechanical strength results showed that the different quantity of C-dots loadings and UV-curing time affect the strength. SEM observations on the cross-sections of the membranes are uniform and have no structural defects, which prove that the C-dots are compatible with the water-soluble PUA resin. The C-dot loading was increased from 0 to 1 g, the maximum tensile stress was nearly 2.67 MPa, but the tensile strain was decreased from 23.4% to 15.1% and 7.2% respectively. QYs results showed that the C-dots in the membrane were stable after 120 h continuous irradiation. Therefore, the C-dots photoluminescent film is the promising material for the flexible devices in the future applications. Copyright © 2016 John Wiley & Sons, Ltd.

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

Regularized linearization for quantum nonlinear optical cavities: application to degenerate optical parametric oscillators.

PubMed

Navarrete-Benlloch, Carlos; Roldán, Eugenio; Chang, Yue; Shi, Tao

2014-10-06

Nonlinear optical cavities are crucial both in classical and quantum optics; in particular, nowadays optical parametric oscillators are one of the most versatile and tunable sources of coherent light, as well as the sources of the highest quality quantum-correlated light in the continuous variable regime. Being nonlinear systems, they can be driven through critical points in which a solution ceases to exist in favour of a new one, and it is close to these points where quantum correlations are the strongest. The simplest description of such systems consists in writing the quantum fields as the classical part plus some quantum fluctuations, linearizing then the dynamical equations with respect to the latter; however, such an approach breaks down close to critical points, where it provides unphysical predictions such as infinite photon numbers. On the other hand, techniques going beyond the simple linear description become too complicated especially regarding the evaluation of two-time correlators, which are of major importance to compute observables outside the cavity. In this article we provide a regularized linear description of nonlinear cavities, that is, a linearization procedure yielding physical results, taking the degenerate optical parametric oscillator as the guiding example. The method, which we call self-consistent linearization, is shown to be equivalent to a general Gaussian ansatz for the state of the system, and we compare its predictions with those obtained with available exact (or quasi-exact) methods. Apart from its operational value, we believe that our work is valuable also from a fundamental point of view, especially in connection to the question of how far linearized or Gaussian theories can be pushed to describe nonlinear dissipative systems which have access to non-Gaussian states.

Polarizable Force Field for DNA Based on the Classical Drude Oscillator: I. Refinement Using Quantum Mechanical Base Stacking and Conformational Energetics.

PubMed

Lemkul, Justin A; MacKerell, Alexander D

2017-05-09

Empirical force fields seek to relate the configuration of a set of atoms to its energy, thus yielding the forces governing its dynamics, using classical physics rather than more expensive quantum mechanical calculations that are computationally intractable for large systems. Most force fields used to simulate biomolecular systems use fixed atomic partial charges, neglecting the influence of electronic polarization, instead making use of a mean-field approximation that may not be transferable across environments. Recent hardware and software developments make polarizable simulations feasible, and to this end, polarizable force fields represent the next generation of molecular dynamics simulation technology. In this work, we describe the refinement of a polarizable force field for DNA based on the classical Drude oscillator model by targeting quantum mechanical interaction energies and conformational energy profiles of model compounds necessary to build a complete DNA force field. The parametrization strategy employed in the present work seeks to correct weak base stacking in A- and B-DNA and the unwinding of Z-DNA observed in the previous version of the force field, called Drude-2013. Refinement of base nonbonded terms and reparametrization of dihedral terms in the glycosidic linkage, deoxyribofuranose rings, and important backbone torsions resulted in improved agreement with quantum mechanical potential energy surfaces. Notably, we expand on previous efforts by explicitly including Z-DNA conformational energetics in the refinement.

Introduction to dissociative recombination

NASA Technical Reports Server (NTRS)

Guberman, Steven L.; Mitchell, J. Brian A.

1989-01-01

Dissociative recombination (DR) of molecular ions with electrons has important consequences in many areas of physical science. Ab-initio calculations coupled with resonant scattering theory and multichannel quantum defect studies have produced detailed results illuminating the role of ion vibrational excitation, the quantum yields of the DR products, and the role of Rydberg states. The theoretical and experimental results are discussed.

Quantum Mechanics in Insulators

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

Aeppli, G.; Department of Physics and Astronomy, University College of London, London

Atomic physics is undergoing a large revival because of the possibility of trapping and cooling ions and atoms both for individual quantum control as well as collective quantum states, such as Bose-Einstein condensates. The present lectures start from the 'atomic' physics of isolated atoms in semiconductors and insulators and proceed to coupling them together to yield magnets undergoing quantum phase transitions as well as displaying novel quantum states with no classical analogs. The lectures are based on: G.-Y. Xu et al., Science 317, 1049-1052 (2007); G. Aeppli, P. Warburton, C. Renner, BT Technology Journal, 24, 163-169 (2006); H. M. Ronnowmore » et al., Science 308, 392-395 (2005) and N. Q. Vinh et al., PNAS 105, 10649-10653 (2008).« less

An Acoustic Charge Transport Imager for High Definition Television Applications: Reliability Modeling and Parametric Yield Prediction of GaAs Multiple Quantum Well Avalanche Photodiodes. Degree awarded Oct. 1997

NASA Technical Reports Server (NTRS)

Hunt, W. D.; Brennan, K. F.; Summers, C. J.; Yun, Ilgu

1994-01-01

Reliability modeling and parametric yield prediction of GaAs/AlGaAs multiple quantum well (MQW) avalanche photodiodes (APDs), which are of interest as an ultra-low noise image capture mechanism for high definition systems, have been investigated. First, the effect of various doping methods on the reliability of GaAs/AlGaAs multiple quantum well (MQW) avalanche photodiode (APD) structures fabricated by molecular beam epitaxy is investigated. Reliability is examined by accelerated life tests by monitoring dark current and breakdown voltage. Median device lifetime and the activation energy of the degradation mechanism are computed for undoped, doped-barrier, and doped-well APD structures. Lifetimes for each device structure are examined via a statistically designed experiment. Analysis of variance shows that dark-current is affected primarily by device diameter, temperature and stressing time, and breakdown voltage depends on the diameter, stressing time and APD type. It is concluded that the undoped APD has the highest reliability, followed by the doped well and doped barrier devices, respectively. To determine the source of the degradation mechanism for each device structure, failure analysis using the electron-beam induced current method is performed. This analysis reveals some degree of device degradation caused by ionic impurities in the passivation layer, and energy-dispersive spectrometry subsequently verified the presence of ionic sodium as the primary contaminant. However, since all device structures are similarly passivated, sodium contamination alone does not account for the observed variation between the differently doped APDs. This effect is explained by the dopant migration during stressing, which is verified by free carrier concentration measurements using the capacitance-voltage technique.

Quantum key distribution with 1.25 Gbps clock synchronization.

PubMed

Bienfang, J; Gross, A; Mink, A; Hershman, B; Nakassis, A; Tang, X; Lu, R; Su, D; Clark, Charles; Williams, Carl; Hagley, E; Wen, Jesse

2004-05-03

We have demonstrated the exchange of sifted quantum cryptographic key over a 730 meter free-space link at rates of up to 1.0 Mbps, two orders of magnitude faster than previously reported results. A classical channel at 1550 nm operates in parallel with a quantum channel at 845 nm. Clock recovery techniques on the classical channel at 1.25 Gbps enable quantum transmission at up to the clock rate. System performance is currently limited by the timing resolution of our silicon avalanche photodiode detectors. With improved detector resolution, our technique will yield another order of magnitude increase in performance, with existing technology.

Comparative analysis of salt stress, duration and intensity, on the chloroplast ultrastructure and photosynthetic apparatus in Thellungiella salsuginea.

PubMed

Goussi, Rahma; Manaa, Arafet; Derbali, Walid; Cantamessa, Simone; Abdelly, Chedly; Barbato, Roberto

2018-06-01

Salinity is one of the most important abiotic stress affecting plant growth and productivity worldwide. Photosynthesis, together with cell growth, is among the primary process affected by salinity. Here, we report the effects of salt stress on photosynthesis in the model halophyte Thellungiella salsuginea. Plants were grown in hydroponic system and then treated for 2 weeks with different NaCl concentrations (0, 100, 200 and 400 mM). Leaf analysis using both photonic and transmission electron microscopes showed some changes in mesophyll cell organization, including shape and dimension. Under high NaCl concentration (400 mM) a swelling of thylakoids and starch accumulation was also observed. The obtained results also showed a change in the photosynthetic efficiency of both photosystems (PSI and PSII), depending on both NaCl concentrations and duration of the stress treatment. Under moderate salinity (100 and 200 mM NaCl) no significant variation was observed in PSI and PSII yield parameters. Chlorophyll a fluorescence transient showed some variations in OJ, JI and IP phases under salt stress depending also on NaCl levels and the duration of stress. Under high salinity PSII donor side was affected as well as quantum yield of PSI which also showed a donor side limitation. A significant decrease on quantum yields Y(I) and Y(II) under high salt treatment (400 mM NaCl) for prolonged period of time (15 days) was observed. The decrease of these parameters was quantitatively compensated by a corresponding increase of energy thermal dissipation Y(NPQ) in photosystem II and a increase in the Y(ND) in PSI. Analysis of derived parameters from the OJIP transient curve revealed that ABS/RC decreased under NaCl treatment by reason of the increase in size of antenna of active reaction centers. An increase in the performance index PI (ABS) , a slight decrease in the rate of DI O /RC, TR O /RC and the level of electron transport per PSII RC (ET O /RC) were observed during the first days of salt stress treatment reflecting a high PSII efficiency. Copyright © 2018 Elsevier B.V. All rights reserved.