NASA Astrophysics Data System (ADS)
Semenov, S. G.; Bedrina, M. E.
2014-02-01
The intermediates of hypothetical photochemical reactions that accompany the quenching of the 3C{60/*} triplet state by triplet oxygen are studied by the (U)PBE0 quantum-chemical method. The diradical C60-O-O formed from 3O2 and photoexcited buckminsterfullerene 3C{60/*} is characterized by a negative binding energy -1.11 eV (with respect to C60 and 3O2), the singlet-triplet splitting Δ E ST of 0.07 eV, and the dipole moment of 3.2 D at the equilibrium internuclear separations 1.522 Å (CO) and 1.294 Å (OO). Its decay produces 1O2. The formation of a dioxetane circle lowers the energy by 0.8 eV. The ground-state energy of diketone C58(C=O)2 is 2.0 eV lower than the energy of C60-O-O. The metastable centrosymmetric diradical C60-C60, formed upon ineffective light absorption by clusters (C60)N, has a single interpolyhedral C-C bond (1.657 Å). Its triplet state T 1 lies 0.16 eV higher than the S 1 singlet. The S 1 → S 0 relaxation leads to the formation of a stable C60-C60 dimer with a shorter (1.584 Å) bis-single exothermic (+0.24 eV) bond of polyhedra. The photoexcited C60-C60 dimer is able to form isomeric metastable diradicals C60-C60-O-O.
Photoelectron Quantum Yields of the Amino Acids
Dam, Rudy J.; Burke, Charles A.; Griffith, O. Hayes
1974-01-01
The photoelectron quantum yields of 21 common amino acids and 15 polyamino acids were measured in the 180-240 nm wavelength region. On the average, the quantum yields of these two groups exhibit quite similar wavelength dependence. For λ > 220 nm all amino acid and polyamino acid quantum yields are ≤10-7 electrons/(incident) photon. The mean yields increase to about 5 × 10-7 electrons/photon at 200 nm and 5 × 10-6 electrons/photon at 180 nm. L-tryptophan, L-tyrosine, and poly-L-tryptophan exhibit above average yields between 180 and 200 nm. Comparison with the dye phthalocyanine indicates that the quantum yield of the dye is two orders of magnitude greater than that of the amino acids from 200 to 240 nm, suggesting the feasibility of photoelectron labeling studies of biological surfaces. PMID:4836100
Ke, Hanzhong; Li, Wenbin; Zhang, Tao; Zhu, Xunjin; Tam, Hoi-Lam; Hou, Anxin; Kwong, Daniel W J; Wong, Wai-Kwok
2012-04-21
Several acetylene bridged porphyrin-monophthalocyaninato ytterbium(III) hybrids, PZn-PcYb, PH(2)-PcYb and PPd-PcYb, have been prepared and characterized by (1)H and (31)P NMR, mass spectrometry, and UV-vis spectroscopy. Their photophysical and photochemical properties, especially the relative singlet oxygen ((1)O(2)) quantum yields and the two-photon absorption cross-section (σ(2)), were investigated. These three newly synthesized compounds exhibited very large σ(2) values and substantial (1)O(2) quantum yields upon photo-excitation, making them potential candidates as one- and two-photon photodynamic therapeutic agents.
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.
Quantum Yield of Gold-Cathode Photomultipliers
NASA Technical Reports Server (NTRS)
Childs, Charles B.
1961-01-01
Two gold-cathode EMI 6255G tubes have been investigated for their quantum yield between 3100 and 1900 A. The tubes had cathodes of different appearances. One of these, numbered 3012, had a slight bluish tinge and was very transparent to visible light; the other, numbered 3021, had a definite gold coloration. The relative quantum yield of each tube was determined with the aid of a Cary model 14 recording spectrophotometer used as a monochromator. The monochromator relative-energy output was determined from the current output of a sodium-salicylate-coated RCA 1P21 photomultiplier. Each gold-cathode tube was then operated at 3000 v, and the central 1.8 cm cube of the cathode was exposed to the monochromator output.
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.
NASA Astrophysics Data System (ADS)
Shimizu, Okiyasu; Watanabe, Jun; Imakubo, Keiichi; Naito, Shizuo
1998-11-01
The phosphorescence quantum yield Φ P (=einsteins emitted/einsteins absorbed by sensitizer) of singlet oxygen (1O2) was measured for an air-saturated CCl4 solution of phenalenone (PH) used as a photosensitizer, by means of a photon-counting technique based on the use of a near-IR-sensitive photomultiplier. Employment of steady-state excitation allowed for the determination of the absolute quantum yield of Φ P=(1.38±0.05)×10-3 in CCl4. The result was obtained by direct comparison of the areas under the corrected emission spectra of 1O2 and of quinine bisulfate (QBS) in 1N H2SO4 as a luminescence standard.
New Ru(II) Complexes for Dual Photoreactivity: Ligand Exchange and 1O2 Generation
Knoll, Jessica D.; Albani, Bryan A.; Turro, Claudia
2016-01-01
CONSPECTUS Uncovering the factors that govern the electronic structure of Ru(II)–polypyridyl complexes is critical in designing new compounds for desired photochemical reactions, and strategies to tune excited states for ligand dissociation and 1O2 production are discussed herein. The generally accepted mechanism for photoinduced ligand dissociation proposes that population of the dissociative triplet ligand field (3LF) state proceeds through thermal population from the vibrationally cooled triplet metal-to-ligand charge transfer (3MLCT) state; however, temperature-dependent emission spectroscopy provides varied activation energies using the emission and ligand exchange quantum yields for [Ru(bpy)2(L)2]2+ (bpy = 2,2′-bipyridine; L = CH3CN or py). This suggests that population of the 3LF state proceeds from the vibrationally excited 3MLCT state. Because the quantum yield of ligand dissociation for nitriles is much more efficient than that for py, steric bulk was introduced into the ligand set to distort the pseudo-octahedral geometry and lower the energy of the 3LF state. The py dissociation quantum yield with 500 nm irradiation in a series of [Ru(tpy)(NN)(py)]2+ complexes (tpy = 2,2′:6′,2″-terpyridine; NN = bpy, 6,6′-dimethyl-2,2′-bipyridine (Me2bpy), 2,2′-biquinoline (biq)) increases by 2–3 orders of magnitude with the sterically bulky Me2bpy and biq ligands relative to bpy. Ultrafast transient absorption spectroscopy reveals population of the 3LF state within 3–7 ps when NN is bulky, and density functional theory calculations support stabilized 3LF states. Dual activity via ligand dissociation and 1O2 production can be achieved by careful selection of the ligand set to tune the excited-state dynamics. Incorporation of an extended π system in Ru(II) complexes such as [Ru(bpy)(dppn)(CH3CN)2]2+ (dppn = benzo[i]dipyrido[3,2-a:2′,3′-c]phenazine) and [Ru(tpy)(Me2dppn)(py)]2+ (Me2dppn = 3,6-dimethylbenzo[i]dipyrido[3,2-a:2′,3
Orfield, Noah J; McBride, James R; Wang, Feng; Buck, Matthew R; Keene, Joseph D; Reid, Kemar R; Htoon, Han; Hollingsworth, Jennifer A; Rosenthal, Sandra J
2016-02-23
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. Herein, 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, 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". Therefore, in contrast to conventional QDs, ensemble photoluminescence quantum yield is principally defined by charging processes rather than the existence of dark g-QDs.
On the photoelectric quantum yield of small dust particles
NASA Astrophysics Data System (ADS)
Kimura, Hiroshi
2016-07-01
Photoelectron emission is crucial to electric charging of dust particles around main-sequence stars and gas heating in various dusty environments. An estimate of the photoelectric processes contains an ill-defined parameter called the photoelectric quantum yield, which is the total number of electrons ejected from a dust particle per absorbed photon. Here we revisit the so-called small particle effect of photoelectron emission and provide an analytical model to estimate photoelectric quantum yields of small dust particles in sizes down to nanometers. We show that the small particle effect elevates the photoelectric quantum yields of nanoparticles up to by a factor of 103 for carbon, water ice, and organics, and a factor of 102 for silicate, silicon carbide, and iron. We conclude the surface curvature of the particles is a quantity of great importance to the small particle effect, unless the particles are submicrometers in radius or larger.
Unity quantum yield of photogenerated charges and band-like transport in quantum-dot solids.
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.
High quantum yield ZnO quantum dots synthesizing via an ultrasonication microreactor method.
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. PMID:27245962
High quantum yield ZnO quantum dots synthesizing via an ultrasonication microreactor method.
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.
Quantum Yield of Single Surface Plasmons Generated by a Quantum Dot Coupled with a Silver Nanowire.
Li, Qiang; Wei, Hong; Xu, Hongxing
2015-12-01
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.
Quantum yield of conversion of the dental photoinitiator camphorquinone
NASA Astrophysics Data System (ADS)
Chen, Yin-Chu; Ferracane, Jack L.; Prahl, Scott A.
2005-06-01
The primary absorber in dental resins is the photoinitiators, which start the photo polymerization process. We studied the quantum yield of conversion of camphorquinone (CQ), a blue light photoinitiator, using 3M FreeLight LED lamp as the light curing unit. The molar extinction coefficient, ɛ469, of CQ was measured to be 46+/-2 cm-1/(mol/L) at 469 nm. The absorption coefficient change to the radiant exposure was measured at three different irradiances. The relationship between the CQ absorption coefficient and curing lamp radiant exposure was the same for different irradiances and fit an exponential function: μa469(H)= μao exp(-H/Hthreshold), where μao is 4.46+/-0.05 cm-1, and Hthreshold=43+/-4 J/cm2. Combining this exponential relationship with CQ molar extinction coefficient and the absorbed photon energy (i.e., the product of the radiant exposure with the absorption coefficient), we plotted CQ concentration [number of molecules/cm3] as a function of the accumulated absorbed photons per volume. The slope of the relationship is the quantum yield of the CQ conversion. Therefore, in our formulation (0.7 w% CQ with reducing agents 0.35 w% DMAEMA and 0.05 w% BHT) the quantum yield was solved to be 0.07+/-0.01 CQ conversion per absorbed photon.
New Ru(II) Complex for Dual Activity: Photoinduced Ligand Release and (1)O2 Production.
Loftus, Lauren M; White, Jessica K; Albani, Bryan A; Kohler, Lars; Kodanko, Jeremy J; Thummel, Randolph P; Dunbar, Kim R; Turro, Claudia
2016-03-01
The new complex [Ru(pydppn)(biq)(py)](2+) (1) undergoes both py photodissociation in CH3CN with Φ500 =0.0070(4) and (1)O2 production with ΦΔ =0.75(7) in CH3 OH from a long-lived (3) ππ* state centered on the pydppn ligand (pydppn=3-(pyrid-2-yl)benzo[i]dipyrido[3,2-a:2',3'-c]phenazine; biq = 2,2'-biquinoline; py=pyridine). This represents an order of magnitude decrease in the Φ500 compared to the previously reported model compound [Ru(tpy)(biq)(py)](2+) (3) (tpy=2,2':6',2''-terpyridine) that undergoes only ligand exchange. The effect on the quantum yields by the addition of a second deactivation pathway through the low-lying (3) ππ* state necessary for dual reactivity was investigated using ultrafast and nanosecond transient absorption spectroscopy, revealing a significantly shorter (3) MLCT lifetime in 1 relative to that of the model complex 3. Due to the structural similarities between the two compounds, the lower values of Φ500 and ΦΔ compared to that of [Ru(pydppn)(bpy)(py)](2+) (2) (bpy=2,2'-bipyridine) are attributed to a competitive excited state population between the (3) LF states involved in ligand dissociation and the long-lived (3) ππ* state in 1. Complex 1 represents a model compound for dual activity that may be applied to photochemotherapy. PMID:26715085
Accurate fluorescence quantum yield determination by fluorescence correlation spectroscopy.
Kempe, Daryan; Schöne, Antonie; Fitter, Jörg; Gabba, Matteo
2015-04-01
Here, we present a comparative method for the accurate determination of fluorescence quantum yields (QYs) by fluorescence correlation spectroscopy. By exploiting the high sensitivity of single-molecule spectroscopy, we obtain the QYs of samples in the microliter range and at (sub)nanomolar concentrations. Additionally, in combination with fluorescence lifetime measurements, our method allows the quantification of both static and collisional quenching constants. Thus, besides being simple and fast, our method opens up the possibility to photophysically characterize labeled biomolecules under application-relevant conditions and with low sample consumption, which is often important in single-molecule studies.
Spatial mapping of fluorophore quantum yield in diffusive media.
Zhao, Yanyu; Roblyer, Darren
2015-08-01
Fluorescence quantum yield (QY) indicates the efficiency of the fluorescence process. The QY of many fluorophores is sensitive to local tissue environments, highlighting the possibility of using QY as an indicator of important parameters such as pH or temperature. QY is commonly measured by comparison to a well-known standard in nonscattering media. We propose a new imaging method, called quantum yield imaging (QYI), to spatially map the QY of a fluorophore within an optically diffusive media. QYI utilizes the wide-field diffuse optical technique spatial frequency domain imaging (SFDI) as well as planar fluorescence imaging. SFDI is used to measure the optical properties of the background media and the absorption contributed by the fluorophore. The unknown QY is then calculated by combining information from both modalities. A fluorescent sample with known QY is used to account for instrument response. To demonstrate QYI, rhodamine B and SNARF-5 were imaged in liquid phantoms with different background optical properties. The methanol:water ratio and pH were changed for rhodamine B and SNARF-5 solvents, respectively, altering the QY of each through a wide range. QY was determined with an agreement of 0.021 and 0.012 for rhodamine B and SNARF-5, respectively. PMID:26308165
Synthesis of Luminescent Graphene Quantum Dots with High Quantum Yield and Their Toxicity Study
Jiang, Dan; Chen, Yunping; Li, Na; Li, Wen; Wang, Zhenguo; Zhu, Jingli; Zhang, Hong; Liu, Bin; Xu, Shan
2015-01-01
High fluorescence quantum yield graphene quantum dots (GQDs) have showed up as a new generation for bioimaging. In this work, luminescent GQDs were prepared by an ameliorative photo-Fenton reaction and a subsequent hydrothermal process using graphene oxide sheets as the precursor. The as-prepared GQDs were nanomaterials with size ranging from 2.3 to 6.4 nm and emitted intense green luminescence in water. The fluorescence quantum yield was as high as 24.6% (excited at 340 nm) and the fluorescence was strongest at pH 7. Moreover, the influences of low-concentration (12.5, 25 μg/mL) GQDs on the morphology, viability, membrane integrity, internal cellular reactive oxygen species level and mortality of HeLa cells were relatively weak, and the in vitro imaging demonstrated GQDs were mainly in the cytoplasm region. More strikingly, zebrafish embryos were co-cultured with GQDs for in vivo imaging, and the results of heart rate test showed the intake of small amounts of GQDs brought little harm to the cardiovascular of zebrafish. GQDs with high quantum yield and strong photoluminescence show good biocompatibility, thus they show good promising for cell imaging, biolabeling and other biomedical applications. PMID:26709828
New RuII Complex for Dual Activity: Photoinduced Ligand Release and 1O2 Production
Loftus, Lauren M.; White, Jessica K.; Albani, Bryan A.; Kohler, Lars; Kodanko, Jeremy J.; Thummel, Randolph P.
2016-01-01
The new complex [Ru(pydppn)(biq)(py)]2+ (1) undergoes both py photodissociation in CH3CN with Φ500=0.0070(4) and 1O2 production with ΦΔ=0.75(7) in CH3OH from a long-lived 3ππ* state centered on the pydppn ligand (pydppn=3-(pyrid-2-yl)benzo[i]dipyrido[3,2-a:2′,3′-c]phenazine; biq = 2,2′-biquinoline; py= pyridine). This represents an order of magnitude decrease in the Φ500 compared to the previously reported model compound [Ru(tpy)(biq)(py)]2+ (3) (tpy=2,2′:6′,2″-terpyridine) that undergoes only ligand exchange. The effect on the quantum yields by the addition of a second deactivation pathway through the low-lying 3ππ* state necessary for dual reactivity was investigated using ultrafast and nanosecond transient absorption spectroscopy, revealing a significantly shorter 3MLCT lifetime in 1 relative to that of the model complex 3. Due to the structural similarities between the two compounds, the lower values of Φ500 and ΦΔ compared to that of [Ru(pydppn)(bpy)(py)]2+ (2) (bpy=2,2′-bipyridine) are attributed to a competitive excited state population between the 3LF states involved in ligand dissociation and the long-lived 3ππ* state in 1. Complex 1 represents a model compound for dual activity that may be applied to photochemotherapy. PMID:26715085
Luminescence quantum yields of gold nanoparticles varying with excitation wavelengths.
Cheng, Yuqing; Lu, Guowei; He, Yingbo; Shen, Hongming; Zhao, Jingyi; Xia, Keyu; Gong, Qihuang
2016-01-28
Luminescence quantum yields (QYs) of gold nanoparticles including nanorods, nanobipyramids and nanospheres are measured elaborately at a single nanoparticle level with different excitation wavelengths. It is found that the QYs of the nanostructures are essentially dependent on the excitation wavelength. The QY is higher when the excitation wavelength is blue-detuned and close to the nanoparticles' surface plasmon resonance peak. A phenomenological model based on the plasmonic resonator concept is proposed to understand the experimental findings. The excitation wavelength dependent QY is attributed to the wavelength dependent coupling efficiency between the free electron oscillation and the intrinsic plasmon resonant radiative mode. These studies should contribute to the understanding of one-photon luminescence from metallic nanostructures and plasmonic surface enhanced spectroscopy. PMID:26731570
Luminescence quantum yields of gold nanoparticles varying with excitation wavelengths
NASA Astrophysics Data System (ADS)
Cheng, Yuqing; Lu, Guowei; He, Yingbo; Shen, Hongming; Zhao, Jingyi; Xia, Keyu; Gong, Qihuang
2016-01-01
Luminescence quantum yields (QYs) of gold nanoparticles including nanorods, nanobipyramids and nanospheres are measured elaborately at a single nanoparticle level with different excitation wavelengths. It is found that the QYs of the nanostructures are essentially dependent on the excitation wavelength. The QY is higher when the excitation wavelength is blue-detuned and close to the nanoparticles' surface plasmon resonance peak. A phenomenological model based on the plasmonic resonator concept is proposed to understand the experimental findings. The excitation wavelength dependent QY is attributed to the wavelength dependent coupling efficiency between the free electron oscillation and the intrinsic plasmon resonant radiative mode. These studies should contribute to the understanding of one-photon luminescence from metallic nanostructures and plasmonic surface enhanced spectroscopy.
Film quantum yields of EUV& ultra-high PAG photoresists
Hassanein, Elsayed; Higgins, Craig; Naulleau, Patrick; Matyi, Richard; Gallatin, Greg; Denbeaux, Gregory; Antohe, Alin; Thackery, Jim; Spear, Kathleen; Szmanda, Charles; Anderson, Christopher N.; Niakoula, Dimitra; Malloy, Matthew; Khurshid, Anwar; Montgomery, Cecilia; Piscani, Emil C.; Rudack, Andrew; Byers, Jeff; Ma, Andy; Dean, Kim; Brainard, Robert
2008-01-10
Base titration methods are used to determine C-parameters for three industrial EUV photoresist platforms (EUV-2D, MET-2D, XP5496) and twenty academic EUV photoresist platforms. X-ray reflectometry is used to measure the density of these resists, and leads to the determination of absorbance and film quantum yields (FQY). Ultrahigh levels ofPAG show divergent mechanisms for production of photo acids beyond PAG concentrations of 0.35 moles/liter. The FQY of sulfonium PAGs level off, whereas resists prepared with iodonium PAG show FQY s that increase beyond PAG concentrations of 0.35 moles/liter, reaching record highs of 8-13 acids generatedlEUV photons absorbed.
Near-unity photoluminescence quantum yield in MoS₂.
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.
Near-unity photoluminescence quantum yield in MoS₂.
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. PMID:26612948
Bilski, P; Burkhart, J G; Chignell, C F
2003-11-19
Environmental pollutants activated by UV sunlight may have contributed to the recent decline in frog populations and the concomitant increase in malformations in the USA and abroad. UV radiation is able to mutate DNA and to initiate photosensitization processes that generate mutagenic and biologically disruptive oxygen transients. We have examined water from selected sites in Minnesota and Vermont using singlet molecular oxygen (1O(2)), detected by its phosphorescence and free radicals detected by spin trapping, as markers for photosensitization. Water from a pond in Minnesota with malformed frogs, which also causes malformations in the laboratory, photosensitized more 1O(2), even though it absorbed less UV light compared to water from a site that did not cause malformations. This suggested that unknown natural or pollutant agents were present, and that photosensitization may be involved. Although UV irradiation of the two Minnesota water samples in the presence of the spin trap 5,5-dimethyl-1-pyrroline N-oxide (DMPO) revealed the presence of the DMPO/*OH, DMPO/*H(e(aq)-) and DMPO/*C(unknown) adducts there were no qualitative or quantitative differences between them. We also examined water samples from several sites in Vermont, and compared them by measuring the quantum yield of 1O(2) photosensitization. While all the Vermont samples produced a small amount of 1O(2), there was no clear correlation with the incidence of frog malformations. However, the samples differed strongly in absorption spectra and the ability to quench 1O(2). These factors may determine how much UV light is absorbed and converted into chemical reactions. Our results show that photochemical characterization of 1O(2) photosensitization is possible in untreated natural water samples. Photosensitization falls into the category of global factors that may be closely associated with the effects of UV irradiation of the Earth's environments. Thus, photosensitization might be an important component in
Near-unity quantum yields from chloride treated CdTe colloidal quantum dots.
Page, Robert C; Espinobarro-Velazquez, Daniel; Leontiadou, Marina A; Smith, Charles; Lewis, Edward A; Haigh, Sarah J; Li, Chen; Radtke, Hanna; Pengpad, Atip; Bondino, Federica; Magnano, Elena; Pis, Igor; Flavell, Wendy R; O'Brien, Paul; Binks, David J
2015-04-01
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. This 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.
NASA Astrophysics Data System (ADS)
Fery-Forgues*, Suzanne; Lavabre, Dominique
1999-09-01
Fluorescence quantum yields are used to quantify the efficiency of the emission process. In spite of the importance of these data, experimental directions for their acquisition are rarely given. A general procedure for determining the relative fluorescence quantum yield of solutions is described here, drawing attention to the many pitfalls that students may encounter. Starting materials are common yellow and pink highlighter pens.
Local Density Fluctuations Predict Photoisomerization Quantum Yield of Azobenzene-Modified DNA.
Kingsland, Addie; Samai, Soumyadyuti; Yan, Yunqi; Ginger, David S; Maibaum, Lutz
2016-08-01
Azobenzene incorporated into DNA has a photoisomerization quantum yield that depends on the DNA sequence near the azobenzene attachment site. We use Molecular Dynamics computer simulations to elucidate which physical properties of the modified DNA determine the quantum yield. We show for a wide range of DNA sequences that the photoisomerization quantum yield is strongly correlated with the variance of the number of atoms in close proximity to the outer phenyl ring of the azobenzene group. We infer that quantum yield is controlled by the availability of fluctuations that enable the conformational change. We demonstrate that these simulations can be used as a qualitative predictive tool by calculating the quantum yield for several novel DNA sequences, and confirming these predictions using UV-vis spectroscopy. Our results will be useful for the development of a wide range of applications of photoresponsive DNA nanotechnology. PMID:27428569
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.
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.
Electron quantum yields from a barium photocathode illuminated with polarized light
Conde, M.E.; Chattopadhyay, S.; Kim, K.J.; Kwon, S.I.; Leung, K.N.; Young, A.T.
1993-05-01
Photoemission measurements with a barium photo-cathode and a nitrogen laser are reported. The cathode is prepared by evaporating barium onto a copper disc. Radiation from a nitrogen laser (337 nm, 10 ns) is polarized and strikes the cathode surface at variable angles. An electron quantum yield as high as 1 {times} 10{sup {minus}3} is observed. The dependence of the quantum yield on the beam polarization and angle of incidence is investigated. The results indicate that higher quantum yields are achieved when the laser beam is incident at an angle of {approximately}55{degree} and is polarized perpendicular to the plane of incidence.
Gradient CdSe/CdS Quantum Dots with Room Temperature Biexciton Unity Quantum Yield.
Nasilowski, Michel; Spinicelli, Piernicola; Patriarche, Gilles; Dubertret, Benoît
2015-06-10
Auger recombination is a major limitation for the fluorescent emission of quantum dots (QDs). It is the main source of QDs fluorescence blinking at the single-particle level. At high-power excitation, when several charge carriers are formed inside a QD, Auger becomes more efficient and severely decreases the quantum yield (QY) of multiexcitons. This limits the efficiency and the use of colloidal QDs in applications where intense light output is required. Here, we present a new generation of thick-shell CdSe/CdS QDs with dimensions >40 nm and a composition gradient between the core and the shell that exhibits 100% QY for the emission of both the monoexciton and the biexciton in air and at room temperature for all the QDs we have observed. The fluorescence emission of these QDs is perfectly Poissonian at the single-particle level at different excitation levels and temperatures, from 30 to 300 K. In these QDs, the emission of high-order (>2) multiexcitons is quite efficient, and we observe white light emission at the single-QD level when high excitation power is used. These gradient thick shell QDs confirm the suppression of Auger recombination in gradient core/shell structures and help further establish the colloidal QDs with a gradient shell as a very stable source of light even under high excitation.
Gradient CdSe/CdS Quantum Dots with Room Temperature Biexciton Unity Quantum Yield.
Nasilowski, Michel; Spinicelli, Piernicola; Patriarche, Gilles; Dubertret, Benoît
2015-06-10
Auger recombination is a major limitation for the fluorescent emission of quantum dots (QDs). It is the main source of QDs fluorescence blinking at the single-particle level. At high-power excitation, when several charge carriers are formed inside a QD, Auger becomes more efficient and severely decreases the quantum yield (QY) of multiexcitons. This limits the efficiency and the use of colloidal QDs in applications where intense light output is required. Here, we present a new generation of thick-shell CdSe/CdS QDs with dimensions >40 nm and a composition gradient between the core and the shell that exhibits 100% QY for the emission of both the monoexciton and the biexciton in air and at room temperature for all the QDs we have observed. The fluorescence emission of these QDs is perfectly Poissonian at the single-particle level at different excitation levels and temperatures, from 30 to 300 K. In these QDs, the emission of high-order (>2) multiexcitons is quite efficient, and we observe white light emission at the single-QD level when high excitation power is used. These gradient thick shell QDs confirm the suppression of Auger recombination in gradient core/shell structures and help further establish the colloidal QDs with a gradient shell as a very stable source of light even under high excitation. PMID:25990468
NASA Astrophysics Data System (ADS)
Qu, Ailan; Xie, Haolong; Xu, Xinmei; Zhang, Yangyu; Wen, Shengwu; Cui, Yifan
2016-07-01
Graphene quantum dots (GQDs) with high quantum yield (about 23.6% at an excitation wavelength of 320 nm) and GQDs/TiO2 nanotubes (GQDs/TiO2 NTs) composites were achieved by a simple hydrothermal method at low temperature. Photoluminescence characterization showed that the GQDs exhibited the down-conversion PL features at excitation from 300 to 420 nm and up-conversion photoluminescence in the range of 600-800 nm. The photocatalytic activity of prepared GQDs/TiO2 NTs composites on the degradation of methyl orange (MO) was significantly enhanced compared with that of pure TiO2 nanotubes (TiO2 NTs). For the composites coupling with 1.5%, 2.5% and 3.5% GQDs, the degradation of MO after 20 min irradiation under UV-vis light irradiation (λ = 380-780 nm) were 80.52%, 94.64% and 51.91%, respectively, which are much higher than that of pure TiO2 NTs (35.41%). It was inferred from the results of characterization that the improved photocatalytic activity of the GQDs/TiO2 NTs composites was attributed to the synergetic effect of up-conversion properties of the GQDs, enhanced visible light absorption and efficient separation of photogenerated electron-holes of the GQDs/TiO2 composite.
Quantum yield and lifetime data analysis for the UV curable quantum dot nanocomposites
Cheng, Qi; Liu, Cui; Wei, Wenjun; Xu, Heng; You, Qingliang; Zou, Linling; Liu, Xueqing; Liu, Jiyan; Cao, Yuan-Cheng; Zheng, Guang
2016-01-01
The quantum yield (QY) and lifetime are the important parameters for the photoluminescent materials. The data here report the changes of the QY and lifetime for the quantum dot (QD) nanocomposite after the UV curing of the urethane acrylate prepolymer. The data were collected based on the water soluble CdTe QDs and urethane acrylate prepolymer. Colloidal QDs were in various concentration from 0.5×10−3 molL−1 to 10×10−3 molL−1, and 1% (wt%) 1173 was the photoinitiator. The QY before the curing was 56.3%, 57.8% and 58.6% for the QDs 510 nm, 540 nm and 620 nm, respectively. The QY after the curing was changed to 8.9%, 9.6% and 13.4% for the QDs 510 nm, 540 nm and 620 nm, respectively. Lifetime data showed that the lifetime was changed from 23.71 ns, 24.55 ns, 23.52 ns to 1.29 ns, 2.74 ns, 2.45 ns for the QDs 510 nm, 540 nm and 620 nm, respectively. PMID:26909375
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...
Comparison of photoluminescence quantum yield of single gold nanobipyramids and gold nanorods.
Rao, Wenye; Li, Qiang; Wang, Yuanzhao; Li, Tao; Wu, Lijun
2015-03-24
Fluorescent gold nanoparticles with high quantum yield are highly desirable for optical imaging in the fields of biology and materials science. We investigate the one-photon photoluminescence (PL) properties of individual gold nanobipyramids (GNBs) and find they are analogous to those of the extensively studied gold nanorods (GNRs). By combining PL and atomic force microscopy (AFM) measurements with discrete dipole approximation (DDA) simulations, we obtain the PL quantum yield of single GNRs and GNBs. Compared to GNRs in the similar surface plasmon resonance range, the PL quantum yield of GNBs is found to be doubled. The stronger field intensity around GNBs can explain their higher PL quantum yields. Our research would provide deeper understanding of the mechanism of PL from gold nanoparticles as well as be beneficial for finding out optical imaging labels with high contrast.
Primary quantum yields of ketyl radicals in photoreduction by amines. Abstraction of H from N
Inbar, S.; Linschitz, H.; Cohen, S.G.
1980-02-13
Results of laser flash photolysis studies of the primary reaction of benzophenone triplet with aliphatic amines in benzene solution are reported. Quantum yield of formation of benzophenone ketyl radical was 0.9 - 1.0. Quantum yields for reduction of ketone also were determined for various amines, and the effects of tert-butyl alcohol on radical formation was investigated. Data indicated that H is not abstracted from -CH/sub 3/ but is abstracted efficiently from -NH/sub 2/. The very high quantum yields observed with tertiary and secondary amines were thought to imply exciplex formation, but lower quantum yields with primary amines were conditionally attributed to higher ionization potentials. (BLM)
On the possibility of long-wavelength long-lifetime high-quantum-yield luminophores.
Lakowicz, J R; Piszczek, G; Kang, J S
2001-01-01
We describe an approach to creating a new class of luminophores which display both long wavelength emissions exceeding 600 nm and long lifetimes. These luminophores are based on resonance energy transfer (RET) from a long lifetime donor to a short lifetime but long wavelength acceptor. We demonstrated the possibility of obtaining these desirable spectral properties using donors and acceptors noncovalently bound to DNA. The donor was a ruthenium (Ru) metal-ligand complex in which one of the diimine ligands intercalated into double-helix DNA. The acceptors were either nile blue, TOTO-3, or TO-PRO-3. Upon binding of the acceptor to donor-labeled DNA, we found that the acceptor quantum yield was remarkably enhanced so that the wavelength-integrated intensities of the donor and acceptor bound to DNA were many-fold greater than the intensity of the donor and acceptor alone when separately bound to DNA. The origin of this effect is efficient energy transfer from the donor. Under these conditions the effective overall quantum yield approaches that of the acceptor. Importantly, the increased quantum yield can be obtained while maintaining usefully long apparent acceptor lifetimes of 30 to 80 ns. The effect of an increased quantum yield from a low quantum yield donor may find use in assays to detect macromolecular binding interactions. These results suggest the synthesis of covalently linked donor-acceptor pairs with the desirable spectral properties of long wavelength emission, high quantum yield, and moderately long lifetimes for gated detection.
Size-dependent absolute quantum yields for size-separated colloidally-stable silicon nanocrystals.
Mastronardi, Melanie L; Maier-Flaig, Florian; Faulkner, Daniel; Henderson, Eric J; Kübel, Christian; Lemmer, Uli; Ozin, Geoffrey A
2012-01-11
Size-selective precipitation was used to successfully separate colloidally stable allylbenzene-capped silicon nanocrystals into several visible emitting monodisperse fractions traversing the quantum size effect range of 1-5 nm. This enabled the measurement of the absolute quantum yield and lifetime of photoluminescence of allylbenzene-capped silicon nanocrystals as a function of size. The absolute quantum yield and lifetime are found to monotonically decrease with decreasing nanocrystal size, which implies that nonradiative vibrational and surface defect effects overwhelm spatial confinement effects that favor radiative relaxation. Visible emission absolute quantum yields as high as 43% speak well for the development of "green" silicon nanocrystal color-tunable light emitting diodes that can potentially match the performance of their toxic heavy metal chalcogenide counterparts.
Measurements of barium photocathode quantum yields at four excimer laser wavelengths
Van Loy, M.D.; Young, A.T.; Leung, K.N.
1992-06-01
The electron quantum yields from barium cathodes excited by excimer laser radiation at 193, 248, 308, and 351 nm have been determined. Experiments with different cathode surface preparation techniques reveal that deposition of barium film a few microns thick on a clean copper surface under moderate vacuum conditions achieves relatively high quantum efficiencies. Quantum yields measured from surfaces prepared in this manner are 2.3 x 10{sup -3} at 193 nm, 7.6 x 10{sup - 4} at 248 nm, 6.1 x 10{sup -4} at 308 nm, and 4.0 x 10{sup -4} at 351 nm. Other preparation techniques, such as laser cleaning of a solid barium surface, produced quantum yields that were at least an order of magnitude lower than these values.
Ensemble brightening and enhanced quantum yield in size-purified silicon nanocrystals
Miller, Joseph B.; Van Sickle, Austin R.; Anthony, Rebecca J.; Kroll, Daniel M.; Kortshagen, Uwe R.; Hobbie, Erik K.
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
Ensemble brightening and enhanced quantum yield in size-purified silicon nanocrystals
Miller, Joseph B.; Van Sickle, Austin R.; Anthony, Rebecca J.; Kroll, Daniel M.; Kortshagen, Uwe R.; Hobbie, Erik K.
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 the 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.
A graphene quantum dot photodynamic therapy agent with high singlet oxygen generation
Ge, Jiechao; Lan, Minhuan; Zhou, Bingjiang; Liu, Weimin; Guo, Liang; Wang, Hui; Jia, Qingyan; Niu, Guangle; Huang, Xing; Zhou, Hangyue; Meng, Xiangmin; Wang, Pengfei; Lee, Chun-Sing; Zhang, Wenjun; Han, Xiaodong
2014-01-01
Clinical applications of current photodynamic therapy (PDT) agents are often limited by their low singlet oxygen (1O2) quantum yields, as well as by photobleaching and poor biocompatibility. Here we present a new PDT agent based on graphene quantum dots (GQDs) that can produce 1O2 via a multistate sensitization process, resulting in a quantum yield of ~1.3, the highest reported for PDT agents. The GQDs also exhibit a broad absorption band spanning the UV region and the entire visible region and a strong deep-red emission. Through in vitro and in vivo studies, we demonstrate that GQDs can be used as PDT agents, simultaneously allowing imaging and providing a highly efficient cancer therapy. The present work may lead to a new generation of carbon-based nanomaterial PDT agents with overall performance superior to conventional agents in terms of 1O2 quantum yield, water dispersibility, photo- and pH-stability, and biocompatibility. PMID:25105845
A graphene quantum dot photodynamic therapy agent with high singlet oxygen generation.
Ge, Jiechao; Lan, Minhuan; Zhou, Bingjiang; Liu, Weimin; Guo, Liang; Wang, Hui; Jia, Qingyan; Niu, Guangle; Huang, Xing; Zhou, Hangyue; Meng, Xiangmin; Wang, Pengfei; Lee, Chun-Sing; Zhang, Wenjun; Han, Xiaodong
2014-01-01
Clinical applications of current photodynamic therapy (PDT) agents are often limited by their low singlet oxygen ((1)O2) quantum yields, as well as by photobleaching and poor biocompatibility. Here we present a new PDT agent based on graphene quantum dots (GQDs) that can produce (1)O2 via a multistate sensitization process, resulting in a quantum yield of ~1.3, the highest reported for PDT agents. The GQDs also exhibit a broad absorption band spanning the UV region and the entire visible region and a strong deep-red emission. Through in vitro and in vivo studies, we demonstrate that GQDs can be used as PDT agents, simultaneously allowing imaging and providing a highly efficient cancer therapy. The present work may lead to a new generation of carbon-based nanomaterial PDT agents with overall performance superior to conventional agents in terms of (1)O2 quantum yield, water dispersibility, photo- and pH-stability, and biocompatibility.
A graphene quantum dot photodynamic therapy agent with high singlet oxygen generation
NASA Astrophysics Data System (ADS)
Ge, Jiechao; Lan, Minhuan; Zhou, Bingjiang; Liu, Weimin; Guo, Liang; Wang, Hui; Jia, Qingyan; Niu, Guangle; Huang, Xing; Zhou, Hangyue; Meng, Xiangmin; Wang, Pengfei; Lee, Chun-Sing; Zhang, Wenjun; Han, Xiaodong
2014-08-01
Clinical applications of current photodynamic therapy (PDT) agents are often limited by their low singlet oxygen (1O2) quantum yields, as well as by photobleaching and poor biocompatibility. Here we present a new PDT agent based on graphene quantum dots (GQDs) that can produce 1O2 via a multistate sensitization process, resulting in a quantum yield of ~1.3, the highest reported for PDT agents. The GQDs also exhibit a broad absorption band spanning the UV region and the entire visible region and a strong deep-red emission. Through in vitro and in vivo studies, we demonstrate that GQDs can be used as PDT agents, simultaneously allowing imaging and providing a highly efficient cancer therapy. The present work may lead to a new generation of carbon-based nanomaterial PDT agents with overall performance superior to conventional agents in terms of 1O2 quantum yield, water dispersibility, photo- and pH-stability, and biocompatibility.
A graphene quantum dot photodynamic therapy agent with high singlet oxygen generation.
Ge, Jiechao; Lan, Minhuan; Zhou, Bingjiang; Liu, Weimin; Guo, Liang; Wang, Hui; Jia, Qingyan; Niu, Guangle; Huang, Xing; Zhou, Hangyue; Meng, Xiangmin; Wang, Pengfei; Lee, Chun-Sing; Zhang, Wenjun; Han, Xiaodong
2014-01-01
Clinical applications of current photodynamic therapy (PDT) agents are often limited by their low singlet oxygen ((1)O2) quantum yields, as well as by photobleaching and poor biocompatibility. Here we present a new PDT agent based on graphene quantum dots (GQDs) that can produce (1)O2 via a multistate sensitization process, resulting in a quantum yield of ~1.3, the highest reported for PDT agents. The GQDs also exhibit a broad absorption band spanning the UV region and the entire visible region and a strong deep-red emission. Through in vitro and in vivo studies, we demonstrate that GQDs can be used as PDT agents, simultaneously allowing imaging and providing a highly efficient cancer therapy. The present work may lead to a new generation of carbon-based nanomaterial PDT agents with overall performance superior to conventional agents in terms of (1)O2 quantum yield, water dispersibility, photo- and pH-stability, and biocompatibility. PMID:25105845
Shen, Xun-wei; Yuan, Chun-wei
2005-01-01
Heterogeneous photocatalysis in slurry reactors have the particular characteristic that the catalyst particles not only absorb but also scatter photons so the radiation scattering can not be neglected. However, it is very difficult in mathematics to obtain the rigorous solution of the radiative transfer equation. Consequently present methods, in which the apparent quantum yields can be calculated by employing the incident radiation intensity, always underestimate quantum yields calculations. In this paper, a method is developed to produce absolute values of photocatalytic quantum yields in slurry reactor based on cylindrical UV light source. In a typical laboratory reactor (diameter equal to 5.6 cm and length equal to 10 cm) the values for the photocatalytic degradation of phenol are reported under precisely defined conditions. The true value of the local volumetric rate of photon absorption (LVRPA) can be obtained. It was shown that apparent quantum yields differ from true quantum yields 7.08% and that for the same geometric arrangement, vanishing fraction accounts for 1.1% of the incident radiation. The method can be used to compare reactivity of different catalysts or, for a given catalyst, reactivity with different model compounds and as a principle to design a reactor.
Quantum Yields of CAM Plants Measured by Photosynthetic O(2) Exchange.
Adams, W W; Nishida, K; Osmond, C B
1986-05-01
The quantum yield of photosynthetic O(2) exchange was measured in eight species of leaf succulents representative of both malic enzyme type and phosphoenolpyruvate carboxykinase type CAM plants. Measurements were made at 25 degrees C and CO(2) saturation using a leaf disc O(2) electrode system, either during or after deacidification. The mean quantum yield was 0.095 +/- 0.012 (sd) moles O(2) per mole quanta, which compared with 0.094 +/- 0.006 (sd) moles O(2) per mole quanta for spinach leaf discs measured under the same conditions. There were no consistent differences in quantum yield between decarboxylation types or during different phases of CAM metabolism. On the basis of current notions of compartmentation of CAM biochemistry, our observations are interpreted to indicate that CO(2) refixation is energetically independent of gluconeogenesis during deacidification.
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 measurements 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.
Photosynthetic Quantum Yield Dynamics: From Photosystems to Leaves[W][OA
Hogewoning, Sander W.; Wientjes, Emilie; Douwstra, Peter; Trouwborst, Govert; van Ieperen, Wim; Croce, Roberta; Harbinson, Jeremy
2012-01-01
The mechanisms underlying the wavelength dependence of the quantum yield for CO2 fixation (α) and its acclimation to the growth-light spectrum are quantitatively addressed, combining in vivo physiological and in vitro molecular methods. Cucumber (Cucumis sativus) was grown under an artificial sunlight spectrum, shade light spectrum, and blue light, and the quantum yield for photosystem I (PSI) and photosystem II (PSII) electron transport and α were simultaneously measured in vivo at 20 different wavelengths. The wavelength dependence of the photosystem excitation balance was calculated from both these in vivo data and in vitro from the photosystem composition and spectroscopic properties. Measuring wavelengths overexciting PSI produced a higher α for leaves grown under the shade light spectrum (i.e., PSI light), whereas wavelengths overexciting PSII produced a higher α for the sun and blue leaves. The shade spectrum produced the lowest PSI:PSII ratio. The photosystem excitation balance calculated from both in vivo and in vitro data was substantially similar and was shown to determine α at those wavelengths where absorption by carotenoids and nonphotosynthetic pigments is insignificant (i.e., >580 nm). We show quantitatively that leaves acclimate their photosystem composition to their growth light spectrum and how this changes the wavelength dependence of the photosystem excitation balance and quantum yield for CO2 fixation. This also proves that combining different wavelengths can enhance quantum yields substantially. PMID:22623496
Bidault, Sébastien; Devilez, Alexis; Maillard, Vincent; Lermusiaux, Laurent; Guigner, Jean-Michel; Bonod, Nicolas; Wenger, Jérôme
2016-04-26
Minimizing the luminescence lifetime while maintaining a high emission quantum yield is paramount in optimizing the excitation cross-section, radiative decay rate, and brightness of quantum solid-state light sources, particularly at room temperature, where nonradiative processes can dominate. We demonstrate here that DNA-templated 60 and 80 nm diameter gold nanoparticle dimers, featuring one fluorescent molecule, provide single-photon emission with lifetimes that can fall below 10 ps and typical quantum yields in a 45-70% range. Since these colloidal nanostructures are obtained as a purified aqueous suspension, fluorescence spectroscopy can be performed on both fixed and freely diffusing nanostructures to quantitatively estimate the distributions of decay rate and fluorescence intensity enhancements. These data are in excellent agreement with theoretical calculations and demonstrate that millions of bright fluorescent nanostructures, with radiative lifetimes below 100 ps, can be produced in parallel. PMID:26972678
Impact of Vibrational Coherence on the Quantum Yield at a Conical Intersection.
Duan, Hong-Guang; Miller, R J Dwayne; Thorwart, Michael
2016-09-01
We study the vibrationally coherent quantum dynamics of an electronic wave packet in the vicinity of a conical intersection within a three-state two-mode model. By transforming the coherent tuning and coupling modes into the bath, the underdamped dynamics of the resulting effective three-state model is solved efficiently by the numerically exact hierarchy equation of motion approach. The transient excited-state absorption and two-dimensional spectra reveal the impact of vibrational coherence on the relaxation pathways of the wave packet. We find that both the quantum yield and the isomerization rate are crucially influenced by the vibrational coherence of the wave packet. A less coherent wave packet can traverse the conical intersection more rapidly, while the resulting quantum yield is smaller. Finally, we show that repeated passages of the wave packet through the conical intersection can lead to measurable interference effects in the form of Stueckelberg oscillations. PMID:27547995
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.
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.
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…
NASA Astrophysics Data System (ADS)
Dey, Swayandipta; Zhou, Yadong; Tian, Xiangdong; Jenkins, Julie A.; Chen, Ou; Zou, Shengli; Zhao, Jing
2015-04-01
In this work, we systematically investigated the plasmonic effect on blinking, photon antibunching behavior and biexciton emission of single CdSe/CdS core/shell quantum dots (QDs) near gold nanoparticles (NPs) with a silica shell (Au@SiO2). In order to obtain a strong interaction between the plasmons and excitons, the Au@SiO2 NPs and CdSe/CdS QDs of appropriate sizes were chosen so that the plasmon resonance overlaps with the absorption and emission of the QDs. We observed that in the regime of a low excitation power, the photon antibunching and blinking properties of single QDs were modified significantly when the QDs were on the Au@SiO2 substrates compared to those on glass. Most significantly, second-order photon intensity correlation data show that the presence of plasmons increases the ratio of the biexciton quantum yield over the exciton quantum yield (QYBX/QYX). An electrodynamics model was developed to quantify the effect of plasmons on the lifetime, quantum yield, and emission intensity of the biexcitons for the QDs. Good agreement was obtained between the experimentally measured and calculated changes in QYBX/QYX due to Au@SiO2 NPs, showing the validity of the developed model. The theoretical studies also indicated that the relative position of the QDs to the Au NPs and the orientation of the electric field are important factors that regulate the emission properties of the excitons and biexcitons of QDs. The study suggests that the multiexciton emission efficiency in QD systems can be manipulated by employing properly designed plasmonic structures.In this work, we systematically investigated the plasmonic effect on blinking, photon antibunching behavior and biexciton emission of single CdSe/CdS core/shell quantum dots (QDs) near gold nanoparticles (NPs) with a silica shell (Au@SiO2). In order to obtain a strong interaction between the plasmons and excitons, the Au@SiO2 NPs and CdSe/CdS QDs of appropriate sizes were chosen so that the plasmon resonance
Dey, Swayandipta; Zhou, Yadong; Tian, Xiangdong; Jenkins, Julie A; Chen, Ou; Zou, Shengli; Zhao, Jing
2015-04-21
In this work, we systematically investigated the plasmonic effect on blinking, photon antibunching behavior and biexciton emission of single CdSe/CdS core/shell quantum dots (QDs) near gold nanoparticles (NPs) with a silica shell (Au@SiO2). In order to obtain a strong interaction between the plasmons and excitons, the Au@SiO2 NPs and CdSe/CdS QDs of appropriate sizes were chosen so that the plasmon resonance overlaps with the absorption and emission of the QDs. We observed that in the regime of a low excitation power, the photon antibunching and blinking properties of single QDs were modified significantly when the QDs were on the Au@SiO2 substrates compared to those on glass. Most significantly, second-order photon intensity correlation data show that the presence of plasmons increases the ratio of the biexciton quantum yield over the exciton quantum yield (QYBX/QYX). An electrodynamics model was developed to quantify the effect of plasmons on the lifetime, quantum yield, and emission intensity of the biexcitons for the QDs. Good agreement was obtained between the experimentally measured and calculated changes in QYBX/QYX due to Au@SiO2 NPs, showing the validity of the developed model. The theoretical studies also indicated that the relative position of the QDs to the Au NPs and the orientation of the electric field are important factors that regulate the emission properties of the excitons and biexcitons of QDs. The study suggests that the multiexciton emission efficiency in QD systems can be manipulated by employing properly designed plasmonic structures. PMID:25806486
Dey, Swayandipta; Zhou, Yadong; Tian, Xiangdong; Jenkins, Julie A; Chen, Ou; Zou, Shengli; Zhao, Jing
2015-04-21
In this work, we systematically investigated the plasmonic effect on blinking, photon antibunching behavior and biexciton emission of single CdSe/CdS core/shell quantum dots (QDs) near gold nanoparticles (NPs) with a silica shell (Au@SiO2). In order to obtain a strong interaction between the plasmons and excitons, the Au@SiO2 NPs and CdSe/CdS QDs of appropriate sizes were chosen so that the plasmon resonance overlaps with the absorption and emission of the QDs. We observed that in the regime of a low excitation power, the photon antibunching and blinking properties of single QDs were modified significantly when the QDs were on the Au@SiO2 substrates compared to those on glass. Most significantly, second-order photon intensity correlation data show that the presence of plasmons increases the ratio of the biexciton quantum yield over the exciton quantum yield (QYBX/QYX). An electrodynamics model was developed to quantify the effect of plasmons on the lifetime, quantum yield, and emission intensity of the biexcitons for the QDs. Good agreement was obtained between the experimentally measured and calculated changes in QYBX/QYX due to Au@SiO2 NPs, showing the validity of the developed model. The theoretical studies also indicated that the relative position of the QDs to the Au NPs and the orientation of the electric field are important factors that regulate the emission properties of the excitons and biexcitons of QDs. The study suggests that the multiexciton emission efficiency in QD systems can be manipulated by employing properly designed plasmonic structures.
NASA Astrophysics Data System (ADS)
Liu, Pengpeng; Zhang, Changchang; Liu, Xiang; Cui, Ping
2016-04-01
An economic and green approach of manufacturing carbon quantum dots (CQDs) with a high quantum yield (denoted with HQY-CQDs) and the application in labeling bovine serum albumin (BSA) were described in detail in this work. Firstly, the cheap resources of citric acid and glycine were pyrolysed in drying oven for preparing the CQDs. Then the product was immersed in tetrahydrofuran for 8 h. HQY-CQDs were obtained by removing tetrahydrofuran from the supernate and were evaluated that they possessed a much higher quantum yield compared with that without dealing with tetrahydrofuran and a wonderful photo-bleaching resistance. Such HQY-CQDs could be functionalized by N-hydroxysuccinimide and successively combined with BSA covalently. Thus fluorescent labeling on BSA was realized. The HQY-CQDs were demonstrated with transmission electron microscopy and the chemical modification with N-hydroxysuccinimide was proved by infrared and X-ray photoelectron spectra. Labeling BSA with the HQY-CQDs was confirmed by gel electrophoresis and fluorescence imaging.
Quantum yield and excitation rate of single molecules close to metallic nanostructures.
Holzmeister, Phil; Pibiri, Enrico; Schmied, Jürgen J; Sen, Tapasi; Acuna, Guillermo P; Tinnefeld, Philip
2014-01-01
The interaction of dyes and metallic nanostructures strongly affects the fluorescence and can lead to significant fluorescence enhancement at plasmonic hot spots, but also to quenching. Here we present a method to distinguish the individual contributions to the changes of the excitation, radiative and non-radiative rate and use this information to determine the quantum yields for single molecules. The method is validated by precisely placing single fluorescent dyes with respect to gold nanoparticles as well as with respect to the excitation polarization using DNA origami nanostructures. Following validation, measurements in zeromode waveguides reveal that suppression of the radiative rate and enhancement of the non-radiative rate lead to a reduced quantum yield. Because the method exploits the intrinsic blinking of dyes, it can generally be applied to fluorescence measurements in arbitrary nanophotonic environments. PMID:25370834
Quantum yield and excitation rate of single molecules close to metallic nanostructures.
Holzmeister, Phil; Pibiri, Enrico; Schmied, Jürgen J; Sen, Tapasi; Acuna, Guillermo P; Tinnefeld, Philip
2014-11-05
The interaction of dyes and metallic nanostructures strongly affects the fluorescence and can lead to significant fluorescence enhancement at plasmonic hot spots, but also to quenching. Here we present a method to distinguish the individual contributions to the changes of the excitation, radiative and non-radiative rate and use this information to determine the quantum yields for single molecules. The method is validated by precisely placing single fluorescent dyes with respect to gold nanoparticles as well as with respect to the excitation polarization using DNA origami nanostructures. Following validation, measurements in zeromode waveguides reveal that suppression of the radiative rate and enhancement of the non-radiative rate lead to a reduced quantum yield. Because the method exploits the intrinsic blinking of dyes, it can generally be applied to fluorescence measurements in arbitrary nanophotonic environments.
Sample-averaged biexciton quantum yield measured by solution-phase photon correlation.
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.
A quantum yield determination of O/1D/ production from ozone via laser flash photolysis
NASA Technical Reports Server (NTRS)
Philen, D. L.; Davis, D. D.; Watson, R. T.
1977-01-01
The quantum yield of electronically excited atomic oxygen produced from ozone photolysis was measured at 298 K from wavelengths of 293.0 to 316.5 nm. The reaction of the atomic oxygen with N2O to form excited NO2 was used to monitor the O production; a frequency-doubled flashlamp-pumped dye laser which provided tunable ultraviolet in the desired spectral region with 0.1-nm linewidth served as the photolysis source. The atomic oxygen quantum yield was found to be constant below 300 nm, with a sharp decrease centered at 308 nm and a diminution to less than one tenth of the constant value by 313.5 nm.
Yang Ningli; Zhang Shuyi . E-mail: zhangsy@nju.edu.cn; Kuo Paokuang; Qu Min; Fang Jianwen; Li Jiahuang; Hua Zichun
2007-02-23
The photo-dissociations of oxyhemoglobin of several mammals, such as human, bovine, pig, horse, and rabbit, have been studied. By means of optical pump-probe technique, the quantum yields for photo-dissociation of these oxyhemoglobin have been determined at pH 7 and 20 {sup o}C. A nanosecond laser at 532 nm is used as the pumping source, and a xenon lamp through a monochrometer provides a probe light at 432 nm. The experimental results show that the quantum yields of these mammalian oxyhemoglobin are different from each other, especially for that of rabbit. By analyzing the amino acid sequences and tetramer structures as well as the flexibility and hydrophobicity of the different hemoglobin, possible explanations for the differences are proposed.
Sample-Averaged Biexciton Quantum Yield Measured by Solution-Phase Photon Correlation
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
Quantum yield and excitation rate of single molecules close to metallic nanostructures
Holzmeister, Phil; Pibiri, Enrico; Schmied, Jürgen J.; Sen, Tapasi; Acuna, Guillermo P.; Tinnefeld, Philip
2014-01-01
The interaction of dyes and metallic nanostructures strongly affects the fluorescence and can lead to significant fluorescence enhancement at plasmonic hot spots, but also to quenching. Here we present a method to distinguish the individual contributions to the changes of the excitation, radiative and non-radiative rate and use this information to determine the quantum yields for single molecules. The method is validated by precisely placing single fluorescent dyes with respect to gold nanoparticles as well as with respect to the excitation polarization using DNA origami nanostructures. Following validation, measurements in zeromode waveguides reveal that suppression of the radiative rate and enhancement of the non-radiative rate lead to a reduced quantum yield. Because the method exploits the intrinsic blinking of dyes, it can generally be applied to fluorescence measurements in arbitrary nanophotonic environments. PMID:25370834
Photocurrent Quantum Yield in Suspended Carbon Nanotube p-n Junctions.
Aspitarte, Lee; McCulley, Daniel R; Minot, Ethan D
2016-09-14
We study photocurrent generation in individual suspended carbon nanotube p-n junctions using spectrally resolved scanning photocurrent microscopy. Spatial maps of the photocurrent allow us to determine the length of the p-n junction intrinsic region, as well as the role of the n-type Schottky barrier. We show that reverse-bias operation eliminates complications caused by the n-type Schottky barrier and increases the length of the intrinsic region. The absorption cross-section of the CNT is calculated using an empirically verified model, and the effect of substrate reflection is determined using FDTD simulations. We find that the room temperature photocurrent quantum yield is approximately 30% when exciting the carbon nanotube at the S44 and S55 excitonic transitions. The quantum yield value is an order of magnitude larger than previous estimates. PMID:27575386
Laane, C.; Ford, W.E.; Otvos, J.W.; Calvin, M.
1981-04-01
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/sup +/. 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/sup +/ gradients inatthe presence of valinomycin. When vesicles are made with transmembrane potentials, interior more negative, the quantum yield of heptylviologen reduction is doubled, and, converseley, 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.
Feng, X. T.; Zhang, Y.; Liu, X. G.; Zhang, F.; Wang, Y. L.; Yang, Y. Z.
2015-11-23
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 light 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.
Niwa, Kazuki
2016-01-01
Quantum yield (QY), which is defined as the probability of photon production by a single bio/chemiluminescence reaction, is an important factor to characterize luminescence light intensity emitted diffusively from the reaction solution mixture. Here, methods to measure number of photons to determine QY according to the techniques of national radiometry standards are described. As an example, experiments using firefly bioluminescence reactions are introduced. PMID:27424895
Niwa, Kazuki
2016-01-01
Quantum yield (QY), which is defined as the probability of photon production by a single bio/chemiluminescence reaction, is an important factor to characterize luminescence light intensity emitted diffusively from the reaction solution mixture. Here, methods to measure number of photons to determine QY according to the techniques of national radiometry standards are described. As an example, experiments using firefly bioluminescence reactions are introduced.
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. PMID:26691065
Hertel, Tobias; Himmelein, Sabine; Ackermann, Thomas; Stich, Dominik; Crochet, Jared
2010-12-28
Photoluminescence quantum yields and nonradiative decay of the excitonic S(1) state in length fractionated (6,5) single-wall carbon nanotubes (SWNTs) are studied by continuous wave and time-resolved fluorescence spectroscopy. The experimental data are modeled by diffusion limited contact quenching of excitons at stationary quenching sites including tube ends. A combined analysis of the time-resolved photoluminescence decay and the length dependence of photoluminescence quantum yields (PL QYs) from SWNTs in sodium cholate suspensions allows to determine the exciton diffusion coefficient D = 10.7 ± 0.4 cm(2)s(-1) and lifetime τ(PL) for long tubes of 20 ± 1 ps. PL quantum yields Φ(PL) are found to scale with the inverse diffusion coefficient and the square of the mean quenching site distance, here l(d) = 120 ± 25 nm. The results suggest that low PL QYs of SWNTs are due to the combination of high-diffusive exciton mobility with the presence of only a few quenching sites.
Lee, Hyun Ji; Laskin, Alexander; Laskin, Julia; Nizkorodov, Sergey A.
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) 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.
Lee, Hyun Ji Julie; Laskin, Alexander; Laskin, Julia; Nizkorodov, Sergey A
2013-06-01
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.
Photoluminescence quantum yield of PbS nanocrystals in colloidal suspensions
Greben, M.; Fucikova, A.; Valenta, J.
2015-04-14
The absolute photoluminescence (PL) quantum yield (QY) of oleic acid-capped colloidal PbS quantum dots (QDs) in toluene is thoroughly investigated as function of QD size, concentration, excitation photon energy, and conditions of storage. We observed anomalous decrease of QY with decreasing concentration for highly diluted suspensions. The ligand desorption and QD-oxidation are demonstrated to be responsible for this phenomenon. Excess of oleic acid in suspensions makes the QY values concentration-independent over the entire reabsorption-free range. The PL emission is shown to be dominated by surface-related recombinations with some contribution from QD-core transitions. We demonstrate that QD colloidal suspension stability improves with increasing the concentration and size of PbS QDs.
Scurlock, R.D.; Martire, D.O.; Ogilby, P.R. . Dept. of Chemistry); Taylor, V.L.; Clough, R.L. )
1994-08-15
The quantum yield of singlet oxygen (a[sup 1][Delta][sub g]), produced by energy transfer from the photosensitizer acridine, has been determined by two independent spectroscopic methods in solid polystyrene. Upon 355-nm pulsed-laser irradiation of acridine at 1.3 mJ/pulse, the O[sub 2](a[sup 1][Delta][sub g]) quantum yield in polystyrene [[phi][sub [Delta
Shi, Lei; Yang, Jian Hai; Zeng, Hai Bo; Chen, Yong Mei; Yang, Sheng Chun; Wu, Chao; Zeng, Hao; Yoshihito, Osada; Zhang, Qiqing
2016-08-14
In this contribution, we have shown that the organic fluorophores, 5-oxo-3,5-dihydro-2H-thiazolo [3,2-a] pyridine-3,7-dicarboxylic acid (TPDCA) and 5-oxo-3,5-dihydro-2H-thiazolo [3,2-a] pyridine-7-carboxylic acid (TPCA), are the main ingredients and fluorescence origins of N,S-CDs via systematic analyses. It inspires us to deeply analyze and understand the fluorescence origins of carbon dots with high fluorescence quantum yields, which will expand their applications. PMID:27426926
NASA Astrophysics Data System (ADS)
Wesely, E. Jane; Rothberg, Lewis; Geng, Yanhou; Chen, Shaw
2004-03-01
We have studied the photophysics of a liquid crystalline oligofluorene which emits blue light with a quantum efficiency of forty-nine percent.( Y. Geng, S. Culligan, A. Trajkovska, J. Wallace and S. Chen, Chem. Mater; 2003, 15, 542-549.) The fluorescent yield is reduced when the film has been exposed to ultra-violet light and air. The resulting photooxidation creates luminescent defects that have previously been observed in some polyfluorenes.( E. J. W. List, R. Guentner, P. Scanducci de Freitas, and U. Scherf, Adv Mater., 2002, 14, 374-378.) The defects decrease the overall fluorescent yield because they divert energy away from the blue-emitting chromophores and emit at longer wavelengths with low efficiency. In contrast with previous studies of photooxidized polyfluorenes, we observe two emission peaks associated with defects that have distinct intensity dependence and decay dynamics.
NASA Astrophysics Data System (ADS)
Shi, Lei; Yang, Jian Hai; Zeng, Hai Bo; Chen, Yong Mei; Yang, Sheng Chun; Wu, Chao; Zeng, Hao; Yoshihito, Osada; Zhang, Qiqing
2016-07-01
In this contribution, we have shown that the organic fluorophores, 5-oxo-3,5-dihydro-2H-thiazolo [3,2-a] pyridine-3,7-dicarboxylic acid (TPDCA) and 5-oxo-3,5-dihydro-2H-thiazolo [3,2-a] pyridine-7-carboxylic acid (TPCA), are the main ingredients and fluorescence origins of N,S-CDs via systematic analyses. It inspires us to deeply analyze and understand the fluorescence origins of carbon dots with high fluorescence quantum yields, which will expand their applications.In this contribution, we have shown that the organic fluorophores, 5-oxo-3,5-dihydro-2H-thiazolo [3,2-a] pyridine-3,7-dicarboxylic acid (TPDCA) and 5-oxo-3,5-dihydro-2H-thiazolo [3,2-a] pyridine-7-carboxylic acid (TPCA), are the main ingredients and fluorescence origins of N,S-CDs via systematic analyses. It inspires us to deeply analyze and understand the fluorescence origins of carbon dots with high fluorescence quantum yields, which will expand their applications. Electronic supplementary information (ESI) available. See DOI: 10.1039/c6nr00451b
Solvent effect on the relative quantum yield and fluorescence quenching of 2DAM
NASA Astrophysics Data System (ADS)
Nagaraja, D.; Melavanki, R. M.; Patil, N. R.; Kusanur, R. A.
2014-09-01
The relative quantum yield of diethyl 2-acetamido-2-((3-oxo-3H-benzo[f]chromen-1-yl)methyl) malonate [2DAM] is estimated using single point method with quinine sulfate as standard reference. The quantum yield varies between 0.1161 and 0.3181 depending on the nature of the solvent. The rates of radiative and non radiative decay constants are also calculated. The fluorescence quenching of [2DAM] by aniline is studied at room temperature, by steady state, in five different solvents namely acetonitrile (AN), 1,4 dioxane (DX), 1,2 dichloroethane (DCE), tetrahydrofuran (THF) and toluene (TOL), in order to explore various possible quenching mechanisms. The experimental results show a positive deviation in Stern Volmer plots for all solvents. Various parameters for the quenching process are determined by ground state complex, sphere of action static quenching model and finite sink approximation model. The magnitudes of these rate parameters indicate that positive deviation in the Stern Volmer (SV) plot is due to both static and dynamic processes. Further, finite sink approximation model is used to check whether these bimolecular reactions were diffusion limited or not. The values of distance parameter R‧ and diffusion co efficient D are determined and then compared with the values of encounter distance R and diffusion coefficient D calculated using Stokes-Einstein equation.
Nagaraja, D; Melavanki, R M; Patil, N R; Geethanjali, H S; Kusanur, R A
2015-08-01
We estimated the relative florescence quantum yield (Φ) of 8-methoxy-3-[1-(4,5-dicarbomethoxy-1,2,3-triazoloacetyl)]coumarin [8MDTC] using a single-point method with quinine sulfate in 0.1 M of sulfuric acid used as a standard reference. The fluorescence lifetimes, radiative and non-radiative decay rate constants are calculated. Relative quantum yields were found to be less in the non-polar solvents, indicating that the solute exhibits less fluorescence in a non-polar environment. The fluorescence quenching of [8MDTC] by aniline was studied at room temperature by examining the steady state in five different solvents in order to explore various possible quenching mechanisms. The experimental results show a positive deviation in Stern-Volmer plots in all solvents. Ground state complex and sphere of action static quenching models were used to interpret the results. Many quenching rate parameters were calculated using these models. The values of these parameters suggest that the sphere of action static quenching model agrees well with the experimental results. Further, a finite sink approximation model was used to check whether these bimolecular reactions were diffusion limited or not. The values of the distance parameter R' and the diffusion coefficient D were determined and are compared with the values of the encounter distance R and diffusion coefficient D calculated using the Stokes-Einstein equation.
Investigation of the CO2 Dependence of Quantum Yield and Respiration in Eucalyptus pauciflora
Kirschbaum, Miko U. F.; Farquhar, Graham D.
1987-01-01
In leaves of C3 plants, the rate of nonphotorespiratory respiration appears to be higher in darkness than in the light. This change from a high to a low rate of carbon loss with increasing photon flux density leads to an increase in the apparent quantum yield of photosynthetic CO2 assimilation at low photon flux densities (Kok effect). The mechanism of this suppression of nonphotorespiratory respiration is not understood, but biochemical evidence and the observation that a Kok effect is often not observed under low O2, has led to the suggestion that photorespiration might be involved in some way. This hypothesis was tested with snowgum (Eucalyptus pauciflora Sieb. ex Spreng.) using gas exchange methods. The test was based on the assumption that if photorespiration were involved, then it would be expected that the intercellular partial pressure of CO2 would also have an influence on the Kok effect. Under normal atmospheric levels of CO2 and O2, a Kok effect was found. Changing the intercellular partial pressure of CO2, however, did not affect the estimate of nonphotorespiratory respiraton, and it was concluded that its decrease with increasing photon flux density did not involve photorespiration. Concurrent measurements showed that the quantum yield of net assimilation of CO2 increased with increasing intercellular partial pressure of CO2, and this increase agreed closely with predictions based on recent models of photosynthesis. PMID:16665319
Accuracy of quantum sensors measuring yield photon flux and photosynthetic photon flux
NASA Technical Reports Server (NTRS)
Barnes, C.; Tibbitts, T.; Sager, J.; Deitzer, G.; Bubenheim, D.; Koerner, G.; Bugbee, B.; Knott, W. M. (Principal Investigator)
1993-01-01
Photosynthesis is fundamentally driven by photon flux rather than energy flux, but not all absorbed photons yield equal amounts of photosynthesis. Thus, two measures of photosynthetically active radiation have emerged: photosynthetic photon flux (PPF), which values all photons from 400 to 700 nm equally, and yield photon flux (YPF), which weights photons in the range from 360 to 760 nm according to plant photosynthetic response. We selected seven common radiation sources and measured YPF and PPF from each source with a spectroradiometer. We then compared these measurements with measurements from three quantum sensors designed to measure YPF, and from six quantum sensors designed to measure PPF. There were few differences among sensors within a group (usually <5%), but YPF values from sensors were consistently lower (3% to 20%) than YPF values calculated from spectroradiometric measurements. Quantum sensor measurements of PPF also were consistently lower than PPF values calculated from spectroradiometric measurements, but the differences were <7% for all sources, except red-light-emitting diodes. The sensors were most accurate for broad-band sources and least accurate for narrow-band sources. According to spectroradiometric measurements, YPF sensors were significantly less accurate (>9% difference) than PPF sensors under metal halide, high-pressure sodium, and low-pressure sodium lamps. Both sensor types were inaccurate (>18% error) under red-light-emitting diodes. Because both YPF and PPF sensors are imperfect integrators, and because spectroradiometers can measure photosynthetically active radiation much more accurately, researchers should consider developing calibration factors from spectroradiometric data for some specific radiation sources to improve the accuracy of integrating sensors.
Accuracy of quantum sensors measuring yield photon flux and photosynthetic photon flux.
Barnes, C; Tibbitts, T; Sager, J; Deitzer, G; Bubenheim, D; Koerner, G; Bugbee, B
1993-12-01
Photosynthesis is fundamentally driven by photon flux rather than energy flux, but not all absorbed photons yield equal amounts of photosynthesis. Thus, two measures of photosynthetically active radiation have emerged: photosynthetic photon flux (PPF), which values all photons from 400 to 700 nm equally, and yield photon flux (YPF), which weights photons in the range from 360 to 760 nm according to plant photosynthetic response. We selected seven common radiation sources and measured YPF and PPF from each source with a spectroradiometer. We then compared these measurements with measurements from three quantum sensors designed to measure YPF, and from six quantum sensors designed to measure PPF. There were few differences among sensors within a group (usually <5%), but YPF values from sensors were consistently lower (3% to 20%) than YPF values calculated from spectroradiometric measurements. Quantum sensor measurements of PPF also were consistently lower than PPF values calculated from spectroradiometric measurements, but the differences were <7% for all sources, except red-light-emitting diodes. The sensors were most accurate for broad-band sources and least accurate for narrow-band sources. According to spectroradiometric measurements, YPF sensors were significantly less accurate (>9% difference) than PPF sensors under metal halide, high-pressure sodium, and low-pressure sodium lamps. Both sensor types were inaccurate (>18% error) under red-light-emitting diodes. Because both YPF and PPF sensors are imperfect integrators, and because spectroradiometers can measure photosynthetically active radiation much more accurately, researchers should consider developing calibration factors from spectroradiometric data for some specific radiation sources to improve the accuracy of integrating sensors.
Schmidt, R.; Seikel, K.; Brauer, H.D. )
1989-06-01
The quantum yield of singlet oxygen ({sup 1}O{sub 2}) {sup 1}{Delta}{sub g} (v = 0) {yields} {sup 1}{Sigma}{sub g}{sup {minus}} (v = O) phosphorescence was determined in acetonitrile, chloroform, carbon disulfide, carbon tetrachloride, and Freon 113 relative to the respective emission in benzene, using the known {sup 1}O{sub 2} phosphorescence quantum yield in benzene as standard. Quantum yields were not found to depend on sensitizer (dicyanoanthracene, rubicene, tetraphenylporphine) but to depend strongly on solvent. The {sup 1}O{sub 2} phosphorescence quantum yields are surprisingly large. The maximum value measured is Qp (Freon 113) = 0.15. The emission quantum yields correlate linearly with {sup 1}O{sub 2} lifetimes for all solvents, including benzene. Consequently the rate constant of {sup 1}O{sub 2} phosphorescence is independent of solvent. It amounts to k{sub p} = 1.3 s{sup {minus}1}. Thus the radiative rate constant is approximately 5000 times larger in liquid solution than for an isolated {sup 1}O{sub 2} molecule.
NASA Astrophysics Data System (ADS)
Meneses-Nava, M. A.; Barbosa-García, O.; Díaz-Torres, L. A.; Chávez-Cerda, S.; Torres-Cisneros, M.; King, T. A.
2001-08-01
The fluorescence quantum yield of quinine sulfate in sol-gel and PMMA impregnated glasses is measured. The observed quantum yield improvement in the sol-gel matrix, compared to ethanol, is interpreted as a reduction of non-radiative relaxation channels by isolation of the molecules by the cage of the glass. PMMA impregnated sol-gel glasses show an extra improvement of the fluorescence yield, which is interpreted as a reduction of the free space and the rigid fixation of the molecules to the matrix.
SU-E-T-191: First Principle Calculation of Quantum Yield in Photodynamic Therapy
Abolfath, R; Guo, F; Chen, Z; Nath, R
2014-06-01
Purpose: We present a first-principle method to calculate the spin transfer efficiency in oxygen induced by any photon fields especially in MeV energy range. The optical pumping is mediated through photosensitizers, e.g., porphyrin and/or ensemble of quantum dots. Methods: Under normal conditions, oxygen molecules are in the relatively non-reactive triplet state. In the presence of certain photosensitizer compounds such as porphyrins, electromagnetic radiation of specific wavelengths can excite oxygen to highly reactive singlet state. With selective uptake of photosensitizers by certain malignant cells, photon irradiation of phosensitized tumors can lead to selective killing of cancer cells. This is the basis of photodynamic therapy (PDT). Despite several attempts, PDT has not been clinically successful except in limited superficial cancers. Many parameters such as photon energy, conjugation with quantum dots etc. can be potentially combined with PDT in order to extend the role of PDT in cancer management. The key quantity for this optimization is the spin transfer efficiency in oxygen by any photon field. The first principle calculation model presented here, is an attempt to fill this need. We employ stochastic density matrix description of the quantum jumps and the rate equation methods in quantum optics based on Markov/Poisson processes and calculate time evolution of the population of the optically pumped singlet oxygen. Results: The results demonstrate the feasibility of our model in showing the dependence of the optical yield in generating spin-singlet oxygen on the experimental conditions. The adjustable variables can be tuned to maximize the population of the singlet oxygen hence the efficacy of the photodynamic therapy. Conclusion: The present model can be employed to fit and analyze the experimental data and possibly to assist researchers in optimizing the experimental conditions in photodynamic therapy.
NASA Astrophysics Data System (ADS)
Gupta, Sharad; Ico, Gerardo; Matsumura, Paul; Rao, A. L. N.; Vullev, Valentine; Anvari, Bahman
2012-03-01
We recently reported construction of a new type of optical nano-construct composed of genome-depleted plant infecting brome mosaic virus (BMV) doped with Indocyanine green (ICG), an FDA-approved chromophore. We refer to these constructs as optical viral ghosts (OVGs) since only the capsid protein (CP) subunits of BMV remain to encapsulate ICG. To utilize OVGs as effective nano-probes in fluorescence imaging applications, their fluorescence quantum yield needs to be maximized. In this study, we investigate the effect of altering the CP to ICG mass ratio on the fluorescent quantum yield of OVGs. Results of this study provide the basis for construction of OVGs with optimal amounts of CP and ICG to yield maximal fluorescence quantum yield.
Overview of southern coastline looking towards Piers O1, O2, and ...
Overview of southern coastline looking towards Piers O-1, O-2, and O-3, Facility 177 to left, Dry Dock No. 4 in center - U.S. Naval Base, Pearl Harbor, Coal Dock, End of South Avenue near Dry Dock No. 4, Pearl City, Honolulu County, HI
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.
Quantum yields for the light adaptations in Anabaena sensory rhodopsin and bacteriorhodopsin
NASA Astrophysics Data System (ADS)
Wada, Yoichiro; Kawanabe, Akira; Furutani, Yuji; Kandori, Hideki; Ohtani, Hiroyuki
2008-02-01
Archael-type rhodopsin has an all- trans or a 13- cis retinal. The light-induced interconversion between these two forms has been found in Anabaena sensory rhodopsin, even though only the photoreaction from the 13- cis form to the all- trans form exists in bacteriorhodopsin. In this study, we obtained the quantum yields for the 13- cis → all- trans and all- trans → 13- cis reactions of Anabaena sensory rhodopsin (0.24 ± 0.03 and 0.38 ± 0.07, respectively) and concluded that these values were independent of the wavelength of the excitation light as well as bacteriorhodopsin. In other words, no excess energy effects can be found in these reactions.
Surface structures for enhancement of quantum yield in broad spectrum emission nanocrystals
Schreuder, Michael A.; McBride, James R.; Rosenthal, Sandra J.
2014-07-22
Disclosed are inorganic nanoparticles comprising a body comprising cadmium and/or zinc crystallized with selenium, sulfur, and/or tellurium; a multiplicity of phosphonic acid ligands comprising at least about 20% of the total surface ligand coverage; wherein the nanocrystal is capable of absorbing energy from a first electromagnetic region and capable of emitting light in a second electromagnetic region, wherein the maximum absorbance wavelength of the first electromagnetic region is different from the maximum emission wavelength of the second electromagnetic region, thereby providing a Stokes shift of at least about 20 nm, wherein the second electromagnetic region comprises an at least about 100 nm wide band of wavelengths, and wherein the nanoparticle exhibits has a quantum yield of at least about 10%. This abstract is intended as a scanning tool for purposes of searching in the particular art and is not intended to be limiting of the present invention.
Photonic effects on the radiative decay rate and luminescence quantum yield of doped nanocrystals.
Senden, Tim; Rabouw, Freddy T; Meijerink, Andries
2015-02-24
Nanocrystals (NCs) doped with luminescent ions form an emerging class of materials. In contrast to excitonic transitions in semiconductor NCs, the optical transitions are localized and not affected by quantum confinement. The radiative decay rates of the dopant emission in NCs are nevertheless different from their bulk analogues due to photonic effects, and also the luminescence quantum yield (QY, important for applications) is affected. In the past, different theoretical models have been proposed to describe the photonic effects for dopant emission in NCs, with little experimental validation. In this work we investigate the photonic effects on the radiative decay rate of luminescent doped NCs using 4 nm LaPO4 NCs doped with Ce(3+) or Tb(3+) ions in different refractive index solvents and bulk crystals. We demonstrate that the measured influence of the refractive index on the radiative decay rate of the Ce(3+) emission, having near unity QY, is in excellent agreement with the theoretical nanocrystal-cavity model. Furthermore, we show how the nanocrystal-cavity model can be used to quantify the nonunity QY of Tb(3+)-doped LaPO4 NCs and demonstrate that, as a general rule, the QY is higher in media with higher refractive index.
Inbar, S.; Linschitz, H.; Cohen, S.G.
1981-03-11
Nanosecond flash photolysis, steady irradiation, and deuterium substitution studies have been carried out on solutions of benzophenone with added reductants. Quantum yields (phi/sub ketyl/) for reduction in benzene of benzophenone triplet to ketyl radical, based on phi = 2 for benzhydrol (I), were approx. 1 for cyclohexane (II), tert-butylamine (III), 2-aminobutane (IV), cyclohexylamine (V), di-n-propylamine (VI), and triethylamine (VII), approx. 0.7 for 1,4-diazabicyclo(2.2.2)octane (VIII), and approx. 0 for tert-butyl alcohol (IX). Thus, quenching, without radical formation by H abstraction from N and/or ..cap alpha..-C, does not occur with common aliphatic amines but does with Dabco (VIII). The latter quenching is markedly increased by small additions of acetonitrile; the flash spectrum from this compound indicates formation of a triplet amine CT complex or radical ion pair. Triplet-reductant interaction rate constants, k/sur ir/, are high for the amines (approx. 10/sup 8/-10/sup 9/ M/sup -1/ s/sup -1/) but also show significant deuterium kinetic isotope effects: 1.9 with III-N-d/sub 2/; 1.4 with IV-N-d/sub 2/; 1.2-1.3 with IV-..cap alpha..-C-d. It is proposed that k/sub ir/ measures H atom abstraction, favored in the transition state by an initial charge-transfer interaction. Overall steady irradiation quantum yields of reduction by amines, phi/sub Red/, are much lower than phi/sub ketyl/. This is attributed to disproportionationreactions of ketyl and alkylaminyl radicals for primary and secondary amines, and, possibly, aminoalkyl radicals for tertiary amines. In the case of tert-butylamine, the rate constant for disproportionation is obtained from the decay kinetics of ketyl radical and leads to phi/sub Red/ in agreement with that directly measured.
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(+).
Solution-based synthesis of high yield CZTS (Cu2ZnSnS4) spherical quantum dots
NASA Astrophysics Data System (ADS)
Rajesh, G.; Muthukumarasamy, N.; Subramanian, E. P.; Venkatraman, M. R.; Agilan, S.; Ragavendran, V.; Thambidurai, M.; Velumani, S.; Yi, Junsin; Velauthapillai, Dhayalan
2015-01-01
High yield CZTS quantum dots have been synthesized using simple precursors by chemical precipitation technique. Formation mechanism of CZTS spherical quantum dots also has been investigated. According to the mechanism, copper sulfide nuclei firstly forms, and serves as the starting point for the nucleation and growth of CZTS. X-ray diffraction pattern, X-ray photoelectron spectra (XPS) and Raman spectra reveals the formation of pure kesterite structure Cu2ZnSnS4 nanoparticles. HRTEM analysis reveals the formation of CZTS quantum dots with an average particle size of ∼8.3 nm. The elemental distribution of CZTS quantum dots studied using STEM elemental mapping reveals that Cu, Zn, Sn and S are present in the sample. The photoluminescence spectra of CZTS exhibit a broad red emission band at 657 nm. The optical band gap is shifted to the higher energy side and it shows the presence of quantum confinement effect.
Absolute Photoluminescence Quantum Yields of IR-26 Dye, PbS, and PbSe Quantum Dots
Semonin, Octavi Escala; Johnson, Justin C; Luther, Joseph M; Midgett, Aaron G; Nozik, Arthur J; Beard, Matthew C
2010-08-19
In this study, we have directly measured the photoluminescence quantum yield (Φ{sub PL}) of IR-26 at a range of concentrations and the Φ{sub PL} of PbS and PbSe QDs for a range of sizes. We find that the Φ{sub PL} of IR-26 has a weak concentration dependence due to reabsorption, with a Φ{sub PL} of 0.048 ± 0.002% for low concentrations, lower than previous reports by a full order of magnitude. We also find that there is a dramatic size dependence for both PbS and PbSe QDs, with the smallest dots exhibiting a Φ{sub PL} in excess of 60%, while larger dots fall below 3%. A model, including nonradiative transition between electronic states and energy transfer to ligand vibrations, appears to explain this size dependence. These findings provide both a better characterization of photoluminescence for near-infrared emitters and some insight into how improved QDs can be developed.
Chapman, Gala; Henary, Maged; Patonay, Gabor
2011-01-01
The effect of varying short-chain alkyl substitution of the indole nitrogens on the spectroscopic properties of cyanine dyes was examined. Molar absorptivities and fluorescence quantum yields were determined for a set of pentamethine dyes and a set of heptamethine dyes for which the substitution of the indole nitrogen was varied. For both sets of dyes, increasing alkyl chain length resulted in no significant change in quantum yield or molar absorptivity. These results may be useful in designing new cyanine dyes for analytical applications and predicting their spectroscopic properties. PMID:21760707
Determination of the Fluorescence Quantum Yield by Oceanic Phytoplankton in Their Natural Habitat
NASA Astrophysics Data System (ADS)
Maritorena, Stéphane; Morel, André; Gentili, Bernard
2000-12-01
Sun-stimulated chlorophyll a fluorescence has been measured in situ , within the upward and downward light fields, in oceanic waters with chlorophyll concentrations of 0.04 3 mg m 3 . We combined these signals with phytoplankton absorption spectra to derive the fluorescence quantum yield, (number of photons emitted by fluorescence number of absorbed photons). was derived separately from hyperspectral (upward and downward) irradiance measurements (with a LI-COR Instruments spectroradiometer) and from nadir radiance near 683 nm (with a Biospherical Instruments profiler). The contribution of inelastic Raman scattering to the signal in the red band was assessed and subtracted. Raman-corrected values derived from the two instruments compared well. Vertical profiles were strongly structured, with maximal (5 6%) values at depth, whereas was 1% in near-surface waters (measurements made approximately at solar noon). These near-surface values are needed for interpretation of remotely sensed fluorescence signals. This optical study shows that the fluorescence yield of algae in their natural environment can be accurately derived in a nonintrusive way with available instrumentation and adequate protocols.
A Reactive 1O2 - Responsive Combined Treatment System of Photodynamic and Chemotherapy for Cancer
NASA Astrophysics Data System (ADS)
Wang, Xiaojun; Meng, Guoqing; Zhang, Song; Liu, Xinli
2016-07-01
The development of reactive oxygen species (ROS)-responsive drug delivery and drug release has gradually attracted much attention in recent years as a promising therapeutic strategy. Singlet oxygen (1O2) as the major ROS species is widely used in photodynamic therapy (PDT) of cancer. In the present study, we introduce a combined treatment using ROS-sensitive thioketal (TK) linkage as a linker between upconversion nanoparticles (UNs)-based PDT and doxorubicin (DOX)-based chemotherapy. UNs can not only play a role in PDT, but can also be used as a nanocarrier for drug delivery of DOX. Moreover, the products of 1O2 during PDT are able to cleave TK linker inducing the release of DOX which can further achieve the goal of chemotherapy. By using this 1O2-responsive nanocarrier delivery system, DOX can easily reach the tumor site and be accumulated in the nuclei to effectively kill the cancer cells, and therefore decreasing the side effects of chemotherapy on the body. Thus, PDT also has the function of controlling drug release in this combination treatment strategy. Compared with monotherapy, the combination of PDT with chemotherapy also possesses excellent drug loading capability and anticancer efficiency.
A Reactive 1O2 - Responsive Combined Treatment System of Photodynamic and Chemotherapy for Cancer
Wang, Xiaojun; Meng, Guoqing; Zhang, Song; Liu, Xinli
2016-01-01
The development of reactive oxygen species (ROS)-responsive drug delivery and drug release has gradually attracted much attention in recent years as a promising therapeutic strategy. Singlet oxygen (1O2) as the major ROS species is widely used in photodynamic therapy (PDT) of cancer. In the present study, we introduce a combined treatment using ROS-sensitive thioketal (TK) linkage as a linker between upconversion nanoparticles (UNs)-based PDT and doxorubicin (DOX)-based chemotherapy. UNs can not only play a role in PDT, but can also be used as a nanocarrier for drug delivery of DOX. Moreover, the products of 1O2 during PDT are able to cleave TK linker inducing the release of DOX which can further achieve the goal of chemotherapy. By using this 1O2-responsive nanocarrier delivery system, DOX can easily reach the tumor site and be accumulated in the nuclei to effectively kill the cancer cells, and therefore decreasing the side effects of chemotherapy on the body. Thus, PDT also has the function of controlling drug release in this combination treatment strategy. Compared with monotherapy, the combination of PDT with chemotherapy also possesses excellent drug loading capability and anticancer efficiency. PMID:27443831
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...
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.
Hausmann, David; Kuzmanoski, Ana; Feldmann, Claus
2016-04-21
The reaction of manganese(ii) bromide and the crown ether 18-crown-6 in the ionic liquid [(n-Bu)3MeN][N(Tf)2] under mild conditions (80-130 °C) resulted in the formation of three different coordination compounds: MnBr2(18-crown-6) (), Mn3Br6(18-crown-6)2 () and Mn3Br6(18-crown-6) (). In general, the local coordination and the crystal structure of all compounds are driven by the mismatch between the small radius of the Mn(2+) cation (83 pm) and the ring opening of 18-crown-6 as a chelating ligand (about 300 pm). This improper situation leads to different types of coordination and bonding. MnBr2(18-crown-6) represents a molecular compound with Mn(2+) coordinated by two bromine atoms and only five oxygen atoms of 18-crown-6. Mn3Br6(18-crown-6)2 falls into a [MnBr(18-crown-6)](+) cation - with Mn(2+) coordinated by six oxygen atoms and Br - and a [MnBr(18-crown-6)MnBr4](-) anion. In this anion, Mn(2+) is coordinated by five oxygen atoms of the crown ether as well as by two bromine atoms, one of them bridging to an isolated (MnBr4) tetrahedron. Mn3Br6(18-crown-6), finally, forms an infinite, non-charged [Mn2(18-crown-6)(MnBr6)] chain. Herein, 18-crown-6 is exocyclically coordinated by two Mn(2+) cations. All compounds show intense luminescence in the yellow to red spectral range and exhibit remarkable quantum yields of 70% (Mn3Br6(18-crown-6)) and 98% (Mn3Br6(18-crown-6)2). The excellent quantum yield of Mn3Br6(18-crown-6)2 and its differentiation from MnBr2(18-crown-6) and Mn3Br6(18-crown-6) can be directly correlated to the local coordination. PMID:26956783
Xu, Suying; Bai, Xilin; Ma, Jingwen; Xu, Minmin; Hu, Gaofei; James, Tony D; Wang, Leyu
2016-08-01
The use of fluorescence probes for biomedical imaging has attracted significant attention over recent years owing to their high resolution at cellular level. The probes are available in many formats including small particle size based imaging agents which are considered to be promising candidates, due to their excellent stabilities. Yet, concerns over the potential cytotoxicity effects of inorganic luminescent particles have led to questions about their suitability for imaging applications. Exploration of alternatives inspired us to use organic fluorophores with aggregation-induced emission (AIE), prepared by functionalizing the amine group on tetraphenylethene with 3,5-bis(trifluoromethyl)phenyl isocyanate. The as-synthesized novel AIE fluorophore (TPE-F) display enhanced quantum yield and longer lifetime as compared with its counterparts (4,4',4″,4‴-(ethene-1,1,2,2-tetrayl)tetraaniline, TPE-AM). Furthermore, the TPE-F was encapsulated into small-size organic nanoparticles (NPs; dynamic light scattering size, ∼10 nm) with polysuccinimide (PSI). The biocompatibility, excellent stability, bright fluorescence, and selective cell targeting of these NPs enable the as-prepared TPE-F NPs to be suitable for specific fluorescence cell imaging. PMID:27349933
Cheminal, Alexandre; Léonard, Jérémie; Kim, So-Young; Jung, Kwang-Hwan; Kandori, Hideki; Haacke, Stefan
2015-10-14
Anabaena Sensory Rhodopsin (ASR) stands out among the microbial retinal proteins in that, under light-adaptation (LA) conditions, it binds both the 13-cis isomer and the all-trans isomer of the protonated Schiff base of retinal (PSBR). In the dark-adapted (DA) state, more than 95% of the proteins bear all-trans PSBR, and the protein environment adopts a different equilibrium state. We report the excited state and photo-isomerization kinetics of ASR under different LA conditions. The full data set allows confirming that the photoisomerization of the 13C isomer occurs within 100 fs and indications of an excited and ground state wavepacket launched by the ultrafast non-adiabatic reaction are reported. Even though this recalls the record isomerization time and the coherent reaction scenario of 11-cis PSBR in rhodopsin, the photoisomerization quantum yield (QY) is much lower, actually the lowest value ever reported for retinal proteins (<15%). Noticeably, in ASR the excited state lifetime (ESL) is at least five times larger and the QY is more than twice as large for AT PSBR as compared to 13C PSBR. We argue that ESL and QY cannot be expected to be correlated at all, but that the latter is decided on, as often anticipated, by the wavepacket pathways leading to the conical intersection seam.
Meiling, Till T; Cywiński, Piotr J; Bald, Ilko
2016-01-01
In this study, a new reliable, economic, and environmentally-friendly one-step synthesis is established to obtain carbon nanodots (CNDs) with well-defined and reproducible photoluminescence (PL) properties via the microwave-assisted hydrothermal treatment of starch and Tris-acetate-EDTA (TAE) buffer as carbon sources. Three kinds of CNDs are prepared using different sets of above mentioned starting materials. The as-synthesized CNDs: C-CND (starch only), N-CND 1 (starch in TAE) and N-CND 2 (TAE only) exhibit highly homogenous PL and are ready to use without need for further purification. The CNDs are stable over a long period of time (>1 year) either in solution or as freeze-dried powder. Depending on starting material, CNDs with PL quantum yield (PLQY) ranging from less than 1% up to 28% are obtained. The influence of the precursor concentration, reaction time and type of additives on the optical properties (UV-Vis absorption, PL emission spectrum and PLQY) is carefully investigated, providing insight into the chemical processes that occur during CND formation. Remarkably, upon freeze-drying the initially brown CND-solution turns into a non-fluorescent white/slightly brown powder which recovers PL in aqueous solution and can potentially be applied as fluorescent marker in bio-imaging, as a reduction agent or as a photocatalyst. PMID:27334409
Ibrahim, H.; Lasa, H. de
1999-09-01
Photocatalytic conversion of a model pollutant (toluene) is studied in a newly designed batch photoreactor, called Photo-CREC-Air. In this unit TiO{sub 2} is supported on a filter mesh with good contact with near UV light, TiO{sub 2}, and air. Photo-CREC-Air is designed with special features including a Venturi section and a heated perforated plate. The heated perforated plate minimizes water adsorption on the mesh and consequently water effects on the reaction rate. The system performance is examined for different toluene concentrations and two humidity levels. After assessing the insignificant toluene adsorption observed under the selected operating conditions, a pseudohomogeneous model is postulated for kinetics modeling. Initial photodegradation rates of toluene at 100 C in Photo-CREC-Air, in the range of model pollutant concentrations and humidity level studied, were 0.005--0.05 {mu}mol/(gcat s). Apparent quantum yields were estimated to be in many cases greater than 100% and as high as 450%.
Oktyabrsky, Serge; Yakimov, Michael; Tokranov, Vadim; Murat, Pavel
2016-03-30
Here, a picosecond-range timing of charged particles and photons is a long-standing challenge for many high-energy physics, biophysics, medical and security applications. We present a design, technological pathway and challenges, and some properties important for realization of an ultrafast high-efficient room-temperature semiconductor scintillator based on self-assembled InAs quantum dots (QD) embedded in a GaAs matrix. Low QD density (<; 1015 cm-3), fast (~5 ps) electron capture, luminescence peak redshifted by 0.2-0.3 eV from GaAs absorption edge with fast decay time (0.5-1 ns) along with the efficient energy transfer in the GaAs matrix (4.2 eV/pair) allows for fabrication of a semiconductormore » scintillator with the unsurpassed performance parameters. The major technological challenge is fabrication of a large volume (> 1 cm3 ) of epitaxial QD medium. This requires multiple film separation and bonding, likely using separate epitaxial films as waveguides for improved light coupling. Compared to traditional inorganic scintillators, the semiconductor-QD based scintillators could have about 5x higher light yield and 20x faster decay time, opening a way to gamma detectors with the energy resolution better than 1% and sustaining counting rates MHz. Picosecond-scale timing requires segmented low-capacitance photodiodes integrated with the scintillator. For photons, the proposed detector inherently provides the depth-of-interaction information.« less
Girdling effects on fruit set and quantum yield efficiency of PSII in two Citrus cultivars.
Rivas, F; Gravina, A; Agustí, M
2007-04-01
Girdling effects on fruitlet abscission, leaf chlorophyll, chlorophyll a fluorescence and carbohydrate concentration in various flowering and vegetative shoots were studied during natural fruit drop in two Citrus cultivars. Irrespective of shoot type, girdling delayed fruitlet abscission, but only fruitlets borne on leafy shoots had increased final fruit set. Chlorophyll a fluorescence analysis revealed differences in quantum yield efficiency of photosystem II of light adapted leaves (Phi(PSII)) among shoot types and in response to girdling. In young leaves of vegetative shoots, girdling decreased Phi(PSII), whereas Phi(PSII) increased from Day 30 after girdling in young leaves of leafy flowering shoots; however, Phi(PSII) did not change in mature leaves during fruit set in either control or girdled trees. Girdling altered leaf carbohydrate concentrations and the photosynthetic performance of the various shoot types. Our results indicate that, in Citrus, several carbohydrate-based regulatory mechanisms of photosynthesis coexist during carbohydrate accumulation brought about by girdling. It is concluded that the delay in fruitlet abscission and the increase in Phi(PSII )observed in girdled leafy flowering shoots are the mechanisms underlying the enhancement of fruit set after girdling.
Meiling, Till T.; Cywiński, Piotr J.; Bald, Ilko
2016-01-01
In this study, a new reliable, economic, and environmentally-friendly one-step synthesis is established to obtain carbon nanodots (CNDs) with well-defined and reproducible photoluminescence (PL) properties via the microwave-assisted hydrothermal treatment of starch and Tris-acetate-EDTA (TAE) buffer as carbon sources. Three kinds of CNDs are prepared using different sets of above mentioned starting materials. The as-synthesized CNDs: C-CND (starch only), N-CND 1 (starch in TAE) and N-CND 2 (TAE only) exhibit highly homogenous PL and are ready to use without need for further purification. The CNDs are stable over a long period of time (>1 year) either in solution or as freeze-dried powder. Depending on starting material, CNDs with PL quantum yield (PLQY) ranging from less than 1% up to 28% are obtained. The influence of the precursor concentration, reaction time and type of additives on the optical properties (UV-Vis absorption, PL emission spectrum and PLQY) is carefully investigated, providing insight into the chemical processes that occur during CND formation. Remarkably, upon freeze-drying the initially brown CND-solution turns into a non-fluorescent white/slightly brown powder which recovers PL in aqueous solution and can potentially be applied as fluorescent marker in bio-imaging, as a reduction agent or as a photocatalyst. PMID:27334409
NASA Astrophysics Data System (ADS)
Meiling, Till T.; Cywiński, Piotr J.; Bald, Ilko
2016-06-01
In this study, a new reliable, economic, and environmentally-friendly one-step synthesis is established to obtain carbon nanodots (CNDs) with well-defined and reproducible photoluminescence (PL) properties via the microwave-assisted hydrothermal treatment of starch and Tris-acetate-EDTA (TAE) buffer as carbon sources. Three kinds of CNDs are prepared using different sets of above mentioned starting materials. The as-synthesized CNDs: C-CND (starch only), N-CND 1 (starch in TAE) and N-CND 2 (TAE only) exhibit highly homogenous PL and are ready to use without need for further purification. The CNDs are stable over a long period of time (>1 year) either in solution or as freeze-dried powder. Depending on starting material, CNDs with PL quantum yield (PLQY) ranging from less than 1% up to 28% are obtained. The influence of the precursor concentration, reaction time and type of additives on the optical properties (UV-Vis absorption, PL emission spectrum and PLQY) is carefully investigated, providing insight into the chemical processes that occur during CND formation. Remarkably, upon freeze-drying the initially brown CND-solution turns into a non-fluorescent white/slightly brown powder which recovers PL in aqueous solution and can potentially be applied as fluorescent marker in bio-imaging, as a reduction agent or as a photocatalyst.
Laisk, A.; Oja, V.; Rasulov, B.; Eichelmann, H.; Sumberg, A.
1997-01-01
Sunflower (Helianthus annuus L.), cotton (Gossypium hirsutum L.), tobacco (Nicotiana tabacum L.), sorghum (Sorghum bicolor Moench.), amaranth (Amaranthus cruentus L.), and cytochrome b6f complex-deficient transgenic tobacco leaves were used to test the response of plants exposed to differnt light intensities and CO2 concentrations before and after photoinhibition at 4000 [mu]mol photons m-2 s-1 and to thermoinhibition up to 45[deg]C. Quantum yields of photochemical and nonphotochemical excitation quenching (YP and YN) and the corresponding relative rate constants for excitation capture from the antenna-primary radical pair equilibrium system (k[prime]P and k[prime]N) were calculated from measured fluorescence parameters. The above treatments resulted in decreases in YP and K[prime]P and in approximately complementary increases in YN and K[prime]N under normal and inhibitory conditions. The results were reproduced by a mathematical model of electron/proton transport and O2 evolution/CO2 assimilation in photosynthesis based on budget equations for the intermediates of photosynthesis. Quantitative differences between model predictions and experiments are explainable, assuming that electron transport is organized into domains that contain relatively complete electron and proton transport chains (e.g. thylakoids). With the complementation that occurs between the photochemical and nonphotochemical excitation quenching, the regulatory system can constantly maintain the shortest lifetime of excitation necessary to avoid the formation of chlorophyll triplet states and singlet oxygen. PMID:12223845
Girdling effects on fruit set and quantum yield efficiency of PSII in two Citrus cultivars.
Rivas, F; Gravina, A; Agustí, M
2007-04-01
Girdling effects on fruitlet abscission, leaf chlorophyll, chlorophyll a fluorescence and carbohydrate concentration in various flowering and vegetative shoots were studied during natural fruit drop in two Citrus cultivars. Irrespective of shoot type, girdling delayed fruitlet abscission, but only fruitlets borne on leafy shoots had increased final fruit set. Chlorophyll a fluorescence analysis revealed differences in quantum yield efficiency of photosystem II of light adapted leaves (Phi(PSII)) among shoot types and in response to girdling. In young leaves of vegetative shoots, girdling decreased Phi(PSII), whereas Phi(PSII) increased from Day 30 after girdling in young leaves of leafy flowering shoots; however, Phi(PSII) did not change in mature leaves during fruit set in either control or girdled trees. Girdling altered leaf carbohydrate concentrations and the photosynthetic performance of the various shoot types. Our results indicate that, in Citrus, several carbohydrate-based regulatory mechanisms of photosynthesis coexist during carbohydrate accumulation brought about by girdling. It is concluded that the delay in fruitlet abscission and the increase in Phi(PSII )observed in girdled leafy flowering shoots are the mechanisms underlying the enhancement of fruit set after girdling. PMID:17241995
Effects of inter-nanocrystal distance on luminescence quantum yield in ensembles of Si nanocrystals
Valenta, J. Greben, M.; Gutsch, S.; Hiller, D.; Zacharias, M.
2014-12-15
The absolute photoluminescence (PL) quantum yield (QY) of multilayers of Silicon nanocrystals (SiNCs) separated by SiO{sub 2} barriers were thoroughly studied as function of the barrier thickness, excitation wavelength, and temperature. By mastering the plasma-enhanced chemical vapor deposition growth, we produce a series of samples with the same size-distribution of SiNCs but variable interlayer barrier distance. These samples enable us to clearly demonstrate that the increase of barrier thickness from ∼1 to larger than 2 nm induces doubling of the PL QY value, which corresponds to the change of number of close neighbors in the hcp structure. The temperature dependence of PL QY suggests that the PL QY changes are due to a thermally activated transport of excitation into non-radiative centers in dark NCs or in the matrix. We estimate that dark NCs represent about 68% of the ensemble of NCs. The PL QY excitation spectra show no significant changes upon changing the barrier thickness and no clear carrier multiplication effects. The dominant effect is the gradual decrease of the PL QY with increasing excitation photon energy.
Action spectra of photosystems II and I and quantum yield of photosynthesis in leaves in State 1.
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.
Johnston, D.B.; Lipsky, S. )
1991-05-02
The fluorescence quantum yield of benzene vapor excited at 253.7 nm and at pressures from 10 to 50 Torr has been determined at 22C by comparison with the fluorescence from a dilute solution of benzene in cyclohexane. The value thus obtained is 0.044 {plus minus} 0.006, which is significantly lower than has been reported in all previous investigations. Although the origin of the discrepancy remains unknown, a theoretical argument is presented that tends to support the lower value.
Purchase, R L; de Groot, H J M
2015-06-01
This contribution discusses why we should consider developing artificial photosynthesis with the tandem approach followed by the Dutch BioSolar Cells consortium, a current operational paradigm for a global artificial photosynthesis project. We weigh the advantages and disadvantages of a tandem converter against other approaches, including biomass. Owing to the low density of solar energy per unit area, artificial photosynthetic systems must operate at high efficiency to minimize the land (or sea) area required. In particular, tandem converters are a much better option than biomass for densely populated countries and use two photons per electron extracted from water as the raw material into chemical conversion to hydrogen, or carbon-based fuel when CO2 is also used. For the average total light sum of 40 mol m(-2) d(-1) for The Netherlands, the upper limits are many tons of hydrogen or carbon-based fuel per hectare per year. A principal challenge is to forge materials for quantitative conversion of photons to chemical products within the physical limitation of an internal potential of ca 2.9 V. When going from electric charge in the tandem to hydrogen and back to electricity, only the energy equivalent to 1.23 V can be stored in the fuel and regained. A critical step is then to learn from nature how to use the remaining difference of ca 1.7 V effectively by triple use of one overpotential for preventing recombination, kinetic stabilization of catalytic intermediates and finally generating targeted heat for the release of oxygen. Probably the only way to achieve this is by using bioinspired responsive matrices that have quantum-classical pathways for a coherent conversion of photons to fuels, similar to what has been achieved by natural selection in evolution. In appendix A for the expert, we derive a propagator that describes how catalytic reactions can proceed coherently by a convergence of time scales of quantum electron dynamics and classical nuclear dynamics. We
Purchase, R L; de Groot, H J M
2015-06-01
This contribution discusses why we should consider developing artificial photosynthesis with the tandem approach followed by the Dutch BioSolar Cells consortium, a current operational paradigm for a global artificial photosynthesis project. We weigh the advantages and disadvantages of a tandem converter against other approaches, including biomass. Owing to the low density of solar energy per unit area, artificial photosynthetic systems must operate at high efficiency to minimize the land (or sea) area required. In particular, tandem converters are a much better option than biomass for densely populated countries and use two photons per electron extracted from water as the raw material into chemical conversion to hydrogen, or carbon-based fuel when CO2 is also used. For the average total light sum of 40 mol m(-2) d(-1) for The Netherlands, the upper limits are many tons of hydrogen or carbon-based fuel per hectare per year. A principal challenge is to forge materials for quantitative conversion of photons to chemical products within the physical limitation of an internal potential of ca 2.9 V. When going from electric charge in the tandem to hydrogen and back to electricity, only the energy equivalent to 1.23 V can be stored in the fuel and regained. A critical step is then to learn from nature how to use the remaining difference of ca 1.7 V effectively by triple use of one overpotential for preventing recombination, kinetic stabilization of catalytic intermediates and finally generating targeted heat for the release of oxygen. Probably the only way to achieve this is by using bioinspired responsive matrices that have quantum-classical pathways for a coherent conversion of photons to fuels, similar to what has been achieved by natural selection in evolution. In appendix A for the expert, we derive a propagator that describes how catalytic reactions can proceed coherently by a convergence of time scales of quantum electron dynamics and classical nuclear dynamics. We
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.
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.
Influence of temperature and photon energy on quantum yield of photoemission from real iron surfaces
NASA Astrophysics Data System (ADS)
Momose, Yoshihiro; Suzuki, Daisuke; Sakurai, Takao; Nakayama, Keiji
2014-07-01
The influence of temperature and incident photon energy on the photoemission quantum yield, Y s, of real iron surfaces has been investigated by thermally assisted photoemission (TAPE). Measurements were carried out using a Geiger counter under a gaseous atmosphere of He containing 1 % isobutane vapor at normal atmospheric pressure in the temperature range 25-353 °C under UV irradiation with wavelengths of 200, 210, 220, and 230 nm. The Y s obtained under irradiation at a given wavelength was found to increase with temperature, particularly more rapidly with wavelengths of greater photon energy. From the Arrhenius plots, the Y s values were found to have activation energies of 0.112-0.040 eV, depending on the photon energy. The chemical composition of the surfaces after TAPE measurements at different temperatures was examined by X-ray photoelectron spectroscopy (XPS). The intensity of species thermally removed from the surface was also measured by temperature desorption spectroscopy (TDS). XPS and TDS results showed the removal of the surface water and weakly bound carbon material from the surface with temperature. It was concluded that the removal of these species with increasing temperature enabled the incident light to penetrate through the surface into the metal, causing the increase in the Y s. The dependence of the activation energies on the photon energy was explained by the change of UV light absorption spectra of the surface water, and the enhancement of the Y s with temperature was also attributed to the influence of iron cations (Fe3+) corresponding to positive holes produced in the surface oxide layer by UV light.
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.
Measurement of quantum yield of up-conversion Luminescence in Er(3+)-doped nano-glass-ceramics.
Rodríguez, V D; Tikhomirov, V K; Méndez-Ramos, J; del-Castillo, J; Görller-Walrand, C
2009-03-01
A measurement of quantum yield of up-conversion luminescence has been done for the Er(3+)-doped transparent oxyfluoride glass-ceramics 32(SiO,)9(AlO1.5)31.5(CdF2)18.5(PbF2)5.5(ZnF2): 3.5(ErF3) mol%, where most of Er3+ dopants partition in 8 nm diameter nano-crystals Er10Pb25F65. The yield was found by newly proposed method using the pump power dependence of the resonant luminescence. The result of the measurement points out that a theoretical maximum of 50% may be reached for the up-conversion luminescence yield in this material. This high yield is shown to be due to low phonon energy and short inter-dopant distances in the nano-crystals.
Wei, Zhangwen; Gu, Zhi-Yuan; Arvapally, Ravi K.; Chen, Ying-Pin; 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.
Wei, ZW; Gu, ZY; Arvapally, RK; Chen, YP; McDougald, RN; Ivy, JF; Yakovenko, AA; Feng, DW; Omary, MA; Zhou, HC
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.
Zhao, Jing; Nair, Gautham; Fisher, Brent R.; Bawendi, Moungi G.
2010-04-16
Semiconductor nanocrystals emit light intermittently; i.e., they “blink,” under steady illumination. The dark periods have been widely assumed to be due to photoluminescence (PL) quenching by an Auger-like process involving a single additional charge present in the nanocrystal. Our results challenge this long-standing assumption. Close examination of exciton PL intensity time traces of single CdSe(CdZnS) core(shell) nanocrystals reveals that the dark state PL quantum yield can be 10 times less than the biexciton PL quantum yield. In addition, we observe spectrally resolved multiexciton emission and find that it also blinks with an on/off ratio greater than 10:1 . These results directly contradict the predictions of the charging model.
Wang, Zhong-Xia; Li, Peng-Fei; Liao, Wei-Qiang; Tang, Yuanyuan; Ye, Heng-Yun; Zhang, Yi
2016-04-01
Two new manganese(II) based organic-inorganic hybrid compounds, C11H21Cl3MnN2 (1) and C11H22Cl4MnN2 (2), with prominent photoluminescence and dielectric properties were synthesized by solvent modulation. Compound 1 with novel trigonal bipyramidal geometry exhibits bright red luminescence with a lifetime of 2.47 ms and high quantum yield of 35.8 %. Compound 2 with tetrahedral geometry displays intense long-lived (1.54 ms) green light emission with higher quantum yield of 92.3 %, accompanied by reversible solid-state phase transition at 170 K and a distinct switchable dielectric property. The better performance of 2 results from the structure, including a discrete organic cation moiety and inorganic metal anion framework, which gives the cations large freedom of motion.
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.
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. PMID:27548639
Zou Xubo; Mathis, W.
2005-08-15
We propose experimental schemes to implement ancilla-free 1{yields}3 optimal phase covariant quantum cloning machines for x-y and x-z equatorial qubits by interfering a polarized photon, which we wish to clone, with different light resources at a six-port symmetric beam splitter. The scheme requires linear optical elements and three-photon coincidence detection, and is feasible with current experimental technology.
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).
Meusinger, Carl; Johnson, Matthew S.; Berhanu, Tesfaye A.; Erbland, Joseph; Savarino, Joel
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 a 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.
Total inhibition of (1)O2-induced oxidative damage to guanine bases of DNA/RNA by turmeric extracts.
Joshi, Prakash C; Li, Hsin H; Merchant, Monique; Keane, Thomas C
2014-09-26
The guanine base of nucleic acids is known to be very reactive towards degradation by (1)O2-induced oxidative stress. Oxidative reactions of DNA are linked to many human diseases including cancer. Among the various forms of reactive O2 species (OH, (1)O2 or O2(-)), the oxidative stress caused by (1)O2 is of particular physiologic importance because of its selectively long life in aqueous medium and its ability to diffuse through a cell membrane. In this study we investigated the degradation of a model compound guanosine (Guo) by (1)O2, which was generated by riboflavin-induced photosensitization and by molybdate ion catalyzed disproportionation of H2O2. We observed the remarkable ability of an aqueous and alcoholic extracts of Turmeric (Curcuma longa) as an extraordinary scavenger of (1)O2 to completely inhibit the degradation of Guo. The alcoholic extracts were more effective in their antioxidant activity than the corresponding water extract. This naturally occurring antioxidant offers a most economical supplement to protect biologically significant molecules from the oxidative stress induced by (1)O2. PMID:25181345
Purchase, R. L.; de Groot, H. J. M.
2015-01-01
This contribution discusses why we should consider developing artificial photosynthesis with the tandem approach followed by the Dutch BioSolar Cells consortium, a current operational paradigm for a global artificial photosynthesis project. We weigh the advantages and disadvantages of a tandem converter against other approaches, including biomass. Owing to the low density of solar energy per unit area, artificial photosynthetic systems must operate at high efficiency to minimize the land (or sea) area required. In particular, tandem converters are a much better option than biomass for densely populated countries and use two photons per electron extracted from water as the raw material into chemical conversion to hydrogen, or carbon-based fuel when CO2 is also used. For the average total light sum of 40 mol m−2 d−1 for The Netherlands, the upper limits are many tons of hydrogen or carbon-based fuel per hectare per year. A principal challenge is to forge materials for quantitative conversion of photons to chemical products within the physical limitation of an internal potential of ca 2.9 V. When going from electric charge in the tandem to hydrogen and back to electricity, only the energy equivalent to 1.23 V can be stored in the fuel and regained. A critical step is then to learn from nature how to use the remaining difference of ca 1.7 V effectively by triple use of one overpotential for preventing recombination, kinetic stabilization of catalytic intermediates and finally generating targeted heat for the release of oxygen. Probably the only way to achieve this is by using bioinspired responsive matrices that have quantum–classical pathways for a coherent conversion of photons to fuels, similar to what has been achieved by natural selection in evolution. In appendix A for the expert, we derive a propagator that describes how catalytic reactions can proceed coherently by a convergence of time scales of quantum electron dynamics and classical nuclear dynamics
Nardello, Véronique; Barbillat, Jacques; Marko, Jean; Witte, Peter T; Alsters, Paul L; Aubry, Jean-Marie
2003-01-20
The decomposition of hydrogen peroxide into singlet molecular oxygen-(1)O(2) ((1)Delta(g))-in the presence of lanthanum(iii) salts was studied by monitoring its characteristic IR luminescence at 1270 nm. The process was found to be heterogeneously catalyzed by La(III), provided that the heterogeneous catalyst is generated in situ. The yield of (1)O(2) generation was assessed as 45+/-5 % both in water and in methanol. The pH-dependence on the rate of (1)O(2) generation corresponds to a bell-shaped curve from pH 4.5 to 13 with a maximum around pH 8. The study of the influence of H(2)O(2) showed that the formation of (1)O(2) begins as soon as one equivalent of H(2)O(2) is introduced. It then increases drastically up to two equivalents and more smoothly above. Unlike all other metal salt catalyst systems known to date for H(2)O(2) disproportionation, this chemical source of (1)O(2) is able to generate (1)O(2) not only in basic media, but also under neutral and slightly acidic conditions. In addition, this La-based catalyst system has a very low tendency to induce unwanted oxygenating side reactions, such as epoxidation of alkenes. These two characteristics of the heterogeneous lanthanum catalyst system allow non-photochemical (i.e., "dark") singlet oxygenation of substrate classes that cannot be peroxidized successfully with conventional molybdate catalysts, such as allylic alcohols and alkenyl amines.
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.
Avilov, Sergiy; Berardozzi, Romain; Gunewardene, Mudalige S.; Adam, Virgile; Hess, Samuel T.; Bourgeois, Dominique
2014-01-01
Single-molecule localization microscopy of biological samples requires a precise knowledge of the employed fluorescent labels. Photoactivation, photoblinking and photobleaching of phototransformable fluorescent proteins influence the data acquisition and data processing strategies to be used in (Fluorescence) Photoactivation Localization Microscopy ((F)-PALM), notably for reliable molecular counting. As these parameters might depend on the local environment, they should be measured in cellulo in biologically relevant experimental conditions. Here, we measured phototransformation quantum yields for Dendra2 fused to actin in fixed mammalian cells in typical (F)-PALM experiments. To this aim, we developed a data processing strategy based on the clustering optimization procedure proposed by Lee et al (PNAS 109, 17436–17441, 2012). Using simulations, we estimated the range of experimental parameters (molecular density, molecular orientation, background level, laser power, frametime) adequate for an accurate determination of the phototransformation yields. Under illumination at 561 nm in PBS buffer at pH 7.4, the photobleaching yield of Dendra2 fused to actin was measured to be (2.5±0.4)×10−5, whereas the blinking-off yield and thermally-activated blinking-on rate were measured to be (2.3±0.2)×10−5 and 11.7±0.5 s−1, respectively. These phototransformation yields differed from those measured in poly-vinyl alcohol (PVA) and were strongly affected by addition of the antifading agent 1,4-diazabicyclo[2.2.2]octane (DABCO). In the presence of DABCO, the photobleaching yield was reduced 2-fold, the blinking-off yield was decreased more than 3-fold, and the blinking-on rate was increased 2-fold. Therefore, DABCO largely improved Dendra2 photostability in fixed mammalian cells. These findings are consistent with redox-based bleaching and blinking mechanisms under (F)-PALM experimental conditions. Finally, the green-to-red photoconversion quantum yield of Dendra2 was
CO quantum yield in the photolysis of CO2 at wavelength 1470 and wavelengths 1500-1670.
NASA Technical Reports Server (NTRS)
Inn, E. C. Y.
1972-01-01
The results of carbon monoxide quantum yield measurements of carbon dioxide photolysis by radiation at 1470 A and in the region from 1500 to 1670 A are presented in tabular form. The experimental technique and equipment developed by Inn and Heimerl (1971) were used. These measurements, together with some previously reported ones for a longer wavelength region, are intended to provide a uniform set of values based on the same experimental technique for the entire spectral region that is relevant to the carbon-dioxide photochemistry in the atmospheres of Mars and Venus.
Hirohara, Shiho; Obata, Makoto; Alitomo, Hiroki; Sharyo, Kohei; Ando, Tsuyoshi; Yano, Shigenobu; Tanihara, Masao
2009-05-20
5,10,15,20-Tetrakis(4-(2,3,4,6-tetra-O-acetyl-beta-d-glucopyranosylthio)-2,3,5,6-tetrafluorophenyl)porphyrin 2a and its Zn(II), Pd(II), and Pt(II) complexes 2b, 2c, and 2d were prepared in excellent yields by nucleophilic substitution of the corresponding free-base porphyrin and metalloporphyrins with acetyl 2,3,4,6-tetra-O-acetyl-1-thio-beta-d-glucopyranoside. Deprotection of 2a, 2b, 2c, and 2d by alkaline hydrolysis afforded the corresponding S-glucosylated porphyrin 3a and its metal complexes 3b, 3c, and 3d. The structures and purity of all new photosensitizers were confirmed by elemental analysis and (1)H, (13)C, and (19)F NMR, UV-vis, and steady-state luminescence spectroscopy. The relative efficiency of singlet oxygen ((1)O(2)) production increased in the order of free-base fluoroporphyrins (2a and 3a) < Zn(II) complexes (2b and 3b) < Pd(II) complexes (2c and 3c), which can be explained in terms of the heavy-atom effect, while the (1)O(2)-producing efficiency of Pt(II) complexes (2d and 3d) were exceptionally low. In vitro photocytotoxicity of these eight S-glucosylated photosensitizers was examined in HeLa cells. Although all protected photosensitizers 2a, 2b, 2c, and 2d showed no photocytotoxicity, the photosensitizers 3a, 3b, and 3c exerted potent photocytotoxicity. These results clearly indicated that the sugar moieties of 3a, 3b, and 3c act as not only water-solubility-enhancing functionalities but also cellular-uptake-enhancing elements. Photocytotoxicity testing of 3a, 3b, and 3c in the presence of reactive oxygen species inhibitors suggested that (1)O(2) is the major mediator of cell death. Hence, the Zn(II) and Pd(II) complexes 3b and 3c are promising photosensitizers having cellular uptake-facilitating units (sugar moieties) and enhanced (1)O(2) generation due to the heavy-atom effect.
Bartusik, Dorota; Aebisher, David; Lyons, Alan M; Greer, Alexander
2012-11-01
A microphotoreactor device was developed to generate bubbles (1.4 mm diameter, 90 μL) containing singlet oxygen at levels toxic to bacteria and fungus. As singlet oxygen decays rapidly to triplet oxygen, the bubbles leave behind no waste or byproducts other than O(2). From a comparative study in deaerated, air saturated, and oxygenated solutions, it was reasoned that the singlet oxygen bubbles inactivate Escherichia coli and Aspergillus fumigatus, mainly by an oxygen gradient inside and outside of the bubble such that singlet oxygen is solvated and diffuses through the aqueous solution until it reacts with the target organism. Thus, singlet oxygen bubble toxicity was inversely proportional to the amount of dissolved oxygen in solution. In a second mechanism, singlet oxygen interacts directly with E. coli that accumulate at the gas-liquid interface although this mechanism operates at a rate approximately 10 times slower. Due to encapsulation in the gaseous core of the bubble and a 0.98 ms lifetime, the bubbles can traverse relatively long 0.39 mm distances carrying (1)O(2) far into the solution; by comparison the diffusion distance of (1)O(2) fully solvated in H(2)O is much shorter (~150 nm). Bubbles that reached the outer air-water interface contained no (1)O(2). The mechanism by which (1)O(2) deactivated organisms was explored through the addition of detergent molecules and Ca(2+) ions. Results indicate that the preferential accumulation of E. coli at the air-water interface of the bubble leads to enhanced toxicity of bubbles containing (1)O(2). The singlet oxygen device offers intriguing possibilities for creating new types of disinfection strategies based on photodynamic ((1)O(2)) bubble carriers.
Yang, Yang; Linke, Martin; von Haimberger, Theodore; Matute, Ricardo; González, Leticia; Schmieder, Peter; Heyne, Karsten
2014-01-01
Photoisomerization of a protein bound chromophore is the basis of light sensing of many photoreceptors. We tracked Z-to-E photoisomerization of Cph1 phytochrome chromophore PCB in the Pr form in real-time. Two different phycocyanobilin (PCB) ground state geometries with different ring D orientations have been identified. The pre-twisted and hydrogen bonded PCB(a) geometry exhibits a time constant of 30 ps and a quantum yield of photoproduct formation of 29%, about six times slower and ten times higher than that for the non-hydrogen bonded PCB(b) geometry. This new mechanism of pre-twisting the chromophore by protein-cofactor interaction optimizes yields of slow photoreactions and provides a scaffold for photoreceptor engineering. PMID:26798771
Rani, Janardhanan R; Oh, Se-I; Woo, Jeong Min; Tarwal, Nilesh L; Kim, Hyun-Woong; Mun, Bongjin Simon; Lee, Sungbae; Kim, Ki-Jeong; Jang, Jae-Hyung
2015-03-18
Highly luminescent graphene oxide (GO)-phosphor hybrid thin films with a maximum quantum yield of 9.6% were synthesized via a simple chemical method. An intense luminescence emission peak at 537 nm and a broad emission peak at 400 nm were observed from the GO-phosphor hybrid films. The maximum quantum yield of the emissions from the hybrid films was found to be 9.6%, which is 48 times higher than that of pristine GO films. The GO-phosphor hybrids were prepared via spin-coating and subsequent postannealing of the films, resulting in scrolling of the GO sheets. The resulting GO nanoscrolls exhibited a length of ∼2 μm with nanoscale interior cavities. Transmission electron microscopy and selected-area electron diffraction analyses revealed that the lattice structure of the tubular scrolls is similar to that of carbon nanotubes. While pristine GO films are p-type, in the GO-phosphor hybrids, the Fermi level shifted upward and fell between the HOMO-LUMO gap due to phosphor attachment via C-N bonding. The highly luminescent GO-phosphor hybrids will find important applications in graphene-based optoelectronic devices.
Enhanced fluorescence yields through cavity quantum-electrodynamic effects in microdroplets
Barnes, M.D.; Whitten, W.B.; Ramsey, J.M. )
1994-07-01
Measurements of the integrated fluorescence yield per molecule of Rhodamine 6G (R6G) in 4--16-[mu]m-diameter levitated microdroplets show a size dependence that is attributed to a net increase in the fluorescence decay rate for the smaller (4--5-[mu]m) droplets. The average fluorescence yield in 4-[mu]m droplets (for which we have previously observed emission-rate enhancement) is approximately a factor of 2 larger than the yield measured for larger droplets for which emission-rate enhancement does not occur. These results suggest that there is little emission-rate inhibition in this system, even though the fluorescence emission spectrum overlaps several cavity resonances. A mechanism based on spectral diffusion is postulated for the apparent absence of cavity-inhibited emission and is illustrated by Monte Carlo calculations using time-dependent line-shape functions.
Low-Pressure Photolysis of 2,3-Pentanedione in Air: Quantum Yields and Reaction Mechanism.
Bouzidi, Hichem; Djehiche, Mokhtar; Gierczak, Tomasz; Morajkar, Pranay; Fittschen, Christa; Coddeville, Patrice; Tomas, Alexandre
2015-12-24
Dicarbonyls in the atmosphere mainly arise from secondary sources as reaction products in the degradation of a large number of volatile organic compounds (VOC). Because of their sensitivity to solar radiation, photodissociation of dicarbonyls can dominate the fate of these VOC and impact the atmospheric radical budget. The photolysis of 2,3-pentanedione (PTD) has been investigated for the first time as a function of pressure in a static reactor equipped with continuous wave cavity ring-down spectroscopy to measure the HO2 radical photostationary concentrations along with stable species. We showed that (i) Stern-Volmer plots are consistent with low OH-radical formation yields in RCO + O2 reactions, (ii) the decrease of the photodissociation rate due to pressure increase from 26 to 1000 mbar is of about 30%, (iii) similarly to other dicarbonyls, the Stern-Volmer analysis shows a curvature at the lower pressure investigated, which may be assigned to the existence of excited singlet and triplet PTD states, (iv) PTD photolysis at 66 mbar leads to CO2, CH2O and CO with yields of (1.16 ± 0.04), (0.33 ± 0.02) and (0.070 ± 0.005), respectively, with CH2O yield independent of pressure up to 132 mbar and CO yield in agreement with that obtained at atmospheric pressure by Bouzidi et al. (2014), and (v) the PTD photolysis mechanism remains unchanged between atmospheric pressure and 66 mbar. As a part of this work, the O2 broadening coefficient for the absorption line of HO2 radicals at 6638.21 cm(-1) has been determined (γO2 = 0.0289 cm(-1) atm(-1)). PMID:26608471
Alrawashdeh, Lubna R; Cronin, Michael P; Woodward, Clifford E; Day, Anthony I; Wallace, Lynne
2016-07-01
The weaker emission typically seen for iridium(III) cyclometalated complexes in aqueous medium can be reversed via encapsulation in cucurbit[10]uril (Q[10]). The Q[10] cavity is shown to effectively maximize quantum yields for the complexes, compared to any other medium. This may provide significant advantages for a number of sensor applications. NMR studies show that the complexes are accommodated similarly within the host molecule, even with cationic substituents attached to the ppy ligands, indicating that the hydrophobic effect is the dominant driving force for binding. Cavity-encapsulated 1:1 host-guest species dominate the emission, but 1:2 species are also indicated, which also give some enhancement of intensity. Results demonstrate that the enhancement is due primarily to much lower rates of nonradiative decay but also suggest that the encapsulation can cause a change in character of the emitting state.
BRODY, M; EMERSON, R
1959-11-01
Quantum yield measurements were made with the red alga Porphyridium cruentum, cultured so as to give different proportions of chlorophyll and phycobilins. Totally absorbing suspensions were used so that there was no uncertainty in the amount of energy absorbed. These measurements have shown that chlorophyll, in this alga, has a photosynthetic efficiency as high as in other algal groups, and higher than the phycobilins-at least at wave lengths shorter than about 650 mmicro. Wave lengths longer than this are beyond the range of maximum efficiency of chlorophyll. Under specified conditions of temperature and supplementary light full efficiency may be extended to longer wave lengths. The results of these measurements have made it unnecessary to suppose that in red algae chlorophyll plays a minor role while the phycobilins are the photosynthetic sensitizers of primary importance.
Lindle, D.W.; Ferrett, T.A.; Heimann, P.A.; Shirley, D.A.
1986-08-01
The quantum yield of the visible scintillator sodium salicylate is found to increase in the incident photon-energy range 80--270 eV. Because of its use as a photon-flux monitor in recent gas-phase photoelectron spectroscopy measurements, previously reported partial cross sections for Hg (4f-italic, 5p-italic, and 5d-italic subshells) and CH/sub 3/I (I 4d-italic subshell) in this energy range are corrected, and new values are reported. For Hg, the correction brings the experimental data into better overall agreement with theory. However, considerable uncertainty remains in the absolute scale derived from previous Hg photoabsorption measurements, and no single rescaling of the subshell cross sections could simultaneously bring all three into agreement with available theoretical calculations.
Freund, Christelle; Porzio, William; Giovanella, Umberto; Vignali, Francesco; Pasini, Mariacecilia; Destri, Silvia; Mech, Agnieszka; Di Pietro, Sebastiano; Di Bari, Lorenzo; Mineo, Placido
2011-06-20
The synthesis and the molecular and photophysical characterization, together with solid state and solution structure analysis, of a series of europium complexes based on β-diketonate ligands are reported. The Eu(III) complex emission, specifically its photoluminescence quantum yield (PL-QY), can be tuned by changing ligands which finely modifies the environment of the metal ion. Steady-state and time-resolved emission spectroscopy and overall PL-QY measurements are reported and related to geometrical features observed in crystal structures of some selected compounds. Moreover, paramagnetic NMR, based on the analogous complexes with other lanthanides, are use to demonstrate that there is a significant structural reorganization upon dissolution, which justifies the observed differences in the emission properties between solid and solution states. The energy of the triplet levels of the ligands and the occurrence of nonradiative deactivation processes clearly account for the luminescence efficiencies of the complexes in the series.
NASA Technical Reports Server (NTRS)
Ryason, P. R.
1977-01-01
Water decomposition by a cyclic photoredox process is discussed in general terms. Thermodynamics determines the wavelength of the charge-transfer band corresponding to electron transfer to or from water of hydration of a cation. These relationships indicate that it is unlikely that a photoreduction reaction resulting in water decomposition will occur in the sea-level solar range of wavelengths. Such is not the case for photooxidation, and an example is known: the photolysis of Eu(2+) in aqueous solution. Hydrogen quantum yields have been determined for this reaction. They are sufficiently high (about 0.3) as to offer encourangement for the further exploration of photoredox reactions as a means of solar energy conversion.
Alrawashdeh, Lubna R; Cronin, Michael P; Woodward, Clifford E; Day, Anthony I; Wallace, Lynne
2016-07-01
The weaker emission typically seen for iridium(III) cyclometalated complexes in aqueous medium can be reversed via encapsulation in cucurbit[10]uril (Q[10]). The Q[10] cavity is shown to effectively maximize quantum yields for the complexes, compared to any other medium. This may provide significant advantages for a number of sensor applications. NMR studies show that the complexes are accommodated similarly within the host molecule, even with cationic substituents attached to the ppy ligands, indicating that the hydrophobic effect is the dominant driving force for binding. Cavity-encapsulated 1:1 host-guest species dominate the emission, but 1:2 species are also indicated, which also give some enhancement of intensity. Results demonstrate that the enhancement is due primarily to much lower rates of nonradiative decay but also suggest that the encapsulation can cause a change in character of the emitting state. PMID:27315543
NASA Astrophysics Data System (ADS)
Yu, Yong Qiang; Zhang, Quan Sheng; Tang, Yong Zheng; Li, Xue Meng; Liu, Hong Liang; Li, Li Xia
2013-07-01
In this study, a three-way factorial experimental design was used to investigate the diurnal changes of photosynthetic activity of the intertidal macroalga Sargassum thunbergii in response to temperature, tidal pattern and desiccation during a simulated diurnal light cycle. The maximum (Fv/Fm) and effective (ΦPSII) quantum yields of photosystem II (PSII) were estimated by chlorophyll fluorescence using a pulse amplitude modulated fluorometer. Results showed that this species exhibited sun-adapted characteristics, as evidenced by the daily variation of Fv/Fm and ΦPSII. Both yield values decreased with increasing irradiance towards noon and recovered rapidly in the afternoon suggesting a dynamic photoinhibition. The photosynthetic quantum yield of S. thunbergii thalli varied significantly with temperature, tidal pattern and desiccation. Thalli were more susceptible to light-induced damage at high temperature of 25 °C and showed complete recovery of photosynthetic activity only when exposed to 8 °C. In contrast with the mid-morning low tide period, although there was an initial increase in photosynthetic yield during emersion, thalli showed a greater degree of decline at the end of emersion and remained less able to recover when low tide occurred at mid-afternoon. Short-term air exposure of 2 h did not significantly influence the photosynthesis. However, when exposed to moderate conditions (4 h desiccation at 15 °C or 6 h desiccation at 8 °C), a significant inhibition of photosynthesis was followed by partial or complete recovery upon re-immersion in late afternoon. Only extreme conditions (4 h desiccation at 25 °C or 6 h desiccation at 15 °C or 25 °C) resulted in the complete inhibition, with little indication of recovery until the following morning, implying the occurrence of chronic PSII damage. Based on the magnitude of effect, desiccation was the predominant negative factor affecting the photosynthesis under the simulated daytime irradiance period. These
Zhao, Jiang; Yu, Yue; Yang, Xiaolong; Yan, Xiaogang; Zhang, Huiming; Xu, Xianbin; Zhou, Guijiang; Wu, Zhaoxin; Ren, Yixia; Wong, Wai-Yeung
2015-11-11
A series of heteroleptic functional Ir(III) complexes bearing different fluorinated aromatic sulfonyl groups has been synthesized. Their photophysical features, electrochemical behaviors, and electroluminescent (EL) properties have been characterized in detail. These complexes emit intense yellow phosphorescence with exceptionally high quantum yields (ΦP > 0.9) at room temperature, and the emission maxima of these complexes can be finely tuned depending upon the number of the fluorine substituents on the pendant phenyl ring of the sulfonyl group. Furthermore, the electrochemical properties and electron injection/transporting (EI/ET) abilities of these Ir(III) phosphors can also be effectively tuned by the fluorinated aromatic sulfonyl group to furnish some desired characters for enhancing the EL performance. Hence, the maximum luminance efficiency (ηL) of 81.2 cd A(-1), corresponding to power efficiency (ηP) of 64.5 lm W(-1) and external quantum efficiency (ηext) of 19.3%, has been achieved, indicating the great potential of these novel phosphors in the field of organic light-emitting diodes (OLEDs). Furthermore, a clear picture has been drawn for the relationship between their optoelectronic properties and chemical structures. These results should provide important information for developing highly efficient phosphors. PMID:26458215
Zhao, Jiang; Yu, Yue; Yang, Xiaolong; Yan, Xiaogang; Zhang, Huiming; Xu, Xianbin; Zhou, Guijiang; Wu, Zhaoxin; Ren, Yixia; Wong, Wai-Yeung
2015-11-11
A series of heteroleptic functional Ir(III) complexes bearing different fluorinated aromatic sulfonyl groups has been synthesized. Their photophysical features, electrochemical behaviors, and electroluminescent (EL) properties have been characterized in detail. These complexes emit intense yellow phosphorescence with exceptionally high quantum yields (ΦP > 0.9) at room temperature, and the emission maxima of these complexes can be finely tuned depending upon the number of the fluorine substituents on the pendant phenyl ring of the sulfonyl group. Furthermore, the electrochemical properties and electron injection/transporting (EI/ET) abilities of these Ir(III) phosphors can also be effectively tuned by the fluorinated aromatic sulfonyl group to furnish some desired characters for enhancing the EL performance. Hence, the maximum luminance efficiency (ηL) of 81.2 cd A(-1), corresponding to power efficiency (ηP) of 64.5 lm W(-1) and external quantum efficiency (ηext) of 19.3%, has been achieved, indicating the great potential of these novel phosphors in the field of organic light-emitting diodes (OLEDs). Furthermore, a clear picture has been drawn for the relationship between their optoelectronic properties and chemical structures. These results should provide important information for developing highly efficient phosphors.
2015-01-01
Several nonradiative processes compete with tryptophan fluorescence emission. The difficulty in spectral interpretation lies in associating specific molecular environmental features with these processes and thereby utilizing the fluorescence spectral data to identify the local environment of tryptophan. Here, spectroscopic and molecular modeling study of Lys-Trp dipeptide charged species shows that backbone-ring interactions are undistinguished. Instead, quantum mechanical ground state isosurfaces reveal variations in indole π electron distribution and density that parallel charge (as a function of pK1, pK2, and pKR) on the backbone and residues. A pattern of aromaticity-associated quantum yield and fluorescence lifetime changes emerges. Where quantum yield is high, isosurfaces have a charge distribution similar to the highest occupied molecular orbital (HOMO) of indole, which is the dominant fluorescent ground state of the 1La transition dipole moment. Where quantum yield is low, isosurface charge distribution over the ring is uneven, diminished, and even found off ring. At pH 13, the indole amine is deprotonated, and Lys-Trp quantum yield is extremely low due to tautomer structure that concentrates charge on the indole amine; the isosurface charge distribution bears scant resemblance to the indole HOMO. Such greatly diminished fluorescence has been observed for proteins where the indole nitrogen is hydrogen bonded, lending credence to the association of aromaticity changes with diminished quantum yield in proteins as well. Thus tryptophan ground state isosurfaces are an indicator of indole aromaticity, signaling the partition of excitation energy between radiative and nonradiative processes. PMID:24882092
NASA Astrophysics Data System (ADS)
Reader, H. E.; Miller, W. L.
2010-12-01
Photochemical oxidation of chromophoric dissolved organic matter (CDOM) is the major source of carbon monoxide to the surface ocean. Bacterial consumption and air-sea exchange comprise the two known sinks for CO in marine systems. Though the two loss terms are relatively efficient, CO remains supersaturated with respect to the atmosphere in the surface ocean. Global oceanic estimates of CO photoproduction range from 30-84Tg CO/year (Zafiriou 2003, Fichot and Miller 2010). The variation in estimates is largely due to the difficulty in predicting the efficiency of photoproduction (i.e. Apparent Quantum Yield; AQY). Though the AQY for CO photoproduction appears to be relatively constant, there is indication that terrestrially derived sources, such as those found in estuarine environments, produce CO more efficiently than marine derived sources (Ziolkowski 2000). Since variation among sources is likely in the global ocean, accurate assignment of AQY to variable water types is required to accurately predict CO photoproduction. Deriving the correct apparent quantum yield from remotely sensed data would lead to better predictions of large scale CO photoproduction from optical data. Thirty-eight (38) AQY spectra for CO photoproduction were determined by monthly sampling during spring tides in three dark water locations on the coast of Georgia, USA, from November 2008 to September 2009. Sapelo Sound, a marine dominated system, receives little to no freshwater input over the year, while Altamaha Sound drains the largest watershed in the state of Georgia, and has largely variably freshwater input. Doboy Sound, situated between Sapelo Sound and Altamaha Sound, is largely marine dominated, though in periods of high flow on the Altamaha River, receives some fresh water overflow. The coast of Georgia is dominated by Spartina alterniflora salt marshes, and thus also has a strong non-point source of terrestrially derived carbon. CO apparent quantum yields were determined by
NASA Astrophysics Data System (ADS)
Hitomi, Y.; Arakaki, T.
2009-12-01
Redox cycles of iron in the aquatic environment affect formation of reactive oxygen species such as hydrogen peroxide and hydroxyl radicals, which in turn determines lifetimes of many organic compounds. Although aqueous Fe(III)-dicarboxylate complexes are considered to be important sources of photo-formed Fe(II), molar absorptivity and quantum yield of Fe(II) formation for individual species are not well understood. We initiated a study to characterize Fe(II) photo-formation from Fe(III)-dicarboxylates with the concentration ranges that are relevant to the natural aquatic environment. The Visual MINTEQ computer program was used to calculate the equilibrium concentrations of individual Fe(III)-dicarboxylate species. The molar absorptivity of Fe(III)-dicarboxylate species was obtained by UV-VIS spectrophotometer, and the product of the quantum yield and the molar absorptivity of Fe(III)-dicarboxylate species were obtained from photochemical experiments. These experimental data were combined with the calculated equilibrium Fe(III)-dicarboxylate concentrations to determine individual molar absorptivity and quantum yield of Fe(II) photo-formation for a specific Fe(III)-dicarboxylate species. We used initial concentrations of less than 10 micromolar Fe(III) to study the photochemical formation of Fe(II). Dicarboxylate compounds studied include oxalate, malonate, succinate, malate, and phthalate. We report molar absorptivity and concentration-dependent quantum yields of Fe(II) photo-formation of individual Fe(III)-dicarboxylates.
NASA Astrophysics Data System (ADS)
Hou, Juan; Wang, Wei; Zhou, Tianyu; Wang, Bo; Li, Huiyu; Ding, Lan
2016-05-01
Heteroatom doped carbon dots (CDs) have received increasing attention due to their unique properties and related applications. However, previously reported CDs generally show strong emission only in the blue-light region, thus restricting their further applications. And the fundamental investigation on the preparation process is always neglected. Herein, we have developed a simple and solvent-free synthetic strategy to fabricate nitrogen-doped CDs (N-CDs) from citric acid and dicyandiamide. The as-prepared N-CDs exhibited a uniform size distribution, strong yellowish-green fluorescence emission and a high quantum yield of 73.2%. The products obtained at different formation stages were detailedly characterized by transmission electron microscopy, X-ray diffraction spectrometer, X-ray photoelectron spectroscopy and UV absorbance spectroscopy. A possible formation mechanism has thus been proposed including dehydration, polymerization and carbonization. Furthermore, the N-CDs could serve as a facile and label-free probe for the detection of iron and fluorine ions with detection limits of 50 nmol L-1 and 75 nmol L-1, respectively.Heteroatom doped carbon dots (CDs) have received increasing attention due to their unique properties and related applications. However, previously reported CDs generally show strong emission only in the blue-light region, thus restricting their further applications. And the fundamental investigation on the preparation process is always neglected. Herein, we have developed a simple and solvent-free synthetic strategy to fabricate nitrogen-doped CDs (N-CDs) from citric acid and dicyandiamide. The as-prepared N-CDs exhibited a uniform size distribution, strong yellowish-green fluorescence emission and a high quantum yield of 73.2%. The products obtained at different formation stages were detailedly characterized by transmission electron microscopy, X-ray diffraction spectrometer, X-ray photoelectron spectroscopy and UV absorbance spectroscopy. A
MacDougall, Sean K. W.; Ivaturi, Aruna; Marques-Hueso, Jose; Richards, Bryce S.
2014-06-15
The internal photoluminescent quantum yield (iPLQY) – defined as the ratio of emitted photons to those absorbed – is an important parameter in the evaluation and application of luminescent materials. The iPLQY is rarely reported due to the complexities in the calibration of such a measurement. Herein, an experimental method is proposed to correct for re-emission, which leads to an underestimation of the absorption under broadband excitation. Although traditionally the iPLQY is measured using monochromatic sources for linear materials, this advancement is necessary for nonlinear materials with wavelength dependent iPLQY, such as the application of up-conversion to solar energy harvesting. The method requires an additional measurement of the emission line shape that overlaps with the excitation and absorption spectra. Through scaling of the emission spectrum, at the long wavelength edge where an overlap of excitation does not occur, it is possible to better estimate the value of iPLQY. The method has been evaluated for a range of nonlinear material concentrations and under various irradiances to analyze the necessity and boundary conditions that favor the proposed method. Use of this refined method is important for a reliable measurement of iPLQY under a broad illumination source such as the Sun.
NASA Astrophysics Data System (ADS)
Tomes, John J.; Finlayson, Chris E.
2016-09-01
We report upon the exploitation of the latest 3D printing technologies to provide low-cost instrumentation solutions, for use in an undergraduate level final-year project. The project addresses prescient research issues in optoelectronics, which would otherwise be inaccessible to such undergraduate student projects. The experimental use of an integrating sphere in conjunction with a desktop spectrometer presents opportunities to use easily handled, low cost materials as a means to illustrate many areas of physics such as spectroscopy, lasers, optics, simple circuits, black body radiation and data gathering. Presented here is a 3rd year undergraduate physics project which developed a low cost (£25) method to manufacture an experimentally accurate integrating sphere by 3D printing. Details are given of both a homemade internal reflectance coating formulated from readily available materials, and a robust instrument calibration method using a tungsten bulb. The instrument is demonstrated to give accurate and reproducible experimental measurements of luminescence quantum yield of various semiconducting fluorophores, in excellent agreement with literature values.
Niinemets, Ülo; Sun, Zhihong; Talts, Eero
2015-12-01
Leaf age alters the balance between the use of end-product of plastidic isoprenoid synthesis pathway, dimethylallyl diphosphate (DMADP), in prenyltransferase reactions leading to synthesis of pigments of photosynthetic machinery and in isoprene synthesis, but the implications of such changes on environmental responses of isoprene emission have not been studied. Because under light-limited conditions, isoprene emission rate is controlled by DMADP pool size (SDMADP ), shifts in the share of different processes are expected to particularly strongly alter the light dependency of isoprene emission. We examined light responses of isoprene emission in young fully expanded, mature and old non-senescent leaves of hybrid aspen (Populus tremula x P. tremuloides) and estimated in vivo SDMADP and isoprene synthase activity from post-illumination isoprene release. Isoprene emission capacity was 1.5-fold larger in mature than in young and old leaves. The initial quantum yield of isoprene emission (αI ) increased by 2.5-fold with increasing leaf age primarily as the result of increasing SDMADP . The saturating light intensity (QI90 ) decreased by 2.3-fold with increasing leaf age, and this mainly reflected limited light-dependent increase of SDMADP possibly due to feedback inhibition by DMADP. These major age-dependent changes in the shape of the light response need consideration in modelling canopy isoprene emission.
Implications of interveinal distance for quantum yield in C4 grasses: a modeling and meta-analysis.
Ogle, Kiona
2003-08-01
The distance between veins has the potential to affect photosynthesis in C(4) grasses because photon capture and photosynthetic carbon reduction are primarily restricted to vascular bundle sheath cells (BSC). For example, BSC density should increase as interveinal distance (IVD) decreases, and thus IVD may influence photon capture and photosynthesis in C(4) grasses. The objective of this study is to evaluate the potential importance of IVD to the function of C(4) grasses, and a literature survey is conducted to test the hypothesis that quantum yield of photosynthesis (Phi) increases with decreasing IVD. First, a meta-analysis of Phi and IVD values obtained for 12 C(4) grass species supports this hypothesis as Phi and IVD are significantly negatively correlated (r=-0.61). Second, a regression of carbon isotope discrimination (delta) versus IVD was conducted and the regression equation was used in a simple biochemical model that relates Phi to Delta and leakage of CO(2) from the BSC. The modeling analysis also supports the hypothesis that Phi decreases with increasing IVD in C(4) grasses. C(4) grasses are virtually absent from shaded habitats, and the biochemical model is employed to examine the implications of IVD for shade-tolerance in C(4) grasses. The model predicts that only those species with uncommonly small IVD values are able to tolerate prolonged shade.
Li, Feng; Wang, Jing; Sun, Shuqing; Wang, Hai; Tang, Zhiyong; Nie, Guangjun
2015-04-24
A green-light emitting germanium nanocrystal-based biosensor to monitor lysosomal pH changes is developed. The Ge nanocrystals are synthesized in an aqueous solution with a significantly enhanced photoluminescence quantum yield of 26%. This synthesis involves a facile solution based route which avoided the use of toxic or environmentally unfriendly agents. Importantly, the photoluminescence intensity of the synthesized Ge nanocrystals is particularly sensitive to changes in pH between 5 and 6. When incubated with cultured cells, the nanocrystals are internalized and subsequently translocated via the lysosomal pathway, and the Ge nanocrystals' fluorescence are greatly enhanced, even when the lysosomal pH is only slightly increased. These results reveal that the Ge nanocrystals possess high pH sensitivity compared to a commercially available dye, LysoSensor Green DND-189. The fluorescent properties of the Ge nanocrystals are demonstrated to be dependent on both the crystal form and their surface chemistry. The superior fluorescence properties and bioapplicability of the Ge nanocrystals makes them a promising intracellular bioimaging probe for monitoring various pH-sensitive processes in cells.
Quantum yield spectra and I-V properties of a GaAs solar cell grown on a Ge substrate
NASA Astrophysics Data System (ADS)
Partain, L. D.; Virshup, G. F.; Kaminar, N. R.
A measured quantum yield spectrum showed a weak Ge junction in tandem with a strong GaAs junction for a heteroface p/n GaAs junction grown by MOCVD (metal-organic chemical vapor deposition) on an n-Ge substrate. In natural sunlight, this device had a notched-shaped I-V that limited its fill factor (FF) to 0.612 and its efficiency to 18 percent AM2.6D, which are values below those typical of similar heteroface p/n GaAs junctions grown on n-GaAs substrates. The notch disappeared and the FF increased to 0.806 under infrared-rich incandescent light. The notch deepened and the FF decreased to 0.606 under infrared-poor xenon light. This is modeled as a Ge junction with a soft I-V in tandem with a standard GaAs p/n junction. Calculations of the relative infrared content of sunlight predicts that this cell's FF should progressively decrease as the air mass spectrum progressively loses infrared content in going from AM2.6 through AM1.5 to AM0. The best model found for the Ge junction transport properties is an n-GaAs/n-Ge isotype heterojunction possibly controlled by space-charge-limited-current mechanisms.
Hou, Juan; Wang, Wei; Zhou, Tianyu; Wang, Bo; Li, Huiyu; Ding, Lan
2016-06-01
Heteroatom doped carbon dots (CDs) have received increasing attention due to their unique properties and related applications. However, previously reported CDs generally show strong emission only in the blue-light region, thus restricting their further applications. And the fundamental investigation on the preparation process is always neglected. Herein, we have developed a simple and solvent-free synthetic strategy to fabricate nitrogen-doped CDs (N-CDs) from citric acid and dicyandiamide. The as-prepared N-CDs exhibited a uniform size distribution, strong yellowish-green fluorescence emission and a high quantum yield of 73.2%. The products obtained at different formation stages were detailedly characterized by transmission electron microscopy, X-ray diffraction spectrometer, X-ray photoelectron spectroscopy and UV absorbance spectroscopy. A possible formation mechanism has thus been proposed including dehydration, polymerization and carbonization. Furthermore, the N-CDs could serve as a facile and label-free probe for the detection of iron and fluorine ions with detection limits of 50 nmol L(-1) and 75 nmol L(-1), respectively. PMID:27180833
NASA Astrophysics Data System (ADS)
Bower, Jonathan P.; Anastasio, Cort
2013-08-01
Much attention has focused on the highly reactive hydroxyl radical in the oxidation of trace organic compounds on snow and ice (and subsequent release of volatile organics to the atmospheric boundary layer) but other oxidants are likely also important in this processing. Here we examine the ice chemistry of singlet molecular oxygen (1O2*), which can be significant in atmospheric water drops but has not been examined in ice or snow. To examine 1O2* on ice we illuminate laboratory ices containing Rose Bengal (RB) as the source of 1O2*, furfuryl alcohol (FFA) as the probe, and Na2SO4 to control the total solute concentration. We find that the 1O2*-mediated loss of FFA (and, thus, the 1O2* concentration) is up to 11,000 times greater on ice than in the equivalent liquid sample at the same photon flux. We attribute this large increase in the 1O2* steady-state concentration to the freeze-concentration of solutes into liquid-like regions (LLRs) in/on ice: compared to the initial solution, in the LLRs of ice the sources for 1O2* are highly concentrated, while the concentration of the dominant sink for 1O2* (i.e., water) remains largely unchanged. Similar to results expected in liquid solution, rates of FFA loss in ice depend on both the initial sensitizer concentration and temperature, providing evidence that these reactions occur in LLRs. However, we find that the enhancement in 1O2* concentrations on ice does not follow predictions from freezing-point depression, likely because experiments were conducted below the eutectic temperature for sodium sulfate, where all of the salt should have precipitated. We also explore a method for separating 1O2* and rad OH contributions to FFA oxidation in laboratory ices and show its application to two natural snow samples. We find that 1O2* concentrations in these snows are approximately 100 times higher than observed in polluted, mid-latitude fog waters, showing that the enhancement of 1O2* on ice is environmentally relevant and that
2015-01-01
The synthesis, electrochemistry, and photophysical characterization of a 10,10-dimethylbiladiene tetrapyrrole bearing ancillary pentafluorophenyl groups at the 5- and 15-meso positions (DMBil1) is presented. This nonmacrocyclic tetrapyrrole platform is robust and can serve as an excellent ligand scaffold for Zn2+ and Cu2+ centers. X-ray diffraction studies conducted for DMBil1 along with the corresponding Zn[DMBil1] and Cu[DMBil1] complexes show that this ligand scaffold binds a single metal ion within the tetrapyrrole core. Additionally, electrochemical experiments revealed that all three of the aforementioned compounds display an interesting redox chemistry as the DMBil1 framework can be both oxidized and reduced by two electrons. Spectroscopic and photophysical experiments carried out for DMBil1, Zn[DMBil1], and Cu[DMBil1] provide a basic picture of the electronic properties of these platforms. All three biladiene derivatives strongly absorb light in the visible region and are weakly emissive. The ability of these compounds to sensitize the formation of 1O2 at wavelengths longer than 500 nm was probed. Both the free base and Zn2+ 10,10-dimethylbiladiene architectures show modest efficiencies for 1O2 sensitization. The combination of structural, electrochemical, and photophysical data detailed herein provides a basis for the design of additional biladiene constructs for the activation of O2 and other small molecules. PMID:25187099
Morajkar, Pranay; Bossolasco, Adriana; Schoemaecker, Coralie; Fittschen, Christa
2014-06-01
Radical quantum yields have been measured following the 248 nm photolysis of acetaldehyde, CH3CHO. 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 HO2 radicals by reaction with O2. The CH3 radical yield has been determined using the same technique following their conversion into CH3O2. Absolute yields have been deduced for HCO radicals and H atoms through fitting of time resolved HO2 profiles, obtained under various O2 concentrations, to a complex model, while the CH3 yield has been determined relative to the CH3 yield from 248 nm photolysis of CH3I. Time resolved HO2 profiles under very low O2 concentrations suggest that another unknown HO2 forming reaction path exists in this reaction system besides the conversion of HCO radicals and H atoms by reaction with O2. HO2 profiles can be well reproduced under a large range of experimental conditions with the following quantum yields: CH3CHO + hν(248nm) → CH3CHO*, CH3CHO* → CH3 + HCO ϕ(1a) = 0.125 ± 0.03, CH3CHO* → CH3 + H + CO ϕ(1e) = 0.205 ± 0.04, CH3CHO*[Formula: see text]CH3CO + HO2 ϕ(1f) = 0.07 ± 0.01. The CH3O2 quantum yield has been determined in separate experiments as ϕ(CH₃) = 0.33 ± 0.03 and is in excellent agreement with the CH3 yields derived from the HO2 measurements considering that the triple fragmentation (R1e) is an important reaction path in the 248 nm photolysis of CH3CHO. From arithmetic considerations taking into account the HO2 and CH3 measurements we deduce a remaining quantum yield for the molecular pathway: CH3CHO* → CH4 + CO ϕ(1b) = 0.6. All experiments can be consistently explained with absence of the formerly considered pathway: CH3CHO* → CH3CO + H ϕ(1c) = 0. PMID:24908009
Bagratashvili, V N; Tsypina, S I; Chutko, E A; Gerasimova, V I; Gordienko, V M
2008-08-31
The kinetics of photoluminescence of a EuFOD{sub 3} metalloorganic compound doped into a nanoporous Vycor glass by the method of supercritical fluid impregnation is studied. The lifetime of luminescence of EuFOD{sub 3} molecules in pores excited by an excimer XeCl laser was 40 {mu}s, which is considerably smaller than this lifetime (150-890 {mu}s) in solutions. The quantum yield of luminescence of EuFOD{sub 3} was estimate as {approx}4x10{sup -4}. (laser applications and other topics in quantum electronics)
NASA Astrophysics Data System (ADS)
Bashtanov, M. E.; Drozdova, N. N.; Krasnovskii, A. A.
1999-12-01
An investigation was made of the ratios of the intensity Idf of the singlet-oxygen(1O2)-sensitised delayed fluorescence of the zinc complex of tetra(4-tert-butyl)phthalocyanine (ZnTBPc), with the maximum at λ = 685 nm, to the intensity I1270 of the photosensitised phosphorescence of 1O2 with the maximum at λ = 1270 nm in deuterated benzene when excited with λ = 337 nm nitrogen-laser pulses. Depending on the energy density of the laser radiation (0.25 — 0.7 mJ cm-2) and on the concentration of ZnTBPc (0.06 — 3.4 μM), the ratio of the zero-time intensities of the delayed fluorescence of ZnTBPc and of the singlet-oxygen phosphorescence Idf0/I12700 varied from 0.01 to 0.2 in air-saturated solutions of ZnTBPc. The intensity Idf0 decreased fivefold as a result of saturation with oxygen of air-saturated solutions. The quantum efficiency of the delayed fluorescence was represented by the coefficient α =(Idf0/I12700)kr/(γf[1O2]0[ZnTBPc]), where [1O2]0 is the zero-time concentration of 1O2 after a laser shot; kr is the rate constant of radiative deactivation of 1O2 in the investigated solvent; γf is the quantum yield of the ZnTBPc fluorescence. It was established that in the case of air-saturated solutions of ZnTBPc this coefficient was approximately 200 times less than for metal-free tetra(4-tert-butyl)phthalocyanine and its absolute value was ~2 × 1011 M-2 s-1.
NASA Astrophysics Data System (ADS)
Sueishi, Yoshimi; Fujita, Tomonori; Nakatani, Shinichiro; Inazumi, Naoya; Osawa, Yoshihiro
2013-10-01
The association constants (K) for the inclusion complexation of four kinds of cyclodextrins (CDs (β- and γ-), 2,6-di-O-methylated β-CD, and 2,3,6-tri-O-methylated β-CD) and cucurbit[7]uril (CB[7]) with 1,8- and 2,6-anilinonaphthalene sulfonic acids (ANSs) were determined from fluorescence spectra enhanced by inclusion. Various CDs and CB[7] form stable 1:1 inclusion complexes with 1,8- and 2,6-ANSs: K = 80-11 700 M-1 for 2,6-ANS and 50-195 M-1 for 1,8-ANS. The high stability of the inclusion complexes of 2,6-ANS with CB[7] and 2,6-di-O-methylated β-CD is shown. Further, we determined the fluorescence quantum yields (Φ values) for the inclusion complexes of ANSs by using a fluorescence spectrophotometer equipped with a half-moon unit. The Φ values of 1,8- and 2,6-ANSs were largely enhanced by the inclusion of methylated β-CDs and did not correlate with the degree of stability (K) of the inclusion complexes. We characterized the structures of the inclusion complexes by 2D ROESY-NMR measurements. In addition, the microenvironmental polarity inside the hydrophobic CD and CB[7] cavities was evaluated using the fluorescence probe 2,6-ANS. Based on the emission mechanism and the aspect of inclusion in a hydrophobic cavity, we have suggested that the microenvironmental polarity and viscosity for the excited state of ANS plays an important role for the Φ values of inclusion complexes.
Sueishi, Yoshimi; Fujita, Tomonori; Nakatani, Shinichiro; Inazumi, Naoya; Osawa, Yoshihiro
2013-10-01
The association constants (K) for the inclusion complexation of four kinds of cyclodextrins (CDs (β- and γ-), 2,6-di-O-methylated β-CD, and 2,3,6-tri-O-methylated β-CD) and cucurbit[7]uril (CB[7]) with 1,8- and 2,6-anilinonaphthalene sulfonic acids (ANSs) were determined from fluorescence spectra enhanced by inclusion. Various CDs and CB[7] form stable 1:1 inclusion complexes with 1,8- and 2,6-ANSs: K=80-11700 M(-1) for 2,6-ANS and 50-195 M(-1) for 1,8-ANS. The high stability of the inclusion complexes of 2,6-ANS with CB[7] and 2,6-di-O-methylated β-CD is shown. Further, we determined the fluorescence quantum yields (Φ values) for the inclusion complexes of ANSs by using a fluorescence spectrophotometer equipped with a half-moon unit. The Φ values of 1,8- and 2,6-ANSs were largely enhanced by the inclusion of methylated β-CDs and did not correlate with the degree of stability (K) of the inclusion complexes. We characterized the structures of the inclusion complexes by 2D ROESY-NMR measurements. In addition, the microenvironmental polarity inside the hydrophobic CD and CB[7] cavities was evaluated using the fluorescence probe 2,6-ANS. Based on the emission mechanism and the aspect of inclusion in a hydrophobic cavity, we have suggested that the microenvironmental polarity and viscosity for the excited state of ANS plays an important role for the Φ values of inclusion complexes.
Fischer, Stefan; Goldschmidt, Jan Christoph; Johnson, Noah J. J.; Pichaandi, Jothirmayanantham; Veggel, Frank C. J. M. van
2015-11-21
Colloidal upconverter nanocrystals (UCNCs) that convert near-infrared photons to higher energies are promising for applications ranging from life sciences to solar energy harvesting. However, practical applications of UCNCs are hindered by their low upconversion quantum yield (UCQY) and the high irradiances necessary to produce relevant upconversion luminescence. Achieving high UCQY under practically relevant irradiance remains a major challenge. The UCQY is severely limited due to non-radiative surface quenching processes. We present a rate equation model for migration of the excitation energy to show that surface quenching does not only affect the lanthanide ions directly at the surface but also many other lanthanide ions quite far away from the surface. The average migration path length is on the order of several nanometers and depends on the doping as well as the irradiance of the excitation. Using Er{sup 3+}-doped β-NaYF{sub 4} UCNCs, we show that very isotropic and thick (∼10 nm) β-NaLuF{sub 4} inert shells dramatically reduce the surface-related quenching processes, resulting in much brighter upconversion luminescence at simultaneously considerably lower irradiances. For these UCNCs embedded in poly(methyl methacrylate), we determined an internal UCQY of 2.0% ± 0.2% using an irradiance of only 0.43 ± 0.03 W/cm{sup 2} at 1523 nm. Normalized to the irradiance, this UCQY is 120× higher than the highest values of comparable nanomaterials in the literature. Our findings demonstrate the important role of isotropic and thick shells in achieving high UCQY at low irradiances from UCNCs. Additionally, we measured the additional short-circuit current due to upconversion in silicon solar cell devices as a proof of concept and to support our findings determined using optical measurements.
NASA Astrophysics Data System (ADS)
Jackson, William M.
2016-10-01
VUV photodissociation above 10.5 eV is considered the primary region for photochemical destruction of CO2 by solar radiation. There is enough photon energy in this region so that in addition to ground state O(3PJ) and CO(1Σ +) that can be produced during photodissociation excited species such as atomic oxygen O(1D) and O(1S), as well as excited carbon monoxide CO(a3Π, a'3Σ+) also can be formed. Electronic excited oxygen atom and carbon monoxide are the species that are responsible for the airglows in atmospheres of the solar planets and comets. Therefore, detail photodissociation quantum yields for these excited species from CO2 are critical in interpreting the chemistry in these solar system bodies. We have previously shown that the time-sliced velocity-mapped imaging (TS-VMI) technique can provide detailed branching ratio information about photodissociation of diatomic molecules.1, 2 However, to date we have not been able to show how this technique can be use to determine absolute quantum yields for the products produced in the VUV photodissociation of CO2. In this talk we will describe how the known quantum yields for the photodissociation O2 to O(3P2), O(3P1), O(3P0) and O(1D) can be used to determine quantum yields of similar products in the photodissociation of CO2.[1] Yu Song, Hong Gao, Yih Chung Chang, D. Hammouténe, H. Ndome, M. Hochlaf, William M. Jackson, and C. Y. Ng, Ap. J., 819:23 (13pp), 2016; doi:10.3847/0004-637X/819/1/23.[2] Hong Gao, Yu Song, William M. Jackson and C. Y. Ng, J. Chem. Phys, 138, 191102, 2013.
NASA Astrophysics Data System (ADS)
Zhang, Jiaxiang; Wildmann, Johannes S.; Ding, Fei; Trotta, Rinaldo; Huo, Yongheng; Zallo, Eugenio; Huber, Daniel; Rastelli, Armando; Schmidt, Oliver G.
2015-12-01
Triggered sources of entangled photon pairs are key components in most quantum communication protocols. For practical quantum applications, electrical triggering would allow the realization of compact and deterministic sources of entangled photons. Entangled-light-emitting-diodes based on semiconductor quantum dots are among the most promising sources that can potentially address this task. However, entangled-light-emitting-diodes are plagued by a source of randomness, which results in a very low probability of finding quantum dots with sufficiently small fine structure splitting for entangled-photon generation (~10-2). Here we introduce strain-tunable entangled-light-emitting-diodes that exploit piezoelectric-induced strains to tune quantum dots for entangled-photon generation. We demonstrate that up to 30% of the quantum dots in strain-tunable entangled-light-emitting-diodes emit polarization-entangled photons. An entanglement fidelity as high as 0.83 is achieved with fast temporal post selection. Driven at high speed, that is 400 MHz, strain-tunable entangled-light-emitting-diodes emerge as promising devices for high data-rate quantum applications.
Zhang, Jiaxiang; Wildmann, Johannes S; Ding, Fei; Trotta, Rinaldo; Huo, Yongheng; Zallo, Eugenio; Huber, Daniel; Rastelli, Armando; Schmidt, Oliver G
2015-01-01
Triggered sources of entangled photon pairs are key components in most quantum communication protocols. For practical quantum applications, electrical triggering would allow the realization of compact and deterministic sources of entangled photons. Entangled-light-emitting-diodes based on semiconductor quantum dots are among the most promising sources that can potentially address this task. However, entangled-light-emitting-diodes are plagued by a source of randomness, which results in a very low probability of finding quantum dots with sufficiently small fine structure splitting for entangled-photon generation (∼10(-2)). Here we introduce strain-tunable entangled-light-emitting-diodes that exploit piezoelectric-induced strains to tune quantum dots for entangled-photon generation. We demonstrate that up to 30% of the quantum dots in strain-tunable entangled-light-emitting-diodes emit polarization-entangled photons. An entanglement fidelity as high as 0.83 is achieved with fast temporal post selection. Driven at high speed, that is 400 MHz, strain-tunable entangled-light-emitting-diodes emerge as promising devices for high data-rate quantum applications.
Zhang, Jiaxiang; Wildmann, Johannes S.; Ding, Fei; Trotta, Rinaldo; Huo, Yongheng; Zallo, Eugenio; Huber, Daniel; Rastelli, Armando; Schmidt, Oliver G.
2015-01-01
Triggered sources of entangled photon pairs are key components in most quantum communication protocols. For practical quantum applications, electrical triggering would allow the realization of compact and deterministic sources of entangled photons. Entangled-light-emitting-diodes based on semiconductor quantum dots are among the most promising sources that can potentially address this task. However, entangled-light-emitting-diodes are plagued by a source of randomness, which results in a very low probability of finding quantum dots with sufficiently small fine structure splitting for entangled-photon generation (∼10−2). Here we introduce strain-tunable entangled-light-emitting-diodes that exploit piezoelectric-induced strains to tune quantum dots for entangled-photon generation. We demonstrate that up to 30% of the quantum dots in strain-tunable entangled-light-emitting-diodes emit polarization-entangled photons. An entanglement fidelity as high as 0.83 is achieved with fast temporal post selection. Driven at high speed, that is 400 MHz, strain-tunable entangled-light-emitting-diodes emerge as promising devices for high data-rate quantum applications. PMID:26621073
Jacob, Maik H; Dsouza, Roy N; Ghosh, Indrajit; Norouzy, Amir; Schwarzlose, Thomas; Nau, Werner M
2013-01-10
effective FRET rate and the recovered donor-acceptor distance depend on the quantum yield, most strongly in the absence of diffusion, which has to be accounted for in the interpretation of distance trends monitored by FRET.
Smith, C A; Maki, A H
1993-01-01
The radiative quantum yield, phi op, of the triplet state of human alpha-lactalbumin (HLA) has been measured in the temperature range between 6 K and the softening point of the aqueous glass (approximately 150 K). phi op has little temperature dependence below approximately 30 K, but above this it decreases sharply with increasing temperature. The unusual temperature dependence is fitted by a phenomenological two-state model in which the phosphorescence originates primarily from a donor, tryptophan (Trp) 104, and an acceptor, Trp 60, the populations of which are coupled by a thermally activated triplet-triplet energy transfer process. The model assumes that the acceptor (Trp 60) triplet state undergoes radiationless deactivation by a proximal disulfide residue, while the donor (Trp 104) has no such extrinsic quencher. The decrease of phi op with increasing temperature is accounted for by the thermally activated triplet-triplet energy transfer process. The disulfide quenching rate constant itself is assumed to be temperature independent, in accord with recent measurements of simple disulfide quenching in long chain snake venom neurotoxins (Schlyer, B. D., E. Lau, and A. H. Maki. 1992. Biochemistry. 31:4375-4383; Li, Z., A. Bruce, and W. C. Galley. 1992. Biophys. J. 61:1364-1371). We find that the phosphorescence quenching in HLA occurs with an activation energy of 97 cm-1, which we associate with a barrier to the energy transfer process. The data are fit well by the model if we assume a value for the temperature-independent disulfide quenching constant of kQ > 3 s-1 that is consistent with recent measurements on indole-disulfide model systems (Li, Z., A. Bruce, and W. C. Galley. 1992. Biophys. J. 61:1364-1371). Similar results are reported for bovine alpha-lactalbumin (BLA) and for hen egg-white lysozyme (HEWL) that contains the structural equivalents of Trp 104 and Trp 60 of HLA. HLA provides the best agreement with calculations since it is the simplest, lacking
Pennacchietti, Francesca; Losi, Aba; Xu, Xiu-ling; Zhao, Kai-hong; Gärtner, Wolfgang; Viappiani, Cristiano; Cella, Francesca; Diaspro, Alberto; Abbruzzetti, Stefania
2015-02-01
The protein encoded by the gene slr1393 from the cyanobacterium Synechocystis sp. PCC6803 (Slr1393) is composed of three GAF domains, a PAS domain, and a histidine kinase motif. The third GAF domain (referred to as GAF3) was previously characterized as the sole domain in this protein, being able to carry phycocyanobilin (PCB) as the chromophore and to accomplish photochemistry. GAF3 shows photochromicity, and is able to switch between a red-absorbing parental state (GAF3R, λmax = 649 nm) and a green-absorbing photoproduct state (GAF3G, λmax = 536 nm) upon appropriate irradiation. In this study we have determined the photochemical quantum yields for the interconversion between both forms using two methods: an "absolute" method and a reference-based control. The latter is a comparative procedure which exploits a well-characterized blue-light photoreceptor, YtvA from Bacillus subtilis, and the cyanobacterial phytochrome Cph1 as actinometers. The former is an ad hoc developed, four laser-based setup where two cw lasers provide the pump beams to induce photoswitching (red to green and green to red, respectively) and two cw lasers simultaneously monitor the appearance and disappearance of the two species. Interestingly, fit analysis of the recorded transient absorbance changes provided a quantum yield for the green → red conversion (≈0.3) at least three times larger than for the red → green conversion (≈0.08). These data are in agreement with the results from the comparative method documenting the usefulness of the 'direct' method developed here for quantum yields' determination. The light-induced switching capability of this photochromic protein allowed measuring the kinetics of GAF3 immobilized on a glass plate, and within living, overexpressing Escherichia coli cells. PMID:25358617
Q-Machine Plasmas Yielding New Experimental Methodologies of Sheared-Flow and Nano-Quantum Physics
Hatakeyama, Rikizo; Kaneko, Toshiro
2008-10-15
The traditional Q machine has been modified in accordance with the evolution of experimental methodologies ranging from modern plasma physics to extreme nanoscience. A special emphasis is placed on physics of sheared-flow related electron-temperature-gradient modes and nano-quantum physics or electronics based on fullerene and carbon nanotubes.
Zhou, Pingwei; Zhu, Yongsheng; Xu, Wen; Xu, Lin; Song, Hongwei
2013-11-01
In this work, rare earth (RE) ions tri-doped YV(1-x)P(x)O(4): RE(3+) (RE = Tm, Dy, Eu) inverse opal photonic crystals (IOPCs) were fabricated by the PMMA template method, which demonstrated efficient white light emissions under ultraviolet excitation. It is significant to observe that the chrominance of the white light could be largely modulated by the photonic stop band of the IOPCs. And more, the photoluminescence quantum yield in the IOPCs was largely improved over the grinded reference (REF) because the undesired energy transfer (ET) process was effectively restrained. PMID:24216800
NASA Astrophysics Data System (ADS)
Läuter, Almuth; Suresh, Dhanya; Volpp, Hans-Robert
2003-04-01
The dynamics of chlorine and hydrogen atom formation in the 193.3 nm gas-phase laser photolysis of room-temperature 1,1-dichloro-1-fluoroethane, CH3CFCl2 (HCFC-141b), were studied by means of the pulsed-laser-photolysis and laser-induced fluorescence (LIF) "pump-and-probe" technique. Nascent ground-state Cl(2P3/2) and spin-orbit excited Cl*(2P1/2) as well as H(2S) atom photofragments were detected under collision-free conditions by pulsed Doppler-resolved laser-induced fluorescence measurements employing narrow-band vacuum ultraviolet probe laser radiation, generated via resonant third-order sum-difference frequency conversion of dye laser radiation in krypton. Using HCl photolysis as a reference source of well-defined Cl(2P3/2), Cl*(2P1/2), and H atom concentrations, values for the chlorine-atom spin-orbit branching ratio [Cl*]/[Cl]=0.36±0.08, the total chlorine atom quantum yield (ΦCl+Cl*=1.01±0.14), and the H atom quantum yield (ΦH=0.04±0.01) were determined by means of a photolytic calibration method. From the measured Cl and Cl* atom Doppler profiles the mean relative translational energy of the chlorine fragments could be determined to be ET(Cl)=157±12 kJ/mol and ET(Cl*)=165±12 kJ/mol. The corresponding average values 0.56 and 0.62 of the fraction of total available energy channeled into CH3CFCl+Cl/Cl* product translational energy were found to lie between the limiting values 0.36 and 0.85 predicted by a soft impulsive and a rigid rotor model of the CH3CFCl2→CH3CFCl+Cl/Cl* dissociation processes, respectively. The measured total chlorine atom quantum yield along with the rather small H atom quantum yield as well as the observed energy disposal indicates that direct C-Cl bond cleavage is the most important primary fragmentation mechanism for CH3CFCl2 after photoexcitation in the first absorption band.
Gao, Tang; Xu, Pengfei; Liu, Meihui; Bi, Anyao; Hu, Pengzhi; Ye, Bin; Wang, Wei; Zeng, Wenbin
2015-05-01
A novel fluorescent probe with a high quantum yield (0.41), large Stokes shifts (255 nm), and red emission (635 nm) was designed to detect all typical oxidation states of palladium species (0, +2, +4) by palladium-mediated terminal propargyl ethers cleavage reaction in water solution without any organic media. The probe showed a high selectivity and excellent sensitivity for palladium species, with a detection as low as 57 nM (6.2 μg L(-1)).
Ghosh, Buddhadeb; Papanastasiou, Dimitrios K.; Burkholder, James B.
2012-10-28
Oxalyl chloride, (ClCO){sub 2}, has been used as a Cl atom photolytic precursor in numerous laboratory kinetic and photochemical studies. In this study, the UV/vis absorption spectrum of (ClCO){sub 2} and the Cl atom quantum yields in its photolysis at 193, 248, and 351 nm are reported. The UV/vis spectrum was measured between 200 and 450 nm at 296 K using diode array spectroscopy in conjunction with an absolute cross section obtained at 213.9 nm. Our results are in agreement with the spectrum reported by Baklanov and Krasnoperov [J. Phys. Chem. A 105, 97-103 (2001)], which was obtained at 11 discrete wavelengths between 193.3 and 390 nm. Cl atom quantum yields, {Phi}({lambda}), were measured using pulsed laser photolysis coupled with time resolved atomic resonance fluorescence detection of Cl. The UV photolysis of (ClCO){sub 2} has been shown in previous studies to occur via an impulsive three-body dissociation mechanism, (COCl){sub 2}+ hv{yields} ClCO*+ Cl + CO (2), where the excited ClCO radical, ClCO*, either dissociates or stabilizes ClCO*{yields} Cl + CO (3a), {yields} ClCO (3b). ClCO is thermally unstable at the temperatures (253-298 K) and total pressures (13-128 Torr) used in our experiments ClCO + M {yields} Cl + CO + M (4) leading to the formation of a secondary Cl atom that was resolvable in the Cl atom temporal profiles obtained in the 248 and 351 nm photolysis of (ClCO){sub 2}. {Phi}(193 nm) was found to be 2.07 {+-} 0.37 independent of bath gas pressure (25.8-105.7 Torr, N{sub 2}), i.e., the branching ratio for channel 2a or the direct formation of 2Cl + 2CO in the photolysis of (ClCO){sub 2} is >0.95. At 248 nm, the branching ratio for channel 2a was determined to be 0.79 {+-} 0.15, while the total Cl atom yield, i.e., following the completion of reaction (4), was found to be 1.98 {+-} 0.26 independent of bath gas pressure (15-70 Torr, N{sub 2}). {Phi}(351 nm) was found to be pressure dependent between 7.8 and 122.4 Torr (He, N{sub 2}). The low
Rosner, J. L.; Alexander, J. P.; Cassel, D. G.; Duboscq, J. E.; Ehrlich, R.; Fields, L.; Gibbons, L.; Gray, R.; Gray, S. W.; Hartill, D. L.; Heltsley, B. K.; Hertz, D.; Jones, C. D.; Kandaswamy, J.; Kreinick, D. L.; Kuznetsov, V. E.; Mahlke-Krueger, H.; Mohapatra, D.; Onyisi, P. U. E.; Patterson, J. R.
2008-06-06
We exploit the quantum coherence between pair-produced D{sup 0} and D{sup 0} in {psi}(3770) decays to study charm mixing, which is characterized by the parameters x and y, and to make a first determination of the relative strong phase {delta} between D{sup 0}{yields}K{sup +}{pi}{sup -} and D{sup 0}{yields}K{sup +}{pi}{sup -}. Using 281 pb{sup -1} of e{sup +}e{sup -} collision data collected with the CLEO-c detector at E{sub cm}=3.77 GeV, as well as branching fraction input and time-integrated measurements of R{sub M}{identical_to}(x{sup 2}+y{sup 2})/2 and R{sub WS}{identical_to}{gamma}(D{sup 0}{yields}K{sup +}{pi}{sup -})/{gamma}(D{sup 0}{yields}K{sup +}{pi}{sup -}) from other experiments, we find cos{delta}=1.03{sub -0.17}{sup +0.31}{+-}0.06, where the uncertainties are statistical and systematic, respectively. By further including other mixing parameter measurements, we obtain an alternate measurement of cos{delta}=1.10{+-}0.35{+-}0.07, as well as xsin{delta}=(4.4{sub -1.8}{sup +2.7}{+-}2.9)x10{sup -3} and {delta}=(22{sub -12-11}{sup +11+9}) deg.
Liu, Li; Zhao, Zhe; Zhang, Xiaomin; Cui, Daan; Tu, Baofeng; Ou, Dingrong; Cheng, Mojie
2013-01-28
The YSZ electrolyte fuel cell with a ternary cathode composed of LSM-YSZ-Ce(0.9)Mn(0.1)O(2-δ) exhibits ca. 2.6 times higher current density than that with a binary cathode composed of LSM-YSZ at 600 °C.
Oberhuber, W.; Edwards, G. E.
1993-02-01
The temperature dependence of quantum yields of electron transport from photosystem II (PSII) ([phi]II, determined from chlorophyll a fluorescence) and CO2 assimilation ([phi]CO2, apparent quantum yield for CO2 assimilation) were determined simultaneously in vivo. With C4 species representing NADP-malic enzyme, NAD-malic enzyme, and phosphoenolpyruvate carboxykinase subgroups, the ratio of [phi]II/[phi]CO2 was constant over the temperature range from 15 to 40[deg]C at high light intensity (1100 [mu]mol quanta m-2 s-1). A similar response was obtained at low light intensity (300 [mu]mol quanta m-2 s-1), except the ratio of [phi]II/[phi]CO2 increased at high temperature. When the true quantum yield for CO2 fixation ([phi]CO2*) was calculated by correcting for respiration in the light (estimated from temperature dependence of dark respiration), the ratio of [phi]II/[phi]C02* remained constant with varying temperature and under both light intensities in all C4 species examined. Because the [phi]II/[phi]CO2* ratio was the same in C4 monocots representing the three subgroups, the ratio was not affected by differences in the bio-chemical mechanism of concentrating CO2 in the bundle sheath cells. The results suggest that PSII activity is closely linked to the true rate of CO2 fixation in C4 plants. The close relationship between [phi]II and [phi]CO2* in C4 species under varying temperature and light intensity conditions is apparently due to a common low level of photorespiration and a primary requirement for reductive power in the C3 pathway. In contrast, in a C3 plant the [phi] II/[phi]CO2* ratio is higher under normal atmospheric conditions than under nonphotorespiratory conditions and it increases with rising temperature. This decrease in efficiency in utilizing energy derived from PSII for CO2 fixation is due to an increase in photorespiration. In both the C3 and C4 species, photochemistry is limited under low temperature, and thus excess energy must be dissipated by
Ghosh, Buddhadeb; Papanastasiou, Dimitrios K; Burkholder, James B
2012-10-28
Oxalyl chloride, (ClCO)(2), has been used as a Cl atom photolytic precursor in numerous laboratory kinetic and photochemical studies. In this study, the UV/vis absorption spectrum of (ClCO)(2) and the Cl atom quantum yields in its photolysis at 193, 248, and 351 nm are reported. The UV∕vis spectrum was measured between 200 and 450 nm at 296 K using diode array spectroscopy in conjunction with an absolute cross section obtained at 213.9 nm. Our results are in agreement with the spectrum reported by Baklanov and Krasnoperov [J. Phys. Chem. A 105, 97-103 (2001)], which was obtained at 11 discrete wavelengths between 193.3 and 390 nm. Cl atom quantum yields, Φ(λ), were measured using pulsed laser photolysis coupled with time resolved atomic resonance fluorescence detection of Cl. The UV photolysis of (ClCO)(2) has been shown in previous studies to occur via an impulsive three-body dissociation mechanism, (COCl)(2) + hv → ClCO* + Cl + CO (2), where the excited ClCO radical, ClCO*, either dissociates or stabilizes ClCO* → Cl + CO (3a), → ClCO (3b). ClCO is thermally unstable at the temperatures (253-298 K) and total pressures (13-128 Torr) used in our experiments ClCO + M → Cl + CO + M (4) leading to the formation of a secondary Cl atom that was resolvable in the Cl atom temporal profiles obtained in the 248 and 351 nm photolysis of (ClCO)(2). Φ(193 nm) was found to be 2.07 ± 0.37 independent of bath gas pressure (25.8-105.7 Torr, N(2)), i.e., the branching ratio for channel 2a or the direct formation of 2Cl + 2CO in the photolysis of (ClCO)(2) is >0.95. At 248 nm, the branching ratio for channel 2a was determined to be 0.79 ± 0.15, while the total Cl atom yield, i.e., following the completion of reaction (4), was found to be 1.98 ± 0.26 independent of bath gas pressure (15-70 Torr, N(2)). Φ(351 nm) was found to be pressure dependent between 7.8 and 122.4 Torr (He, N(2)). The low-pressure limit of the total Cl atom quantum yield, Φ(0)(351 nm), was 2
NASA Astrophysics Data System (ADS)
Le Roy, Robert J.; Walji, Sadru; Sentjens, Katherine
2013-06-01
Alkali hydride diatomic molecules have long been the object of spectroscopic studies. However, their small reduced mass makes them species for which the conventional semiclassical-based methods of analysis tend to have the largest errors. To date, the only quantum-mechanically accurate direct-potential-fit (DPF) analysis for one of these molecules was the one for LiH reported by Coxon and Dickinson. The present paper extends this level of analysis to NaH, and reports a DPF analysis of all available spectroscopic data for the A ^1Σ^+-X ^1Σ^+ system of NaH which yields analytic potential energy functions for these two states that account for those data (on average) to within the experimental uncertainties. W.C. Stwalley, W.T. Zemke and S.C. Yang, J. Phys. Chem. Ref. Data {20}, 153-187 (1991). J.A. Coxon and C.S. Dickinson, J. Chem. Phys. {121}, 8378 (2004).
Coropceanu, Igor; Rossinelli, Aurelio; Caram, Justin R; Freyria, Francesca S; Bawendi, Moungi G
2016-03-22
A two-step process has been developed for growing the shell of CdSe/CdS core/shell nanorods. The method combines an established fast-injection-based step to create the initial elongated shell with a second slow-injection growth that allows for a systematic variation of the shell thickness while maintaining a high degree of monodispersity at the batch level and enhancing the uniformity at the single-nanorod level. The second growth step resulted in nanorods exhibiting a fluorescence quantum yield up to 100% as well as effectively complete energy transfer from the shell to the core. This improvement suggests that the second step is associated with a strong suppression of the nonradiative channels operating both before and after the thermalization of the exciton. This hypothesis is supported by the suppression of a defect band, ubiquitous to CdSe-based nanocrystals after the second growth.
NASA Astrophysics Data System (ADS)
Wei, Shutian; Zhu, Zhilin; Wang, Zhixiao; Wei, Gugangfen; Wang, Pingjian; Li, Hai; Hua, Zhen; Lin, Zhonghai
2016-07-01
Size-controllable monodisperse CdSe nanocrystals with different organic capping were prepared based on the hot-injection method. The effective separation of nucleation and growth was achieved by rapidly mixing two highly reactive precursors. As a contrast, we prepared CdSe/CdS nanocrystals (NCs) successfully based on the selective ion layer adsorption and reaction (SILAR) technique. This inorganic capping obtained higher photoluminescence quantum yield (PLQY) of 59.3% compared with organic capping of 40.8%. Furthermore, the CdSe-epoxy resin (EP) composites were prepared by adopting a flexible ex situ method, and showed excellent stability in the ambient environment for one year. So the composites with both high PLQY of nanocrystals and excellent stability are very promising to device application.
Gudkov, N D; Stolovitskiĭ, Iu M; Evstigneev, V B
1978-01-01
The values of absolute quantum yield phi of the formation of free ion-radicals during the illumination of alkohol solutions of chlorophyll alpha (Chl) and rho-benzoquinone (Q) at room temperature were obtained by the method of impulse photoconductance. With an increase of the dielectric constant epsilon of the solvent from approximately 6 to approximately 25 phi increases by two orders ( approximately 10(-3)--approximately 10(-1). That obtained relationship phi (epsilon) is explained by epsilon effect on the efficiency of dissociation of "solvent-shared" ion-radical pair Chls+. Os-. The comparison of experimental data and theoretically expected ones allowed the estimation of some parameters to be obtained which characterize the ion-radical pair: interionic distance (10 A), the dissociation velocity constant ( approximately 10(5)--10(8) s-1), the velocity constant of reverse electron transfer (10(8) s-1), the life time approximately 10(-8) s).
THOMAS, J B; GOVINDJEE
1960-09-01
This paper describes the relation between the quantum yield of photosynthesis in the red alga Porphyridium cruentum, and the spectral composition of light, changed by filtering white light through aqueous phycobilin solutions of increasing optical density. At sufficiently high densities of the filter solution, no measurable photosynthesis can be observed, although chlorophyll a molecules are still being excited at a significant rate, as can be proved by calculations from spectral distribution curves, and is confirmed by the occurrence of a "second Emerson effect" upon addition of orange light. An interpretation of this result, based on other experiments, will be given in a subsequent paper. A modification of the opal glass technique for reducing the effect of scattering when measuring absorption, was developed in connection with this research, and also is described in the paper.
NASA Technical Reports Server (NTRS)
Chatfield, David C.; Friedman, Ronald S.; Lynch, Gillian C.; Truhlar, Donald G.; Schwenke, David W.
1993-01-01
Accurate quantum mechanical dynamics calculations are reported for the reaction probabilities of O(3P) + H2 yields OH + H with zero total angular momentum on a single potential energy surface. The results show that the reactive flux is gated by quantized transition states up to the highest energy studied, which corresponds to a total energy of 1.90 eV. The quantized transition states are assigned and compared to vibrationally adiabatic barrier maxima; their widths and transmission coefficients are determined; and they are classified as variational, supernumerary of the first kind, and supernumerary of the second kind. Their effects on state-selected and state-to-state reactivity are discussed in detail.
A Time-Dependent Quantum Dynamics Study of the H2 + CH3 yields H + CH4 Reaction
NASA Technical Reports Server (NTRS)
Wang, Dunyou; Kwak, Dochan (Technical Monitor)
2002-01-01
We present a time-dependent wave-packet propagation calculation for the H2 + CH3 yields H + CH4 reaction in six degrees of freedom and for zero total angular momentum. Initial state selected reaction probability for different initial rotational-vibrational states are presented in this study. The cumulative reaction probability (CRP) is obtained by summing over initial-state-selected reaction probability. The energy-shift approximation to account for the contribution of degrees of freedom missing in the 6D calculation is employed to obtain an approximate full-dimensional CRP. Thermal rate constant is compared with different experiment results.
Chow, Pui-Keong; Cheng, Gang; Tong, Glenna So Ming; To, Wai-Pong; Kwong, Wai-Lun; Low, Kam-Hung; Kwok, Chi-Chung; Ma, Chensheng; Che, Chi-Ming
2015-02-01
Luminescent pincer-type Pt(II) complexes supported by C-deprotonated π-extended tridentate RC^N^NR' ligands and pentafluorophenylacetylide ligands show emission quantum yields up to almost unity. Femtosecond time-resolved fluorescence measurements and time-dependent DFT calculations together reveal the dependence of excited-state structural distortions of [Pt(RC^N^NR')(CC-C6 F5 )] on the positional isomers of the tridentate ligand. Pt complexes [Pt(R-C^N^NR')(CC-Ar)] are efficient photocatalysts for visible-light-induced reductive CC bond formation. The [Pt(R-C^N^NR')(CC-C6 F5 )] complexes perform strongly as phosphorescent dopants for green- and red-emitting organic light-emitting diodes (OLEDs) with external quantum efficiency values over 22.1 %. These complexes are also applied in two-photon cellular imaging when incorporated into mesoporous silica nanoparticles (MSNs).
Rong, Mingcong; Cai, Zhixiong; Xie, Lei; Lin, Chunshui; Song, Xinhong; Luo, Feng; Wang, Yiru; Chen, Xi
2016-06-27
Graphitic carbon nitride nanodots (g-C3 N4 nanodots), as a new kind of heavy-metal-free quantum dots, have attracted considerable attention because of their unique physical and chemical properties. Although various methods to obtain g-C3 N4 nanodots have been reported, it is still a challenge to synthesize g-C3 N4 nanodots with ultrahigh fluorescence quantum yield (QY). In this study, highly fluorescent phosphorus/oxygen-doped graphitic carbon nitride (P,O-g-C3 N4 ) nanodots were prepared by chemical oxidation and hydrothermal etching of bulk P-g-C3 N4 derived from the pyrolysis of phytic acid and melamine. The as-prepared P,O-g-C3 N4 nanodots showed strong blue fluorescence and a relatively high QY of up to 90.2 %, which can be ascribed to intrinsic phosphorus/oxygen-containing groups, and surface-oxidation-related fluorescence enhancement. In addition, the P,O-g-C3 N4 nanodots were explored for cell imaging with excellent stability and biocompatibility, which suggest that they have great potential in biological applications. PMID:27249019
NASA Astrophysics Data System (ADS)
Beard, Matthew C.; Semonin, Octavi E.; Johnson, Justin C.; Marshall, Ashley; Zhang, Jianbing; Chernomordik, Boris D.
2016-03-01
PbS and PbSe quantum dots (QDs) are promising strong infrared emitters. We have developed several synthetic routes to producing PbS and PbSe QDs with a variety of sizes such that the bandgap can be continuously tuned from 2000 to 1000 nm. We provide a simple and accurate synthetic route to reproducibly produce PbS QDs with a narrow size-distribution and high chemical yield. The different synthetic routes lead to differences in their surface chemistry and to differences in their air stability and photoluminescence quantum yields (PLQY). To characterize the PLQY we directly measured the PLQY IR-26 (a standard IR emitting organic dye) at a range of concentrations as well as the PLQY of PbS and PbSe QDs for a range of sizes. We find that the PLQY of IR-26 has a weak concentration dependence due to reabsorption, with a PLQY of 0:048_0:002% for low concentrations, lower than previous reports by a full order of magnitude. We also find a dramatic size dependence for both PbS and PbSe QDs, with the smallest dots exhibiting a PLQY in excess of 60% while larger dots fall below 3%. A model, including nonradiative transition between electronic states and energy transfer to ligand vibrations, appears to explain this size dependence. These findings provide both a better characterization of photoluminescence for near infrared emitters. Halogen surface passivation provides both a larger PLQY (~ 30% improvement) as well as increased air stability.
Porcel, Rosa; Redondo-Gómez, Susana; Mateos-Naranjo, Enrique; Aroca, Ricardo; Garcia, Rosalva; Ruiz-Lozano, Juan Manuel
2015-08-01
Rice is the most important food crop in the world and is a primary source of food for more than half of the world population. However, salinity is considered the most common abiotic stress reducing its productivity. Soil salinity inhibits photosynthetic processes, which can induce an over-reduction of the reaction centres in photosystem II (PSII), damaging the photosynthetic machinery. The arbuscular mycorrhizal (AM) symbiosis may improve host plant tolerance to salinity, but it is not clear how the AM symbiosis affects the plant photosynthetic capacity, particularly the efficiency of PSII. This study aimed at determining the influence of the AM symbiosis on the performance of PSII in rice plants subjected to salinity. Photosynthetic activity, plant gas-exchange parameters, accumulation of photosynthetic pigments and rubisco activity and gene expression were also measured in order to analyse comprehensively the response of the photosynthetic processes to AM symbiosis and salinity. Results showed that the AM symbiosis enhanced the actual quantum yield of PSII photochemistry and reduced the quantum yield of non-photochemical quenching in rice plants subjected to salinity. AM rice plants maintained higher net photosynthetic rate, stomatal conductance and transpiration rate than nonAM plants. Thus, we propose that AM rice plants had a higher photochemical efficiency for CO2 fixation and solar energy utilization and this increases plant salt tolerance by preventing the injury to the photosystems reaction centres and by allowing a better utilization of light energy in photochemical processes. All these processes translated into higher photosynthetic and rubisco activities in AM rice plants and improved plant biomass production under salinity.
Porcel, Rosa; Redondo-Gómez, Susana; Mateos-Naranjo, Enrique; Aroca, Ricardo; Garcia, Rosalva; Ruiz-Lozano, Juan Manuel
2015-08-01
Rice is the most important food crop in the world and is a primary source of food for more than half of the world population. However, salinity is considered the most common abiotic stress reducing its productivity. Soil salinity inhibits photosynthetic processes, which can induce an over-reduction of the reaction centres in photosystem II (PSII), damaging the photosynthetic machinery. The arbuscular mycorrhizal (AM) symbiosis may improve host plant tolerance to salinity, but it is not clear how the AM symbiosis affects the plant photosynthetic capacity, particularly the efficiency of PSII. This study aimed at determining the influence of the AM symbiosis on the performance of PSII in rice plants subjected to salinity. Photosynthetic activity, plant gas-exchange parameters, accumulation of photosynthetic pigments and rubisco activity and gene expression were also measured in order to analyse comprehensively the response of the photosynthetic processes to AM symbiosis and salinity. Results showed that the AM symbiosis enhanced the actual quantum yield of PSII photochemistry and reduced the quantum yield of non-photochemical quenching in rice plants subjected to salinity. AM rice plants maintained higher net photosynthetic rate, stomatal conductance and transpiration rate than nonAM plants. Thus, we propose that AM rice plants had a higher photochemical efficiency for CO2 fixation and solar energy utilization and this increases plant salt tolerance by preventing the injury to the photosystems reaction centres and by allowing a better utilization of light energy in photochemical processes. All these processes translated into higher photosynthetic and rubisco activities in AM rice plants and improved plant biomass production under salinity. PMID:26291919
NASA Astrophysics Data System (ADS)
Gorrotxategi-Carbajo, P.; Fasci, E.; Ventrillard, I.; Carras, M.; Maisons, G.; Romanini, D.
2013-03-01
We report on the first application of Optical Feedback-Cavity Enhanced Absorption Spectroscopy to formaldehyde trace gas analysis at mid-infrared wavelengths. A continuous-wave room-temperature, distributed-feedback quantum cascade laser emitting around 1,769 cm-1 has been successfully coupled to an optical cavity with finesse 10,000 in an OF-CEAS spectrometer operating on the ν2 fundamental absorption band of formaldehyde. This compact setup (easily transportable) is able to monitor H2CO at ambient concentrations within few seconds, presently limited by the sample exchange rate. The minimum detectable absorption is 1.6 × 10-9 cm-1 for a single laser scan (100 ms, 100 data points), with a detectable H2CO mixing ratio of 60 pptv at 10 Hz. The corresponding detection limit at 1 Hz is 5 × 10-10 cm-1, with a normalized figure of merit of 5 × 10-11cm^{-1}/sqrtHz (100 data points recorded in each spectrum taken at 10 Hz rate). A preliminary Allan variance analysis shows white noise averaging down to a minimum detection limit of 5 pptv at an optimal integration time of 10 s, which is significantly better than previous results based on multi-pass or cavity-enhanced tunable QCL absorption spectroscopy.
Au/Ce0.72Zr0.18Pr0.1O2 nanodisperse catalyst for oxidation of carbon monoxide
NASA Astrophysics Data System (ADS)
Liberman, E. Yu.; Naumkin, A. V.; Mikhailichenko, A. I.; Batrakova, M. K.; Maslakov, K. I.; Revina, A. A.; Papkova, M. V.; Kon'kova, T. V.; Grunskii, V. N.; Gasparyan, M. D.; Karpovich, A. L.; Lizunova, A. A.
2016-01-01
The nanodisperse Au/Ce0.72Zr0.18Pr0.1O2 catalysts for low-temperature oxidation of carbon monoxide were synthesized. The compounds were identified by XRD, XPS, TEM, ISP-MS, and gas chromatography. The samples containing gold nanoparticles obtained by radiation chemical reduction in reverse micellar dispersion exhibited higher activity than the catalysts obtained by deposition-precipitation (DP) despite the higher content of the active component.
Hurley, J.K.; Sinai, N.; Linschitz, H.
1982-11-15
The extinction coefficient epsilon/sub T/, of triplet benzophenone in benzene has been directly determined by absolute measurements of absorbed energy and triplet absorbance, ..delta..D/sup 0//sub T/, under demonstrably linear conditions where incident excitation energy, E/sub 0/, and ground state absorbance, A/sub 0/, are both extrapolated to zero. The result, 7220 +- 320 M/sup -1/ cm/sup -1/ at 530 nm, validates and corrects many measurements of triplet and radical extinctions and yields, using the energy-transfer method. As E/sub 0/ and A/sub 0/ both decrease, ..delta..D/sup 0//sub T/ becomes proportional to their product. In this situation, the ratio R = (1/A/sub 0/) (d..delta..D/sup 0//sub T//dE/sub 0/) = (epsilon/sub T/ /sup -/ epsilon/sub G/)phi/sub T/. Measurements of R, referred to benzophenone, give (epsilon/sub T/ - epsilon/sub G/)phi/sub T/ for any substance, without necessity for absolute energy calibration. Both absolute and relative laser flash measurements on zinc tetraphenyl porphyrin (epsilon/sub T/ - epsilon/sub G/ at 470 nm = 7.3 x 10/sup 4/ M/sup -1/ cm/sup -1/) give phi/sub T/ = 0.83 +- 0.04. 6 figures, 2 tables.
NASA Astrophysics Data System (ADS)
Duan, Hongyan; Jiang, Yang; Zhang, Yugang; Sun, Dapeng; Liu, Chao; Huang, Jian; Lan, Xinzheng; Zhou, Hongyang; Chen, Lei; Zhong, Honghai
2013-07-01
Composition-controllable ternary CdSexS1-x quantum dots (QDs) with multiple emission colors were obtained via a hot-injection-like method at a relatively low injection temperature (230 ° C) in octadecene. Then highly fluorescent CdSexS1-x/ZnS core/shell (CS) QDs were synthesized by a facile single-molecular precursor approach. The fluorescent quantum yield of the resulting green (λem = 523 nm), yellow (λem = 565 nm) and red (λem = 621 nm) emission of CS QDs in toluene reached up to 85%, 55% and 39%, respectively. Moreover, a QDs white light-emitting diode (QDs-WLED) was fabricated by hybridizing green-, yellow- and red-emitting CdSexS1-x/ZnS CS QDs/epoxy composites on a blue InGaN chip. The resulting four-band RYGB QDs-WLED showed good performance with CIE-1931 coordinates of (0.4137, 0.3955), an Ra of 81, and a Tc of 3360 K at 30 mA, which indicated the combination of multiple-color QDs with high fluorescence QYs in LEDs as a promising approach to obtain warm WLEDs with good color rendering.
Ouzounis, Theoharis; Razi Parjikolaei, Behnaz; Fretté, Xavier; Rosenqvist, Eva; Ottosen, Carl-Otto
2015-01-01
To evaluate the effect of blue light intensity and timing, two cultivars of lettuce [Lactuca sativa cv. “Batavia” (green) and cv. “Lollo Rossa” (red)] were grown in a greenhouse compartment in late winter under natural light and supplemental high pressure sodium (SON-T) lamps yielding 90 (±10) μmol m−2 s−1 for up to 20 h, but never between 17:00 and 21:00. The temperature in the greenhouse compartments was 22/11°C day/night, respectively. The five light-emitting diode (LED) light treatments were Control (no blue addition), 1B 06-08 (Blue light at 45 μmol m−2 s−1 from 06:00 to 08:00), 1B 21-08 (Blue light at 45 μmol m−2 s−1 from 21:00 to 08:00), 2B 17-19 (Blue at 80 μmol m−2 s−1 from 17:00 to 19:00), and 1B 17-19 (Blue at 45 μmol m−2 s−1 from 17:00 to 19:00). Total fresh and dry weight was not affected with additional blue light; however, plants treated with additional blue light were more compact. The stomatal conductance in the green lettuce cultivar was higher for all treatments with blue light compared to the Control. Photosynthetic yields measured with chlorophyll fluorescence showed different response between the cultivars; in red lettuce, the quantum yield of PSII decreased and the yield of non-photochemical quenching increased with increasing blue light, whereas in green lettuce no difference was observed. Quantification of secondary metabolites showed that all four treatments with additional blue light had higher amount of pigments, phenolic acids, and flavonoids compared to the Control. The effect was more prominent in red lettuce, highlighting that the results vary among treatments and compounds. Our results indicate that not only high light level triggers photoprotective heat dissipation in the plant, but also the specific spectral composition of the light itself at low intensities. However, these plant responses to light are cultivar dependent. PMID:25767473
Hennig, Carsten; Schmatz, Stefan
2005-06-15
The exothermic gas-phase bimolecular nucleophilic substitution (S{sub N}2) reaction Cl{sup -}+CH{sub 3}Br ({upsilon}{sub 1}{sup '},{upsilon}{sub 2}{sup '},{upsilon}{sub 3}{sup '}){yields}ClCH{sub 3} ({upsilon}{sub 1},{upsilon}{sub 2},{upsilon}{sub 3})+Br{sup -} and the corresponding endothermic reverse reaction have been studied by time-independent quantum scattering calculations in hyperspherical coordinates on a coupled-cluster potential-energy surface. The dimensionality-reduced model takes four degrees of freedom into account [Cl-C and C-Br stretching modes (quantum numbers {upsilon}{sub 3}{sup '} and {upsilon}{sub 3}); totally symmetric modes of the methyl group, i.e., C-H stretching ({upsilon}{sub 1}{sup '} and {upsilon}{sub 1}) and umbrella bending vibrations ({upsilon}{sub 2}{sup '} and {upsilon}{sub 2})]. Diagonalization of the Hamiltonian was performed employing the Lanczos algorithm with a variation of partial reorthogonalization. A narrow grid in the total energy was employed so that long-living resonance states could be resolved and extracted. While excitation of the reactant umbrella bending mode already leads to a considerable enhancement of the reaction probability, its combination with vibrational excitation of the broken C-Br bond, (0, 1, 1), results in a strong synergic effect that can be rationalized by the similarity with the classical transitional normal mode. Exciting the C-H stretch has a non-negligible effect on the reaction probability, while for larger translational energies this mode follows the expected spectatorlike behavior. Combination of C-Br stretch and symmetric C-H, (1,0,1), stretch does not show a cooperative effect. Contrary to the spectator mode concept, energy originally stored in the C-H stretching mode is by no means conserved, but almost completely released in other modes of the reaction products. Products are most likely formed in states with a high degree of excitation in the new C-Cl bond, while the internal modes of
Belnap, J.; Phillips, S.L.; Smith, S.D.
2007-01-01
Biological soil crusts are an integral part of dryland ecosystems. We monitored the cover of lichens and mosses, cyanobacterial biomass, concentrations of UV-protective pigments in both free-living and lichenized cyanobacteria, and quantum yield in the soil lichen species Collema in an undisturbed Mojave Desert shrubland. During our sampling time, the site received historically high and low levels of precipitation, whereas temperatures were close to normal. Lichen cover, dominated by Collema tenax and C. coccophorum, and moss cover, dominated by Syntrichia caninervis, responded to both increases and decreases in precipitation. This finding for Collema spp. at a hot Mojave Desert site is in contrast to a similar study conducted at a cool desert site on the Colorado Plateau in SE Utah, USA, where Collema spp. cover dropped in response to elevated temperatures, but did not respond to changes in rainfall. The concentrations of UV-protective pigments in free-living cyanobacteria at the Mojave Desert site were also strongly and positively related to rainfall received between sampling times (R2 values ranged from 0.78 to 0.99). However, pigment levels in the lichenized cyanobacteria showed little correlation with rainfall. Quantum yield in Collema spp. was closely correlated with rainfall. Climate models in this region predict a 3.5-4.0 ??C rise in temperature and a 15-20% decline in winter precipitation by 2099. Based on our data, this rise in temperature is unlikely to have a strong effect on the dominant species of the soil crusts. However, the predicted drop in precipitation will likely lead to a decrease in soil lichen and moss cover, and high stress or mortality in soil cyanobacteria as levels of UV-protective pigments decline. In addition, surface-disturbing activities (e.g., recreation, military activities, fire) are rapidly increasing in the Mojave Desert, and these disturbances quickly remove soil lichens and mosses. These stresses combined are likely to lead to
Tsai, Chia Nung; Mazumder, Shivnath; Zhang, Xiu Zhu; Schlegel, H Bernhard; Chen, Yuan Jang; Endicott, John F
2016-08-01
Metal to ligand charge-transfer (MLCT) excited state emission quantum yields, ϕem, are reported in 77 K glasses for a series of pentaammine and tetraammine ruthenium(II) complexes with monodentate aromatic acceptor ligands (Ru-MDA) such as pyridine and pyrazine. These quantum yields are only about 0.2-1% of those found for their Ru-bpy (bpy = 2,2'-bipyridine) analogs in similar excited state energy ranges (hνem). The excited state energy dependencies of the emission intensity are characterized by mean radiative decay rate constants, kRAD, resolved from ϕem/τobs = kRAD (τobs = the observed emission decay lifetime; τobs(-1) = kRAD + kNRD; kNRD = nonradiative decay rate constant). Except for the Ru-pz chromophores in alcohol glasses, the values of kNRD for the Ru-MDA chromophores are slightly smaller, and their dependences on excited state energies are very similar to those of related Ru-bpy chromophores. In principle, one expects kRAD to be proportional to the product of (hνem)(3) and the square of the transition dipole moment (Me,g).(2) However, from experimental studies of Ru-bpy chromophores, an additional hνem dependence has been found that originates in an intensity stealing from a higher energy excited state with a much larger value of Me,g. This additional hνem dependence is not present in the kRAD energy dependence for Ru-MDA chromophores in the same energy regime. Intensity stealing in the phosphorescence of these complexes is necessary since the triplet-to-singlet transition is only allowed through spin-orbit coupling and since the density functional theory modeling implicates configurational mixing between states in the triplet spin manifold; this is treated by setting Me,g equal to the product of a mixing coefficient and the difference between the molecular dipole moments of the states involved, which implicates an experimental first order dependence of kRAD on hνem. The failure to observe intensity stealing for the Ru-MDA complexes suggests
Tsai, Chia Nung; Mazumder, Shivnath; Zhang, Xiu Zhu; Schlegel, H Bernhard; Chen, Yuan Jang; Endicott, John F
2016-08-01
Metal to ligand charge-transfer (MLCT) excited state emission quantum yields, ϕem, are reported in 77 K glasses for a series of pentaammine and tetraammine ruthenium(II) complexes with monodentate aromatic acceptor ligands (Ru-MDA) such as pyridine and pyrazine. These quantum yields are only about 0.2-1% of those found for their Ru-bpy (bpy = 2,2'-bipyridine) analogs in similar excited state energy ranges (hνem). The excited state energy dependencies of the emission intensity are characterized by mean radiative decay rate constants, kRAD, resolved from ϕem/τobs = kRAD (τobs = the observed emission decay lifetime; τobs(-1) = kRAD + kNRD; kNRD = nonradiative decay rate constant). Except for the Ru-pz chromophores in alcohol glasses, the values of kNRD for the Ru-MDA chromophores are slightly smaller, and their dependences on excited state energies are very similar to those of related Ru-bpy chromophores. In principle, one expects kRAD to be proportional to the product of (hνem)(3) and the square of the transition dipole moment (Me,g).(2) However, from experimental studies of Ru-bpy chromophores, an additional hνem dependence has been found that originates in an intensity stealing from a higher energy excited state with a much larger value of Me,g. This additional hνem dependence is not present in the kRAD energy dependence for Ru-MDA chromophores in the same energy regime. Intensity stealing in the phosphorescence of these complexes is necessary since the triplet-to-singlet transition is only allowed through spin-orbit coupling and since the density functional theory modeling implicates configurational mixing between states in the triplet spin manifold; this is treated by setting Me,g equal to the product of a mixing coefficient and the difference between the molecular dipole moments of the states involved, which implicates an experimental first order dependence of kRAD on hνem. The failure to observe intensity stealing for the Ru-MDA complexes suggests
Ananyev, Gennady; Gates, Colin; Dismukes, G Charles
2016-09-01
We have measured flash-induced oxygen quantum yields (O2-QYs) and primary charge separation (Chl variable fluorescence yield, Fv/Fm) in vivo among phylogenetically diverse microalgae and cyanobacteria. Higher O2-QYs can be attained in cells by releasing constraints on charge transfer at the Photosystem II (PSII) acceptor side by adding membrane-permeable benzoquinone (BQ) derivatives that oxidize plastosemiquinone QB(-) and QBH2. This method allows uncoupling PSII turnover from its natural regulation in living cells, without artifacts of isolating PSII complexes. This approach reveals different extents of regulation across species, controlled at the QB(-) acceptor site. Arthrospira maxima is confirmed as the most efficient PSII-WOC (water oxidizing complex) and exhibits the least regulation of flux. Thermosynechococcus elongatus exhibits an O2-QY of 30%, suggesting strong downregulation. WOC cycle simulations with the most accurate model (VZAD) show that a light-driven backward transition (net addition of an electron to the WOC, distinct from recombination) occurs in up to 25% of native PSIIs in the S2 and S3 states, while adding BQ prevents backward transitions and increases the lifetime of S2 and S3 by 10-fold. Backward transitions occur in PSIIs that have plastosemiquinone radicals in the QB site and are postulated to be physiologically regulated pathways for storing light energy as proton gradient through direct PSII-cyclic electron flow (PSII-CEF). PSII-CEF is independent of classical PSI/cyt-b6f-CEF and provides an alternative proton translocation pathway for energy conversion. PSII-CEF enables variable fluxes between linear and cyclic electron pathways, thus accommodating species-dependent needs for redox and ion-gradient energy sources powered by a single photosystem.
Ananyev, Gennady; Gates, Colin; Dismukes, G Charles
2016-09-01
We have measured flash-induced oxygen quantum yields (O2-QYs) and primary charge separation (Chl variable fluorescence yield, Fv/Fm) in vivo among phylogenetically diverse microalgae and cyanobacteria. Higher O2-QYs can be attained in cells by releasing constraints on charge transfer at the Photosystem II (PSII) acceptor side by adding membrane-permeable benzoquinone (BQ) derivatives that oxidize plastosemiquinone QB(-) and QBH2. This method allows uncoupling PSII turnover from its natural regulation in living cells, without artifacts of isolating PSII complexes. This approach reveals different extents of regulation across species, controlled at the QB(-) acceptor site. Arthrospira maxima is confirmed as the most efficient PSII-WOC (water oxidizing complex) and exhibits the least regulation of flux. Thermosynechococcus elongatus exhibits an O2-QY of 30%, suggesting strong downregulation. WOC cycle simulations with the most accurate model (VZAD) show that a light-driven backward transition (net addition of an electron to the WOC, distinct from recombination) occurs in up to 25% of native PSIIs in the S2 and S3 states, while adding BQ prevents backward transitions and increases the lifetime of S2 and S3 by 10-fold. Backward transitions occur in PSIIs that have plastosemiquinone radicals in the QB site and are postulated to be physiologically regulated pathways for storing light energy as proton gradient through direct PSII-cyclic electron flow (PSII-CEF). PSII-CEF is independent of classical PSI/cyt-b6f-CEF and provides an alternative proton translocation pathway for energy conversion. PSII-CEF enables variable fluxes between linear and cyclic electron pathways, thus accommodating species-dependent needs for redox and ion-gradient energy sources powered by a single photosystem. PMID:27117512
Zhang, Yongqiang; Liu, Xingyuan; Fan, Yi; Guo, Xiaoyang; Zhou, Lei; Lv, Ying; Lin, Jie
2016-08-18
A one-step microwave synthesis of N-doped hydroxyl-functionalized carbon dots (CDs) with ultra-high fluorescence quantum yields (QYs) of 99% is reported. These ultra-high QY CDs were synthesized using citric acid and amino compound-containing hydroxyls like ethanolamine and tris(hydroxylmethyl)aminomethane. Amino and carboxyl moieties can form amides through dehydration condensation reactions, and these amides act as bridges between carboxyl and hydroxyl groups, and modify hydroxyl groups on the surface of the CDs. The entire reaction can be carried out within 5 min. When the molar ratio of reactants is 1 : 1, the hydroxyl and graphitic nitrogen content is the highest, and the synergy leads to a high ratio between the radiative transition rate and nonradiative transition rate as well as a high QY. The developed pathway to N-doped hydroxyl-functionalized CDs can provide unambiguous and remarkable insights into the design of highly luminescent functionalized carbon dots, and expedite the applications of CDs. PMID:27500530
NASA Astrophysics Data System (ADS)
Jiang, Z. C.; Lin, T. N.; Lin, H. T.; Talite, M. J.; Tzeng, T. T.; Hsu, C. L.; Chiu, K. P.; Lin, C. A. J.; Shen, J. L.; Yuan, C. T.
2016-01-01
Solution-processed, non-toxic carbon dots (CDs) have attracted much attention due to their unique photoluminescence (PL) properties. They are promising emissive layers for flexible light-emitting devices. To this end, the CDs in pristine aqueous solutions need to be transferred to form solid-state thin films without sacrificing their original PL characteristics. Unfortunately, solid-state PL quenching induced by extra non-radiative (NR) energy transfer among CDs would significantly hinder their practical applications in optoelectronics. Here, a facile, low-cost and effective method has been utilized to fabricate high-performance CD/polymer light-emitting flexible films with submicron-structured patterns. The patterned polymers can serve as a solid matrix to disperse and passivate CDs, thus achieving high internal quantum yields of 61%. In addition, they can act as an out-coupler to mitigate the waveguide-mode losses, approximately doubling the external light-extraction efficiency. Such CD/polymer composites also exhibit good photo-stability, and thus can be used as eco-friendly, low-cost phosphors for solid-state lighting.
Yang, Renqiang; Garcia, Andres; Korystov, Dmitry; Mikhailovsky, Alexander; Bazan, Guillermo C; Nguyen, Thuc-Quyen
2006-12-27
Simple procedures are provided for exchanging charge-compensating ions in conjugated polyelectrolytes by progressive dilution of the original species and for determining the degree of ion exchange by using X-ray photoelectron spectroscopy. By using these methods, the bromide ions in poly[(9,9-bis(6'-N,N,N-trimethylammoniumbromide)hexyl)fluorene-co-alt-4,7-(2,1,3-benzothiadiazole)]were exchanged with BF4-, CF3SO3-, PF6-, BPh4-, and B(3,5-(CF3)2C6H3)4- (BArF4-). Absorption, photoluminescence (PL), and PL quantum yields (Phi) were measured in different solvents and in solid films cast from methanol. Examination of the resulting trends, together with the spectral bandshapes in different solvents, suggests that increasing the counteranion (CA) size decreases interchain contacts and aggregation and leads to a substantial increase of Phi in the bulk. Size analysis of polymers containing Br- and BArF4- in water by dynamic light scattering techniques indicates suppression of aggregation by BArF4-. Nanoscale current-voltage measurements of films using conducting atomic force microscopy show that hole mobilities and, more significantly, charge injection barriers are CA dependent. These results show that it is possible to significantly modify the optoelectronic properties of conjugated polyelectrolytes by choosing different counterions. A parent conjugated backbone can thus be fine-tuned for specific applications. PMID:17177402
Jiang, Z. C.; Lin, T. N.; Lin, H. T.; Talite, M. J.; Tzeng, T. T.; Hsu, C. L.; Chiu, K. P.; Lin, C. A. J.; Shen, J. L.; Yuan, C. T.
2016-01-01
Solution-processed, non-toxic carbon dots (CDs) have attracted much attention due to their unique photoluminescence (PL) properties. They are promising emissive layers for flexible light-emitting devices. To this end, the CDs in pristine aqueous solutions need to be transferred to form solid-state thin films without sacrificing their original PL characteristics. Unfortunately, solid-state PL quenching induced by extra non-radiative (NR) energy transfer among CDs would significantly hinder their practical applications in optoelectronics. Here, a facile, low-cost and effective method has been utilized to fabricate high-performance CD/polymer light-emitting flexible films with submicron-structured patterns. The patterned polymers can serve as a solid matrix to disperse and passivate CDs, thus achieving high internal quantum yields of 61%. In addition, they can act as an out-coupler to mitigate the waveguide-mode losses, approximately doubling the external light-extraction efficiency. Such CD/polymer composites also exhibit good photo-stability, and thus can be used as eco-friendly, low-cost phosphors for solid-state lighting. PMID:26822337
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.
NASA Astrophysics Data System (ADS)
Yaiphaba, N.; Ningthoujam, R. S.; Singh, N. Shanta; Vatsa, R. K.; Singh, N. Rajmuhon; Dhara, Sangita; Misra, N. L.; Tewari, R.
2010-02-01
Crystalline nanoneedles of Eu3+-doped GdPO4 and Eu3+-doped GdPO4 covered with GdPO4 shell (core shell) have been prepared at relatively low temperature of 150 °C in ethylene glycol medium. From luminescence study, asymmetric ratio of Eu3+ emission at 612 nm (electric dipole transition) to 592 nm (magnetic dipole transition) is found to be less than one. Maximum luminescence was observed from the nanoparticles with Eu3+ concentration of 5 at. %. For a fixed concentration of Eu3+ doping, there is an improvement in emission intensity for core-shell nanoparticles compared to that for core. This has been attributed to effective removal of surface inhomogeneities around Eu3+ ions present on the surface of core as well as the passivation of inevitable surface states, defects or capping ligand (ethylene glycol) of core nanoparticles by bonding to the shell. Lifetime for D50 level of Eu3+ was found to increase three times for core-shell nanoparticles compared to that for core confirming the more Eu3+ ions with symmetry environment in core shell. For 5 at. % Eu3+-doped GdPO4, quantum yield of 19% is obtained. These nanoparticles are redispersible in water, ethanol, or chloroform and thus will be useful in biological labeling. The dispersed particles are incorporated in polymer-based films that will be useful in display devices.
Jiang, Z C; Lin, T N; Lin, H T; Talite, M J; Tzeng, T T; Hsu, C L; Chiu, K P; Lin, C A J; Shen, J L; Yuan, C T
2016-01-01
Solution-processed, non-toxic carbon dots (CDs) have attracted much attention due to their unique photoluminescence (PL) properties. They are promising emissive layers for flexible light-emitting devices. To this end, the CDs in pristine aqueous solutions need to be transferred to form solid-state thin films without sacrificing their original PL characteristics. Unfortunately, solid-state PL quenching induced by extra non-radiative (NR) energy transfer among CDs would significantly hinder their practical applications in optoelectronics. Here, a facile, low-cost and effective method has been utilized to fabricate high-performance CD/polymer light-emitting flexible films with submicron-structured patterns. The patterned polymers can serve as a solid matrix to disperse and passivate CDs, thus achieving high internal quantum yields of 61%. In addition, they can act as an out-coupler to mitigate the waveguide-mode losses, approximately doubling the external light-extraction efficiency. Such CD/polymer composites also exhibit good photo-stability, and thus can be used as eco-friendly, low-cost phosphors for solid-state lighting. PMID:26822337
NASA Astrophysics Data System (ADS)
Beeks, Ivan; Kumar, Ajith G.; Sardar, Dhiraj K.
2015-03-01
A series of broadly color tunable upconversion phosphors were synthesized from M2O2S (M=Y,Gd,La) using a flux fusion method. We investigate their upconversion properties as a function of the dopant concentrations and excitation power density. The phosphor compositions were determined for their upconversion characteristics under 800, 980 and 1550 nm excitations. By measuring the quantum yield and luminous brightness, we investigate their potential applications in biomedical imaging as well as NIR display applications. Results are compared with the well-known upconversion phosphor NaYF4:Yb/Er/Ho/Tm and found that the M2O2S phosphor systems are more efficient compared to NaYF4. By adopting various synthesis protocols, we were able to examine M2O2S in the size range of 10 nm to 10 μm. This research is supported by the National Science Foundation Partnerships for Research and Education in Materials (NSF-PREM) Grant N0-DMR-0934218.
NASA Astrophysics Data System (ADS)
Jain, Akhil; Hirata, G. A.; Farías, M. H.; Castillón, F. F.
2016-02-01
We report the surface modification of nanocrystalline Gd2O3:Eu3+ phosphor by (3-Aminopropyl)trimethoxysilane (APTMS). The nanoparticles were first coated with silica using the Stöber process, and then annealed at 650 °C for 2 h. Afterwards, APTMS was functionalized onto the silica layer to obtain Gd2O3:Eu3+ nanoparticles bearing amine groups on the surface. The effect of silica coating, and the subsequent annealing process on the crystallization of the nanophosphor were analyzed by x-ray diffraction (XRD). High-resolution transmission electron microscopy (HR-TEM) confirmed the presence of a silica layer of ∼45 nm thickness. X-ray photoelectron (XPS) and Fourier transform infrared (FTIR) spectroscopy confirmed the presence of silica and the amine groups. Photoluminescence (PL) analysis demonstrated an increased emission after functionalization of nanoparticles. Absolute quantum yield (QY) measurements revealed an 18% enhancement in QY in functionalized nanoparticles compared with unmodified nanoparticles, which is of great importance for their biomedical applications.
Lasitha, P; Prasad, Edamana
2016-07-18
Perylene diimide (PDI) derivatives exhibit a high propensity for aggregation, which causes the aggregation-induced quenching of emission from the system. Host-guest chemistry is one of the best-known methods for preventing aggregation through the encapsulation of guest molecules. Herein we report the use of 18-crown-6 (18-C-6) as a host system to disaggregate suitably substituted PDI derivatives in methanol. 18-C-6 formed complexes with amino-substituted PDIs in methanol, which led to disaggregation and enhanced emission from the systems. Furthermore, the embedding of the PDI⋅18-C-6 complexes in poly(vinyl alcohol) (PVA) films generated remarkably high emission quantum yields (60-70 %) from the PDI derivatives. More importantly, the host-guest systems were tested for their ability to conduct electricity in PVA films. The electrical conductivities of the self-assembled systems in PVA were measured by electrochemical impedance spectroscopy (EIS) and the highest conductivity observed was 2.42×10(-5) S cm(-1) .
Jain, Akhil; Hirata, G A; Farías, M H; Castillón, F F
2016-02-12
We report the surface modification of nanocrystalline Gd2O3:Eu(3+) phosphor by (3-Aminopropyl)trimethoxysilane (APTMS). The nanoparticles were first coated with silica using the Stöber process, and then annealed at 650 °C for 2 h. Afterwards, APTMS was functionalized onto the silica layer to obtain Gd2O3:Eu(3+) nanoparticles bearing amine groups on the surface. The effect of silica coating, and the subsequent annealing process on the crystallization of the nanophosphor were analyzed by x-ray diffraction (XRD). High-resolution transmission electron microscopy (HR-TEM) confirmed the presence of a silica layer of ∼45 nm thickness. X-ray photoelectron (XPS) and Fourier transform infrared (FTIR) spectroscopy confirmed the presence of silica and the amine groups. Photoluminescence (PL) analysis demonstrated an increased emission after functionalization of nanoparticles. Absolute quantum yield (QY) measurements revealed an 18% enhancement in QY in functionalized nanoparticles compared with unmodified nanoparticles, which is of great importance for their biomedical applications. PMID:26684579
Adiabatically implementing quantum gates
Sun, Jie; Lu, Songfeng Liu, Fang
2014-06-14
We show that, through the approach of quantum adiabatic evolution, all of the usual quantum gates can be implemented efficiently, yielding running time of order O(1). This may be considered as a useful alternative to the standard quantum computing approach, which involves quantum gates transforming quantum states during the computing process.
Li, Zong-Yu; Wu, Yun-Tse; Tseng, Wei-Lung
2015-10-28
The use of DNA as a template has been demonstrated as an effective method for synthesizing different-sized silver nanoclusters. Although DNA-templated silver nanoclusters show outstanding performance as fluorescent probes for chemical sensing and cellular imaging, the synthesis of DNA-stabilized gold nanoclusters (AuNCs) with high fluorescence intensity remains a challenge. Here a facile, reproducible, scalable, NaBH4-free, UV-light-assisted method was developed to prepare AuNCs using repeats of 30 adenosine nucleotides (A30). The maximal fluorescence of A30-stabilized AuNCs appeared at 475 nm with moderate quantum yield, two fluorescence lifetimes, and a small amount of Au(+) on the surface of the Au core. Results of size-exclusion chromatography revealed that A30-stabilized AuNCs were more compact than A30. A series of control experiments showed that UV light played a dual role in the reduction of gold-ion precursors and the decomposition of citrate ions. A30 also acted as a stabilizer to prevent the aggregation of AuNCs. In addition, single-stranded DNA (ssDNA) consisting of an AuNC-nucleation sequence and a hybridization sequence was utilized to develop a AuNC-based ratiometric fluorescent probe in the presence of the double-strand-chelating dye SYBR Green I (SG). Under conditions of single-wavelength excitation, the combination of AuNC/SG-bearing ssDNA and perfectly matched DNA emitted fluorescence at 475 and 525 nm, respectively. The formed AuNC/SG-bearing ssDNA enabled the sensitive, selective, and ratiometric detection of specific nucleic acid targets. Finally, the AuNC-based ratiometric probes were successfully applied to determine specific nucleic acid targets in human serum.
Clement, Sandhya; Deng, Wei; Camilleri, Elizabeth; Wilson, Brian C; Goldys, Ewa M
2016-01-01
Singlet oxygen is a primary cytotoxic agent in photodynamic therapy. We show that CeF3 nanoparticles, pure as well as conjugated through electrostatic interaction with the photosensitizer verteporfin, are able to generate singlet oxygen as a result of UV light and 8 keV X-ray irradiation. The X-ray stimulated singlet oxygen quantum yield was determined to be 0.79 ± 0.05 for the conjugate with 31 verteporfin molecules per CeF3 nanoparticle, the highest conjugation level used. From this result we estimate the singlet oxygen dose generated from CeF3-verteporfin conjugates for a therapeutic dose of 60 Gy of ionizing radiation at energies of 6 MeV and 30 keV to be (1.2 ± 0.7) × 10(8) and (2.0 ± 0.1) × 10(9) singlet oxygen molecules per cell, respectively. These are comparable with cytotoxic doses of 5 × 10(7)-2 × 10(9) singlet oxygen molecules per cell reported in the literature for photodynamic therapy using light activation. We confirmed that the CeF3-VP conjugates enhanced cell killing with 6 MeV radiation. This work confirms the feasibility of using X- or γ- ray activated nanoparticle-photosensitizer conjugates, either to supplement the radiation treatment of cancer, or as an independent treatment modality.
NASA Astrophysics Data System (ADS)
Clement, Sandhya; Deng, Wei; Camilleri, Elizabeth; Wilson, Brian C.; Goldys, Ewa M.
2016-01-01
Singlet oxygen is a primary cytotoxic agent in photodynamic therapy. We show that CeF3 nanoparticles, pure as well as conjugated through electrostatic interaction with the photosensitizer verteporfin, are able to generate singlet oxygen as a result of UV light and 8 keV X-ray irradiation. The X-ray stimulated singlet oxygen quantum yield was determined to be 0.79 ± 0.05 for the conjugate with 31 verteporfin molecules per CeF3 nanoparticle, the highest conjugation level used. From this result we estimate the singlet oxygen dose generated from CeF3-verteporfin conjugates for a therapeutic dose of 60 Gy of ionizing radiation at energies of 6 MeV and 30 keV to be (1.2 ± 0.7) × 108 and (2.0 ± 0.1) × 109 singlet oxygen molecules per cell, respectively. These are comparable with cytotoxic doses of 5 × 107-2 × 109 singlet oxygen molecules per cell reported in the literature for photodynamic therapy using light activation. We confirmed that the CeF3-VP conjugates enhanced cell killing with 6 MeV radiation. This work confirms the feasibility of using X- or γ- ray activated nanoparticle-photosensitizer conjugates, either to supplement the radiation treatment of cancer, or as an independent treatment modality.
Clement, Sandhya; Deng, Wei; Camilleri, Elizabeth; Wilson, Brian C.; Goldys, Ewa M.
2016-01-01
Singlet oxygen is a primary cytotoxic agent in photodynamic therapy. We show that CeF3 nanoparticles, pure as well as conjugated through electrostatic interaction with the photosensitizer verteporfin, are able to generate singlet oxygen as a result of UV light and 8 keV X-ray irradiation. The X-ray stimulated singlet oxygen quantum yield was determined to be 0.79 ± 0.05 for the conjugate with 31 verteporfin molecules per CeF3 nanoparticle, the highest conjugation level used. From this result we estimate the singlet oxygen dose generated from CeF3-verteporfin conjugates for a therapeutic dose of 60 Gy of ionizing radiation at energies of 6 MeV and 30 keV to be (1.2 ± 0.7) × 108 and (2.0 ± 0.1) × 109 singlet oxygen molecules per cell, respectively. These are comparable with cytotoxic doses of 5 × 107–2 × 109 singlet oxygen molecules per cell reported in the literature for photodynamic therapy using light activation. We confirmed that the CeF3-VP conjugates enhanced cell killing with 6 MeV radiation. This work confirms the feasibility of using X- or γ- ray activated nanoparticle-photosensitizer conjugates, either to supplement the radiation treatment of cancer, or as an independent treatment modality. PMID:26818819
Hanf, A; Volpp, H-R; Sharma, P; Mittal, J P; Vatsa, R K
2010-07-14
Using pulsed H-atom Lyman-alpha laser-induced fluorescence spectroscopy along with a photolytic calibration approach, absolute H-atom product quantum yields of phi(H-b13d) = (0.32+/-0.04) and phi(H-b12d) = (0.36+/-0.04) were measured under collision-free conditions for the 193 nm gas-phase laser flash photolysis of buta-1,3- and buta-1,2-diene at room temperature, which demonstrate that nascent H-atom formation is of comparable importance for both parent molecules. Comparison of the available energy fraction, f(T-b13d) = (0.22+/-0.03) and f(T-b12d) = (0.13+/-0.01), released as H+C(4)H(5) product translational energy with results of impulsive and statistical energy partitioning modeling calculations indicates that for both, buta-1,3- and buta-1,2-diene, H-atom formation is preceded by internal conversion to the respective electronic ground state (S(0)) potential energy surfaces. In addition, values of sigma(b-1,3-d-L alpha) = (3.5+/-0.2)x10(-17) cm(2) and sigma(b-1,2-d-L alpha) = (4.4+/-0.2)x10(-17) cm(2) for the previously unknown Lyman-alpha (121.6 nm) radiation photoabsorption cross sections of buta-1,3- and buta-1,2-diene in the gas-phase were determined.
Scharinger, Eva J.; Dietrich, Richard; Kleinsteuber, Ina; Märtlbauer, Erwin
2016-01-01
Cronobacter sakazakii is a foodborne pathogen associated with rare but often lethal infections in neonates. Powdered infant formula (PIF) represents the most frequent source of infection. Out of the identified serotypes (O1 to O7), O1, O2, and O3 are often isolated from clinical and PIF samples. Serotype-specific monoclonal antibodies (MAbs) suitable for application in enzyme immunoassays (EIAs) for the rapid detection of C. sakazakii have not yet been developed. In this study, we created specific MAbs with the ability to bind to C. sakazakii of serotypes O1, O2, and O3. Characterization by indirect EIAs, immunofluorescence, motility assays, and immunoblotting identified lipopolysaccharide (LPS) and exopolysaccharide (EPS) as the antigenic determinants of the MAbs. The established sandwich EIAs were highly sensitive and were able to detect between 2 × 103 and 9 × 106 CFU/ml. Inclusivity tests confirmed that 93% of serotype O1 strains, 100% of O2 strains, and 87% of O3 strains were detected at low cell counts. No cross-reactivity with >100 strains of Cronobacter spp. and other Enterobacteriaceae was observed, except for that with C. sakazakii serotype O3 and Cronobacter muytjensii serotype O1. Moreover, the sandwich EIAs detected C. sakazakii in PIF samples artificially contaminated with 1 to 10 bacterial cells per 10 g of sample after 15 h of preenrichment. The use of these serotype-specific MAbs not only allows the reliable detection of C. sakazakii strains but also enables simultaneous serotyping in a simple sandwich EIA method. PMID:26850303
Janka, Eshetu; Körner, Oliver; Rosenqvist, Eva; Ottosen, Carl-Otto
2015-05-01
Under a dynamic greenhouse climate control regime, temperature is adjusted to optimise plant physiological responses to prevailing irradiance levels; thus, both temperature and irradiance are used by the plant to maximise the rate of photosynthesis, assuming other factors are not limiting. The control regime may be optimised by monitoring plant responses, and may be promptly adjusted when plant performance is affected by extreme microclimatic conditions, such as high irradiance or temperature. To determine the stress indicators of plants based on their physiological responses, net photosynthesis (Pn) and four chlorophyll-a fluorescence parameters: maximum photochemical efficiency of PSII [Fv/Fm], electron transport rate [ETR], PSII operating efficiency [F'q/F'm], and non-photochemical quenching [NPQ] were assessed for potted chrysanthemum (Dendranthema grandiflora Tzvelev) 'Coral Charm' under different temperature (20, 24, 28, 32, 36 °C) and daily light integrals (DLI; 11, 20, 31, and 43 mol m(-2) created by a PAR of 171, 311, 485 and 667 μmol m(-2) s(-1) for 16 h). High irradiance (667 μmol m(-2) s(-1)) combined with high temperature (>32 °C) significantly (p < 0.05) decreased Fv/Fm. Under high irradiance, the maximum Pn and ETR were reached at 24 °C. Increased irradiance decreased the PSII operating efficiency and increased NPQ, while both high irradiance and temperature had a significant effect on the PSII operating efficiency at temperatures >28 °C. Under high irradiance and temperature, changes in the NPQ determined the PSII operating efficiency, with no major change in the fraction of open PSII centres (qL) (indicating a QA redox state). We conclude that 1) chrysanthemum plants cope with excess irradiance by non-radiative dissipation or a reversible stress response, with the effect on the Pn and quantum yield of PSII remaining low until the temperature reaches 28 °C and 2) the integration of online measurements to monitor photosynthesis and PSII
NASA Astrophysics Data System (ADS)
Lacroix, O.; Rahmouni, K.; Sirat, A.; Takenouti, H.; Deslouis, C.; Keddam, M.; Sala, B.
2014-12-01
Because of their high ionic conduction even at relatively low temperatures, proton conducting ceramics are one of the most promising electrolytes for fuel cell. In contrast to oxide-ion conductors, proton-conducting systems, especially in an electrolyser plant, could operate below 600 °C, critical temperature for mechanical and hot corrosion resistance of common stainless steels. Proton conduction in perovskite type ceramic was analysed under the water molecules insertion to maximize proton conduction. To this end, the SrZr0.9Ln0.1O2.95 electrolyte and its microstructure, particularly grain size was investigated. The insertion and release of water in the perovskite structure was followed by impedance spectroscopy and by using the so-called Brick Layer Model (BLM) to separate the bulk and grain boundary conductivities. It was found that the conductivity in both zones increases namely with steam pressure. It was also verified that the bulk conductivity is higher than that of grain boundaries. Consequently both the operating steam pressure and the grain size appear as the main parameters that can be tuned to enhance the proton conduction.
Apel, Klaus
2013-01-01
Chloroplast development depends on the synthesis and import of a large number of nuclear-encoded proteins. The synthesis of some of these proteins is affected by the functional state of the plastid via a process known as retrograde signaling. Retrograde plastid-to-nucleus signaling has been often characterized in seedlings of Arabidopsis thaliana exposed to norflurazon (NF), an inhibitor of carotenoid biosynthesis. Results of this work suggested that, throughout seedling development, a factor is released from the plastid to the cytoplasm that indicates a perturbation of plastid homeostasis and represses nuclear genes required for normal chloroplast development. The identity of this factor is still under debate. Reactive oxygen species (ROS) were among the candidates discussed as possible retrograde signals in NF-treated plants. In the present work, this proposed role of ROS has been analyzed. In seedlings grown from the very beginning in the presence of NF, ROS-dependent signaling was not detectable, whereas, in seedlings first exposed to NF after light-dependent chloroplast formation had been completed, enhanced ROS production occurred and, among others, 1O2-mediated and EXECUTER-dependent retrograde signaling was induced. Hence, depending on the developmental stage at which plants are exposed to NF, different retrograde signaling pathways may be activated, some of which are also active in non-treated plants under light stress. PMID:23376773
Morajkar, Pranay; Schoemaecker, Coralie; Fittschen, Christa; Bossolasco, Adriana
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{sub 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
Maruyama, N.; Honma, T.; Komatsu, T.
2009-02-15
Transparent crystallized glasses consisting of nonlinear optical Ba{sub 2}TiSi{sub 2}O{sub 8} nanocrystals (diameter: {approx}100 nm) are prepared through the crystallization of 40BaO-20TiO{sub 2}-40SiO{sub 2}-0.5Dy{sub 2}O{sub 3} glass (in the molar ratio), and photoluminescence quantum yields of Dy{sup 3+} ions in the visible region are evaluated directly by using a photoluminescence spectrometer with an integrating sphere. The incorporation of Dy{sup 3+} ions into Ba{sub 2}TiSi{sub 2}O{sub 8} nanocrystals is confirmed from the X-ray diffraction analyses. The total quantum yields of the emissions at the bands of {sup 4}F{sub 9/2}{yields}{sup 6}H{sub 15/2} (blue: 484 nm), {sup 4}F{sub 9/2}{yields}{sup 6}H{sub 13/2} (yellow: 575 nm), and {sup 4}F{sub 9/2}{yields}{sup 6}H{sub 11/2} (red: 669 nm) in the crystallized glasses are {approx}15%, being about four times larger compared with the precursor glass. It is found that the intensity of yellow (575 nm) emissions and the branching ratio of the yellow (575 nm)/blue (484 nm) intensity ratio increase largely due to the crystallization. It is suggested from Judd-Ofelt analyses that the site symmetry of Dy{sup 3+} ions in the crystallized glasses is largely distorted, giving a large increase in the yellow emissions. It is proposed that Dy{sup 3+} ions substitute Ba{sup 2+} sites in Ba{sub 2}TiSi{sub 2}O{sub 8} nanocrystals. - Grapical abstract: This figure shows the photoluminescence spectra of Dy{sup 3+} ions in the range of 450-700 nm obtained in the quantum field measurements for the precursor BTS and crystallized (at 770 and 790 deg. C, for 30 min) glasses. The wavelength of the excitation light was 352 nm. By incorporating into Ba{sub 2}TiSi{sub 2}O{sub 8} nanocrystals, the emission intensity of the yellow band of Dy{sup 3+} ions is largely enhanced. This would give an impact in the science and technology of photoluminescence materials.
Ihnken, Sven; Kromkamp, Jacco C; Beardall, John; Silsbe, Greg M
2014-03-01
Photosynthetic energy consumption and non-photosynthetic energy quenching processes are inherently linked. Both processes must be controlled by the cell to allow cell maintenance and growth, but also to avoid photodamage. We used the chlorophyte algae Dunaliella tertiolecta to investigate how the interactive regulation of photosynthetic and non-photosynthetic pathways varies along dissolved inorganic carbon (DIC) and photon flux gradients. Specifically, cells were transferred to DIC-deplete media to reach a CO₂ compensation before being re-supplied with DIC at various concentrations and different photon flux levels. Throughout these experiments we monitored and characterized the photophysiological responses using pulse amplitude modulated fluorescence, oxygen evolution, 77 K fluorescence emission spectra, and fast-repetition rate fluorometry. O₂ uptake was not significantly stimulated at DIC depletion, which suggests that O₂ production rates correspond to assimilatory photosynthesis. Fluorescence-based measures of relative electron transport rates (rETRs) over-estimated oxygen-based photosynthetic measures due to a strong state-transitional response that facilitated high effective quantum yields. Adoption of an alternative fluorescence-based rETR calculation that accounts for state-transitions resulted in improved linear oxygen versus rETR correlation. This study shows the extraordinary capacity of D. tertiolecta to maintain stable effective quantum yields by flexible regulation of state-transitions. Uncertainties about the control mechanisms of state-transitions are presented.
Huber, Alexandra; Behnke, Thomas; Würth, Christian; Jaeger, Christian; Resch-Genger, Ute
2012-04-17
The rational design of nano- and micrometer-sized particles with tailor-made optical properties for biological, diagnostic, and photonic applications requires tools to characterize the signal-relevant properties of these typically scattering bead suspensions. This includes methods for the preferably nondestructive quantification of the number of fluorophores per particle and the measurement of absolute fluorescence quantum yields and absorption coefficients of suspensions of fluorescent beads for material performance optimization and comparison. Here, as a first proof-of-concept, we present the first time determination of the number of dye molecules per bead using nondestructive quantitative ((19)F) NMR spectroscopy and 1000 nm-sized carboxylated polystyrene particles loaded with varying concentrations of the laser dye coumarin 153 containing a CF(3) group. Additionally, the signal-relevant optical properties of these dye-loaded particles were determined in aqueous suspension in comparison to the free dye in solvents of different polarity with a custom-built integrating sphere setup that enables spectrally resolved measurements of emission, transmission, and reflectance as well absolute fluorescence quantum yields. These measurements present an important step toward absolute brightness values and quantitative fluorescence analysis with particle systems that can be exploited, for example, for optical imaging techniques and different fluorescence assays as well as for the metrological traceability of fluorescence methods. PMID:22404690
Saeed, S.; Jong, E. M. L. D. de; Gregorkiewicz, T.
2015-02-14
We investigate the excitation dependence of the efficiency of the Si nanocrystals-mediated photoluminescence from Er{sup 3+} ions embedded in a SiO{sub 2} matrix. We show that the quantum yield of this emission increases in a step-like manner with excitation energy. The subsequent thresholds of this characteristic dependence are approximately given by the sum of the Si nanocrystals bandgap energy and multiples of 0.8 eV, corresponding to the energy of the first excited state of Er{sup 3+} ions. By comparing differently prepared materials, we explicitly demonstrate that the actual values of the threshold energies and the rate of the observed increase of the external quantum yield depend on sample characteristics—the size, the optical activity and the concentration of Si nanocrystals as well Er{sup 3+} ions to Si nanocrystals concentration ratio. In that way, detailed insights into the efficient excitation of Er{sup 3+} ions are obtained. In particular, the essential role of the hot-carrier-mediated Er excitation route is established, with a possible application perspective for highly efficient future-generation photovoltaics.
Byrdin, M; Rimke, I; Schlodder, E; Stehlik, D; Roelofs, T A
2000-01-01
Transfer and trapping of excitation energy in photosystem I (PS I) trimers isolated from Synechococcus elongatus have been studied by an approach combining fluorescence induction experiments with picosecond time-resolved fluorescence measurements, both at room temperature (RT) and at low temperature (5 K). Special attention was paid to the influence of the oxidation state of the primary electron donor P700. A fluorescence induction effect has been observed, showing a approximately 12% increase in fluorescence quantum yield upon P700 oxidation at RT, whereas at temperatures below 160 K oxidation of P700 leads to a decrease in fluorescence quantum yield ( approximately 50% at 5 K). The fluorescence quantum yield for open PS I (with P700 reduced) at 5 K is increased by approximately 20-fold and that for closed PS I (with P700 oxidized) is increased by approximately 10-fold, as compared to RT. Picosecond fluorescence decay kinetics at RT reveal a difference in lifetime of the main decay component: 34 +/- 1 ps for open PS I and 37 +/- 1 ps for closed PS I. At 5 K the fluorescence yield is mainly associated with long-lived components (lifetimes of 401 ps and 1.5 ns in closed PS I and of 377 ps, 1.3 ns, and 4.1 ns in samples containing approximately 50% open and 50% closed PS I). The spectra associated with energy transfer and the steady-state emission spectra suggest that the excitation energy is not completely thermally equilibrated over the core-antenna-RC complex before being trapped. Structure-based modeling indicates that the so-called red antenna pigments (A708 and A720, i.e., those with absorption maxima at 708 nm and 720 nm, respectively) play a decisive role in the observed fluorescence kinetics. The A720 are preferentially located at the periphery of the PS I core-antenna-RC complex; the A708 must essentially connect the A720 to the reaction center. The excited-state decay kinetics turn out to be neither purely trap limited nor purely transfer (to the trap
NASA Technical Reports Server (NTRS)
Nikzad, Shouleh; Hoenk, M. E.; Carver, A. G.; Jones, T. J.; Greer, F.; Hamden, E.; Goodsall, T.
2013-01-01
In this paper we discuss the high throughput end-to-end post fabrication processing of high performance delta-doped and superlattice-doped silicon imagers for UV, visible, and NIR applications. As an example, we present our results on far ultraviolet and ultraviolet quantum efficiency (QE) in a photon counting, detector array. We have improved the QE by nearly an order of magnitude over microchannel plates (MCPs) that are the state-of-the-art UV detectors for many NASA space missions as well as defense applications. These achievements are made possible by precision interface band engineering of Molecular Beam Epitaxy (MBE) and Atomic Layer Deposition (ALD).
Hong, Jiyun; Jeon, SuKyung; Kim, Janice J.; Devi, Diane; Chacon-Madrid, Kelly; Lee, Wynee; Koo, Seung Moh; Wildeman, Jurjen; Sfeir, Matthew Y.; Peteanu, Linda A.; Wen, Jin; Ma, Jing
2014-07-24
Oligomeric thiophenes are commonly-used components in organic electronics and solar cells. These molecules stack and/or aggregate readily under the processing conditions used to form thin films for these applications, significantly altering their optical and charge-transport properties. To determine how these effects depend on the substitution pattern of the thiophene main chains, nano-aggregates of three sexi-thiophene (6T) oligomers having different alkyl substitution patterns were formed using solvent poisoning techniques and studied using steady-state and time-resolved emission spectroscopy. The results indicate the substantial role played by the side-chain substituents in determining the emissive properties of these species. Both the measured spectral changes and their dependence on substitution are well modeled by combined quantum chemistry and molecular dynamics simulations. The simulations connect the side-chain-induced disorder, which determines the favorable chain packing configurations within the aggregates, with their measured electronic spectra.
Odinokov, A. V.; Basilevsky, M. V.; Petrov, N. Kh.
2011-10-14
This work explains the unordinary solvent effect which was observed in the photochemical decay kinetics for the cyanine dye thiacarbocyanine iodide (Cy{sup +}I{sup -}) in binary solvent mixtures toluene/dimethylsulfoxide. The interpretation is formulated in terms of the probability density F(R) describing the distribution of interionic distances R in the ion pair Cy{sup +}I{sup -} and depending on the solvent composition. The proper normalization of this distribution is expressed via the degree of association {alpha} for the ion pair in a given solvent mixture. The {alpha} values are, in turn, extracted by means of the mass action law from the ionic association constants computed in a separate publication. The detailed kinetic scheme includes the empirical parametrization of the R-dependent kinetic constants for different decay channels. The multiparameter fitting procedure represents, with the reasonable parameter values, the dependence of the observed quantum yields on the solvent composition.
Hu Mei; Liu Xinguo; Tan Ruishan; Li Hongzheng; Xu Wenwu
2013-05-07
A new global potential energy surface for the ground electronic state (1{sup 2}A Prime ) of the Ar+H{sub 2}{sup +}{yields}ArH{sup +}+H reaction has been constructed by multi-reference configuration interaction method with Davidson correction and a basis set of aug-cc-pVQZ. Using 6080 ab initio single-point energies of all the regions for the dynamics, a many-body expansion function form has been used to fit these points. The quantum reactive scattering dynamics calculations taking into account the Coriolis coupling (CC) were carried out on the new potential energy surface over a range of collision energies (0.03-1.0 eV). The reaction probabilities and integral cross sections for the title reaction were calculated. The significance of including the CC quantum scattering calculation has been revealed by the comparison between the CC and the centrifugal sudden approximation calculation. The calculated cross section is in agreement with the experimental result at collision energy 1.0 eV.
Angermund, H.; Bandyopadhyay, A.K.; Grevels, F.; Mark, F. )
1989-06-21
Multiple photosubstitution of CO groups in pentacarbonyliron by an olefin has been investigated by using (E)-cyclooctene as a model olefin exhibiting exceptional coordination properties. The quantum yields {Phi}{sub 1} and {Phi}{sub 2} for sequential conversion of Fe(CO){sub 5} into ({eta}{sup 2}-(E)-C{sub 8}H{sub 14})Fe(CO){sub 4} (1) and ({eta}{sup 2}-(E)-C{sub 8}H{sub 14}){sub 2}Fe(CO){sub 3} (2), respectively, when evaluated using the appropriate formalism for internal light filter corrections (presented in detail in the Appendix), are found to be constant up to high conversion: {Phi}{sub 1} = 0.80 at 302 nm and 0.77 at 254 nm, {Phi}{sub 2} = 0.59 at 302 nm and 0.82 at 254 nm. The wavelength dependence of {Phi}{sub 2} is interpreted in terms of 2 different ligand field excited states of 1, providing for varying CO vs olefin photodetachment. The overall quantum yield for the generation of 2 from Fe(CO){sub 5} (ca. 0.20 at 60% conversion of pentacarbonyliron) is discussed in the context of carbonyliron photocatalyzed olefin isomerization, which is known to involve (labile) ({eta}{sup 2}-olefin){sub 2}Fe(CO){sub 3} as the active catalyst. The synthesis of ({eta}{sup 2}-(E)-C{sub 8}H{sub 14}){sub 3}Fe(CO){sub 2} (3), which is the first isolated representative of this type of complex, is achieved by irradiation of 2 in the presence of excess (E)-cyclooctene, whereby liberated CO is required to be rigorously removed by an inert-gas stream.
Hong, Jiyun; Jeon, SuKyung; Kim, Janice J.; Devi, Diane; Chacon-Madrid, Kelly; Lee, Wynee; Koo, Seung Moh; Wildeman, Jurjen; Sfeir, Matthew Y.; Peteanu, Linda A.; et al
2014-07-24
Oligomeric thiophenes are commonly-used components in organic electronics and solar cells. These molecules stack and/or aggregate readily under the processing conditions used to form thin films for these applications, significantly altering their optical and charge-transport properties. To determine how these effects depend on the substitution pattern of the thiophene main chains, nano-aggregates of three sexi-thiophene (6T) oligomers having different alkyl substitution patterns were formed using solvent poisoning techniques and studied using steady-state and time-resolved emission spectroscopy. The results indicate the substantial role played by the side-chain substituents in determining the emissive properties of these species. Both the measured spectral changesmore » and their dependence on substitution are well modeled by combined quantum chemistry and molecular dynamics simulations. The simulations connect the side-chain-induced disorder, which determines the favorable chain packing configurations within the aggregates, with their measured electronic spectra.« less
NASA Astrophysics Data System (ADS)
Khandale, A. P.; Bhoga, S. S.
2014-12-01
The (100 - x)Nd1.8Ce0.2CuO4+δ:(x)Ce0.9Gd0.1O2-δ (x = 00, 10, 20 and 30 vol.%) composite systems are obtained by impregnating a stoichiometric solution of cerium and gadolinium nitrates followed by sintering at 900 °C for 4 h. Impregnating the Ce0.9Gd0.1O2-δ not only inhibits the growth of the host Nd1.8Ce0.2CuO4+δ grains during sintering but also enlarges the oxygen reduction reaction zone by introducing a nanosized phase that is ionically conductive, which significantly decreases the electrode polarization resistance of the composite cathode. A minimum polarization resistance value of 0.23 ± 0.02 Ω cm2 is obtained at 700 °C for a (80)Nd1.8Ce0.2CuO4+δ:(20)Ce0.9Gd0.1O2-δ composite cathode, and this value is attributed to the optimal dispersion into the porous Nd1.8Ce0.2CuO4+δ matrix. The impedance spectra are modeled using an electrical equivalent model that consists of a mid-frequency ZR1 -CPE circuit (parallel combination of R1 and constant phase element (CPE)) and a low-frequency Gerischer impedance. The Gerischer impedance decreases significantly when Ce0.9Gd0.1O2-δ infiltrates the Nd1.8Ce0.2CuO4+δ matrix. The oxygen partial pressure-dependent polarization study suggests a medium-frequency response, which is due to charge transfer step; however, the low-frequency response corresponds to the non-charge transfer oxygen adsorption-desorption and the diffusion process during the overall oxygen reduction reaction process.
Uhlík, Filip; Slanina, Zdeněk; Nagase, Shigeru
2015-01-22
The contribution reports computations for Al@C{sub 82}, Sc@C{sub 82}, Y@C{sub 82} and La@C{sub 82} based on encapsulation into the IPR (isolated pentagon rule) C{sub 2ν} C{sub 82} cage and also on Mg@C{sub 74}, Ca@C{sub 74}, Sr@C{sub 74} and Ba@C{sub 74} based on encapsulation into the only C{sub 74} IPR cage as well as for three selected lanthanoids La@C{sub 74}, Yb@C{sub 74}, and Lu@C{sub 74}. Their structural and energetic characteristics are used for evaluations of the relative production yields, using the encapsulation Gibbs-energy and saturated metal pressures. It is shown that the results can be well related to the ionization potentials of the free metal atoms.
Jägerbrand, Annika K.; Kudo, Gaku
2016-01-01
There is limited knowledge available on the thermal acclimation processes for bryophytes, especially when considering variation between populations or sites. This study investigated whether short-term ex situ thermal acclimation of different populations showed patterns of site dependency and whether the maximum quantum yield of PSII (Fv/Fm) could be used as an indicator of adaptation or temperature stress in two bryophyte species: Pleurozium schreberi (Willd. ex Brid.) Mitt. and Racomitrium lanuginosum (Hedw.) Brid. We sought to test the hypothesis that differences in the ability to acclimate to short-term temperature treatment would be revealed as differences in photosystem II maximum yield (Fv/Fm). Thermal treatments were applied to samples from 12 and 11 populations during 12 or 13 days in growth chambers and comprised: (1) 10/5 °C; (2) 20/10 °C; (3) 25/15 °C; (4) 30/20 °C (12 hours day/night temperature). In Pleurozium schreberi, there were no significant site-dependent differences before or after the experiment, while site dependencies were clearly shown in Racomitrium lanuginosum throughout the study. Fv/Fm in Pleurozium schreberi decreased at the highest and lowest temperature treatments, which can be interpreted as a stress response, but no similar trends were shown by Racomitrium lanuginosum. PMID:27135242
Jägerbrand, Annika K; Kudo, Gaku
2016-01-01
There is limited knowledge available on the thermal acclimation processes for bryophytes, especially when considering variation between populations or sites. This study investigated whether short-term ex situ thermal acclimation of different populations showed patterns of site dependency and whether the maximum quantum yield of PSII (Fv/Fm) could be used as an indicator of adaptation or temperature stress in two bryophyte species: Pleurozium schreberi (Willd. ex Brid.) Mitt. and Racomitrium lanuginosum (Hedw.) Brid. We sought to test the hypothesis that differences in the ability to acclimate to short-term temperature treatment would be revealed as differences in photosystem II maximum yield (Fv/Fm). Thermal treatments were applied to samples from 12 and 11 populations during 12 or 13 days in growth chambers and comprised: (1) 10/5 °C; (2) 20/10 °C; (3) 25/15 °C; (4) 30/20 °C (12 hours day/night temperature). In Pleurozium schreberi, there were no significant site-dependent differences before or after the experiment, while site dependencies were clearly shown in Racomitrium lanuginosum throughout the study. Fv/Fm in Pleurozium schreberi decreased at the highest and lowest temperature treatments, which can be interpreted as a stress response, but no similar trends were shown by Racomitrium lanuginosum. PMID:27135242
Jägerbrand, Annika K; Kudo, Gaku
2016-04-26
There is limited knowledge available on the thermal acclimation processes for bryophytes, especially when considering variation between populations or sites. This study investigated whether short-term ex situ thermal acclimation of different populations showed patterns of site dependency and whether the maximum quantum yield of PSII (Fv/Fm) could be used as an indicator of adaptation or temperature stress in two bryophyte species: Pleurozium schreberi (Willd. ex Brid.) Mitt. and Racomitrium lanuginosum (Hedw.) Brid. We sought to test the hypothesis that differences in the ability to acclimate to short-term temperature treatment would be revealed as differences in photosystem II maximum yield (Fv/Fm). Thermal treatments were applied to samples from 12 and 11 populations during 12 or 13 days in growth chambers and comprised: (1) 10/5 °C; (2) 20/10 °C; (3) 25/15 °C; (4) 30/20 °C (12 hours day/night temperature). In Pleurozium schreberi, there were no significant site-dependent differences before or after the experiment, while site dependencies were clearly shown in Racomitrium lanuginosum throughout the study. Fv/Fm in Pleurozium schreberi decreased at the highest and lowest temperature treatments, which can be interpreted as a stress response, but no similar trends were shown by Racomitrium lanuginosum.
NASA Astrophysics Data System (ADS)
Semenov, Andrew G.; Zaikin, Andrei D.
2016-07-01
Quantum phase slips (QPSs) generate voltage fluctuations in superconducting nanowires. Employing the Keldysh technique and making use of the phase-charge duality arguments, we develop a theory of QPS-induced voltage noise in such nanowires. We demonstrate that quantum tunneling of the magnetic flux quanta across the wire yields quantum shot noise which obeys Poisson statistics and is characterized by a power-law dependence of its spectrum SΩ on the external bias. In long wires, SΩ decreases with increasing frequency Ω and vanishes beyond a threshold value of Ω at T →0 . The quantum coherent nature of QPS noise yields nonmonotonous dependence of SΩ on T at small Ω .
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.
Intermediate quantum maps for quantum computation
Giraud, O.; Georgeot, B.
2005-10-15
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.
Xu, Xin-Xin; Cui, Zhong-Ping; Gao, Xin; Liu, Xiao-Xia
2014-06-21
To improve photocatalytic activity of a coordination polymer (CP) in the visible light region, five different transition metal ions (Fe(3+), Cr(3+), Ru(3+), Co(2+) and Ni(2+)) were introduced into its framework through an ion-exchange process. Among all the resulting transition metal ion doped coordination polymers (TMI/CPs), the one doped with Fe(3+) took on the most excellent photocatalytic activity and the highest quantum yields in the visible light region, decomposing 94% Rhodamine B (RhB) in 8 hours. It can be attributed to the doping of Fe(3+), which reduced the band gap (Eg) of the original CP, facilitating photocatalysis of the obtained polymer. Compared with the coordination polymer with Fe(3+) as a dopant, products doped with other metal ions presented weaker photocatalytic activities in the visible light region, while under the irradiation of ultraviolet light, they showed favorable photocatalytic properties. The results suggest that to dope transition metal ions into the framework of CPs would be an ideal option for enhancing the photocatalytic activity of coordination polymers.
NASA Astrophysics Data System (ADS)
Qiu, Wenda; Xia, Jian; Chen, Liuping; Dahn, J. R.
2016-06-01
The effectiveness of methyl phenyl carbonate and diphenyl carbonate as electrolyte additives either singly or in combination with methylene methyl disulfonate and tris(-trimethyl-silyl)-phosphite has been systematically investigated in LiNi0.8Mn0.1Co0.1O2/graphite pouch cells. Experiments conducted included ultrahigh precision coulometry, electrochemical impedance spectroscopy, automated storage, gas evolution measurements as well as long-term cycling. The results showed that adding methyl phenyl or diphenyl carbonate increases the coulombic efficiency, reduces charge end-point capacity slippage rate, decreases the self-discharge rate during storage and improves the capacity retention during long-term cycling compared to cells with control electrolyte [1 M LiPF6 ethylene carbonate:ethyl methyl carbonate 3:7] or control electrolyte with 2% vinylene carbonate. 1% diphenyl carbonate appears to be the best among the systems studied. Based on these experiments, diphenyl carbonate seems to be a very beneficial additive for improving the performance of high voltage LiNi0.8Mn0.1Co0.1O2/graphite pouch cells.
Osborne, Tobias J.; Eisert, Jens; Verstraete, Frank
2010-12-31
We show how continuous matrix product states of quantum fields can be described in terms of the dissipative nonequilibrium dynamics of a lower-dimensional auxiliary boundary field by demonstrating that the spatial correlation functions of the bulk field correspond to the temporal statistics of the boundary field. This equivalence (1) illustrates an intimate connection between the theory of continuous quantum measurement and quantum field theory, (2) gives an explicit construction of the boundary field allowing the extension of real-space renormalization group methods to arbitrary dimensional quantum field theories without the introduction of a lattice parameter, and (3) yields a novel interpretation of recent cavity QED experiments in terms of quantum field theory, and hence paves the way toward observing genuine quantum phase transitions in such zero-dimensional driven quantum systems.
Long, S.P. ); Drake, B.G. )
1991-05-01
CO{sub 2} concentration was elevated throughout 3 years around stands of the C{sub 3} sedge Scirpus olneyi on a tidal marsh of the Chesapeake Bay. The hypothesis that tissues developed in an elevated CO{sub 2} atmosphere will show an acclimatory decrease in photosynthetic capacity under light-limiting conditions was examined. The absorbed light quantum yield of CO{sub 2} uptake ({phi}{sub abs}) and the efficiency of photosystem II photochemistry were determined for plants which had developed in open top chambers with CO{sub 2} concentrations in air of 680 micromoles per mole, and of 351 micromoles per mole as controls. When measured in an atmosphere with 10 millimoles per mole O{sub 2} to suppress photorespiration, shoots showed a {phi}{sub abs} of 0.093 {plus minus} 0.003, with no statistically significant difference between shoots grown in elevated or control CO{sub 2} concentration. Efficiency of photosystem II photochemistry was also unchanged by development in an elevated CO{sub 2} atmosphere. Shoots grown and measured in 680 micromoles per mole of CO{sub 2} in air showed a {phi}{sub abs} of 0.078 {plus minus} 0.004 compared with 0.065 {plus minus} for leaves grown and measured in 351 micromoles per mole CO{sub 2} in air; a highly significant increase. In accordance with the change in {phi}{sub abs}, the light compensation point of photosynthesis decreased from 51 {plus minus} 3 to 31 {plus minus} 3 micromoles per square meter per second for stems grown and measured in 351 and 680 micromoles per mole of CO{sub 2} in air, respectively.
Quantum computing of semiclassical formulas.
Georgeot, B; Giraud, O
2008-04-01
We show that semiclassical formulas such as the Gutzwiller trace formula can be implemented on a quantum computer more efficiently than on a classical device. We give explicit quantum algorithms which yield quantum observables from classical trajectories, and which alternatively test the semiclassical approximation by computing classical actions from quantum evolution. The gain over classical computation is in general quadratic, and can be larger in some specific cases.
Li, Shu-Shen; Long, Gui-Lu; Bai, Feng-Shan; Feng, Song-Lin; Zheng, Hou-Zhi
2001-01-01
Quantum computing is a quickly growing research field. This article introduces the basic concepts of quantum computing, recent developments in quantum searching, and decoherence in a possible quantum dot realization. PMID:11562459
Rychlewska, Urszula; Warzajtis, Beata; Dimitrijević, Mirjana Dj.; Draskovic, Nenad S.; Djuran, Miloš I.
2009-01-01
The title compound, {[Cd2(C2H3O3)2(SO4)(H2O)4]·H2O}n, was obtained unintentionally in a transmetallation reaction. The crystal structure contains a two-dimensional metal–organic framework based on CdII–(μ-hydroxyacetato-κ4 O 1,O 2:O 1,O 1′)–CdII zigzag chains joined together by bridging SO4 anions. The resulting layers are shifted with respect to each other and are stacked along the c axis. Their construction is supported by hydrogen bonds between water molecules and between water molecules and carboxylate or sulfate groups. Neighbouring layers are bridged by hydrogen bonds between the hydroxyl substituent and a sulfate anion. The sulfate anion and solvent water molecule are located on twofold axes. The results demonstrate that care must be taken when preparing ethylenediaminetetraacetic acid-type complexes by transmetallation, in order to avoid precipitation of metal complexes with the α-hydroxyacetate ligand. PMID:21583014
NASA Astrophysics Data System (ADS)
Xia, Tian; Brüll, Annelise; Grimaud, Alexis; Fourcade, Sébastien; Mauvy, Fabrice; Zhao, Hui; Grenier, Jean-Claude; Bassat, Jean-Marc
2014-09-01
A-site deficient perovskite La0.57Sr0.15TiO3 (LSTO) materials are synthesized by a modified polyacrylamide gel route. X-ray diffraction pattern of LSTO indicates an orthorhombic structure. The thermal expansion coefficient of LSTO is 10.0 × 10-6 K-1 at 600 °C in 5%H2/Ar. LSTO shows an electrical conductivity of 2 S cm-1 at 600 °C in 3%H2O/H2. A new composite material, containing the porous LSTO backbone impregnated with small amounts of Ce0.9Gd0.1O2-δ (CGO) (3.4-8.3 wt.%) and Ni/Cu (2.0-6.3 wt.%), is investigated as an alternative anode for solid oxide fuel cells (SOFCs). Because of the substantial electro-catalytic activity of the fine and well-dispersed Ni particles on the surface of the ceramic framework, the polarization resistance of 6.3%Ni-8.3%CGO-LSTO anode reaches 0.73 Ω cm2 at 800 °C in 3%H2O/H2. In order to further improve the anodic performance, corn starch and carbon black are used as pore-formers to optimize the microstructure of anodes.
NASA Astrophysics Data System (ADS)
Kiebach, Ragnar; Zhang, Wei-Wei; Zhang, Wei; Chen, Ming; Norrman, Kion; Wang, Hsiang-Jen; Bowen, Jacob R.; Barfod, Rasmus; Hendriksen, Peter Vang
2015-06-01
Degradation phenomena of La0.58Sr0.4Co0.2Fe0.8O3/Ce0.9Gd0.1O2 (LSCF/CGO) cathodes were investigated via post-mortem analyses of an experimental solid oxide fuel cell (SOFC) stack tested at 700 °C for 2000 h using advanced electron microscopy (SEM-EDS, HR-TEM-EDS) and time-of-flight secondary ion mass spectrometry (TOF-SIMS). Similar studies were carried out on non-tested reference cells for comparison. The analysis focused on the LSCF/CGO cathode and the CGO barrier layer, as the cathode degradation can be a major contributor to the overall degradation in this type of SOFC. SEM-EDS and TOF-SIMS were used to investigate inter-diffusion across the barrier layer-electrolyte interface and the barrier layer-cathode interface. In addition, TOF-SIMS data were employed to investigate impurity distribution before and after testing. HR-TEM-EDS was used to investigate possible phase segregation in the LSCF and to look for reaction between the phases. The results show that phase separation and inter-diffusion across the cathode-barrier layer interface and the barrier layer-electrolyte interface happened mainly during sintering and cathode firing, and to a very little degree during the test period.
NASA Astrophysics Data System (ADS)
Auletta, Gennaro; Fortunato, Mauro; Parisi, Giorgio
2014-01-01
Introduction; Part I. Basic Features of Quantum Mechanics: 1. From classical mechanics to quantum mechanics; 2. Quantum observable and states; 3. Quantum dynamics; 4. Examples of quantum dynamics; 5. Density matrix; Part II. More Advanced Topics: 6. Angular momentum and spin; 7. Identical particles; 8. Symmetries and conservation laws; 9. The measurement problem; Part III. Matter and Light: 10. Perturbations and approximation methods; 11. Hydrogen and helium atoms; 12. Hydrogen molecular ion; 13. Quantum optics; Part IV. Quantum Information: State and Correlations: 14. Quantum theory of open systems; 15. State measurement in quantum mechanics; 16. Entanglement: non-separability; 17. Entanglement: quantum information; References; Index.
NASA Astrophysics Data System (ADS)
Fan, Wenjiang; Lawrie, Benjamin J.; Pooser, Raphael C.
2015-11-01
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 with a classical optical readout in this configuration. The theoretical potential of this technique points to resolving particle concentrations with more accuracy than is possible via classical approaches to optical transduction.
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 with 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.
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
NASA Astrophysics Data System (ADS)
Nakazato, Hiromichi; Namiki, Mikio; Pascazio, Saverio; Rauch, Helmut
1995-02-01
The limit of infinitely frequent measurements (continuous observation), yielding the quantum Zeno paradox, is critically analyzed and shown to be unphysical. A specific example involving neutron spin is considered and some practical estimates are given.
NASA Astrophysics Data System (ADS)
Le Gouët, Jean-Louis; Moiseev, Sergey
2012-06-01
Interaction of quantum radiation with multi-particle ensembles has sparked off intense research efforts during the past decade. Emblematic of this field is the quantum memory scheme, where a quantum state of light is mapped onto an ensemble of atoms and then recovered in its original shape. While opening new access to the basics of light-atom interaction, quantum memory also appears as a key element for information processing applications, such as linear optics quantum computation and long-distance quantum communication via quantum repeaters. Not surprisingly, it is far from trivial to practically recover a stored quantum state of light and, although impressive progress has already been accomplished, researchers are still struggling to reach this ambitious objective. This special issue provides an account of the state-of-the-art in a fast-moving research area that makes physicists, engineers and chemists work together at the forefront of their discipline, involving quantum fields and atoms in different media, magnetic resonance techniques and material science. Various strategies have been considered to store and retrieve quantum light. The explored designs belong to three main—while still overlapping—classes. In architectures derived from photon echo, information is mapped over the spectral components of inhomogeneously broadened absorption bands, such as those encountered in rare earth ion doped crystals and atomic gases in external gradient magnetic field. Protocols based on electromagnetic induced transparency also rely on resonant excitation and are ideally suited to the homogeneous absorption lines offered by laser cooled atomic clouds or ion Coulomb crystals. Finally off-resonance approaches are illustrated by Faraday and Raman processes. Coupling with an optical cavity may enhance the storage process, even for negligibly small atom number. Multiple scattering is also proposed as a way to enlarge the quantum interaction distance of light with matter. The
NASA Astrophysics Data System (ADS)
Weinfurter, Harald; Zeilinger, Anton
Quantum entanglement lies at the heart of the new field of quantum communication and computation. For a long time, entanglement was seen just as one of those fancy features which make quantum mechanics so counterintuitive. But recently, quantum information theory has shown the tremendous importance of quantum correlations for the formulation of new methods of information transfer and for algorithms exploiting the capabilities of quantum computers.This chapter describes the first experimental realizations of quantum communication schemes using entangled photon pairs. We show how to make communication secure against eavesdropping using entanglement-based quantum cryptography, how to increase the information capacity of a quantum channel by quantum dense coding and, finally, how to communicate quantum information itself in the process of quantum teleportation.
NASA Astrophysics Data System (ADS)
Georgescu, I. M.; Ashhab, S.; Nori, Franco
2014-01-01
Simulating quantum mechanics is known to be a difficult computational problem, especially when dealing with large systems. However, this difficulty may be overcome by using some controllable quantum system to study another less controllable or accessible quantum system, i.e., quantum simulation. Quantum simulation promises to have applications in the study of many problems in, e.g., condensed-matter physics, high-energy physics, atomic physics, quantum chemistry, and cosmology. Quantum simulation could be implemented using quantum computers, but also with simpler, analog devices that would require less control, and therefore, would be easier to construct. A number of quantum systems such as neutral atoms, ions, polar molecules, electrons in semiconductors, superconducting circuits, nuclear spins, and photons have been proposed as quantum simulators. This review outlines the main theoretical and experimental aspects of quantum simulation and emphasizes some of the challenges and promises of this fast-growing field.
Quantum Mechanics in Insulators
Aeppli, G.
2009-08-20
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. Ronnow et al., Science 308, 392-395 (2005) and N. Q. Vinh et al., PNAS 105, 10649-10653 (2008).
Quantum Criticality and Black Holes
Sachdev, Subir
2007-08-22
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.
Quantum Criticality and Black Holes
Sachdev, Subir [Harvard University, Cambridge, Massachusetts, United States
2016-07-12
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.
Martinez, Rodrigo; Lucas, Josep M.; Gimenez, Xavier; Aguilar, Antonio; Gonzalez, Miguel
2006-04-14
The close-coupling hyperspherical (CCH) exact quantum method was used to study the title barrierless reaction up to a collision energy (E{sub T}) of 0.75 eV, and the results compared with quasiclassical trajectory (QCT) calculations to determine the importance of quantum effects. The CCH integral cross section decreased with E{sub T} and, although the QCT results were in general quite similar to the CCH ones, they presented a significant deviation from the CCH data within the 0.2-0.6 eV collision energy range, where the QCT method did not correctly describe the reaction probability. A very good accord between both methods was obtained for the OH{sup +} vibrational distribution, where no inversion of population was found. For the OH{sup +} rotational distributions, the agreement between the CCH and QCT results was not as good as in the vibrational case, but it was satisfactory in many conditions. The kk{sup '} angular distribution showed a preferential forward character, and the CCH method produced higher forward peaks than the QCT one. All the results were interpreted considering the potential energy surface and plots of a representative sampling of reactive trajectories.
Quantum reduction to Bianchi I models in loop quantum gravity
NASA Astrophysics Data System (ADS)
Bodendorfer, N.
2015-04-01
We propose a quantum symmetry reduction of loop quantum gravity to Bianchi I spacetimes. To this end, we choose the diagonal metric gauge for the spatial diffeomorphism constraint at the classical level, leading to an RBohr gauge theory, and quantize the resulting theory via loop quantum gravity methods. Constraints which lead classically to a suitable reduction are imposed at the quantum level. The dynamics of the resulting model turn out to be very simple and manifestly coincide with those of a polymer quantization of a Bianchi I model for the simplest choice of full theory quantum states compatible with the Bianchi I reduction. In particular, the "improved" μ ¯ dynamics of loop quantum cosmology can be obtained by modifying the regularization of the Hamiltonian constraint with similar ideas, in turn yielding insights into the full theory dynamics.
Cloning of a quantum measurement
Bisio, Alessandro; D'Ariano, Giacomo Mauro; Perinotti, Paolo; Sedlak, Michal
2011-10-15
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. 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.
Stapp, H.P.
1988-12-01
Quantum ontologies are conceptions of the constitution of the universe that are compatible with quantum theory. The ontological orientation is contrasted to the pragmatic orientation of science, and reasons are given for considering quantum ontologies both within science, and in broader contexts. The principal quantum ontologies are described and evaluated. Invited paper at conference: Bell's Theorem, Quantum Theory, and Conceptions of the Universe, George Mason University, October 20-21, 1988. 16 refs.
Quantum Computer Games: Quantum Minesweeper
ERIC Educational Resources Information Center
Gordon, Michal; Gordon, Goren
2010-01-01
The computer game of quantum minesweeper is introduced as a quantum extension of the well-known classical minesweeper. Its main objective is to teach the unique concepts of quantum mechanics in a fun way. Quantum minesweeper demonstrates the effects of superposition, entanglement and their non-local characteristics. While in the classical…
Pfeiffer, P.; Egusquiza, I. L.; Di Ventra, M.; Sanz, M.; Solano, E.
2016-01-01
Technology based on memristors, resistors with memory whose resistance depends on the history of the crossing charges, has lately enhanced the classical paradigm of computation with neuromorphic architectures. However, in contrast to the known quantized models of passive circuit elements, such as inductors, capacitors or resistors, the design and realization of a quantum memristor is still missing. Here, we introduce the concept of a quantum memristor as a quantum dissipative device, whose decoherence mechanism is controlled by a continuous-measurement feedback scheme, which accounts for the memory. Indeed, we provide numerical simulations showing that memory effects actually persist in the quantum regime. Our quantization method, specifically designed for superconducting circuits, may be extended to other quantum platforms, allowing for memristor-type constructions in different quantum technologies. The proposed quantum memristor is then a building block for neuromorphic quantum computation and quantum simulations of non-Markovian systems. PMID:27381511
Pfeiffer, P; Egusquiza, I L; Di Ventra, M; Sanz, M; Solano, E
2016-01-01
Technology based on memristors, resistors with memory whose resistance depends on the history of the crossing charges, has lately enhanced the classical paradigm of computation with neuromorphic architectures. However, in contrast to the known quantized models of passive circuit elements, such as inductors, capacitors or resistors, the design and realization of a quantum memristor is still missing. Here, we introduce the concept of a quantum memristor as a quantum dissipative device, whose decoherence mechanism is controlled by a continuous-measurement feedback scheme, which accounts for the memory. Indeed, we provide numerical simulations showing that memory effects actually persist in the quantum regime. Our quantization method, specifically designed for superconducting circuits, may be extended to other quantum platforms, allowing for memristor-type constructions in different quantum technologies. The proposed quantum memristor is then a building block for neuromorphic quantum computation and quantum simulations of non-Markovian systems. PMID:27381511
Pfeiffer, P; Egusquiza, I L; Di Ventra, M; Sanz, M; Solano, E
2016-07-06
Technology based on memristors, resistors with memory whose resistance depends on the history of the crossing charges, has lately enhanced the classical paradigm of computation with neuromorphic architectures. However, in contrast to the known quantized models of passive circuit elements, such as inductors, capacitors or resistors, the design and realization of a quantum memristor is still missing. Here, we introduce the concept of a quantum memristor as a quantum dissipative device, whose decoherence mechanism is controlled by a continuous-measurement feedback scheme, which accounts for the memory. Indeed, we provide numerical simulations showing that memory effects actually persist in the quantum regime. Our quantization method, specifically designed for superconducting circuits, may be extended to other quantum platforms, allowing for memristor-type constructions in different quantum technologies. The proposed quantum memristor is then a building block for neuromorphic quantum computation and quantum simulations of non-Markovian systems.
NASA Astrophysics Data System (ADS)
Pfeiffer, P.; Egusquiza, I. L.; di Ventra, M.; Sanz, M.; Solano, E.
2016-07-01
Technology based on memristors, resistors with memory whose resistance depends on the history of the crossing charges, has lately enhanced the classical paradigm of computation with neuromorphic architectures. However, in contrast to the known quantized models of passive circuit elements, such as inductors, capacitors or resistors, the design and realization of a quantum memristor is still missing. Here, we introduce the concept of a quantum memristor as a quantum dissipative device, whose decoherence mechanism is controlled by a continuous-measurement feedback scheme, which accounts for the memory. Indeed, we provide numerical simulations showing that memory effects actually persist in the quantum regime. Our quantization method, specifically designed for superconducting circuits, may be extended to other quantum platforms, allowing for memristor-type constructions in different quantum technologies. The proposed quantum memristor is then a building block for neuromorphic quantum computation and quantum simulations of non-Markovian systems.
NASA Technical Reports Server (NTRS)
Hess, W. P.; Kohler, S. J.; Haugen, H. K.; Leone, S. R.
1986-01-01
Initial measurements on I-asterisk yields of alkyl iodides at 266 nm are reported using gain vs. absorption spectroscopy with an InGaAsP diode probe laser. The results are 102 percent + or - 4 percent, 102 percent + or - 7 percent, and 73 percent + or - 4 percent for n-C3F7I, i-C3F7I, and CH3I respectively. Future prospects for the development of diode laser systems and for their use in dynamical studies are discussed.
Yield Improvement in Steel Casting (Yield II)
Richard A. Hardin; Christoph Beckermann; Tim Hays
2002-02-18
This report presents work conducted on the following main projects tasks undertaken in the Yield Improvement in Steel Casting research program: Improvement of Conventional Feeding and Risering Methods, Use of Unconventional Yield Improvement Techniques, and Case Studies in Yield Improvement. Casting trials were conducted and then simulated using the precise casting conditions as recorded by the participating SFSA foundries. These results present a statistically meaningful set of experimental data on soundness versus feeding length. Comparisons between these casting trials and casting trials performed more than forty years ago by Pellini and the SFSA are quite good and appear reasonable. Comparisons between the current SFSA feeding rules and feeding rules based on the minimum Niyama criterion reveal that the Niyama-based rules are generally less conservative. The niyama-based rules also agree better with both the trials presented here, and the casting trails performed by Pellini an d the SFSA years ago. Furthermore, the use of the Niyama criterion to predict centerline shrinkage for horizontally fed plate sections has a theoretical basis according to the casting literature reviewed here. These results strongly support the use of improved feeding rules for horizontal plate sections based on the Niyama criterion, which can be tailored to the casting conditions for a given alloy and to a desired level of soundness. The reliability and repeatability of ASTM shrinkage x-ray ratings was investigated in a statistical study performed on 128 x-rays, each of which were rated seven different times. A manual ''Feeding and Risering Guidelines for Steel Castings' is given in this final report. Results of casting trials performed to test unconventional techniques for improving casting yield are presented. These use a stacked arrangement of castings and riser pressurization to increase the casting yield. Riser pressurization was demonstrated to feed a casting up to four time s the
NASA Astrophysics Data System (ADS)
Brzeziński, Tomasz; Fairfax, Simon A.
2012-11-01
Algebras of functions on quantum weighted projective spaces are introduced, and the structure of quantum weighted projective lines or quantum teardrops is described in detail. In particular the presentation of the coordinate algebra of the quantum teardrop in terms of generators and relations and classification of irreducible *-representations are derived. The algebras are then analysed from the point of view of Hopf-Galois theory or the theory of quantum principal bundles. Fredholm modules and associated traces are constructed. C*-algebras of continuous functions on quantum weighted projective lines are described and their K-groups computed.
Izumi, Yudai; Nakagawa, Kazumichi
2011-08-01
One of the leading hypotheses regarding the origin of prebiotic molecules on primitive Earth is that they formed from inorganic molecules in extraterrestrial environments and were delivered by meteorites, space dust and comets. To evaluate the availability of extraterrestrial amino acids, it is necessary to examine their decomposition and oligomerization rates as induced by extraterrestrial energy sources, such as vacuum ultraviolet (VUV) and X-ray photons and high energy particles. This paper reports the quantum yields of decomposition ((8.2 ± 0.7) × 10(-2) photon(-1)) and homo-dimerization ((1.2 ± 0.3) × 10(-3) photon(-1)) and decomposition of the dimer (0.24 ± 0.06 photon(-1)) of solid L-alanine (Ala) induced by VUV light with an energy of 7.2 eV. Using these quantum yields, the half-life of L-Ala on the surface of a space object in the present earth orbit was estimated to be about 52 days, even when only photons with an energy of 7.2 eV emitted from the present Sun were considered. The actual half-life of solid L-Ala on the surface of a space object orbit around the present day Earth would certainly be much shorter than our estimate, because of the added effect of photons and particles of other energies. Thus, we propose that L-Ala needs to be shielded from solar VUV in protected environments, such as the interior of a meteorite, within a time scale of days after synthesis to ensure its arrival on the primitive Earth.
Atmospheric Nitrogen Fluorescence Yield
NASA Technical Reports Server (NTRS)
Adams, J. H., Jr.; Christl, M. J.; Fountain, W. F.; Gregory, J. C.; Martens, K. U.; Sokolsky, Pierre; Whitaker, Ann F. (Technical Monitor)
2001-01-01
Several existing and planned experiments estimate the energies of ultra-high energy cosmic rays from air showers using the atmospheric nitrogen fluorescence. The nitrogen fluorescence yield from air shower electrons depends on the atmospheric composition. We will discuss the uncertainties in the fluorescence yield form electrons in the real atmosphere and describe a concept for a small balloon payload to measure the atmospheric fluorescence yield as a function of attitude.
Zurek, Wojciech H
2008-01-01
Quantum Darwinism - proliferation, in the environment, of multiple records of selected states of the system (its information-theoretic progeny) - explains how quantum fragility of individual state can lead to classical robustness of their multitude.
Pfeiffer, P.; Egusquiza, I. L.; Di Ventra, M.; Sanz, M.; Solano, E.
2016-07-06
Technology based on memristors, resistors with memory whose resistance depends on the history of the crossing charges, has lately enhanced the classical paradigm of computation with neuromorphic architectures. However, in contrast to the known quantized models of passive circuit elements, such as inductors, capacitors or resistors, the design and realization of a quantum memristor is still missing. Here, we introduce the concept of a quantum memristor as a quantum dissipative device, whose decoherence mechanism is controlled by a continuous-measurement feedback scheme, which accounts for the memory. Indeed, we provide numerical simulations showing that memory effects actually persist in the quantummore » regime. Our quantization method, specifically designed for superconducting circuits, may be extended to other quantum platforms, allowing for memristor-type constructions in different quantum technologies. As a result, the proposed quantum memristor is then a building block for neuromorphic quantum computation and quantum simulations of non-Markovian systems.« less
NASA Astrophysics Data System (ADS)
Coleman, Piers; Schofield, Andrew J.
2005-01-01
As we mark the centenary of Albert Einstein's seminal contribution to both quantum mechanics and special relativity, we approach another anniversary - that of Einstein's foundation of the quantum theory of solids. But 100 years on, the same experimental measurement that puzzled Einstein and his contemporaries is forcing us to question our understanding of how quantum matter transforms at ultra-low temperatures.
Probing deformed quantum commutators
NASA Astrophysics Data System (ADS)
Rossi, Matteo A. C.; Giani, Tommaso; Paris, Matteo G. A.
2016-07-01
Several quantum gravity theories predict a minimal length at the order of magnitude of the Planck length, under which the concepts of space and time lose their physical meaning. In quantum mechanics, the insurgence of such a minimal length can be described by introducing a modified position-momentum commutator, which in turn yields a generalized uncertainty principle, where the uncertainty on position measurements has a lower bound. The value of the minimal length is not predicted by theories and must be estimated experimentally. In this paper, we address the quantum bound to the estimability of the minimal uncertainty length by performing measurements on a harmonic oscillator, which is analytically solvable in the deformed algebra induced by the deformed commutation relations.
NASA Astrophysics Data System (ADS)
Brown, Matthew J.
2014-02-01
The framework of quantum frames can help unravel some of the interpretive difficulties i the foundation of quantum mechanics. In this paper, I begin by tracing the origins of this concept in Bohr's discussion of quantum theory and his theory of complementarity. Engaging with various interpreters and followers of Bohr, I argue that the correct account of quantum frames must be extended beyond literal space-time reference frames to frames defined by relations between a quantum system and the exosystem or external physical frame, of which measurement contexts are a particularly important example. This approach provides superior solutions to key EPR-type measurement and locality paradoxes.
NASA Astrophysics Data System (ADS)
Moulick, Subhayan Roy; Panigrahi, Prasanta K.
2016-06-01
We propose the idea of a quantum cheque scheme, a cryptographic protocol in which any legitimate client of a trusted bank can issue a cheque, that cannot be counterfeited or altered in anyway, and can be verified by a bank or any of its branches. We formally define a quantum cheque and present the first unconditionally secure quantum cheque scheme and show it to be secure against any no-signalling adversary. The proposed quantum cheque scheme can been perceived as the quantum analog of Electronic Data Interchange, as an alternate for current e-Payment Gateways.
NASA Astrophysics Data System (ADS)
Zurek, Wojciech Hubert
2009-03-01
Quantum Darwinism describes the proliferation, in the environment, of multiple records of selected states of a quantum system. It explains how the quantum fragility of a state of a single quantum system can lead to the classical robustness of states in their correlated multitude; shows how effective `wave-packet collapse' arises as a result of the proliferation throughout the environment of imprints of the state of the system; and provides a framework for the derivation of Born's rule, which relates the probabilities of detecting states to their amplitudes. Taken together, these three advances mark considerable progress towards settling the quantum measurement problem.
NASA Astrophysics Data System (ADS)
Fehr, Serge
2010-05-01
Quantum cryptography makes use of the quantum-mechanical behavior of nature for the design and analysis of cryptographic schemes. Optimally (but not always), quantum cryptography allows for the design of cryptographic schemes whose security is guaranteed solely by the laws of nature. This is in sharp contrast to standard cryptographic schemes, which can be broken in principle, i.e., when given sufficient computing power. From a theory point of view, quantum cryptography offers a beautiful interplay between the mathematics of adversarial behavior and quantum information theory. In this review article, we discuss the traditional application of quantum cryptography, quantum key distribution (QKD), from a modern perspective, and we discuss some recent developments in the context of quantum two-party cooperation (2PC). QKD allows two distant parties to communicate in a provably-secure way in the presence of an outside eavesdropper, whereas 2PC is concerned with protecting information against possibly malicious insiders. We show the basic idea of constructing quantum cryptographic schemes, but we also show some connections to quantum information theory as needed for the rigorous security analyses, and we discuss some of the relevant quantum-information-theoretic results.
Quantum graph as a quantum spectral filter
Turek, Ondrej; Cheon, Taksu
2013-03-15
We study the transmission of a quantum particle along a straight input-output line to which a graph {Gamma} is attached at a point. In the point of contact we impose a singularity represented by a certain properly chosen scale-invariant coupling with a coupling parameter {alpha}. We show that the probability of transmission along the line as a function of the particle energy tends to the indicator function of the energy spectrum of {Gamma} as {alpha}{yields}{infinity}. This effect can be used for a spectral analysis of the given graph {Gamma}. Its applications include a control of a transmission along the line and spectral filtering. The result is illustrated with an example where {Gamma} is a loop exposed to a magnetic field. Two more quantum devices are designed using other special scale-invariant vertex couplings. They can serve as a band-stop filter and as a spectral separator, respectively.
NASA Astrophysics Data System (ADS)
Orvil Scully, Marlan; Zubairy, Muhammad Suhail
1997-09-01
Quantum optics has witnessed significant theoretical and experimental developments in recent years. This book provides an in-depth and wide-ranging introduction to the subject, emphasizing throughout the basic principles and their applications. The book begins by developing the basic tools of quantum optics, and goes on to show the application of these tools in a variety of quantum optical systems, including lasing without inversion, squeezed states, and atom optics. The final four chapters discuss quantum optical tests of the foundations of quantum mechanics, and particular aspects of measurement theory. Assuming only a background of standard quantum mechanics and electromagnetic theory, and containing many problems and references, this book will be invaluable to graduate students of quantum optics, as well as to researchers in this field.
... Secondhand Smoke Smokeless Products Youth Tobacco Prevention Tobacco Industry and Products Federal Tax Increase Tobacco Ingredient Reporting ... be used. 3 In the past, the tobacco industry categorized low-yield cigarettes using measurements of tar ...
NASA Technical Reports Server (NTRS)
Callis, S. L.; Sakamoto, C.
1984-01-01
A model based on multiple regression was developed to estimate soybean yields for the country of Argentina. A meteorological data set was obtained for the country by averaging data for stations within the soybean growing area. Predictor variables for the model were derived from monthly total precipitation and monthly average temperature. A trend variable was included for the years 1969 to 1978 since an increasing trend in yields due to technology was observed between these years.
NASA Technical Reports Server (NTRS)
Callis, S. L.; Sakamoto, C.
1984-01-01
A model based on multiple regression was developed to estimate corn yields for the country of Argentina. A meteorological data set was obtained for the country by averaging data for stations within the corn-growing area. Predictor variables for the model were derived from monthly total precipitation, average monthly mean temperature, and average monthly maximum temperature. A trend variable was included for the years 1965 to 1980 since an increasing trend in yields due to technology was observed between these years.
Quantum entanglement, quantum communication and the limits of quantum computing
NASA Astrophysics Data System (ADS)
Ambainis, Andris
Quantum entanglement is a term describing the quantum correlations between different parts of a quantum system. Quantum information theory has developed sophisticated techniques to quantify and study quantum entanglement. In this thesis, we show how to apply those techniques to problems in quantum algorithms, complexity theory, communication and cryptography. The main results are: (1) quantum communication protocols that are exponentially more efficient that conventional (classical) communication protocols, (2) unconditionally secure quantum protocols for cryptographic problems, (3) a new "quantum adversary" method for proving lower bounds on quantum algorithms, (4) a study of "one clean qubit computation", a model related to the experimental implementation of quantum computers using NMR (nucleo-magnetic resonance) technology.
NASA Astrophysics Data System (ADS)
Ryabov, V. A.
2015-08-01
Quantum systems in a mechanical embedding, the breathing mode of a small particles, optomechanical system, etc. are far not the full list of examples in which the volume exhibits quantum behavior. Traditional consideration suggests strain in small systems as a result of a collective movement of particles, rather than the dynamics of the volume as an independent variable. The aim of this work is to show that some problem here might be essentially simplified by introducing periodic boundary conditions. At this case, the volume is considered as the independent dynamical variable driven by the internal pressure. For this purpose, the concept of quantum volume based on Schrödinger’s equation in 𝕋3 manifold is proposed. It is used to explore several 1D model systems: An ensemble of free particles under external pressure, quantum manometer and a quantum breathing mode. In particular, the influence of the pressure of free particle on quantum oscillator is determined. It is shown also that correction to the spectrum of the breathing mode due to internal degrees of freedom is determined by the off-diagonal matrix elements of the quantum stress. The new treatment not using the “force” theorem is proposed for the quantum stress tensor. In the general case of flexible quantum 3D dynamics, quantum deformations of different type might be introduced similarly to monopole mode.
Yamashita, Shin-Ichi; Hamada, Morihiko; Nakanishi, Shunsuke; Saito, Hironobu; Nosaka, Yoshio; Wakida, Shin-Ichi; Biju, Vasudevanpillai
2015-03-23
Despite the bright and tuneable photoluminescence (PL) of semiconductor quantum dots (QDs), the PL instability induced by Auger recombination and oxidation poses a major challenge in single-molecule applications of QDs. The incomplete information about Auger recombination and oxidation is an obstacle in the resolution of this challenge. Here, we report for the first time that Auger-ionized QDs beat self-sensitized oxidation and the non-digitized PL intensity loss. Although high-intensity photoactivation insistently induces PL blinking, the transient escape of QDs into the ultrafast Auger recombination cycle prevents generation of singlet oxygen ((1) O2 ) and preserves the PL intensity. By the detection of the NIR phosphorescence of (1) O2 and evaluation of the photostability of single QDs in aerobic, anaerobic, and (1) O2 scavenger-enriched environments, we disclose relations of Auger ionization and (1) O2 -mediated oxidation to the PL stability of single QDs, which will be useful during the formulation of QD-based single-molecule imaging tools and single-photon devices.
NASA Astrophysics Data System (ADS)
Levy, Amikam; Diósi, Lajos; Kosloff, Ronnie
2016-05-01
In this work we present the concept of a quantum flywheel coupled to a quantum heat engine. The flywheel stores useful work in its energy levels, while additional power is extracted continuously from the device. Generally, the energy exchange between a quantum engine and a quantized work repository is accompanied by heat, which degrades the charging efficiency. Specifically when the quantum harmonic oscillator acts as a work repository, quantum and thermal fluctuations dominate the dynamics. Quantum monitoring and feedback control are applied to the flywheel in order to reach steady state and regulate its operation. To maximize the charging efficiency one needs a balance between the information gained by measuring the system and the information fed back to the system. The dynamics of the flywheel are described by a stochastic master equation that accounts for the engine, the external driving, the measurement, and the feedback operations.
Coleman, Piers; Schofield, Andrew J
2005-01-20
As we mark the centenary of Albert Einstein's seminal contribution to both quantum mechanics and special relativity, we approach another anniversary--that of Einstein's foundation of the quantum theory of solids. But 100 years on, the same experimental measurement that puzzled Einstein and his contemporaries is forcing us to question our understanding of how quantum matter transforms at ultra-low temperatures. PMID:15662409
NASA Astrophysics Data System (ADS)
Lanzagorta, Marco; Jitrik, Oliverio; Uhlmann, Jeffrey; Venegas, Salvador
2016-05-01
A major scientific thrust from recent years has been to try to harness quantum phenomena to increase the performance of a wide variety of information processing devices. In particular, quantum radar has emerged as an intriguing theoretical concept that could revolutionize electromagnetic standoff sensing. In this paper we will discuss how the techniques developed for quantum radar could also be used towards the design of novel seismographs able to detect small ground vibrations., We use a hypothetical earthquake warning system in order to compare quantum seismography with traditional seismographic techniques.
NASA Astrophysics Data System (ADS)
Tartakovskii, Alexander
2012-07-01
Part I. Nanostructure Design and Structural Properties of Epitaxially Grown Quantum Dots and Nanowires: 1. Growth of III/V semiconductor quantum dots C. Schneider, S. Hofling and A. Forchel; 2. Single semiconductor quantum dots in nanowires: growth, optics, and devices M. E. Reimer, N. Akopian, M. Barkelid, G. Bulgarini, R. Heeres, M. Hocevar, B. J. Witek, E. Bakkers and V. Zwiller; 3. Atomic scale analysis of self-assembled quantum dots by cross-sectional scanning tunneling microscopy and atom probe tomography J. G. Keizer and P. M. Koenraad; Part II. Manipulation of Individual Quantum States in Quantum Dots Using Optical Techniques: 4. Studies of the hole spin in self-assembled quantum dots using optical techniques B. D. Gerardot and R. J. Warburton; 5. Resonance fluorescence from a single quantum dot A. N. Vamivakas, C. Matthiesen, Y. Zhao, C.-Y. Lu and M. Atature; 6. Coherent control of quantum dot excitons using ultra-fast optical techniques A. J. Ramsay and A. M. Fox; 7. Optical probing of holes in quantum dot molecules: structure, symmetry, and spin M. F. Doty and J. I. Climente; Part III. Optical Properties of Quantum Dots in Photonic Cavities and Plasmon-Coupled Dots: 8. Deterministic light-matter coupling using single quantum dots P. Senellart; 9. Quantum dots in photonic crystal cavities A. Faraon, D. Englund, I. Fushman, A. Majumdar and J. Vukovic; 10. Photon statistics in quantum dot micropillar emission M. Asmann and M. Bayer; 11. Nanoplasmonics with colloidal quantum dots V. Temnov and U. Woggon; Part IV. Quantum Dot Nano-Laboratory: Magnetic Ions and Nuclear Spins in a Dot: 12. Dynamics and optical control of an individual Mn spin in a quantum dot L. Besombes, C. Le Gall, H. Boukari and H. Mariette; 13. Optical spectroscopy of InAs/GaAs quantum dots doped with a single Mn atom O. Krebs and A. Lemaitre; 14. Nuclear spin effects in quantum dot optics B. Urbaszek, B. Eble, T. Amand and X. Marie; Part V. Electron Transport in Quantum Dots Fabricated by
Dissipative quantum computing with open quantum walks
Sinayskiy, Ilya; Petruccione, Francesco
2014-12-04
An open quantum walk approach to the implementation of a dissipative quantum computing scheme is presented. The formalism is demonstrated for the example of an open quantum walk implementation of a 3 qubit quantum circuit consisting of 10 gates.
Yield gaps and yield relationships in US soybean production systems
Technology Transfer Automated Retrieval System (TEKTRAN)
The magnitude of yield gaps (YG) (potential yield – farmer yield) provides some indication of the prospects for increasing crop yield to meet the food demands of future populations. Quantile regression analysis was applied to county soybean [Glycine max (L.) Merrill] yields (1971 – 2011) from Kentuc...
Multipartite asymmetric quantum cloning
Iblisdir, S.; Gisin, N.; Acin, A.; Cerf, N.J.; Filip, R.; Fiurasek, J.
2005-10-15
We investigate the optimal distribution of quantum information over multipartite systems in asymmetric settings. We introduce cloning transformations that take N identical replicas of a pure state in any dimension as input and yield a collection of clones with nonidentical fidelities. As an example, if the clones are partitioned into a set of M{sub A} clones with fidelity F{sup A} and another set of M{sub B} clones with fidelity F{sup B}, the trade-off between these fidelities is analyzed, and particular cases of optimal N{yields}M{sub A}+M{sub B} cloning machines are exhibited. We also present an optimal 1{yields}1+1+1 cloning machine, which is an example of a tripartite fully asymmetric cloner. Finally, it is shown how these cloning machines can be optically realized.
NASA Technical Reports Server (NTRS)
Lee, H.; Kok, P.; Dowling, J. P.
2002-01-01
This paper addresses the formal equivalence between the Mach-Zehnder interferometer, the Ramsey spectroscope, and a specific quantum logical gate. Based on this equivalence we introduce the quantum Rosetta Stone, and we describe a projective measurement scheme for generating the desired correlations between the interferometric input states in order to achieve Heisenberg-limited sensitivity.
Trevors, J T; Masson, L
2011-01-01
During his famous 1943 lecture series at Trinity College Dublin, the reknown physicist Erwin Schrodinger discussed the failure and challenges of interpreting life by classical physics alone and that a new approach, rooted in Quantum principles, must be involved. Quantum events are simply a level of organization below the molecular level. This includes the atomic and subatomic makeup of matter in microbial metabolism and structures, as well as the organic, genetic information code of DNA and RNA. Quantum events at this time do not elucidate, for example, how specific genetic instructions were first encoded in an organic genetic code in microbial cells capable of growth and division, and its subsequent evolution over 3.6 to 4 billion years. However, due to recent technological advances, biologists and physicists are starting to demonstrate linkages between various quantum principles like quantum tunneling, entanglement and coherence in biological processes illustrating that nature has exerted some level quantum control to optimize various processes in living organisms. In this article we explore the role of quantum events in microbial processes and endeavor to show that after nearly 67 years, Schrödinger was prophetic and visionary in his view of quantum theory and its connection with some of the fundamental mechanisms of life. PMID:21368338
NASA Astrophysics Data System (ADS)
Coecke, Bob
2010-01-01
Why did it take us 50 years since the birth of the quantum mechanical formalism to discover that unknown quantum states cannot be cloned? Yet, the proof of the 'no-cloning theorem' is easy, and its consequences and potential for applications are immense. Similarly, why did it take us 60 years to discover the conceptually intriguing and easily derivable physical phenomenon of 'quantum teleportation'? We claim that the quantum mechanical formalism doesn't support our intuition, nor does it elucidate the key concepts that govern the behaviour of the entities that are subject to the laws of quantum physics. The arrays of complex numbers are kin to the arrays of 0s and 1s of the early days of computer programming practice. Using a technical term from computer science, the quantum mechanical formalism is 'low-level'. In this review we present steps towards a diagrammatic 'high-level' alternative for the Hilbert space formalism, one which appeals to our intuition. The diagrammatic language as it currently stands allows for intuitive reasoning about interacting quantum systems, and trivialises many otherwise involved and tedious computations. It clearly exposes limitations such as the no-cloning theorem, and phenomena such as quantum teleportation. As a logic, it supports 'automation': it enables a (classical) computer to reason about interacting quantum systems, prove theorems, and design protocols. It allows for a wider variety of underlying theories, and can be easily modified, having the potential to provide the required step-stone towards a deeper conceptual understanding of quantum theory, as well as its unification with other physical theories. Specific applications discussed here are purely diagrammatic proofs of several quantum computational schemes, as well as an analysis of the structural origin of quantum non-locality. The underlying mathematical foundation of this high-level diagrammatic formalism relies on so-called monoidal categories, a product of a fairly
All entangled quantum states are nonlocal.
Buscemi, Francesco
2012-05-18
Departing from the usual paradigm of local operations and classical communication adopted in entanglement theory, we study here the interconversion of quantum states by means of local operations and shared randomness. A set of necessary and sufficient conditions for the existence of such a transformation between two given quantum states is given in terms of the payoff they yield in a suitable class of nonlocal games. It is shown that, as a consequence of our result, such a class of nonlocal games is able to witness quantum entanglement, however weak, and reveal nonlocality in any entangled quantum state. An example illustrating this fact is provided.
Free coherent spinons in quantum square ice
NASA Astrophysics Data System (ADS)
Kourtis, Stefanos; Castelnovo, Claudio
2016-09-01
We investigate the quantum dynamics of monopolelike excitations in quantum square ice, as captured by the strongly anisotropic spin-1/2 XXZ model on the checkerboard lattice. We obtain exact results for excitation dynamics in both analytically solvable effective models and a fully interacting model of quantum square ice on finite clusters. We find that the dispersive lower bound of the dynamic response of freely propagating spinons is recovered in the dynamic structure factor of the interacting system, yielding a marked fingerprint of coherent spinon dispersion. Our results provide unbiased evidence for the formation of coherent quasiparticles propagating freely in the correlated "vacuum" of quantum square ice.
NASA Astrophysics Data System (ADS)
The field of many-body quantum physics has a long history of fundamental discoveries, many of which have gone far beyond our wildest imagination. These include the study of novel states of matter, the observation of previously unseen phase transitions, and the discovery of new macroscopic quantum effects which arise when the intriguing rules of quantum mechanics are no longer restricted to the subatomic world, but rather determine the collective behavior of systems that are observable with the naked eye. In the past, it has often been proven difficult to obtain the underlying theory that yields an accurate description of the collective quantum phenomenon on the microscopic level. A good example is the discovery of superfluidity in liquid 4He by Pyotr Kapitsa, John Allen and Don Misener in 1938 [1, 2], where superfluidity refers to the fact that the liquid can flow without experiencing resistance, which leads for example to the spectacular fountain effect [3]. Since the atoms interact very strongly, the precise internal state of liquid helium is notoriously difficult to determine.
Bifurcation-based adiabatic quantum computation with a nonlinear oscillator network.
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
Bifurcation-based adiabatic quantum computation with a nonlinear oscillator network
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
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.
Bifurcation-based adiabatic quantum computation with a nonlinear oscillator network.
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.
NASA Astrophysics Data System (ADS)
Casati, Giulio; Chirikov, Boris
2006-11-01
Preface; Acknowledgments; Introduction: 1. The legacy of chaos in quantum mechanics G. Casati and B. V. Chirikov; Part I. Classical Chaos and Quantum Localization: 2. Stochastic behaviour of a quantum pendulum under a periodic perturbation G. Casati, B. V. Chirikov, F. M. Izrailev and J. Ford; 3. Quantum dynamics of a nonintegrable system D. R. Grempel, R. E. Prange and S. E. Fishman; 4. Excitation of molecular rotation by periodic microwave pulses. A testing ground for Anderson localization R. Blümel, S. Fishman and U. Smilansky; 5. Localization of diffusive excitation in multi-level systems D. K. Shepelyansky; 6. Classical and quantum chaos for a kicked top F. Haake, M. Kus and R. Scharf; 7. Self-similarity in quantum dynamics L. E. Reichl and L. Haoming; 8. Time irreversibility of classically chaotic quantum dynamics K. Ikeda; 9. Effect of noise on time-dependent quantum chaos E. Ott, T. M. Antonsen Jr and J. D. Hanson; 10. Dynamical localization, dissipation and noise R. F. Graham; 11. Maximum entropy models and quantum transmission in disordered systems J.-L. Pichard and M. Sanquer; 12. Solid state 'atoms' in intense oscillating fields M. S. Sherwin; Part II. Atoms in Strong Fields: 13. Localization of classically chaotic diffusion for hydrogen atoms in microwave fields J. E. Bayfield, G. Casati, I. Guarneri and D. W. Sokol; 14. Inhibition of quantum transport due to 'scars' of unstable periodic orbits R. V. Jensen, M. M. Sanders, M. Saraceno and B. Sundaram; 15. Rubidium Rydberg atoms in strong fields G. Benson, G. Raithel and H. Walther; 16. Diamagnetic Rydberg atom: confrontation of calculated and observed spectra C.-H. Iu, G. R. Welch, M. M. Kash, D. Kleppner, D. Delande and J. C. Gay; 17. Semiclassical approximation for the quantum states of a hydrogen atom in a magnetic field near the ionization limit M. Y. Kuchiev and O. P. Sushkov; 18. The semiclassical helium atom D. Wintgen, K. Richter and G. Tanner; 19. Stretched helium: a model for quantum chaos
NASA Astrophysics Data System (ADS)
Casati, Giulio; Chirikov, Boris
1995-04-01
Preface; Acknowledgments; Introduction: 1. The legacy of chaos in quantum mechanics G. Casati and B. V. Chirikov; Part I. Classical Chaos and Quantum Localization: 2. Stochastic behaviour of a quantum pendulum under a periodic perturbation G. Casati, B. V. Chirikov, F. M. Izrailev and J. Ford; 3. Quantum dynamics of a nonintegrable system D. R. Grempel, R. E. Prange and S. E. Fishman; 4. Excitation of molecular rotation by periodic microwave pulses. A testing ground for Anderson localization R. Blümel, S. Fishman and U. Smilansky; 5. Localization of diffusive excitation in multi-level systems D. K. Shepelyansky; 6. Classical and quantum chaos for a kicked top F. Haake, M. Kus and R. Scharf; 7. Self-similarity in quantum dynamics L. E. Reichl and L. Haoming; 8. Time irreversibility of classically chaotic quantum dynamics K. Ikeda; 9. Effect of noise on time-dependent quantum chaos E. Ott, T. M. Antonsen Jr and J. D. Hanson; 10. Dynamical localization, dissipation and noise R. F. Graham; 11. Maximum entropy models and quantum transmission in disordered systems J.-L. Pichard and M. Sanquer; 12. Solid state 'atoms' in intense oscillating fields M. S. Sherwin; Part II. Atoms in Strong Fields: 13. Localization of classically chaotic diffusion for hydrogen atoms in microwave fields J. E. Bayfield, G. Casati, I. Guarneri and D. W. Sokol; 14. Inhibition of quantum transport due to 'scars' of unstable periodic orbits R. V. Jensen, M. M. Sanders, M. Saraceno and B. Sundaram; 15. Rubidium Rydberg atoms in strong fields G. Benson, G. Raithel and H. Walther; 16. Diamagnetic Rydberg atom: confrontation of calculated and observed spectra C.-H. Iu, G. R. Welch, M. M. Kash, D. Kleppner, D. Delande and J. C. Gay; 17. Semiclassical approximation for the quantum states of a hydrogen atom in a magnetic field near the ionization limit M. Y. Kuchiev and O. P. Sushkov; 18. The semiclassical helium atom D. Wintgen, K. Richter and G. Tanner; 19. Stretched helium: a model for quantum chaos
Atmospheric Fluorescence Yield
NASA Technical Reports Server (NTRS)
Adams, James H., Jr.; Christl, M. J.; Fountain, W. F.; Gregory, J. C.; Martens, K.; Sokolsky, P.; Whitaker, Ann F. (Technical Monitor)
2001-01-01
Several existing and planned experiments estimate the energies of ultra-high energy cosmic rays from air showers using the atmospheric fluorescence from these showers. Accurate knowledge of the conversion from atmospheric fluorescence to energy loss by ionizing particles in the atmosphere is key to this technique. In this paper we discuss a small balloon-borne instrument to make the first in situ measurements versus altitude of the atmospheric fluorescence yield. The instrument can also be used in the lab to investigate the dependence of the fluorescence yield in air on temperature, pressure and the concentrations of other gases that present in the atmosphere. The results can be used to explore environmental effects on and improve the accuracy of cosmic ray energy measurements for existing ground-based experiments and future space-based experiments.
Deterministic quantum teleportation with atoms.
Riebe, M; Häffner, H; Roos, C F; Hänsel, W; Benhelm, J; Lancaster, G P T; Körber, T W; Becher, C; Schmidt-Kaler, F; James, D F V; Blatt, R
2004-06-17
Teleportation of a quantum state encompasses the complete transfer of information from one particle to another. The complete specification of the quantum state of a system generally requires an infinite amount of information, even for simple two-level systems (qubits). Moreover, the principles of quantum mechanics dictate that any measurement on a system immediately alters its state, while yielding at most one bit of information. The transfer of a state from one system to another (by performing measurements on the first and operations on the second) might therefore appear impossible. However, it has been shown that the entangling properties of quantum mechanics, in combination with classical communication, allow quantum-state teleportation to be performed. Teleportation using pairs of entangled photons has been demonstrated, but such techniques are probabilistic, requiring post-selection of measured photons. Here, we report deterministic quantum-state teleportation between a pair of trapped calcium ions. Following closely the original proposal, we create a highly entangled pair of ions and perform a complete Bell-state measurement involving one ion from this pair and a third source ion. State reconstruction conditioned on this measurement is then performed on the other half of the entangled pair. The measured fidelity is 75%, demonstrating unequivocally the quantum nature of the process.
Quantum strategies of quantum measurements
NASA Astrophysics Data System (ADS)
Li, Chuan-Feng; Zhang, Yong-Sheng; Huang, Yun-Feng; Guo, Guang-Can
2001-03-01
In the classical Monty Hall problem, one player can always win with probability 2/3. We generalize the problem to the quantum domain and show that a fair two-party zero-sum game can be carried out if the other player is permitted to adopt quantum measurement strategy.
Quantum physics without quantum philosophy
NASA Astrophysics Data System (ADS)
Dürr, Detlef; Goldstein, Sheldon; Zanghì, Nino
Quantum philosophy, a peculiar twentieth-century malady, is responsible for most of the conceptual muddle plaguing the foundations of quantum physics. When this philosophy is eschewed, one naturally arrives at Bohmian mechanics, which is what emerges from Schrödinger's equation for a nonrelativistic system of particles when we merely insist that 'particles' means particles. While distinctly non-Newtonian, Bohmian mechanics is a fully deterministic theory of particles in motion, a motion choreographed by the wave function. The quantum formalism emerges when measurement situations are analyzed according to this theory. When the quantum formalism is regarded as arising in this way, the paradoxes and perplexities so often associated with quantum theory simply evaporate.
Photodestruction Quantum Yield of Adenine in Aqueous Solution.
ERIC Educational Resources Information Center
Rivera, Mercedes
1989-01-01
In this article, background information on the photochemical properties of nucleic acids is provided and an experiment to illustrate this concept is presented. Sample preparation, procedures, and data analysis are discussed. Sample UV absorption spectra are included. (CW)
The Quantum Yield of NO3 from Peroxyacetyl Nitrate Photolysis
NASA Technical Reports Server (NTRS)
Mazely, Troy L.; Friedl, Randall R.; Sander, Stanley P.
1997-01-01
Peroxyacetyl nitrate (PAN) vapor was photolyzed at 248nm and the NO3 photoproduct was detected by laser induced fluorescence. The excited state flourescence contributions were investigated and a data analysis methodology was established to minimize their effects.
Observable Measure of Quantum Coherence in Finite Dimensional Systems
NASA Astrophysics Data System (ADS)
Girolami, Davide
2014-10-01
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.
Observable measure of quantum coherence in finite dimensional systems.
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.
Observable measure of quantum coherence in finite dimensional systems.
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. PMID:25379903
Regular and chaotic quantum dynamics in atom-diatom reactive collisions
Gevorkyan, A. S.; Nyman, G.
2008-05-15
A new microirreversible 3D theory of quantum multichannel scattering in the three-body system is developed. The quantum approach is constructed on the generating trajectory tubes which allow taking into account influence of classical nonintegrability of the dynamical quantum system. When the volume of classical chaos in phase space is larger than the quantum cell in the corresponding quantum system, quantum chaos is generated. The probability of quantum transitions is constructed for this case. The collinear collision of the Li + (FH) {sup {yields}}(LiF) + H system is used for numerical illustration of a system generating quantum (wave) chaos.
ERIC Educational Resources Information Center
Peterson, Ivars
1989-01-01
An analogy from the game of baseball can be used to examine the philosophy involved in statistics surrounding quantum mechanical events. The "Strong Baseball Principle" is proposed and discussed. (CW)
NASA Astrophysics Data System (ADS)
Stapp, Henry P.
2012-05-01
Robert Griffiths has recently addressed, within the framework of a `consistent quantum theory' that he has developed, the issue of whether, as is often claimed, quantum mechanics entails a need for faster-than-light transfers of information over long distances. He argues that the putative proofs of this property that involve hidden variables include in their premises some essentially classical-physics-type assumptions that are not entailed by the precepts of quantum mechanics. Thus whatever is proved is not a feature of quantum mechanics, but is a property of a theory that tries to combine quantum theory with quasi-classical features that go beyond what is entailed by quantum theory itself. One cannot logically prove properties of a system by establishing, instead, properties of a system modified by adding properties alien to the original system. Hence Griffiths' rejection of hidden-variable-based proofs is logically warranted. Griffiths mentions the existence of a certain alternative proof that does not involve hidden variables, and that uses only macroscopically described observable properties. He notes that he had examined in his book proofs of this general kind, and concluded that they provide no evidence for nonlocal influences. But he did not examine the particular proof that he cites. An examination of that particular proof by the method specified by his `consistent quantum theory' shows that the cited proof is valid within that restrictive version of quantum theory. An added section responds to Griffiths' reply, which cites general possibilities of ambiguities that might make what is to be proved ill-defined, and hence render the pertinent `consistent framework' ill defined. But the vagaries that he cites do not upset the proof in question, which, both by its physical formulation and by explicit identification, specify the framework to be used. Griffiths confirms the validity of the proof insofar as that pertinent framework is used. The section also shows
Quantum correlations and distinguishability of quantum states
Spehner, Dominique
2014-07-15
A survey of various concepts in quantum information is given, with a main emphasis on the distinguishability of quantum states and quantum correlations. Covered topics include generalized and least square measurements, state discrimination, quantum relative entropies, the Bures distance on the set of quantum states, the quantum Fisher information, the quantum Chernoff bound, bipartite entanglement, the quantum discord, and geometrical measures of quantum correlations. The article is intended both for physicists interested not only by collections of results but also by the mathematical methods justifying them, and for mathematicians looking for an up-to-date introductory course on these subjects, which are mainly developed in the physics literature.
NASA Astrophysics Data System (ADS)
Grinberg, Horacio; Freed, Karl F.; Williams, Carl J.
1997-08-01
The analytical infinite order sudden (IOS) quantum theory of triatomic photodissociation, developed in paper I, is applied to study the indirect photodissociation of NOCl through a real or virtual intermediate state. The theory uses the IOS approximation for the dynamics in the final dissociative channels and an Airy function approximation for the continuum functions. The transition is taken as polarized in the plane of the molecule; symmetric top wave functions are used for both the initial and intermediate bound states; and simple semiempirical model potentials are employed for each state. The theory provides analytical expressions for the photofragment yield spectrum for producing particular final fragment ro-vibrational states as a function of the photon excitation energy. Computations are made of the photofragment excitation spectrum of NOCl in the region of the T1(13A″)←S0(11A') transition for producing the NO fragment in the vibrational states nNO=0, 1, and 2. The computed spectra for the unexcited nNO==0 and excited nNO=2 states are in reasonable agreement with experiment. However, some discrepancies are observed for the singly excited nNO=1 vibrational state, indicating deficiencies in the semiempirical potential energy surface. Computations for two different orientations of the in-plane transition dipole moment produce very similar excitation spectra. Calculations of fragment rotational distributions are performed for high values of the total angular momentum J, a feature that would be very difficult to perform with close-coupled methods. Computations are also made of the thermally averaged rotational energy distributions to simulate the conditions in actual supersonic jet experiments.
Nation, L.M.
1992-01-01
This paper briefly reviews a lawsuit which is under appeal by the State of Michigan regarding a takings claim filed over a petroleum exploration site. The dispute arose as a result of a 1987 decision by the Michigan Department of Natural Resources forbidding the property owners from developing the mineral rights leased to Miller Brothers in the Huron/Manistee National Forest. This area is bisected by a trend of Silurian Niagaran reef complexes which has a known production history throughout the State. The dunes area of the national forest has been deemed a wilderness area. As a result of the State's decision, the courts have awarded a sum of 71 million dollars to the developer to cover damages and lost resources. The reserve estimates were taken from adjacent areas which showed that the Niagaran reefs are relatively consistent in their yield.
Rebuilding mathematics on a quantum logical foundation
NASA Astrophysics Data System (ADS)
DeJonghe, Richard J., III
We construct a rich first-order quantum logic which generalizes the standard classical predicate logic used in the development of virtually all of modern mathematics, and we use this quantum logic to build the foundations of a new quantum mathematics. First, we prove both soundness and completeness for the quantum logic we develop, and also prove a powerful new completeness result which heretofore had been known to hold for classical, but not quantum, first-order logic. We then use our quantum logic to develop multiple areas of mathematics, including abstract algebra, axiomatic set theory, and arithmetic. In some preliminary investigations into quantum mathematics, Dunn found that the Peano axioms for arithmetic yield the same theorems using either classical or quantum logic. We prove a similar result for certain classes of abstract algebras, and then show that Dunn's result is not generic by presenting examples of quantum monoids, groups, lattices, vector spaces, and operator algebras, all which differ from their classical counterparts. Moreover, we find natural classes of quantum lattices, vector spaces, and operator algebras which all have a beautiful inter-relationship, and make some preliminary investigations into using these structures as a basis for a new mathematical formulation of quantum mechanics. We also develop a quantum set theory (equivalent to ZFC under classical logic) which is far more tractable than quantum set theory previously developed. We then use this set theory to construct a quantum version of the natural numbers, and develop an arithmetic of these numbers based upon an alternative to Peano's axioms (which avoids Dunn's theorem). Surprisingly, we find that these "quantum natural numbers" satisfy our arithmetical axioms if and only if the underlying truth values form a modular lattice, giving a new arithmetical characterization of this important lattice-theoretic property. Finally, we show that these numbers have a natural interpretation as
NASA Astrophysics Data System (ADS)
Mandl, F.
1992-07-01
The Manchester Physics Series General Editors: D. J. Sandiford; F. Mandl; A. C. Phillips Department of Physics and Astronomy, University of Manchester Properties of Matter B. H. Flowers and E. Mendoza Optics Second Edition F. G. Smith and J. H. Thomson Statistical Physics Second Edition F. Mandl Electromagnetism Second Edition I. S. Grant and W. R. Phillips Statistics R. J. Barlow Solid State Physics Second Edition J. R. Hook and H. E. Hall Quantum Mechanics F. Mandl Particle Physics Second Edition B. R. Martin and G. Shaw The Physics of Stars Second Edition A. C. Phillips Computing for Scientists R. J. Barlow and A. R. Barnett Quantum Mechanics aims to teach those parts of the subject which every physicist should know. The object is to display the inherent structure of quantum mechanics, concentrating on general principles and on methods of wide applicability without taking them to their full generality. This book will equip students to follow quantum-mechanical arguments in books and scientific papers, and to cope with simple cases. To bring the subject to life, the theory is applied to the all-important field of atomic physics. No prior knowledge of quantum mechanics is assumed. However, it would help most readers to have met some elementary wave mechanics before. Primarily written for students, it should also be of interest to experimental research workers who require a good grasp of quantum mechanics without the full formalism needed by the professional theorist. Quantum Mechanics features: A flow diagram allowing topics to be studied in different orders or omitted altogether. Optional "starred" and highlighted sections containing more advanced and specialized material for the more ambitious reader. Sets of problems at the end of each chapter to help student understanding. Hints and solutions to the problems are given at the end of the book.
Introduction to Quantum Simulation
NASA Technical Reports Server (NTRS)
Williams, Colin P.
2005-01-01
This viewgraph presentation addresses the problem of efficiently simulating the evolution of a quantum system. The contents include: 1) Quantum Simulation; 2) Extracting Answers from Quantum Simulations; 3) Quantum Fourier Transform; 4) Eigenvalue Estimation; 5) Fermionic Simulations.
Quantum Physics for Beginners.
ERIC Educational Resources Information Center
Strand, J.
1981-01-01
Suggests a new approach for teaching secondary school quantum physics. Reviews traditional approaches and presents some characteristics of the three-part "Quantum Physics for Beginners" project, including: quantum physics, quantum mechanics, and a short historical survey. (SK)
NASA Astrophysics Data System (ADS)
Le Bellac, Michel
2006-03-01
Quantum physics allows us to understand the nature of the physical phenomena which govern the behavior of solids, semi-conductors, lasers, atoms, nuclei, subnuclear particles and light. In Quantum Physics, Le Bellac provides a thoroughly modern approach to this fundamental theory. Throughout the book, Le Bellac teaches the fundamentals of quantum physics using an original approach which relies primarily on an algebraic treatment and on the systematic use of symmetry principles. In addition to the standard topics such as one-dimensional potentials, angular momentum and scattering theory, the reader is introduced to more recent developments at an early stage. These include a detailed account of entangled states and their applications, the optical Bloch equations, the theory of laser cooling and of magneto-optical traps, vacuum Rabi oscillations, and an introduction to open quantum systems. This is a textbook for a modern course on quantum physics, written for advanced undergraduate and graduate students. Completely original and contemporary approach, using algebra and symmetry principles Introduces recent developments at an early stage, including many topics that cannot be found in standard textbooks. Contains 130 physically relevant exercises
Kendon, Viv
2014-12-04
Quantum versions of random walks have diverse applications that are motivating experimental implementations as well as theoretical studies. Recent results showing quantum walks are “universal for quantum computation” relate to algorithms, to be run on quantum computers. We consider whether an experimental implementation of a quantum walk could provide useful computation before we have a universal quantum computer.
NASA Astrophysics Data System (ADS)
Paek, Seung Weon; Kang, Jae Hyun; Ha, Naya; Kim, Byung-Moo; Jang, Dae-Hyun; Jeon, Junsu; Kim, DaeWook; Chung, Kun Young; Yu, Sung-eun; Park, Joo Hyun; Bae, SangMin; Song, DongSup; Noh, WooYoung; Kim, YoungDuck; Song, HyunSeok; Choi, HungBok; Kim, Kee Sup; Choi, Kyu-Myung; Choi, Woonhyuk; Jeon, JoongWon; Lee, JinWoo; Kim, Ki-Su; Park, SeongHo; Chung, No-Young; Lee, KangDuck; Hong, YoungKi; Kim, BongSeok
2012-03-01
A set of design for manufacturing (DFM) techniques have been developed and applied to 45nm, 32nm and 28nm logic process technologies. A noble technology combined a number of potential confliction of DFM techniques into a comprehensive solution. These techniques work in three phases for design optimization and one phase for silicon diagnostics. In the DFM prevention phase, foundation IP such as standard cells, IO, and memory and P&R tech file are optimized. In the DFM solution phase, which happens during ECO step, auto fixing of process weak patterns and advanced RC extraction are performed. In the DFM polishing phase, post-layout tuning is done to improve manufacturability. DFM analysis enables prioritization of random and systematic failures. The DFM technique presented in this paper has been silicon-proven with three successful tape-outs in Samsung 32nm processes; about 5% improvement in yield was achieved without any notable side effects. Visual inspection of silicon also confirmed the positive effect of the DFM techniques.
Secondary Electron Emission Yields
NASA Technical Reports Server (NTRS)
Krainsky, I.; Lundin, W.; Gordon, W. L.; Hoffman, R. W.
1981-01-01
The secondary electron emission (SEE) characteristics for a variety of spacecraft materials were determined under UHV conditions using a commercial double pass CMA which permits sequential Auger electron electron spectroscopic analysis of the surface. The transparent conductive coating indium tin oxide (ITO) was examined on Kapton and borosilicate glass and indium oxide on FED Teflon. The total SEE coefficient ranges from 2.5 to 2.6 on as-received surfaces and from 1.5 to 1.6 on Ar(+) sputtered surfaces with 5 nm removed. A cylindrical sample carousel provides normal incidence of the primary beam as well as a multiple Faraday cup measurement of the approximately nA beam currents. Total and true secondary yields are obtained from target current measurements with biasing of the carousel. A primary beam pulsed mode to reduce electron beam dosage and minimize charging of insulating coatings was applied to Mg/F2 coated solar cell covers. Electron beam effects on ITO were found quite important at the current densities necessary to do Auger studies.
Universal quantum computation with a nonlinear oscillator network
NASA Astrophysics Data System (ADS)
Goto, Hayato
2016-05-01
We theoretically show that a nonlinear oscillator network with controllable parameters can be used for universal quantum computation. The initialization is achieved by a quantum-mechanical bifurcation based on quantum adiabatic evolution, which yields a Schrödinger cat state. All the elementary quantum gates are also achieved by quantum adiabatic evolution, in which dynamical phases accompanying the adiabatic evolutions are controlled by the system parameters. Numerical simulation results indicate that high gate fidelities can be achieved, where no dissipation is assumed.
Complementarity of quantum discord and classically accessible information
Zwolak, Michael P.; Zurek, Wojciech H.
2013-05-20
The sum of the Holevo quantity (that bounds the capacity of quantum channels to transmit classical information about an observable) and the quantum discord (a measure of the quantumness of correlations of that observable) yields an observable-independent total given by the quantum mutual information. This split naturally delineates information about quantum systems accessible to observers – information that is redundantly transmitted by the environment – while showing that it is maximized for the quasi-classical pointer observable. Other observables are accessible only via correlations with the pointer observable. In addition, we prove an anti-symmetry property relating accessible information and discord. It shows that information becomes objective – accessible to many observers – only as quantum information is relegated to correlations with the global environment, and, therefore, locally inaccessible. Lastly, the resulting complementarity explains why, in a quantum Universe, we perceive objective classical reality while flagrantly quantum superpositions are out of reach.
Complementarity of quantum discord and classically accessible information
Zwolak, Michael P.; Zurek, Wojciech H.
2013-05-20
The sum of the Holevo quantity (that bounds the capacity of quantum channels to transmit classical information about an observable) and the quantum discord (a measure of the quantumness of correlations of that observable) yields an observable-independent total given by the quantum mutual information. This split naturally delineates information about quantum systems accessible to observers – information that is redundantly transmitted by the environment – while showing that it is maximized for the quasi-classical pointer observable. Other observables are accessible only via correlations with the pointer observable. In addition, we prove an anti-symmetry property relating accessible information and discord. Itmore » shows that information becomes objective – accessible to many observers – only as quantum information is relegated to correlations with the global environment, and, therefore, locally inaccessible. Lastly, the resulting complementarity explains why, in a quantum Universe, we perceive objective classical reality while flagrantly quantum superpositions are out of reach.« less
Complementarity of quantum discord and classically accessible information
Zwolak, Michael; Zurek, Wojciech H.
2013-01-01
The sum of the Holevo quantity (that bounds the capacity of quantum channels to transmit classical information about an observable) and the quantum discord (a measure of the quantumness of correlations of that observable) yields an observable-independent total given by the quantum mutual information. This split naturally delineates information about quantum systems accessible to observers – information that is redundantly transmitted by the environment – while showing that it is maximized for the quasi-classical pointer observable. Other observables are accessible only via correlations with the pointer observable. We also prove an anti-symmetry property relating accessible information and discord. It shows that information becomes objective – accessible to many observers – only as quantum information is relegated to correlations with the global environment, and, therefore, locally inaccessible. The resulting complementarity explains why, in a quantum Universe, we perceive objective classical reality while flagrantly quantum superpositions are out of reach.
NASA Astrophysics Data System (ADS)
Sych, Denis; Leuchs, Gerd
2015-12-01
Classical physics allows for the existence of pairs of absolutely identical systems. Pairwise application of identical measurements to each of those systems always leads to exactly alike results irrespectively of the choice of measurements. Here we ask a question how the picture looks like in the quantum domain. Surprisingly, we get a counterintuitive outcome. Pairwise application of identical (but a priori unknown) measurements cannot always lead to exactly alike results. We interpret this as quantum uniqueness—a feature that has no classical analog.
Lincoln, Don
2014-10-24
The laws of quantum mechanics and relativity are quite perplexing however it is when the two theories are merged that things get really confusing. This combined theory predicts that empty space isn’t empty at all – it’s a seething and bubbling cauldron of matter and antimatter particles springing into existence before disappearing back into nothingness. Scientists call this complicated state of affairs “quantum foam.” In this video, Fermilab’s Dr. Don Lincoln discusses this mind-bending idea and sketches some of the experiments that have convinced scientists that this crazy prediction is actually true.
Quantum control limited by quantum decoherence
Xue, Fei; Sun, C. P.; Yu, S. X.
2006-01-15
We describe quantum controllability under the influences of the quantum decoherence induced by the quantum control itself. It is shown that, when the controller is considered as a quantum system, it will entangle with its controlled system and then cause quantum decoherence in the controlled system. In competition with this induced decoherence, the controllability will be limited by some uncertainty relation in a well-armed quantum control process. In association with the phase uncertainty and the standard quantum limit, a general model is studied to demonstrate the possibility of realizing a decoherence-free quantum control with a finite energy within a finite time. It is also shown that if the operations of quantum control are to be determined by the initial state of the controller, then due to the decoherence which results from the quantum control itself, there exists a low bound for quantum controllability.
Brightness-equalized quantum dots
Lim, Sung Jun; Zahid, Mohammad U.; Le, Phuong; Ma, Liang; Entenberg, David; Harney, Allison S.; Condeelis, John; Smith, Andrew M.
2015-01-01
As molecular labels for cells and tissues, fluorescent probes have shaped our understanding of biological structures and processes. However, their capacity for quantitative analysis is limited because photon emission rates from multicolour fluorophores are dissimilar, unstable and often unpredictable, which obscures correlations between measured fluorescence and molecular concentration. Here we introduce a new class of light-emitting quantum dots with tunable and equalized fluorescence brightness across a broad range of colours. The key feature is independent tunability of emission wavelength, extinction coefficient and quantum yield through distinct structural domains in the nanocrystal. Precise tuning eliminates a 100-fold red-to-green brightness mismatch of size-tuned quantum dots at the ensemble and single-particle levels, which substantially improves quantitative imaging accuracy in biological tissue. We anticipate that these materials engineering principles will vastly expand the optical engineering landscape of fluorescent probes, facilitate quantitative multicolour imaging in living tissue and improve colour tuning in light-emitting devices. PMID:26437175
Yengoh, Genesis T; Ardö, Jonas
2014-03-01
Although food crop yields per hectare have generally been increasing in Cameroon since 1961, the food price crisis of 2008 and the ensuing social unrest and fatalities raised concerns about the country's ability to meet the food needs of its population. This study examines the country's potential for increasing crop yields and food production to meet this food security challenge. Fuzzy set theory is used to develop a biophysical spatial suitability model for different crops, which in turn is employed to ascertain whether crop production is carried out in biophysically suited areas. We use linear regression to examine the trend of yield development over the last half century. On the basis of yield data from experimental stations and farmers' fields we assess the yield gap for major food crops. We find that yields have generally been increasing over the last half century and that agricultural policies can have significant effects on them. To a large extent, food crops are cultivated in areas that are biophysically suited for their cultivation, meaning that the yield gap is not a problem of biophysical suitability. Notwithstanding, there are significantly large yield gaps between actual yields on farmers' farms and maximum attainable yields from research stations. We conclude that agronomy and policies are likely to be the reasons for these large yield gaps. A key challenge to be addressed in closing the yield gaps is that of replenishing and properly managing soil nutrients.
2015-01-01
The glmS ribozyme catalyzes a self-cleavage reaction at the phosphodiester bond between residues A-1 and G1. This reaction is thought to occur by an acid–base mechanism involving the glucosamine-6-phosphate cofactor and G40 residue. Herein quantum mechanical/molecular mechanical free energy simulations and pKa calculations, as well as experimental measurements of the rate constant for self-cleavage, are utilized to elucidate the mechanism, particularly the role of G40. Our calculations suggest that an external base deprotonates either G40(N1) or possibly A-1(O2′), which would be followed by proton transfer from G40(N1) to A-1(O2′). After this initial deprotonation, A-1(O2′) starts attacking the phosphate as a hydroxyl group, which is hydrogen-bonded to deprotonated G40, concurrent with G40(N1) moving closer to the hydroxyl group and directing the in-line attack. Proton transfer from A-1(O2′) to G40 is concomitant with attack of the scissile phosphate, followed by the remainder of the cleavage reaction. A mechanism in which an external base does not participate, but rather the proton transfers from A-1(O2′) to a nonbridging oxygen during nucleophilic attack, was also considered but deemed to be less likely due to its higher effective free energy barrier. The calculated rate constant for the favored mechanism is in agreement with the experimental rate constant measured at biological Mg2+ ion concentration. According to these calculations, catalysis is optimal when G40 has an elevated pKa rather than a pKa shifted toward neutrality, although a balance among the pKa’s of A-1, G40, and the nonbridging oxygen is essential. These results have general implications, as the hammerhead, hairpin, and twister ribozymes have guanines at a similar position as G40. PMID:25526516
Bifurcation-based adiabatic quantum computation with a nonlinear oscillator network
NASA Astrophysics Data System (ADS)
Goto, Hayato
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 its bifurcation with a slowly varying parameter. 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. To distinguish them, we refer to the present approach as bifurcation-based adiabatic quantum computation. Our numerical simulation results suggest that quantum superposition and quantum fluctuation work effectively to find optimal solutions.
Sassoli de Bianchi, Massimiliano
2013-09-15
In a letter to Born, Einstein wrote [42]: “Quantum mechanics is certainly imposing. But an inner voice tells me that it is not yet the real thing. The theory says a lot, but does not really bring us any closer to the secret of the ‘old one.’ I, at any rate, am convinced that He does not throw dice.” In this paper we take seriously Einstein’s famous metaphor, and show that we can gain considerable insight into quantum mechanics by doing something as simple as rolling dice. More precisely, we show how to perform measurements on a single die, to create typical quantum interference effects, and how to connect (entangle) two identical dice, to maximally violate Bell’s inequality. -- Highlights: •Rolling a die is a quantum process admitting a Hilbert space representation. •Rolling experiments with a single die can produce interference effects. •Two connected dice can violate Bell’s inequality. •Correlations need to be created by the measurement, to violate Bell’s inequality.
Visser, M. )
1991-01-15
This paper presents an application of quantum-mechanical principles to a microscopic variant of the traversable wormholes recently introduced by Morris and Thorne. The analysis, based on the surgical grafting of two Reissner-Nordstroem spacetimes, proceeds by using a minisuperspace model to approximate the geometry of these wormholes. The thin shell'' formalism is applied to this minisuperspace model to extract the effective Lagrangian appropriate to this one-degree-of-freedom system. This effective Lagrangian is then quantized and the wave function for the wormhole is explicitly exhibited. A slightly more general class of wormholes---corresponding to the addition of some dust'' to the wormhole throat---is analyzed by recourse to WKB techniques. In all cases discussed in this paper, the expectation value of the wormhole radius is calculated to be of the order of the Planck length. Accordingly, though these quantum wormholes are of considerable theoretical interest they do not appear to be useful as a means for interstellar travel. The results of this paper may also have a bearing on the question of topological fluctuations in quantum gravity. These calculations serve to suggest that topology-changing effects might in fact be {ital suppressed} by quantum-gravity effects.
NASA Astrophysics Data System (ADS)
Cheon, Taksu; Tsutsui, Izumi; Fülöp, Tamás
2004-09-01
We show that the point interactions on a line can be utilized to provide U(2) family of qubit operations for quantum information processing. Qubits are realized as states localized in either side of the point interaction which represents a controllable gate. The qubit manipulation proceeds in a manner analogous to the operation of an abacus.
NASA Astrophysics Data System (ADS)
Goradia, Shantilal
2009-11-01
The continuing search for quantum gravity and never ending attempts to unify gravity with other forces of nature represent tremendous waste of public and private funds directing students' energy towards non-creative manipulative work instead of learning from the scientific creativity in Einstein's 1919 paper that unifies gravity with nuclear force. It reflects Einstein's 1919 jump beyond his own 1915 theory of gravity, including that of Newton as implicitly demanded by Newton in 1686. Einstein corrected and retracted his 1917 introduction of cosmological constant in 1919. Dislike of the fact that Einstein did not use quantum mechanics to prove his point has no real value now, because we will use key ingredients (Planck scale and probabilistic aspect) of quantum mechanics and show that they reach the same conclusion. Newton explained the solar system known after Kepler. Likewise, our quantum mechanical approach explains the strong coupling as well the solar system and shows new horizons, otherwise unexplained. Explanation of unexplained observations need no prediction per Hawking, and obviously otherwise.
NASA Technical Reports Server (NTRS)
Dowling, Jonathan P.
2000-01-01
Recently, several researchers, including yours truly, have been able to demonstrate theoretically that quantum photon entanglement has the potential to also revolutionize the entire field of optical interferometry, by providing many orders of magnitude improvement in interferometer sensitivity. The quantum entangled photon interferometer approach is very general and applies to many types of interferometers. In particular, without nonlocal entanglement, a generic classical interferometer has a statistical-sampling shot-noise limited sensitivity that scales like 1/Sqrt[N], where N is the number of particles (photons, electrons, atoms, neutrons) passing through the interferometer per unit time. However, if carefully prepared quantum correlations are engineered between the particles, then the interferometer sensitivity improves by a factor of Sqrt[N] (square root of N) to scale like 1/N, which is the limit imposed by the Heisenberg Uncertainty Principle. For optical (laser) interferometers operating at milliwatts of optical power, this quantum sensitivity boost corresponds to an eight-order-of-magnitude improvement of signal to noise. Applications are to tests of General Relativity such as ground and orbiting optical interferometers for gravity wave detection, Laser Interferometer Gravity Observatory (LIGO) and the European Laser Interferometer Space Antenna (LISA), respectively.
Faraggi, A.E.; Matone, M.
1998-01-09
We show that the quantum Hamilton-Jacobi equation can be written in the classical form with the spatial derivative {partial_derivative}{sub q} replaced by {partial_derivative}{sub q} with dq = dq/{radical}1{minus}{beta}{sup 2}(q), where {beta}{sup 2}(q) is strictly related to the quantum potential. This can be seen as the opposite of the problem of finding the wave function representation of classical mechanics as formulated by Schiller and Rosen. The structure of the above {open_quotes}quantum transformation{close_quotes}, related to the recently formulated equivalence principle, indicates that the potential deforms space geometry. In particular, a result by Flanders implies that both W(q) = V(q) {minus} E and the quantum potential Q are proportional to the curvatures {kappa}{sub W} and {kappa}{sub Q} which arise as natural invariants in an equivalence problem for curves in the projective line. In this formulation the Schroedinger equation takes the geometrical form ({partial_derivative}{sub q}{sup 2} + {kappa}{sub W}){psi} = 0.
NASA Astrophysics Data System (ADS)
Lanzagorta, Marco O.; Gomez, Richard B.; Uhlmann, Jeffrey K.
2003-08-01
In recent years, computer graphics has emerged as a critical component of the scientific and engineering process, and it is recognized as an important computer science research area. Computer graphics are extensively used for a variety of aerospace and defense training systems and by Hollywood's special effects companies. All these applications require the computer graphics systems to produce high quality renderings of extremely large data sets in short periods of time. Much research has been done in "classical computing" toward the development of efficient methods and techniques to reduce the rendering time required for large datasets. Quantum Computing's unique algorithmic features offer the possibility of speeding up some of the known rendering algorithms currently used in computer graphics. In this paper we discuss possible implementations of quantum rendering algorithms. In particular, we concentrate on the implementation of Grover's quantum search algorithm for Z-buffering, ray-tracing, radiosity, and scene management techniques. We also compare the theoretical performance between the classical and quantum versions of the algorithms.
Quantum critical scaling in graphene.
Sheehy, Daniel E; Schmalian, Jörg
2007-11-30
We show that the emergent relativistic symmetry of electrons in graphene near its quantum critical point (QCP) implies a crucial importance of the Coulomb interaction. We derive scaling laws, valid near the QCP, that dictate the nontrivial magnetic and charge response of interacting graphene. Our analysis yields numerous predictions for how the Coulomb interaction will be manifested in experimental observables such as the diamagnetic response and electronic compressibility. PMID:18233313
Teleportation-induced correlated quantum channels.
Caruso, F; Giovannetti, V; Palma, G M
2010-01-15
Quantum teleportation of an n-qubit state performed using as an entangled resource a general bipartite state of 2n qubits instead of n Bell states is equivalent to a correlated Pauli channel. This yields a new characterization of such channels in terms of many-body correlation functions of the teleporting media. It provides a relatively simple method for determining whether a correlated quantum channel is able to reliably convey quantum messages by studying the entanglement properties of the teleportation mediating system. Our model is then generalized to the continuous-variable case.
Quantum roulette: an extended quantum strategy
NASA Astrophysics Data System (ADS)
Wang, Xiang-Bin; Kwek, L. C.; Oh, C. H.
2000-12-01
In a recent paper, Meyer demonstrated that with a quantum computer, an analogous zero-sum classically strategic game played with quantum strategy essentially become a bias game under a mixture of quantum and classical strategy. To illustrate his point, Meyer used a quantum coin tossing event. In this Letter, we generalize Meyer's argument to an N-state game.
Quantum state and quantum entanglement protection using quantum measurements
NASA Astrophysics Data System (ADS)
Wang, Shuchao; Li, Ying; Wang, Xiangbin; Kwek, Leong Chuan; Yu, Zongwen; Zou, Wenjie
2015-03-01
The time evolution of some quantum states can be slowed down or even stopped under frequent measurements. This is the usual quantum Zeno effect. Here we report an operator quantum Zeno effect, in which the evolution of some physical observables is slowed down through measurements even though thequantum state changes randomly with time. Based on the operator quantum Zeno effect, we show how we can protect quantum information from decoherence with two-qubit measurements, realizable with noisy two-qubit interactions. Besides, we report the quantum entanglement protection using weak measurement and measurement reversal scheme. Exposed in the nonzero temperature environment, a quantum system can both lose and gain excitations by interacting with the environment. In this work, we show how to optimally protect quantum states and quantum entanglement in such a situation based on measurement reversal from weak measurement. In particular, we present explicit formulas of protection. We find that this scheme can circumvent the entanglement sudden death in certain conditions.
Invariant-mass distribution of cc in {upsilon}(1S){yields}cc+X
Chung, Hee Sok; Kim, Taewon; Lee, Jungil
2008-12-01
We calculate the invariant-mass distribution for the cc pair produced in the inclusive {upsilon}(1S) decay based on the color-singlet mechanism of the nonrelativistic quantum chromodynamics factorization approach at leading order in the bottom-quark velocity v{sub b} in the meson rest frame. As the short-distance processes, we consider bb{yields}g*gg followed by g*{yields}cc and bb{yields}{gamma}*{yields}cc at leading order in the strong coupling. The invariant-mass distribution of the bb{yields}ccgg contribution has a sharp peak just above the threshold and that of the bb{yields}{gamma}*{yields}cc channel is concentrated at the maximally allowed kinematic end point. We predict that {gamma}[{upsilon}(1S){yields}cc+X]/{gamma}[{upsilon}(1S){yields}light hadrons]=(0.065{+-}0.048){alpha}{sub s}, which is in agreement with a previous result within errors.
Efficient quantum walk on a quantum processor.
Qiang, Xiaogang; Loke, Thomas; Montanaro, Ashley; Aungskunsiri, Kanin; Zhou, Xiaoqi; O'Brien, Jeremy L; Wang, Jingbo B; Matthews, Jonathan C F
2016-01-01
The random walk formalism is used across a wide range of applications, from modelling share prices to predicting population genetics. Likewise, quantum walks have shown much potential as a framework for developing new quantum algorithms. Here we present explicit efficient quantum circuits for implementing continuous-time quantum walks on the circulant class of graphs. These circuits allow us to sample from the output probability distributions of quantum walks on circulant graphs efficiently. We also show that solving the same sampling problem for arbitrary circulant quantum circuits is intractable for a classical computer, assuming conjectures from computational complexity theory. This is a new link between continuous-time quantum walks and computational complexity theory and it indicates a family of tasks that could ultimately demonstrate quantum supremacy over classical computers. As a proof of principle, we experimentally implement the proposed quantum circuit on an example circulant graph using a two-qubit photonics quantum processor. PMID:27146471
Efficient quantum walk on a quantum processor
NASA Astrophysics Data System (ADS)
Qiang, Xiaogang; Loke, Thomas; Montanaro, Ashley; Aungskunsiri, Kanin; Zhou, Xiaoqi; O'Brien, Jeremy L.; Wang, Jingbo B.; Matthews, Jonathan C. F.
2016-05-01
The random walk formalism is used across a wide range of applications, from modelling share prices to predicting population genetics. Likewise, quantum walks have shown much potential as a framework for developing new quantum algorithms. Here we present explicit efficient quantum circuits for implementing continuous-time quantum walks on the circulant class of graphs. These circuits allow us to sample from the output probability distributions of quantum walks on circulant graphs efficiently. We also show that solving the same sampling problem for arbitrary circulant quantum circuits is intractable for a classical computer, assuming conjectures from computational complexity theory. This is a new link between continuous-time quantum walks and computational complexity theory and it indicates a family of tasks that could ultimately demonstrate quantum supremacy over classical computers. As a proof of principle, we experimentally implement the proposed quantum circuit on an example circulant graph using a two-qubit photonics quantum processor.
Efficient quantum walk on a quantum processor.
Qiang, Xiaogang; Loke, Thomas; Montanaro, Ashley; Aungskunsiri, Kanin; Zhou, Xiaoqi; O'Brien, Jeremy L; Wang, Jingbo B; Matthews, Jonathan C F
2016-05-05
The random walk formalism is used across a wide range of applications, from modelling share prices to predicting population genetics. Likewise, quantum walks have shown much potential as a framework for developing new quantum algorithms. Here we present explicit efficient quantum circuits for implementing continuous-time quantum walks on the circulant class of graphs. These circuits allow us to sample from the output probability distributions of quantum walks on circulant graphs efficiently. We also show that solving the same sampling problem for arbitrary circulant quantum circuits is intractable for a classical computer, assuming conjectures from computational complexity theory. This is a new link between continuous-time quantum walks and computational complexity theory and it indicates a family of tasks that could ultimately demonstrate quantum supremacy over classical computers. As a proof of principle, we experimentally implement the proposed quantum circuit on an example circulant graph using a two-qubit photonics quantum processor.
Efficient quantum walk on a quantum processor
Qiang, Xiaogang; Loke, Thomas; Montanaro, Ashley; Aungskunsiri, Kanin; Zhou, Xiaoqi; O'Brien, Jeremy L.; Wang, Jingbo B.; Matthews, Jonathan C. F.
2016-01-01
The random walk formalism is used across a wide range of applications, from modelling share prices to predicting population genetics. Likewise, quantum walks have shown much potential as a framework for developing new quantum algorithms. Here we present explicit efficient quantum circuits for implementing continuous-time quantum walks on the circulant class of graphs. These circuits allow us to sample from the output probability distributions of quantum walks on circulant graphs efficiently. We also show that solving the same sampling problem for arbitrary circulant quantum circuits is intractable for a classical computer, assuming conjectures from computational complexity theory. This is a new link between continuous-time quantum walks and computational complexity theory and it indicates a family of tasks that could ultimately demonstrate quantum supremacy over classical computers. As a proof of principle, we experimentally implement the proposed quantum circuit on an example circulant graph using a two-qubit photonics quantum processor. PMID:27146471
Quantum error correction for quantum memories
NASA Astrophysics Data System (ADS)
Terhal, Barbara M.
2015-04-01
Active quantum error correction using qubit stabilizer codes has emerged as a promising, but experimentally challenging, engineering program for building a universal quantum computer. In this review the formalism of qubit stabilizer and subsystem stabilizer codes and their possible use in protecting quantum information in a quantum memory are considered. The theory of fault tolerance and quantum error correction is reviewed, and examples of various codes and code constructions, the general quantum error-correction conditions, the noise threshold, the special role played by Clifford gates, and the route toward fault-tolerant universal quantum computation are discussed. The second part of the review is focused on providing an overview of quantum error correction using two-dimensional (topological) codes, in particular, the surface code architecture. The complexity of decoding and the notion of passive or self-correcting quantum memories are discussed. The review does not focus on a particular technology but discusses topics that will be relevant for various quantum technologies.
Complementarity relations for quantum coherence
NASA Astrophysics Data System (ADS)
Cheng, Shuming; Hall, Michael J. W.
2015-10-01
Various measures have been suggested recently for quantifying the coherence of a quantum state with respect to a given basis. We first use two of these, the l1-norm and relative entropy measures, to investigate tradeoffs between the coherences of mutually unbiased bases. Results include relations between coherence, uncertainty, and purity; tight general bounds restricting the coherences of mutually unbiased bases; and an exact complementarity relation for qubit coherences. We further define the average coherence of a quantum state. For the l1-norm measure this is related to a natural "coherence radius" for the state and leads to a conjecture for an l2-norm measure of coherence. For relative entropy the average coherence is determined by the difference between the von Neumann entropy and the quantum subentropy of the state and leads to upper bounds for the latter quantity. Finally, we point out that the relative entropy of coherence is a special case of G-asymmetry, which immediately yields several operational interpretations in contexts as diverse as frame alignment, quantum communication, and metrology, and suggests generalizing the property of quantum coherence to arbitrary groups of physical transformations.
Quantum random walks using quantum accelerator modes
Ma, Z.-Y.; Burnett, K.; D'Arcy, M. B.; Gardiner, S. A.
2006-01-15
We discuss the use of high-order quantum accelerator modes to achieve an atom optical realization of a biased quantum random walk. We first discuss how one can create coexistent quantum accelerator modes, and hence how momentum transfer that depends on the atoms' internal state can be achieved. When combined with microwave driving of the transition between the states, a different type of atomic beam splitter results. This permits the realization of a biased quantum random walk through quantum accelerator modes.
Yield: it's now an entitlement
NASA Astrophysics Data System (ADS)
George, Bill
1994-09-01
Only a few years ago, the primary method of cost reduction and productivity improvement in the semiconductor industry was increasing manufacturing yields throughout the process. Many of the remarkable reliability improvements realized over the past decade have come about as a result of actions that were originally taken primarily to improve device yields. Obviously, the practice of productivity improvement through yield enhancement is limited to the attainment of 100% yield, at which point some other mechanism must be employed. Traditionally, new products have been introduced to manufacturing at a point of relative immaturity, and semiconductor producers have relied on the traditional `learning curve' method of yield improvement to attain profitable levels of manufacturing yield. Recently, results of a survey of several fabs by a group of University of California at Berkeley researchers in the Competitive Semiconductor Manufacturing Program indicate that most factories learn at about the same rate after startup, in terms of both line yield and defectivity. If this is indeed generally true, then the most competitive factor is the one that starts with the highest yield, and it is difficult to displace a leader once his lead has been established. The two observations made above carry enormous implications for the semiconductor development or manufacturing professional. First, one must achieve very high yields in order to even play the game. Second, the achievement of competitive yields over time in the life of a factory is determined even before the factory is opened, in the planning and development phase. Third, and perhaps most uncomfortable for those of us who have relied on yield improvement as a cost driver, the winners of the nineties will find new levers to drive costs down, having already gotten the benefit of very high yield. This paper looks at the question of how the winners will achieve the critical measures of success, high initial yield and utilization
Noncommunting observables in quantum detection and estimation theory
NASA Technical Reports Server (NTRS)
Helstrom, C. W.
1971-01-01
In quantum detection theory the optimum detection operators must commute; admitting simultaneous approximate measurement of noncommuting observables cannot yield a lower Bayes cost. The lower bounds on mean square errors of parameter estimates predicted by the quantum-mechanical Cramer-Rao inequality can also not be reduced by such means.
Noncommuting observables in quantum detection and estimation theory
NASA Technical Reports Server (NTRS)
Helstrom, C. W.
1971-01-01
In quantum detection theory, the optimum detection operators must commute; admitting simultaneous approximate measurement of noncommuting observables cannot yield a lower Bayes cost. In addition, the lower bounds on mean square errors of parameter estimates, predicted by the quantum mechanical Cramer-Rao inequality, cannot be reduced by such means.
Quantum gate decomposition algorithms.
Slepoy, Alexander
2006-07-01
Quantum computing algorithms can be conveniently expressed in a format of a quantum logical circuits. Such circuits consist of sequential coupled operations, termed ''quantum gates'', or quantum analogs of bits called qubits. We review a recently proposed method [1] for constructing general ''quantum gates'' operating on an qubits, as composed of a sequence of generic elementary ''gates''.
Lincoln, Don
2016-07-12
The laws of quantum mechanics and relativity are quite perplexing however it is when the two theories are merged that things get really confusing. This combined theory predicts that empty space isnât empty at all â itâs a seething and bubbling cauldron of matter and antimatter particles springing into existence before disappearing back into nothingness. Scientists call this complicated state of affairs âquantum foam.â In this video, Fermilabâs Dr. Don Lincoln discusses this mind-bending idea and sketches some of the experiments that have convinced scientists that this crazy prediction is actually true.
Stapp, H.P.
1988-04-01
It is argued that the validity of the predictions of quantum theory in certain spin-correlation experiments entails a violation of Einstein's locality idea that no causal influence can act outside the forward light cone. First, two preliminary arguments suggesting such a violation are reviewed. They both depend, in intermediate stages, on the idea that the results of certain unperformed experiments are physically determinate. The second argument is entangled also with the problem of the meaning of physical reality. A new argument having neither of these characteristics is constructed. It is based strictly on the orthodox ideas of Bohr and Heisenberg, and has no realistic elements, or other ingredients, that are alien to orthodox quantum thinking.
NASA Astrophysics Data System (ADS)
Murdin, P.
2000-11-01
A development of quantum theory that was initiated in the 1920s by Werner Heisenberg (1901-76) and Erwin Schrödinger (1887-1961). The theory drew on a proposal made in 1925 Prince Louis de Broglie (1892-1987), that particles have wavelike properties (the wave-particle duality) and that an electron, for example, could in some respects be regarded as a wave with a wavelength that depended on its mo...
Efficient Quantum Information Processing via Quantum Compressions
NASA Astrophysics Data System (ADS)
Deng, Y.; Luo, M. X.; Ma, S. Y.
2016-01-01
Our purpose is to improve the quantum transmission efficiency and reduce the resource cost by quantum compressions. The lossless quantum compression is accomplished using invertible quantum transformations and applied to the quantum teleportation and the simultaneous transmission over quantum butterfly networks. New schemes can greatly reduce the entanglement cost, and partially solve transmission conflictions over common links. Moreover, the local compression scheme is useful for approximate entanglement creations from pre-shared entanglements. This special task has not been addressed because of the quantum no-cloning theorem. Our scheme depends on the local quantum compression and the bipartite entanglement transfer. Simulations show the success probability is greatly dependent of the minimal entanglement coefficient. These results may be useful in general quantum network communication.
Demonstration of Light-Matter Micro-Macro Quantum Correlations.
Tiranov, Alexey; Lavoie, Jonathan; Strassmann, Peter C; Sangouard, Nicolas; Afzelius, Mikael; Bussières, Félix; Gisin, Nicolas
2016-05-13
Quantum mechanics predicts microscopic phenomena with undeniable success. Nevertheless, current theoretical and experimental efforts still do not yield conclusive evidence that there is or is not a fundamental limitation on the possibility to observe quantum phenomena at the macroscopic scale. This question prompted several experimental efforts producing quantum superpositions of large quantum states in light or matter. We report on the observation of quantum correlations, revealed using an entanglement witness, between a single photon and an atomic ensemble of billions of ions frozen in a crystal. The matter part of the state involves the superposition of two macroscopically distinguishable solid-state components composed of several tens of atomic excitations. Assuming the insignificance of the time ordering our experiment indirectly shows light-matter micro-macro entanglement. Our approach leverages from quantum memory techniques and could be used in other systems to expand the size of quantum superpositions in matter. PMID:27232010
Deterministic generation of multiparticle entanglement by quantum Zeno dynamics.
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.
Demonstration of Light-Matter Micro-Macro Quantum Correlations.
Tiranov, Alexey; Lavoie, Jonathan; Strassmann, Peter C; Sangouard, Nicolas; Afzelius, Mikael; Bussières, Félix; Gisin, Nicolas
2016-05-13
Quantum mechanics predicts microscopic phenomena with undeniable success. Nevertheless, current theoretical and experimental efforts still do not yield conclusive evidence that there is or is not a fundamental limitation on the possibility to observe quantum phenomena at the macroscopic scale. This question prompted several experimental efforts producing quantum superpositions of large quantum states in light or matter. We report on the observation of quantum correlations, revealed using an entanglement witness, between a single photon and an atomic ensemble of billions of ions frozen in a crystal. The matter part of the state involves the superposition of two macroscopically distinguishable solid-state components composed of several tens of atomic excitations. Assuming the insignificance of the time ordering our experiment indirectly shows light-matter micro-macro entanglement. Our approach leverages from quantum memory techniques and could be used in other systems to expand the size of quantum superpositions in matter.
Demonstration of Light-Matter Micro-Macro Quantum Correlations
NASA Astrophysics Data System (ADS)
Tiranov, Alexey; Lavoie, Jonathan; Strassmann, Peter C.; Sangouard, Nicolas; Afzelius, Mikael; Bussières, Félix; Gisin, Nicolas
2016-05-01
Quantum mechanics predicts microscopic phenomena with undeniable success. Nevertheless, current theoretical and experimental efforts still do not yield conclusive evidence that there is or is not a fundamental limitation on the possibility to observe quantum phenomena at the macroscopic scale. This question prompted several experimental efforts producing quantum superpositions of large quantum states in light or matter. We report on the observation of quantum correlations, revealed using an entanglement witness, between a single photon and an atomic ensemble of billions of ions frozen in a crystal. The matter part of the state involves the superposition of two macroscopically distinguishable solid-state components composed of several tens of atomic excitations. Assuming the insignificance of the time ordering our experiment indirectly shows light-matter micro-macro entanglement. Our approach leverages from quantum memory techniques and could be used in other systems to expand the size of quantum superpositions in matter.
Stapp, Henry
2011-11-10
Robert Griffiths has recently addressed, within the framework of a ‘consistent quantum theory’ (CQT) that he has developed, the issue of whether, as is often claimed, quantum mechanics entails a need for faster-than-light transfers of information over long distances. He argues, on the basis of his examination of certain arguments that claim to demonstrate the existence of such nonlocal influences, that such influences do not exist. However, his examination was restricted mainly to hidden-variable-based arguments that include in their premises some essentially classical-physics-type assumptions that are fundamentally incompatible with the precepts of quantum physics. One cannot logically prove properties of a system by attributing to the system properties alien to that system. Hence Griffiths’ rejection of hidden-variable-based proofs is logically warranted. Griffiths mentions the existence of a certain alternative proof that does not involve hidden variables, and that uses only macroscopically described observable properties. He notes that he had examined in his book proofs of this general kind, and concluded that they provide no evidence for nonlocal influences. But he did not examine the particular proof that he cites. An examination of that particular proof by the method specified by his ‘consistent quantum theory’ shows that the cited proof is valid within that restrictive framework. This necessary existence, within the ‘consistent’ framework, of long range essentially instantaneous influences refutes the claim made by Griffiths that his ‘consistent’ framework is superior to the orthodox quantum theory of von Neumann because it does not entail instantaneous influences. An added section responds to Griffiths’ reply, which cites a litany of ambiguities that seem to restrict, devastatingly, the scope of his CQT formalism, apparently to buttress his claim that my use of that formalism to validate the nonlocality theorem is flawed. But the
NASA Astrophysics Data System (ADS)
Schmidt, Alexandre G. M.; da Silva, Ladário
2013-01-01
We quantize the gamble known as Russian roulette and we study it in two versions for two- and three-persons when: (i) players use a fully loaded quantum gun; (ii) the quantum gun has only one quantum bullet.
Interpreting quantum discord through quantum state merging
Madhok, Vaibhav; Datta, Animesh
2011-03-15
We present an operational interpretation of quantum discord based on the quantum state merging protocol. Quantum discord is the markup in the cost of quantum communication in the process of quantum state merging, if one discards relevant prior information. Our interpretation has an intuitive explanation based on the strong subadditivity of von Neumann entropy. We use our result to provide operational interpretations of other quantities like the local purity and quantum deficit. Finally, we discuss in brief some instances where our interpretation is valid in the single-copy scenario.
Quantum probability and quantum decision-making.
Yukalov, V I; Sornette, D
2016-01-13
A rigorous general definition of quantum probability is given, which is valid not only for elementary events but also for composite events, for operationally testable measurements as well as for inconclusive measurements, and also for non-commuting observables in addition to commutative observables. Our proposed definition of quantum probability makes it possible to describe quantum measurements and quantum decision-making on the same common mathematical footing. Conditions are formulated for the case when quantum decision theory reduces to its classical counterpart and for the situation where the use of quantum decision theory is necessary.
Brazil soybean yield covariance model
NASA Technical Reports Server (NTRS)
Callis, S. L.; Sakamoto, C.
1984-01-01
A model based on multiple regression was developed to estimate soybean yields for the seven soybean-growing states of Brazil. The meteorological data of these seven states were pooled and the years 1975 to 1980 were used to model since there was no technological trend in the yields during these years. Predictor variables were derived from monthly total precipitation and monthly average temperature.
Incorporating phenology into yield models
NASA Astrophysics Data System (ADS)
Gray, J. M.; Friedl, M. A.
2015-12-01
Because the yields of many crops are sensitive to meteorological forcing during specific growth stages, phenological information has potential utility in yield mapping and forecasting exercises. However, most attempts to explain the spatiotemporal variability in crop yields with weather data have relied on growth stage definitions that do not change from year-to-year, even though planting, maturity, and harvesting dates show significant interannual variability. We tested the hypothesis that quantifying temperature exposures over dynamically determined growth stages would better explain observed spatiotemporal variability in crop yields than statically defined time periods. Specifically, we used National Agricultural and Statistics Service (NASS) crop progress data to identify the timing of the start of the maize reproductive growth stage ("silking"), and examined the correlation between county-scale yield anomalies and temperature exposures during either the annual or long-term average silking period. Consistent with our hypothesis and physical understanding, yield anomalies were more correlated with temperature exposures during the actual, rather than the long-term average, silking period. Nevertheless, temperature exposures alone explained a relatively low proportion of the yield variability, indicating that other factors and/or time periods are also important. We next investigated the potential of using remotely sensed land surface phenology instead of NASS progress data to retrieve crop growth stages, but encountered challenges related to crop type mapping and subpixel crop heterogeneity. Here, we discuss the potential of overcoming these challenges and the general utility of remotely sensed land surface phenology in crop yield mapping.
Trovato, M.; Reggiani, L.
2011-12-15
By introducing a quantum entropy functional of the reduced density matrix, the principle of quantum maximum entropy is asserted as fundamental principle of quantum statistical mechanics. Accordingly, we develop a comprehensive theoretical formalism to construct rigorously a closed quantum hydrodynamic transport within a Wigner function approach. The theoretical formalism is formulated in both thermodynamic equilibrium and nonequilibrium conditions, and the quantum contributions are obtained by only assuming that the Lagrange multipliers can be expanded in powers of ({h_bar}/2{pi}){sup 2}. In particular, by using an arbitrary number of moments, we prove that (1) on a macroscopic scale all nonlocal effects, compatible with the uncertainty principle, are imputable to high-order spatial derivatives, both of the numerical density n and of the effective temperature T; (2) the results available from the literature in the framework of both a quantum Boltzmann gas and a degenerate quantum Fermi gas are recovered as a particular case; (3) the statistics for the quantum Fermi and Bose gases at different levels of degeneracy are explicitly incorporated; (4) a set of relevant applications admitting exact analytical equations are explicitly given and discussed; (5) the quantum maximum entropy principle keeps full validity in the classical limit, when ({h_bar}/2{pi}){yields}0.
Relativistic quantum cryptography
Molotkov, S. N.
2011-03-15
A new protocol of quantum key distribution is proposed to transmit keys through free space. Along with quantum-mechanical restrictions on the discernibility of nonorthogonal quantum states, the protocol uses additional restrictions imposed by special relativity theory. Unlike all existing quantum key distribution protocols, this protocol ensures key secrecy for a not strictly one-photon source of quantum states and an arbitrary length of a quantum communication channel.
Quantum information does exist
NASA Astrophysics Data System (ADS)
Duwell, Armond
2008-01-01
This paper advocates a concept of quantum information whose origins can be traced to Schumacher [1995. Quantum coding. Physical Review A 51, 2738-2747]. The concept of quantum information advocated is elaborated using an analogy to Shannon's theory provided by Schumacher coding. In particular, this paper extends Timpson's [2004. Quantum information theory and the foundations of quantum mechanics. Ph.D. dissertation, University of Oxford. Preprint, quant-ph/0412063] framework for interpreting Shannon information theory to the quantum context. Entanglement fidelity is advocated as the appropriate success criterion for the reproduction of quantum information. The relationship between the Shannon theory and quantum information theory is discussed.
Interference of quantum market strategies
NASA Astrophysics Data System (ADS)
Piotrowski, Edward W.; Sładkowski, Jan; Syska, Jacek
2003-02-01
Recent development in quantum computation and quantum information theory allows to extend the scope of game theory for the quantum world. The paper is devoted to the analysis of interference of quantum strategies in quantum market games.
Quantum confinement effects across two-dimensional planes in MoS{sub 2} quantum dots
Gan, Z. X.; Liu, L. Z.; Wu, H. Y.; Hao, Y. L.; Shan, Y.; Wu, X. L. E-mail: paul.chu@cityu.edu.hk; Chu, Paul K. E-mail: paul.chu@cityu.edu.hk
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.
A quantum reduction to spherical symmetry in loop quantum gravity
NASA Astrophysics Data System (ADS)
Bodendorfer, N.; Lewandowski, J.; Świeżewski, J.
2015-07-01
Based on a recent purely geometric construction of observables for the spatial diffeomorphism constraint, we propose two distinct quantum reductions to spherical symmetry within full 3 + 1-dimensional loop quantum gravity. The construction of observables corresponds to using the radial gauge for the spatial metric and allows to identify rotations around a central observer as unitary transformations in the quantum theory. Group averaging over these rotations yields our first proposal for spherical symmetry. Hamiltonians of the full theory with angle-independent lapse preserve this spherically symmetric subsector of the full Hilbert space. A second proposal consists in implementing the vanishing of a certain vector field in spherical symmetry as a constraint on the full Hilbert space, leading to a close analogue of diffeomorphisms invariant states. While this second set of spherically symmetric states does not allow for using the full Hamiltonian, it is naturally suited to implement the spherically symmetric midisuperspace Hamiltonian, as an operator in the full theory, on it. Due to the canonical structure of the reduced variables, the holonomy-flux algebra behaves effectively as a one parameter family of 2 + 1-dimensional algebras along the radial coordinate, leading to a diagonal non-vanishing volume operator on 3-valent vertices. The quantum dynamics thus becomes tractable, including scenarios like spherically symmetric dust collapse.
Decomposing global crop yield variability
NASA Astrophysics Data System (ADS)
Ben-Ari, Tamara; Makowski, David
2014-11-01
Recent food crises have highlighted the need to better understand the between-year variability of agricultural production. Although increasing future production seems necessary, the globalization of commodity markets suggests that the food system would also benefit from enhanced supplies stability through a reduction in the year-to-year variability. Here, we develop an analytical expression decomposing global crop yield interannual variability into three informative components that quantify how evenly are croplands distributed in the world, the proportion of cultivated areas allocated to regions of above or below average variability and the covariation between yields in distinct world regions. This decomposition is used to identify drivers of interannual yield variations for four major crops (i.e., maize, rice, soybean and wheat) over the period 1961-2012. We show that maize production is fairly spread but marked by one prominent region with high levels of crop yield interannual variability (which encompasses the North American corn belt in the USA, and Canada). In contrast, global rice yields have a small variability because, although spatially concentrated, much of the production is located in regions of below-average variability (i.e., South, Eastern and South Eastern Asia). Because of these contrasted land use allocations, an even cultivated land distribution across regions would reduce global maize yield variance, but increase the variance of global yield rice. Intermediate results are obtained for soybean and wheat for which croplands are mainly located in regions with close-to-average variability. At the scale of large world regions, we find that covariances of regional yields have a negligible contribution to global yield variance. The proposed decomposition could be applied at any spatial and time scales, including the yearly time step. By addressing global crop production stability (or lack thereof) our results contribute to the understanding of a key
Grapevine canopy reflectance and yield
NASA Technical Reports Server (NTRS)
Minden, K. A.; Philipson, W. R.
1982-01-01
Field spectroradiometric and airborne multispectral scanner data were applied in a study of Concord grapevines. Spectroradiometric measurements of 18 experimental vines were collected on three dates during one growing season. Spectral reflectance, determined at 30 intervals from 0.4 to 1.1 microns, was correlated with vine yield, pruning weight, clusters/vine, and nitrogen input. One date of airborne multispectral scanner data (11 channels) was collected over commercial vineyards, and the average radiance values for eight vineyard sections were correlated with the corresponding average yields. Although some correlations were significant, they were inadequate for developing a reliable yield prediction model.
Quantum recurrences: probe to study quantum chaos
Saif
2000-11-01
We study the phase space of periodically modulated gravitational cavity by means of quantum recurrence phenomena. We report that the quantum recurrences serve as a tool to connect phase space of the driven system with a spectrum in the quantum domain. With the help of quantum recurrences we investigate the quasienergy spectrum of the system for a certain fixed modulation strength. In addition, we study transition of spectrum from discrete to continuum as a function of modulation strength. PMID:11101963
Quantum teleportation of optical quantum gates.
Bartlett, Stephen D; Munro, William J
2003-03-21
We show that a universal set of gates for quantum computation with optics can be quantum teleported through the use of EPR entangled states, homodyne detection, and linear optics and squeezing operations conditioned on measurement outcomes. This scheme may be used for fault-tolerant quantum computation in any optical scheme (qubit or continuous-variable). The teleportation of nondeterministic nonlinear gates employed in linear optics quantum computation is discussed.
Yang, C.-D. . E-mail: cdyang@mail.ncku.edu.tw
2006-12-15
This paper gives a thorough investigation on formulating and solving quantum problems by extended analytical mechanics that extends canonical variables to complex domain. With this complex extension, we show that quantum mechanics becomes a part of analytical mechanics and hence can be treated integrally with classical mechanics. Complex canonical variables are governed by Hamilton equations of motion, which can be derived naturally from Schroedinger equation. Using complex canonical variables, a formal proof of the quantization axiom p {sup {yields}} p = -ih{nabla}, which is the kernel in constructing quantum-mechanical systems, becomes a one-line corollary of Hamilton mechanics. The derivation of quantum operators from Hamilton mechanics is coordinate independent and thus allows us to derive quantum operators directly under any coordinate system without transforming back to Cartesian coordinates. Besides deriving quantum operators, we also show that the various prominent quantum effects, such as quantization, tunneling, atomic shell structure, Aharonov-Bohm effect, and spin, all have the root in Hamilton mechanics and can be described entirely by Hamilton equations of motion.
Quantum Steganography and Quantum Error-Correction
ERIC Educational Resources Information Center
Shaw, Bilal A.
2010-01-01
Quantum error-correcting codes have been the cornerstone of research in quantum information science (QIS) for more than a decade. Without their conception, quantum computers would be a footnote in the history of science. When researchers embraced the idea that we live in a world where the effects of a noisy environment cannot completely be…
Quantum Hall effect in quantum electrodynamics
Penin, Alexander A.
2009-03-15
We consider the quantum Hall effect in quantum electrodynamics and find a deviation from the quantum-mechanical prediction for the Hall conductivity due to radiative antiscreening of electric charge in an external magnetic field. A weak dependence of the universal von Klitzing constant on the magnetic field strength, which can possibly be observed in a dedicated experiment, is predicted.
Quantum critical behavior in heavy electron materials
Yang, Yi-feng; Pines, David
2014-01-01
Quantum critical behavior in heavy electron materials is typically brought about by changes in pressure or magnetic field. In this paper, we develop a simple unified model for the combined influence of pressure and magnetic field on the effectiveness of the hybridization that plays a central role in the two-fluid description of heavy electron emergence. We show that it leads to quantum critical and delocalization lines that accord well with those measured for CeCoIn5, yields a quantitative explanation of the field and pressure-induced changes in antiferromagnetic ordering and quantum critical behavior measured for YbRh2Si2, and provides a valuable framework for describing the role of magnetic fields in bringing about quantum critical behavior in other heavy electron materials. PMID:24912172
Practical characterization of quantum devices without tomography
NASA Astrophysics Data System (ADS)
Landon-Cardinal, Olivier; Flammia, Steven; Silva, Marcus; Liu, Yi-Kai; Poulin, David
2012-02-01
Quantum tomography is the main method used to assess the quality of quantum information processing devices, but its complexity presents a major obstacle for the characterization of even moderately large systems. Part of the reason for this complexity is that tomography generates much more information than is usually sought. Taking a more targeted approach, we develop schemes that enable (i) estimating the ?delity of an experiment to a theoretical ideal description, (ii) learning which description within a reduced subset best matches the experimental data. Both these approaches yield a signi?cant reduction in resources compared to tomography. In particular, we show how to estimate the ?delity between a predicted pure state and an arbitrary experimental state using only a constant number of Pauli expectation values selected at random according to an importance-weighting rule. In addition, we propose methods for certifying quantum circuits and learning continuous-time quantum dynamics that are described by local Hamiltonians or Lindbladians.
Practical characterization of quantum devices without tomography.
da Silva, Marcus P; Landon-Cardinal, Olivier; Poulin, David
2011-11-18
Quantum tomography is the main method used to assess the quality of quantum information processing devices. However, the amount of resources needed for quantum tomography is exponential in the device size. Part of the problem is that tomography generates much more information than is usually sought. Taking a more targeted approach, we develop schemes that enable (i) estimating the fidelity of an experiment to a theoretical ideal description, (ii) learning which description within a reduced subset best matches the experimental data. Both these approaches yield a significant reduction in resources compared to tomography. In particular, we demonstrate that fidelity can be estimated from a number of simple experiments that is independent of the system size, removing an important roadblock for the experimental study of larger quantum information processing units. PMID:22181862
A quantum approach to homomorphic encryption
Tan, Si-Hui; Kettlewell, Joshua A.; Ouyang, Yingkai; Chen, Lin; Fitzsimons, Joseph F.
2016-01-01
Encryption schemes often derive their power from the properties of the underlying algebra on the symbols used. Inspired by group theoretic tools, we use the centralizer of a subgroup of operations to present a private-key quantum homomorphic encryption scheme that enables a broad class of quantum computation on encrypted data. The quantum data is encoded on bosons of distinct species in distinct spatial modes, and the quantum computations are manipulations of these bosons in a manner independent of their species. A particular instance of our encoding hides up to a constant fraction of the information encrypted. This fraction can be made arbitrarily close to unity with overhead scaling only polynomially in the message length. This highlights the potential of our protocol to hide a non-trivial amount of information, and is suggestive of a large class of encodings that might yield better security. PMID:27658349
Sensitive chemical compass assisted by quantum criticality
NASA Astrophysics Data System (ADS)
Cai, C. Y.; Ai, Qing; Quan, H. T.; Sun, C. P.
2012-02-01
A radical-pair-based chemical reaction might be used by birds for navigation via the geomagnetic direction. The inherent physical mechanism is that the quantum coherent transition from a singlet state to triplet states of the radical pair could respond to a weak magnetic field and be sensitive to the direction of such a field; this then results in different photopigments to be sensed by the avian eyes. Here, we propose a quantum bionic setup, inspired by the avian compass, as an ultrasensitive probe of a weak magnetic field based on the quantum phase transition of the environments of the two electrons in the radical pair. We prove that the yield of the chemical products via recombination from the singlet state is determined by the Loschmidt echo of the environments with interacting nuclear spins. Thus quantum criticality of environments could enhance the sensitivity of detection of weak magnetic fields.
A quantum approach to homomorphic encryption
NASA Astrophysics Data System (ADS)
Tan, Si-Hui; Kettlewell, Joshua A.; Ouyang, Yingkai; Chen, Lin; Fitzsimons, Joseph F.
2016-09-01
Encryption schemes often derive their power from the properties of the underlying algebra on the symbols used. Inspired by group theoretic tools, we use the centralizer of a subgroup of operations to present a private-key quantum homomorphic encryption scheme that enables a broad class of quantum computation on encrypted data. The quantum data is encoded on bosons of distinct species in distinct spatial modes, and the quantum computations are manipulations of these bosons in a manner independent of their species. A particular instance of our encoding hides up to a constant fraction of the information encrypted. This fraction can be made arbitrarily close to unity with overhead scaling only polynomially in the message length. This highlights the potential of our protocol to hide a non-trivial amount of information, and is suggestive of a large class of encodings that might yield better security.
NASA Astrophysics Data System (ADS)
Lidar, Daniel A.; Brun, Todd A.
2013-09-01
Prologue; Preface; Part I. Background: 1. Introduction to decoherence and noise in open quantum systems Daniel Lidar and Todd Brun; 2. Introduction to quantum error correction Dave Bacon; 3. Introduction to decoherence-free subspaces and noiseless subsystems Daniel Lidar; 4. Introduction to quantum dynamical decoupling Lorenza Viola; 5. Introduction to quantum fault tolerance Panos Aliferis; Part II. Generalized Approaches to Quantum Error Correction: 6. Operator quantum error correction David Kribs and David Poulin; 7. Entanglement-assisted quantum error-correcting codes Todd Brun and Min-Hsiu Hsieh; 8. Continuous-time quantum error correction Ognyan Oreshkov; Part III. Advanced Quantum Codes: 9. Quantum convolutional codes Mark Wilde; 10. Non-additive quantum codes Markus Grassl and Martin Rötteler; 11. Iterative quantum coding systems David Poulin; 12. Algebraic quantum coding theory Andreas Klappenecker; 13. Optimization-based quantum error correction Andrew Fletcher; Part IV. Advanced Dynamical Decoupling: 14. High order dynamical decoupling Zhen-Yu Wang and Ren-Bao Liu; 15. Combinatorial approaches to dynamical decoupling Martin Rötteler and Pawel Wocjan; Part V. Alternative Quantum Computation Approaches: 16. Holonomic quantum computation Paolo Zanardi; 17. Fault tolerance for holonomic quantum computation Ognyan Oreshkov, Todd Brun and Daniel Lidar; 18. Fault tolerant measurement-based quantum computing Debbie Leung; Part VI. Topological Methods: 19. Topological codes Héctor Bombín; 20. Fault tolerant topological cluster state quantum computing Austin Fowler and Kovid Goyal; Part VII. Applications and Implementations: 21. Experimental quantum error correction Dave Bacon; 22. Experimental dynamical decoupling Lorenza Viola; 23. Architectures Jacob Taylor; 24. Error correction in quantum communication Mark Wilde; Part VIII. Critical Evaluation of Fault Tolerance: 25. Hamiltonian methods in QEC and fault tolerance Eduardo Novais, Eduardo Mucciolo and
Quantum Walk Schemes for Universal Quantum Computation
NASA Astrophysics Data System (ADS)
Underwood, Michael S.
Random walks are a powerful tool for the efficient implementation of algorithms in classical computation. Their quantum-mechanical analogues, called quantum walks, hold similar promise. Quantum walks provide a model of quantum computation that has recently been shown to be equivalent in power to the standard circuit model. As in the classical case, quantum walks take place on graphs and can undergo discrete or continuous evolution, though quantum evolution is unitary and therefore deterministic until a measurement is made. This thesis considers the usefulness of continuous-time quantum walks to quantum computation from the perspectives of both their fundamental power under various formulations, and their applicability in practical experiments. In one extant scheme, logical gates are effected by scattering processes. The results of an exhaustive search for single-qubit operations in this model are presented. It is shown that the number of distinct operations increases exponentially with the number of vertices in the scattering graph. A catalogue of all graphs on up to nine vertices that implement single-qubit unitaries at a specific set of momenta is included in an appendix. I develop a novel scheme for universal quantum computation called the discontinuous quantum walk, in which a continuous-time quantum walker takes discrete steps of evolution via perfect quantum state transfer through small 'widget' graphs. The discontinuous quantum-walk scheme requires an exponentially sized graph, as do prior discrete and continuous schemes. To eliminate the inefficient vertex resource requirement, a computation scheme based on multiple discontinuous walkers is presented. In this model, n interacting walkers inhabiting a graph with 2n vertices can implement an arbitrary quantum computation on an input of length n, an exponential savings over previous universal quantum walk schemes. This is the first quantum walk scheme that allows for the application of quantum error correction
Optimal quantum cloning via spin networks
Chen Qing; Cheng Jianhua; Wang Kelin; Du Jiangfeng
2006-09-15
In this paper we demonstrate that optimal 1{yields}M phase-covariant cloning quantum cloning is available via free dynamical evolution of spin networks. By properly designing the network and the couplings between spins, we show that optimal 1{yields}M phase-covariant cloning can be achieved if the initial state is prepared as a specific symmetric state. Especially, when M is an odd number, the optimal phase-covariant cloning can be achieved without ancillas. Moreover, we demonstrate that the same framework is capable for optimal 1{yields}2 universal cloning.
Brazil wheat yield covariance model
NASA Technical Reports Server (NTRS)
Callis, S. L.; Sakamoto, C.
1984-01-01
A model based on multiple regression was developed to estimate wheat yields for the wheat growing states of Rio Grande do Sul, Parana, and Santa Catarina in Brazil. The meteorological data of these three states were pooled and the years 1972 to 1979 were used to develop the model since there was no technological trend in the yields during these years. Predictor variables were derived from monthly total precipitation, average monthly mean temperature, and average monthly maximum temperature.
Efficient quantum computing using coherent photon conversion.
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
Fission yield measurements at IGISOL
NASA Astrophysics Data System (ADS)
Lantz, M.; Al-Adili, A.; Gorelov, D.; Jokinen, A.; Kolhinen, V. S.; Mattera, A.; Moore, I.; Penttilä, H.; Pomp, S.; Prokofiev, A. V.; Rakopoulos, V.; Rinta-Antila, S.; Simutkin, V.; Solders, A.
2016-06-01
The fission product yields are an important characteristic of the fission process. In fundamental physics, knowledge of the yield distributions is needed to better understand the fission process. For nuclear energy applications good knowledge of neutroninduced fission-product yields is important for the safe and efficient operation of nuclear power plants. With the Ion Guide Isotope Separator On-Line (IGISOL) technique, products of nuclear reactions are stopped in a buffer gas and then extracted and separated by mass. Thanks to the high resolving power of the JYFLTRAP Penning trap, at University of Jyväskylä, fission products can be isobarically separated, making it possible to measure relative independent fission yields. In some cases it is even possible to resolve isomeric states from the ground state, permitting measurements of isomeric yield ratios. So far the reactions U(p,f) and Th(p,f) have been studied using the IGISOL-JYFLTRAP facility. Recently, a neutron converter target has been developed utilizing the Be(p,xn) reaction. We here present the IGISOL-technique for fission yield measurements and some of the results from the measurements on proton induced fission. We also present the development of the neutron converter target, the characterization of the neutron field and the first tests with neutron-induced fission.
Hot Hole Transfer Increasing Polaron Yields in Hybrid Conjugated Polymer/PbS Blends.
Strein, Elisabeth; deQuilettes, Dane W; Hsieh, Stephen T; Colbert, Adam E; Ginger, David S
2014-01-01
We use quasi-steady-state photoinduced absorption (PIA) to study charge generation in blends of poly(3-hexylthiophene-2,5-diyl) (P3HT) with PbS nanocrystal quantum dots as a function of excitation energy. We find that, per photon absorbed, the yield of photogenerated holes present on the conjugated polymer increases with pump energy, even at wavelengths where only the quantum dots absorb. We interpret this result as direct evidence for transfer of hot holes in these conjugated polymer/quantum dot blends. These results help understand the operation of hybrid organic/inorganic photovoltaics.
Acid soil infertility effects on peanut yields and yield components
Blamey, F.P.C.
1983-01-01
The interpretation of soil amelioration experiments with peanuts is made difficult by the unpredictibility of the crop and by the many factors altered when ameliorating acid soils. The present study was conducted to investigate the effects of lime and gypsum applications on peanut kernel yield via the three first order yield components, pods per ha, kernels per pod, and kernel mass. On an acid medium sandy loam soil (typic Plinthustult), liming resulted in a highly significant kernel yield increase of 117% whereas gypsum applications were of no significant benefit. As indicated by path coefficient analysis, an increase in the number of pods per ha was markedly more important in increasing yield than an increase in either the number of kernels per pod or kernel mass. Furthermore, exch. Al was found to be particularly detrimental to pod number. It was postulated that poor peanut yields resulting from acid soil infertility were mainly due to the depressive effect of exch. Al on pod number. Exch. Ca appeared to play a secondary role by ameliorating the adverse effects of exch. Al.
Quantum algorithms for quantum field theories.
Jordan, Stephen P; Lee, Keith S M; Preskill, John
2012-06-01
Quantum field theory reconciles quantum mechanics and special relativity, and plays a central role in many areas of physics. We developed a quantum algorithm to compute relativistic scattering probabilities in a massive quantum field theory with quartic self-interactions (φ(4) theory) in spacetime of four and fewer dimensions. Its run time is polynomial in the number of particles, their energy, and the desired precision, and applies at both weak and strong coupling. In the strong-coupling and high-precision regimes, our quantum algorithm achieves exponential speedup over the fastest known classical algorithm. PMID:22654052
Quantum algorithms for quantum field theories.
Jordan, Stephen P; Lee, Keith S M; Preskill, John
2012-06-01
Quantum field theory reconciles quantum mechanics and special relativity, and plays a central role in many areas of physics. We developed a quantum algorithm to compute relativistic scattering probabilities in a massive quantum field theory with quartic self-interactions (φ(4) theory) in spacetime of four and fewer dimensions. Its run time is polynomial in the number of particles, their energy, and the desired precision, and applies at both weak and strong coupling. In the strong-coupling and high-precision regimes, our quantum algorithm achieves exponential speedup over the fastest known classical algorithm.
Security of counterfactual quantum cryptography
Yin Zhenqiang; Li Hongwei; Chen Wei; Han Zhengfu; Guo Guangcan
2010-10-15
Recently, a 'counterfactual' quantum-key-distribution scheme was proposed by T.-G. Noh [Phys. Rev. Lett. 103, 230501 (2009)]. In this scheme, two legitimate distant peers may share secret keys even when the information carriers are not traveled in the quantum channel. We find that this protocol is equivalent to an entanglement distillation protocol. According to this equivalence, a strict security proof and the asymptotic key bit rate are both obtained when a perfect single-photon source is applied and a Trojan horse attack can be detected. We also find that the security of this scheme is strongly related to not only the bit error rate but also the yields of photons. And our security proof may shed light on the security of other two-way protocols.
Open quantum systems and error correction
NASA Astrophysics Data System (ADS)
Shabani Barzegar, Alireza
Quantum effects can be harnessed to manipulate information in a desired way. Quantum systems which are designed for this purpose are suffering from harming interaction with their surrounding environment or inaccuracy in control forces. Engineering different methods to combat errors in quantum devices are highly demanding. In this thesis, I focus on realistic formulations of quantum error correction methods. A realistic formulation is the one that incorporates experimental challenges. This thesis is presented in two sections of open quantum system and quantum error correction. Chapters 2 and 3 cover the material on open quantum system theory. It is essential to first study a noise process then to contemplate methods to cancel its effect. In the second chapter, I present the non-completely positive formulation of quantum maps. Most of these results are published in [Shabani and Lidar, 2009b,a], except a subsection on geometric characterization of positivity domain of a quantum map. The real-time formulation of the dynamics is the topic of the third chapter. After introducing the concept of Markovian regime, A new post-Markovian quantum master equation is derived, published in [Shabani and Lidar, 2005a]. The section of quantum error correction is presented in three chapters of 4, 5, 6 and 7. In chapter 4, we introduce a generalized theory of decoherence-free subspaces and subsystems (DFSs), which do not require accurate initialization (published in [Shabani and Lidar, 2005b]). In Chapter 5, we present a semidefinite program optimization approach to quantum error correction that yields codes and recovery procedures that are robust against significant variations in the noise channel. Our approach allows us to optimize the encoding, recovery, or both, and is amenable to approximations that significantly improve computational cost while retaining fidelity (see [Kosut et al., 2008] for a published version). Chapter 6 is devoted to a theory of quantum error correction (QEC
NASA Astrophysics Data System (ADS)
Iqbal, Azhar; Abbott, Derek
2009-01-01
A quantum version of the matching pennies (MP) game is proposed that is played using an Einstein-Podolsky-Rosen-Bohm (EPR-Bohm) setting. We construct the quantum game without using state vectors, while considering only the quantum mechanical joint probabilities relevant to the EPR-Bohm setting. We embed the classical game within the quantum game such that the classical MP game results when the quantum mechanical joint probabilities become factorizable. We report new Nash equilibria in the quantum MP game that emerge when the quantum mechanical joint probabilities maximally violate the Clauser-Horne-Shimony-Holt form of Bell’s inequality.
Universal quantum computation by discontinuous quantum walk
Underwood, Michael S.; Feder, David L.
2010-10-15
Quantum walks are the quantum-mechanical analog of random walks, in which a quantum ''walker'' evolves between initial and final states by traversing the edges of a graph, either in discrete steps from node to node or via continuous evolution under the Hamiltonian furnished by the adjacency matrix of the graph. We present a hybrid scheme for universal quantum computation in which a quantum walker takes discrete steps of continuous evolution. This ''discontinuous'' quantum walk employs perfect quantum-state transfer between two nodes of specific subgraphs chosen to implement a universal gate set, thereby ensuring unitary evolution without requiring the introduction of an ancillary coin space. The run time is linear in the number of simulated qubits and gates. The scheme allows multiple runs of the algorithm to be executed almost simultaneously by starting walkers one time step apart.
Secure quantum signatures using insecure quantum channels
NASA Astrophysics Data System (ADS)
Amiri, Ryan; Wallden, Petros; Kent, Adrian; Andersson, Erika
2016-03-01
Digital signatures are widely used in modern communication to guarantee authenticity and transferability of messages. The security of currently used classical schemes relies on computational assumptions. We present a quantum signature scheme that does not require trusted quantum channels. We prove that it is unconditionally secure against the most general coherent attacks, and show that it requires the transmission of significantly fewer quantum states than previous schemes. We also show that the quantum channel noise threshold for our scheme is less strict than for distilling a secure key using quantum key distribution. This shows that "direct" quantum signature schemes can be preferable to signature schemes relying on secret shared keys generated using quantum key distribution.
Randomness: Quantum versus classical
NASA Astrophysics Data System (ADS)
Khrennikov, Andrei
2016-05-01
Recent tremendous development of quantum information theory has led to a number of quantum technological projects, e.g. quantum random generators. This development had stimulated a new wave of interest in quantum foundations. One of the most intriguing problems of quantum foundations is the elaboration of a consistent and commonly accepted interpretation of a quantum state. Closely related problem is the clarification of the notion of quantum randomness and its interrelation with classical randomness. In this short review, we shall discuss basics of classical theory of randomness (which by itself is very complex and characterized by diversity of approaches) and compare it with irreducible quantum randomness. We also discuss briefly “digital philosophy”, its role in physics (classical and quantum) and its coupling to the information interpretation of quantum mechanics (QM).
Bender, Carl M; DeKieviet, Maarten; Klevansky, S. P.
2013-01-01
-symmetric quantum mechanics (PTQM) has become a hot area of research and investigation. Since its beginnings in 1998, there have been over 1000 published papers and more than 15 international conferences entirely devoted to this research topic. Originally, PTQM was studied at a highly mathematical level and the techniques of complex variables, asymptotics, differential equations and perturbation theory were used to understand the subtleties associated with the analytic continuation of eigenvalue problems. However, as experiments on -symmetric physical systems have been performed, a simple and beautiful physical picture has emerged, and a -symmetric system can be understood as one that has a balanced loss and gain. Furthermore, the phase transition can now be understood intuitively without resorting to sophisticated mathe- matics. Research on PTQM is following two different paths: at a fundamental level, physicists are attempting to understand the underlying mathematical structure of these theories with the long-range objective of applying the techniques of PTQM to understanding some of the outstanding problems in physics today, such as the nature of the Higgs particle, the properties of dark matter, the matter–antimatter asymmetry in the universe, neutrino oscillations and the cosmological constant; at an applied level, new kinds of -synthetic materials are being developed, and the phase transition is being observed in many physical contexts, such as lasers, optical wave guides, microwave cavities, superconducting wires and electronic circuits. The purpose of this Theme Issue is to acquaint the reader with the latest developments in PTQM. The articles in this volume are written in the style of mini-reviews and address diverse areas of the emerging and exciting new area of -symmetric quantum mechanics. PMID:23509390
Quantum computing classical physics.
Meyer, David A
2002-03-15
In the past decade, quantum algorithms have been found which outperform the best classical solutions known for certain classical problems as well as the best classical methods known for simulation of certain quantum systems. This suggests that they may also speed up the simulation of some classical systems. I describe one class of discrete quantum algorithms which do so--quantum lattice-gas automata--and show how to implement them efficiently on standard quantum computers.
NASA Astrophysics Data System (ADS)
Cook, Richard J.
1988-01-01
This paper answers the title question by giving an operational definition of quantum jumps based on measurement theory. This definition forms the basis of a theory of quantum jumps which leads to a number of testable predictions. Experiments are proposed to test the theory. The suggested experiments also test the quantum Zeno paradox, i.e., they test the proposition that frequent observation of a quantum system inhibits quantum jumps in that system.
Diagrammatic quantum mechanics
NASA Astrophysics Data System (ADS)
Kauffman, Louis H.; Lomonaco, Samuel J.
2015-05-01
This paper explores how diagrams of quantum processes can be used for modeling and for quantum epistemology. The paper is a continuation of the discussion where we began this formulation. Here we give examples of quantum networks that represent unitary transformations by dint of coherence conditions that constitute a new form of non-locality. Local quantum devices interconnected in space can form a global quantum system when appropriate coherence conditions are maintained.
Probabilistic Cloning and Quantum Computation
NASA Astrophysics Data System (ADS)
Gao, Ting; Yan, Feng-Li; Wang, Zhi-Xi
2004-06-01
We discuss the usefulness of quantum cloning and present examples of quantum computation tasks for which the cloning offers an advantage which cannot be matched by any approach that does not resort to quantum cloning. In these quantum computations, we need to distribute quantum information contained in the states about which we have some partial information. To perform quantum computations, we use a state-dependent probabilistic quantum cloning procedure to distribute quantum information in the middle of a quantum computation.
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.
Engineered semiconductor nanocrystals with enhanced carrier multiplication yields
NASA Astrophysics Data System (ADS)
Klimov, Victor
2014-03-01
Carrier multiplication (CM) is a process whereby absorption of a single photon results in multiple electron-hole pairs (excitons). This process could benefit a number of solar-energy conversion technologies, most notably photocatalysis and photovoltaics. This presentation overviews recent progress in understanding the CM process in semiconductor nanocrystals, motivated by an outstanding challenge in this field - the lack of capability to predict the CM performance of nanocrystals based on their known photophysical properties or documented parameters of parental bulk solids. Here, we present a possible solution to this problem by showing that, using biexciton Auger lifetimes and intraband relaxation rates inferred from ultrafast spectroscopic studies, we can rationalize relative changes in CM yields as a function of nanocrystal composition, size and shape. Further, guided by this model, we demonstrate a two-fold enhancement in multiexciton yields in PbSe nanorods vs. quantum dots attributed to enhanced Coulomb interactions. We also explore the control of competing intra-band cooling for increasing multiexciton production. Specifically, we design a new type of hetero-structured PbSe/CdSe quantum dots with reduced rates of intra-band relaxation and demonstrate a four-fold boost in the multiexciton yield. These studies provide useful guidelines for future efforts to achieve the ultimate, energy-conservation-defined CM efficiencies.
Li, Min; Ni, Qi-liang; Dong, Ning-ning; Chen, Bo
2010-08-01
Photon counting detectors based on microchannel plate have widespread applications in astronomy. The present paper deeply studies secondary electron of microchannel plate in extreme ultraviolet. A theoretical model describing extreme ultraviolet-excited secondary electron yield is presented, and the factor affecting on the secondary electron yields of both electrode and lead glass which consist of microchannel plate is analyzed according to theoretical formula derived from the model. The result shows that the higher secondary electron yield is obtained under appropriate condition that the thickness of material is more than 20 nm and the grazing incidence angle is larger than the critical angle. Except for several wavelengths, the secondary electron yields of both electrode and lead glass decrease along with the increase in the wavelength And also the quantum efficiency of microchannel plate is measured using quantum efficiency test set-up with laser-produced plasmas source as an extreme ultraviolet radiation source, and the result of experiment agrees with theoretical analysis.
Satellite-Based Quantum Communications
Hughes, Richard J; Nordholt, Jane E; McCabe, Kevin P; Newell, Raymond T; Peterson, Charles G
2010-09-20
Single-photon quantum communications (QC) offers the attractive feature of 'future proof', forward security rooted in the laws of quantum physics. Ground based quantum key distribution (QKD) experiments in optical fiber have attained transmission ranges in excess of 200km, but for larger distances we proposed a methodology for satellite-based QC. Over the past decade we have devised solutions to the technical challenges to satellite-to-ground QC, and we now have a clear concept for how space-based QC could be performed and potentially utilized within a trusted QKD network architecture. Functioning as a trusted QKD node, a QC satellite ('QC-sat') could deliver secret keys to the key stores of ground-based trusted QKD network nodes, to each of which multiple users are connected by optical fiber or free-space QC. A QC-sat could thereby extend quantum-secured connectivity to geographically disjoint domains, separated by continental or inter-continental distances. In this paper we describe our system concept that makes QC feasible with low-earth orbit (LEO) QC-sats (200-km-2,000-km altitude orbits), and the results of link modeling of expected performance. Using the architecture that we have developed, LEO satellite-to-ground QKD will be feasible with secret bit yields of several hundred 256-bit AES keys per contact. With multiple ground sites separated by {approx} 100km, mitigation of cloudiness over any single ground site would be possible, potentially allowing multiple contact opportunities each day. The essential next step is an experimental QC-sat. A number of LEO-platforms would be suitable, ranging from a dedicated, three-axis stabilized small satellite, to a secondary experiment on an imaging satellite. to the ISS. With one or more QC-sats, low-latency quantum-secured communications could then be provided to ground-based users on a global scale. Air-to-ground QC would also be possible.
NASA Astrophysics Data System (ADS)
Bojowald, Martin
The universe, ultimately, is to be described by quantum theory. Quantum aspects of all there is, including space and time, may not be significant for many purposes, but are crucial for some. And so a quantum description of cosmology is required for a complete and consistent worldview. At any rate, even if we were not directly interested in regimes where quantum cosmology plays a role, a complete physical description could not stop at a stage before the whole universe is reached. Quantum theory is essential in the microphysics of particles, atoms, molecules, solids, white dwarfs and neutron stars. Why should one expect this ladder of scales to end at a certain size? If regimes are sufficiently violent and energetic, quantum effects are non-negligible even on scales of the whole cosmos; this is realized at least once in the history of the universe: at the big bang where the classical theory of general relativity would make energy densities diverge.
Coropceanu, Igor; Bawendi, Moungi G
2014-07-01
CdSe/CdS core/shell quantum dots (QDs) have been optimized toward luminescent solar concentration (LSC) applications. Systematically increasing the shell thickness continuously reduced reabsorption up to a factor of 45 for the thickest QDs studied (with ca. 14 monolayers of CdS) compared to the initial CdSe cores. Moreover, an improved synthetic method was developed that retains a high-fluorescence quantum yield, even for particles with the thickest shell volume, for which a quantum yield of 86% was measured in solution. These high quantum yield thick shell quantum dots were embedded in a polymer matrix, yielding highly transparent composites to serve as prototype LSCs, which exhibited an optical efficiency as high as 48%. A Monte Carlo simulation was developed to model LSC performance and to identify the major loss channels for LSCs incorporating the materials developed. The results of the simulation are in excellent agreement with the experimental data. PMID:24902615
Quantum optics, cavity QED, and quantum optomechanics
NASA Astrophysics Data System (ADS)
Meystre, Pierre
2013-05-01
Quantum optomechanics provides a universal tool to achieve the quantum control of mechanical motion. It does that in devices spanning a vast range of parameters, with mechanical frequencies from a few Hertz to GHz, and with masses from 10-20 g to several kilos. Its underlying ideas can be traced back to the study of gravitational wave antennas, quantum optics, cavity QED and laser cooling which, when combined with the recent availability of advanced micromechanical and nanomechanical devices, opens a path to the realization of macroscopic mechanical systems that operate deep in the quantum regime. At the fundamental level this development paves the way to experiments that will lead to a more profound understanding of quantum mechanics; and from the point of view of applications, quantum optomechanical techniques will provide motion and force sensing near the fundamental limit imposed by quantum mechanics (quantum metrology) and significantly expand the toolbox of quantum information science. After a brief summary of key historical developments, the talk will give a broad overview of the current state of the art of quantum optomechanics, and comment on future prospects both in applied and in fundamental science. Work supported by NSF, ARO and the DARPA QuASAR and ORCHID programs.
Quantum leadership: the implication for Iranian nursing leaders.
Dargahi, Hossein
2013-07-13
Quantum organizations are referred where stakeholders know how to access the infinite potential of the quantum field. Viewing healthcare organizations from perspective of quantum theory suggest new approaches into management techniques for effective and efficient delivery of healthcare services. This research is aimed to determine the quantum skills, quantum leadership characteristics and functions of Tehran University of Medical Sciences hospitals' nursing administrators. A cross-sectional, descriptive and analytical study was conducted among 25 nursing administrators of Tehran University of Medical Sciences (TUMS) hospitals, Tehran, Iran. The research tool for data collection was a self-constructed questionnaire that measured the quantum skills, quantum leadership characteristics and functions of TUMS hospitals' nursing administrators. The validity of questionnaire was confirmed by 5 management science experts and its reliability was performed by using test-retest method yielded a Cronbach's alpha coefficient of 0.90. Data were collected and analyzed by SPSS software and t-test statistical methods. The results of this research showed that all respondents had desired quantum skills (75.71±5.98), quantum leadership characteristics (82.01±6.77), and quantum leadership functions (78.57±6.28) and total quantum leadership (78.76±4.50). Also, passing management training courses of the respondents was significantly correlated with their quantum leadership. Iranian healthcare organizations require quantum leadership that provides an important resource to advance Iranian nursing leadership to the organizational excellence. We hope Iranian hospitals' nursing leaders who have quantum skills potentially, present a highly developed sense of self and the ability to improve nursing care outcomes in these hospitals.
The yield of N/2D/ atoms in the dissociative recombination of NO/+/
NASA Technical Reports Server (NTRS)
Kley, D.; Lawrence, G. M.; Stone, E. J.
1977-01-01
The quantum yield or branching ratio of N(2D) atoms formed in the reaction e + NO(+) yields N + O was measured to be 76% plus or minus 6%. Photoionization of buffered nitric oxide by a flash lamp was studied using time-resolved atomic absorption. Atoms were produced both by direct photodissociation and by dissociative recombination, and these two effects were separated by means of SF6 as an electron scavenger.
NASA Astrophysics Data System (ADS)
Alvarez-Rodriguez, U.; Sanz, M.; Lamata, L.; Solano, E.
2015-07-01
Quantum information provides fundamentally different computational resources than classical information. We prove that there is no unitary protocol able to add unknown quantum states belonging to different Hilbert spaces. This is an inherent restriction of quantum physics that is related to the impossibility of copying an arbitrary quantum state, i.e., the no-cloning theorem. Moreover, we demonstrate that a quantum adder, in absence of an ancillary system, is also forbidden for a known orthonormal basis. This allows us to propose an approximate quantum adder that could be implemented in the lab. Finally, we discuss the distinct character of the forbidden quantum adder for quantum states and the allowed quantum adder for density matrices.
Expected number of quantum channels in quantum networks.
Chen, Xi; Wang, He-Ming; Ji, Dan-Tong; Mu, Liang-Zhu; Fan, Heng
2015-01-01
Quantum communication between nodes in quantum networks plays an important role in quantum information processing. Here, we proposed the use of the expected number of quantum channels as a measure of the efficiency of quantum communication for quantum networks. This measure quantified the amount of quantum information that can be teleported between nodes in a quantum network, which differs from classical case in that the quantum channels will be consumed if teleportation is performed. We further demonstrated that the expected number of quantum channels represents local correlations depicted by effective circles. Significantly, capacity of quantum communication of quantum networks quantified by ENQC is independent of distance for the communicating nodes, if the effective circles of communication nodes are not overlapped. The expected number of quantum channels can be enhanced through transformations of the lattice configurations of quantum networks via entanglement swapping. Our results can shed lights on the study of quantum communication in quantum networks.
Expected number of quantum channels in quantum networks.
Chen, Xi; Wang, He-Ming; Ji, Dan-Tong; Mu, Liang-Zhu; Fan, Heng
2015-01-01
Quantum communication between nodes in quantum networks plays an important role in quantum information processing. Here, we proposed the use of the expected number of quantum channels as a measure of the efficiency of quantum communication for quantum networks. This measure quantified the amount of quantum information that can be teleported between nodes in a quantum network, which differs from classical case in that the quantum channels will be consumed if teleportation is performed. We further demonstrated that the expected number of quantum channels represents local correlations depicted by effective circles. Significantly, capacity of quantum communication of quantum networks quantified by ENQC is independent of distance for the communicating nodes, if the effective circles of communication nodes are not overlapped. The expected number of quantum channels can be enhanced through transformations of the lattice configurations of quantum networks via entanglement swapping. Our results can shed lights on the study of quantum communication in quantum networks. PMID:26173556
Expected number of quantum channels in quantum networks
Chen, Xi; Wang, He-Ming; Ji, Dan-Tong; Mu, Liang-Zhu; Fan, Heng
2015-01-01
Quantum communication between nodes in quantum networks plays an important role in quantum information processing. Here, we proposed the use of the expected number of quantum channels as a measure of the efficiency of quantum communication for quantum networks. This measure quantified the amount of quantum information that can be teleported between nodes in a quantum network, which differs from classical case in that the quantum channels will be consumed if teleportation is performed. We further demonstrated that the expected number of quantum channels represents local correlations depicted by effective circles. Significantly, capacity of quantum communication of quantum networks quantified by ENQC is independent of distance for the communicating nodes, if the effective circles of communication nodes are not overlapped. The expected number of quantum channels can be enhanced through transformations of the lattice configurations of quantum networks via entanglement swapping. Our results can shed lights on the study of quantum communication in quantum networks. PMID:26173556
Reliable quantum communication over a quantum relay channel
Gyongyosi, Laszlo; Imre, Sandor
2014-12-04
We show that reliable quantum communication over an unreliable quantum relay channels is possible. The coding scheme combines the results on the superadditivity of quantum channels and the efficient quantum coding approaches.
Ancilla-assisted quantum process tomography.
Altepeter, J B; Branning, D; Jeffrey, E; Wei, T C; Kwiat, P G; Thew, R T; O'Brien, J L; Nielsen, M A; White, A G
2003-05-16
Complete and precise characterization of a quantum dynamical process can be achieved via the method of quantum process tomography. Using a source of correlated photons, we have implemented several methods, each investigating a wide range of processes, e.g., unitary, decohering, and polarizing. One of these methods, ancilla-assisted process tomography (AAPT), makes use of an additional "ancilla system," and we have theoretically determined the conditions when AAPT is possible. Surprisingly, entanglement is not required. We present data obtained using both separable and entangled input states. The use of entanglement yields superior results, however. PMID:12785945
Quantum states for Heisenberg-limited interferometry
Uys, H.; Meystre, P.
2007-07-15
The phase sensitivity of interferometers is limited by the so-called Heisenberg limit, which states that the optimum phase sensitivity is inversely proportional to the number of interfering particles N, a 1/{radical}(N) improvement over the standard quantum limit. We have used simulated annealing, a global optimization strategy, to systematically search for quantum interferometer input states that approach the Heisenberg-limited uncertainty in estimates of the interferometer phase shift. We compare the performance of these states to that of other nonclassical states already known to yield Heisenberg-limited uncertainty.
Quantum thermodynamics of general quantum processes.
Binder, Felix; Vinjanampathy, Sai; Modi, Kavan; Goold, John
2015-03-01
Accurately describing work extraction from a quantum system is a central objective for the extension of thermodynamics to individual quantum systems. The concepts of work and heat are surprisingly subtle when generalizations are made to arbitrary quantum states. We formulate an operational thermodynamics suitable for application to an open quantum system undergoing quantum evolution under a general quantum process by which we mean a completely positive and trace-preserving map. We derive an operational first law of thermodynamics for such processes and show consistency with the second law. We show that heat, from the first law, is positive when the input state of the map majorizes the output state. Moreover, the change in entropy is also positive for the same majorization condition. This makes a strong connection between the two operational laws of thermodynamics. PMID:25871066
Schuurmans, R. Milou; van Alphen, Pascal; Schuurmans, J. Merijn; Matthijs, Hans C. P.; Hellingwerf, Klaas J.
2015-01-01
The societal importance of renewable carbon-based commodities and energy carriers has elicited a particular interest for high performance phototrophic microorganisms. Selection of optimal strains is often based on direct comparison under laboratory conditions of maximal growth rate or additional valued features such as lipid content. Instead of reporting growth rate in culture, estimation of photosynthetic efficiency (quantum yield of PSII) by pulse-amplitude modulated (PAM) fluorimetry is an often applied alternative method. Here we compared the quantum yield of PSII and the photonic yield on biomass for the green alga Chlorella sorokiniana 211-8K and the cyanobacterium Synechocystis sp. PCC 6803. Our data demonstrate that the PAM technique inherently underestimates the photosynthetic efficiency of cyanobacteria by rendering a high F0 and a low FM, specifically after the commonly practiced dark pre-incubation before a yield measurement. Yet when comparing the calculated biomass yield on light in continuous culture experiments, we obtained nearly equal values for both species. Using mutants of Synechocystis sp. PCC 6803, we analyzed the factors that compromise its PAM-based quantum yield measurements. We will discuss the role of dark respiratory activity, fluorescence emission from the phycobilisomes, and the Mehler-like reaction. Based on the above observations we recommend that PAM measurements in cyanobacteria are interpreted only qualitatively. PMID:26394153
Schuurmans, R Milou; van Alphen, Pascal; Schuurmans, J Merijn; Matthijs, Hans C P; Hellingwerf, Klaas J
2015-01-01
The societal importance of renewable carbon-based commodities and energy carriers has elicited a particular interest for high performance phototrophic microorganisms. Selection of optimal strains is often based on direct comparison under laboratory conditions of maximal growth rate or additional valued features such as lipid content. Instead of reporting growth rate in culture, estimation of photosynthetic efficiency (quantum yield of PSII) by pulse-amplitude modulated (PAM) fluorimetry is an often applied alternative method. Here we compared the quantum yield of PSII and the photonic yield on biomass for the green alga Chlorella sorokiniana 211-8K and the cyanobacterium Synechocystis sp. PCC 6803. Our data demonstrate that the PAM technique inherently underestimates the photosynthetic efficiency of cyanobacteria by rendering a high F0 and a low FM, specifically after the commonly practiced dark pre-incubation before a yield measurement. Yet when comparing the calculated biomass yield on light in continuous culture experiments, we obtained nearly equal values for both species. Using mutants of Synechocystis sp. PCC 6803, we analyzed the factors that compromise its PAM-based quantum yield measurements. We will discuss the role of dark respiratory activity, fluorescence emission from the phycobilisomes, and the Mehler-like reaction. Based on the above observations we recommend that PAM measurements in cyanobacteria are interpreted only qualitatively. PMID:26394153
Quantum Dimension and Quantum Projective Spaces
NASA Astrophysics Data System (ADS)
Matassa, Marco
2014-09-01
We show that the family of spectral triples for quantum projective spaces introduced by D'Andrea and Dąbrowski, which have spectral dimension equal to zero, can be reconsidered as modular spectral triples by taking into account the action of the element K_{2rho} or its inverse. The spectral dimension computed in this sense coincides with the dimension of the classical projective spaces. The connection with the well known notion of quantum dimension of quantum group theory is pointed out.
Counterfactual quantum cryptography.
Noh, Tae-Gon
2009-12-01
Quantum cryptography allows one to distribute a secret key between two remote parties using the fundamental principles of quantum mechanics. The well-known established paradigm for the quantum key distribution relies on the actual transmission of signal particle through a quantum channel. In this Letter, we show that the task of a secret key distribution can be accomplished even though a particle carrying secret information is not in fact transmitted through the quantum channel. The proposed protocols can be implemented with current technologies and provide practical security advantages by eliminating the possibility that an eavesdropper can directly access the entire quantum system of each signal particle.
NASA Astrophysics Data System (ADS)
Viennot, David; Aubourg, Lucile
2016-02-01
We study a theoretical model of closed quasi-hermitian chain of spins which exhibits quantum analogues of chimera states, i.e. long life classical states for which a part of an oscillator chain presents an ordered dynamics whereas another part presents a disordered dynamics. For the quantum analogue, the chimera behaviour deals with the entanglement between the spins of the chain. We discuss the entanglement properties, quantum chaos, quantum disorder and semi-classical similarity of our quantum chimera system. The quantum chimera concept is novel and induces new perspectives concerning the entanglement of multipartite systems.
Counterfactual quantum cryptography.
Noh, Tae-Gon
2009-12-01
Quantum cryptography allows one to distribute a secret key between two remote parties using the fundamental principles of quantum mechanics. The well-known established paradigm for the quantum key distribution relies on the actual transmission of signal particle through a quantum channel. In this Letter, we show that the task of a secret key distribution can be accomplished even though a particle carrying secret information is not in fact transmitted through the quantum channel. The proposed protocols can be implemented with current technologies and provide practical security advantages by eliminating the possibility that an eavesdropper can directly access the entire quantum system of each signal particle. PMID:20366133
Quantum information causality.
Pitalúa-García, Damián
2013-05-24
How much information can a transmitted physical system fundamentally communicate? We introduce the principle of quantum information causality, which states the maximum amount of quantum information that a quantum system can communicate as a function of its dimension, independently of any previously shared quantum physical resources. We present a new quantum information task, whose success probability is upper bounded by the new principle, and show that an optimal strategy to perform it combines the quantum teleportation and superdense coding protocols with a task that has classical inputs. PMID:23745844
Multiscale quantum optical networks
NASA Astrophysics Data System (ADS)
Jaroszkiewicz, George
2007-04-01
Quantum experiments are described in terms of time-dependent networks of quantum bits, each qubit representing an elementary information gateway. The emphasis is on the signal properties of apparatus rather than on systems under observation (SUOs), with the quantum states of the theory (the labstates) representing the observer's information about the state of their apparatus, rather than of any SUO. The formalism gives an efficient quantum register description related to the formalism of quantum computation. Experiments conventionally described by the PVM and POVM formalisms are treated in identical terms, the formalism providing an efficient modular approach to quantum optics experiments of arbitrary complexity.
Lan, S-Y; Radnaev, A G; Collins, O A; Matsukevich, D N; Kennedy, T A; Kuzmich, A
2009-08-01
A quantum repeater is a system for long-distance quantum communication that employs quantum memory elements to mitigate optical fiber transmission losses. The multiplexed quantum memory (O. A. Collins, S. D. Jenkins, A. Kuzmich, and T. A. B. Kennedy, Phys. Rev. Lett. 98, 060502 (2007)) has been shown theoretically to reduce quantum memory time requirements. We present an initial implementation of a multiplexed quantum memory element in a cold rubidium gas. We show that it is possible to create atomic excitations in arbitrary memory element pairs and demonstrate the violation of Bell's inequality for light fields generated during the write and read processes.
Quantum capacity of quantum black holes
NASA Astrophysics Data System (ADS)
Adami, Chris; Bradler, Kamil
2014-03-01
The fate of quantum entanglement interacting with a black hole has been an enduring mystery, not the least because standard curved space field theory does not address the interaction of black holes with matter. We discuss an effective Hamiltonian of matter interacting with a black hole that has a precise analogue in quantum optics and correctly reproduces both spontaneous and stimulated Hawking radiation with grey-body factors. We calculate the quantum capacity of this channel in the limit of perfect absorption, as well as in the limit of a perfectly reflecting black hole (a white hole). We find that the white hole is an optimal quantum cloner, and is isomorphic to the Unruh channel with positive quantum capacity. The complementary channel (across the horizon) is entanglement-breaking with zero capacity, avoiding a violation of the quantum no-cloning theorem. The black hole channel on the contrary has vanishing capacity, while its complement has positive capacity instead. Thus, quantum states can be reconstructed faithfully behind the black hole horizon, but not outside. This work sheds new light on black hole complementarity because it shows that black holes can both reflect and absorb quantum states without violating the no-cloning theorem, and makes quantum firewalls obsolete.
Quantum optics. Gravity meets quantum physics
Adams, Bernhard W.
2015-02-27
Albert Einstein’s general theory of relativity is a classical formulation but a quantum mechanical description of gravitational forces is needed, not only to investigate the coupling of classical and quantum systems but simply to give a more complete description of our physical surroundings. In this issue of Nature Photonics, Wen-Te Liao and Sven Ahrens reveal a link between quantum and gravitational physics. They propose that in the quantum-optical effect of superradiance, the world line of electromagnetic radiation is changed by the presence of a gravitational field.
Work and quantum phase transitions: quantum latency.
Mascarenhas, E; Bragança, H; Dorner, R; França Santos, M; Vedral, V; Modi, K; Goold, J
2014-06-01
We study the physics of quantum phase transitions from the perspective of nonequilibrium thermodynamics. For first-order quantum phase transitions, we find that the average work done per quench in crossing the critical point is discontinuous. This leads us to introduce the quantum latent work in analogy with the classical latent heat of first order classical phase transitions. For second order quantum phase transitions the irreversible work is closely related to the fidelity susceptibility for weak sudden quenches of the system Hamiltonian. We demonstrate our ideas with numerical simulations of first, second, and infinite order phase transitions in various spin chain models.
Quantum Darwinism in Quantum Brownian Motion
NASA Astrophysics Data System (ADS)
Blume-Kohout, Robin; Zurek, Wojciech H.
2008-12-01
Quantum Darwinism—the redundant encoding of information about a decohering system in its environment—was proposed to reconcile the quantum nature of our Universe with apparent classicality. We report the first study of the dynamics of quantum Darwinism in a realistic model of decoherence, quantum Brownian motion. Prepared in a highly squeezed state—a macroscopic superposition—the system leaves records whose redundancy increases rapidly with initial delocalization. Redundancy appears rapidly (on the decoherence time scale) and persists for a long time.
Quantum Darwinism in quantum Brownian motion.
Blume-Kohout, Robin; Zurek, Wojciech H
2008-12-12
Quantum Darwinism--the redundant encoding of information about a decohering system in its environment--was proposed to reconcile the quantum nature of our Universe with apparent classicality. We report the first study of the dynamics of quantum Darwinism in a realistic model of decoherence, quantum Brownian motion. Prepared in a highly squeezed state--a macroscopic superposition--the system leaves records whose redundancy increases rapidly with initial delocalization. Redundancy appears rapidly (on the decoherence time scale) and persists for a long time.
Quantum Kolmogorov complexity and bounded quantum memory
Miyadera, Takayuki
2011-04-15
The effect of bounded quantum memory in a primitive information protocol has been examined using the quantum Kolmogorov complexity as a measure of information. We employed a toy two-party protocol in which Bob, by using a bounded quantum memory and an unbounded classical memory, estimates a message that was encoded in qubits by Alice in one of the bases X or Z. Our theorem gave a nontrivial effect of the memory boundedness. In addition, a generalization of the uncertainty principle in the presence of quantum memory has been obtained.
Evaluation of a cotton stripper yield monitor
Technology Transfer Automated Retrieval System (TEKTRAN)
The objective of this work was to evaluate the accuracy of a microwave sensor based yield monitor for measuring yield on a cotton stripper harvester and determine if the yield monitor can discriminate differences in yield to the same level as a reference scale system. A new yield monitor was instal...
Quantum Darwinian Evolution Implies Tumor Origination
NASA Astrophysics Data System (ADS)
Cooper, W. Grant
2011-03-01
Quantum uncertainty limits operating on metastable amino DNA protons drive the arrangement, keto-amino ? enol-imine, which contributes to time-dependent stochastic mutations. Product enol-imine protons participate in coupled quantum oscillations at frequencies of about 1013 s-1 until ``measured by'' an evolutionarily selected quantum reader, the transcriptase. This introduces entanglement states between coherent protons and transcriptase components, which ultimately yield an ensemble of decohered, non-reequilibrated enol and imine isomers that participate in ``molecular clock'' base substitutions at G'-C' and *G-*C sites. This introduces a quantum Darwinian evolution model which (a) simulates incidence of cancer data and (b) implies insight into quantum origins of evolutionary extinction. Data identify an inherited ``genetic space,'' s, which is initially mutation-free and satisfies the inequality, 1 = s = 0.97. When accumulated stochastic mutations cause s-values to approach their evolutionarily allowed threshold limit, s 0.97 + e, age-related degenerative disease is manifested. This implies a gain in evolutionary advantage which protects the gene pool against acquiring unsafe levels of mutation. Data requiring coherent states imply that classical duplex DNA contains an embedded microphysical subset of electron lone-pairs and hydrogen bonded protons that govern time-dependent genetic specificity in terms of quantum probability laws.
Converting Coherence to Quantum Correlations
NASA Astrophysics Data System (ADS)
Ma, Jiajun; Yadin, Benjamin; Girolami, Davide; Vedral, Vlatko; Gu, Mile
2016-04-01
Recent results in quantum information theory characterize quantum coherence in the context of resource theories. Here, we study the relation between quantum coherence and quantum discord, a kind of quantum correlation which appears even in nonentangled states. We prove that the creation of quantum discord with multipartite incoherent operations is bounded by the amount of quantum coherence consumed in its subsystems during the process. We show how the interplay between quantum coherence consumption and creation of quantum discord works in the preparation of multipartite quantum correlated states and in the model of deterministic quantum computation with one qubit.
Converting Coherence to Quantum Correlations.
Ma, Jiajun; Yadin, Benjamin; Girolami, Davide; Vedral, Vlatko; Gu, Mile
2016-04-22
Recent results in quantum information theory characterize quantum coherence in the context of resource theories. Here, we study the relation between quantum coherence and quantum discord, a kind of quantum correlation which appears even in nonentangled states. We prove that the creation of quantum discord with multipartite incoherent operations is bounded by the amount of quantum coherence consumed in its subsystems during the process. We show how the interplay between quantum coherence consumption and creation of quantum discord works in the preparation of multipartite quantum correlated states and in the model of deterministic quantum computation with one qubit.
EDITORIAL: Focus on Quantum Control
NASA Astrophysics Data System (ADS)
Rabitz, Herschel
2009-10-01
represent two-photon power spectra of arbitrarily and adaptively shaped broadband laser pulses M A Montgomery and N H Damrauer Accurate and efficient implementation of the von Neumann representation for laser pulses with discrete and finite spectra Frank Dimler, Susanne Fechner, Alexander Rodenberg, Tobias Brixner and David J Tannor Coherent strong-field control of multiple states by a single chirped femtosecond laser pulse M Krug, T Bayer, M Wollenhaupt, C Sarpe-Tudoran, T Baumert, S S Ivanov and N V Vitanov Quantum-state measurement of ionic Rydberg wavepackets X Zhang and R R Jones On the paradigm of coherent control: the phase-dependent light-matter interaction in the shaping window Tiago Buckup, Jurgen Hauer and Marcus Motzkus Use of the spatial phase of a focused laser beam to yield mechanistic information about photo-induced chemical reactions V J Barge, Z Hu and R J Gordon Coherent control of multiple vibrational excitations for optimal detection S D McGrane, R J Scharff, M Greenfield and D S Moore Mode selectivity with polarization shaping in the mid-IR David B Strasfeld, Chris T Middleton and Martin T Zanni Laser-guided relativistic quantum dynamics Chengpu Liu, Markus C Kohler, Karen Z Hatsagortsyan, Carsten Muller and Christoph H Keitel Continuous quantum error correction as classical hybrid control Hideo Mabuchi Quantum filter reduction for measurement-feedback control via unsupervised manifold learning Anne E B Nielsen, Asa S Hopkins and Hideo Mabuchi Control of the temporal profile of the local electromagnetic field near metallic nanostructures Ilya Grigorenko and Anatoly Efimov Laser-assisted molecular orientation in gaseous media: new possibilities and applications Dmitry V Zhdanov and Victor N Zadkov Optimization of laser field-free orientation of a state-selected NO molecular sample Arnaud Rouzee, Arjan Gijsbertsen, Omair Ghafur, Ofer M Shir, Thomas Back, Steven Stolte and Marc J J Vrakking Controlling the sense of molecular rotation Sharly Fleischer
Kendon, Vivien M; Nemoto, Kae; Munro, William J
2010-08-13
We briefly review what a quantum computer is, what it promises to do for us and why it is so hard to build one. Among the first applications anticipated to bear fruit is the quantum simulation of quantum systems. While most quantum computation is an extension of classical digital computation, quantum simulation differs fundamentally in how the data are encoded in the quantum computer. To perform a quantum simulation, the Hilbert space of the system to be simulated is mapped directly onto the Hilbert space of the (logical) qubits in the quantum computer. This type of direct correspondence is how data are encoded in a classical analogue computer. There is no binary encoding, and increasing precision becomes exponentially costly: an extra bit of precision doubles the size of the computer. This has important consequences for both the precision and error-correction requirements of quantum simulation, and significant open questions remain about its practicality. It also means that the quantum version of analogue computers, continuous-variable quantum computers, becomes an equally efficient architecture for quantum simulation. Lessons from past use of classical analogue computers can help us to build better quantum simulators in future.
Self-assembled quantum dots in a nanowire system for quantum photonics
NASA Astrophysics Data System (ADS)
Heiss, M.; Fontana, Y.; Gustafsson, A.; Wüst, G.; Magen, C.; O'Regan, D. D.; Luo, J. W.; Ketterer, B.; Conesa-Boj, S.; Kuhlmann, A. V.; Houel, J.; Russo-Averchi, E.; Morante, J. R.; Cantoni, M.; Marzari, N.; Arbiol, J.; Zunger, A.; Warburton, R. J.; Fontcuberta I Morral, A.
2013-05-01
Quantum dots embedded within nanowires represent one of the most promising technologies for applications in quantum photonics. Whereas the top-down fabrication of such structures remains a technological challenge, their bottom-up fabrication through self-assembly is a potentially more powerful strategy. However, present approaches often yield quantum dots with large optical linewidths, making reproducibility of their physical properties difficult. We present a versatile quantum-dot-in-nanowire system that reproducibly self-assembles in core-shell GaAs/AlGaAs nanowires. The quantum dots form at the apex of a GaAs/AlGaAs interface, are highly stable, and can be positioned with nanometre precision relative to the nanowire centre. Unusually, their emission is blue-shifted relative to the lowest energy continuum states of the GaAs core. Large-scale electronic structure calculations show that the origin of the optical transitions lies in quantum confinement due to Al-rich barriers. By emitting in the red and self-assembling on silicon substrates, these quantum dots could therefore become building blocks for solid-state lighting devices and third-generation solar cells.
Self-assembled quantum dots in a nanowire system for quantum photonics.
Heiss, M; Fontana, Y; Gustafsson, A; Wüst, G; Magen, C; O'Regan, D D; Luo, J W; Ketterer, B; Conesa-Boj, S; Kuhlmann, A V; Houel, J; Russo-Averchi, E; Morante, J R; Cantoni, M; Marzari, N; Arbiol, J; Zunger, A; Warburton, R J; Fontcuberta i Morral, A
2013-05-01
Quantum dots embedded within nanowires represent one of the most promising technologies for applications in quantum photonics. Whereas the top-down fabrication of such structures remains a technological challenge, their bottom-up fabrication through self-assembly is a potentially more powerful strategy. However, present approaches often yield quantum dots with large optical linewidths, making reproducibility of their physical properties difficult. We present a versatile quantum-dot-in-nanowire system that reproducibly self-assembles in core-shell GaAs/AlGaAs nanowires. The quantum dots form at the apex of a GaAs/AlGaAs interface, are highly stable, and can be positioned with nanometre precision relative to the nanowire centre. Unusually, their emission is blue-shifted relative to the lowest energy continuum states of the GaAs core. Large-scale electronic structure calculations show that the origin of the optical transitions lies in quantum confinement due to Al-rich barriers. By emitting in the red and self-assembling on silicon substrates, these quantum dots could therefore become building blocks for solid-state lighting devices and third-generation solar cells. PMID:23377293
Distinguishability of generic quantum states
NASA Astrophysics Data System (ADS)
Puchała, Zbigniew; Pawela, Łukasz; Życzkowski, Karol
2016-06-01
Properties of random mixed states of dimension N distributed uniformly with respect to the Hilbert-Schmidt measure are investigated. We show that for large N , due to the concentration of measure, the trace distance between two random states tends to a fixed number D ˜=1 /4 +1 /π , which yields the Helstrom bound on their distinguishability. To arrive at this result, we apply free random calculus and derive the symmetrized Marchenko-Pastur distribution, which is shown to describe numerical data for the model of coupled quantum kicked tops. Asymptotic value for the root fidelity between two random states, √{F }=3/4 , can serve as a universal reference value for further theoretical and experimental studies. Analogous results for quantum relative entropy and Chernoff quantity provide other bounds on the distinguishablity of both states in a multiple measurement setup due to the quantum Sanov theorem. We study also mean entropy of coherence of random pure and mixed states and entanglement of a generic mixed state of a bipartite system.
Efficient Quantum Pseudorandomness
NASA Astrophysics Data System (ADS)
Brandão, Fernando G. S. L.; Harrow, Aram W.; Horodecki, Michał
2016-04-01
Randomness is both a useful way to model natural systems and a useful tool for engineered systems, e.g., in computation, communication, and control. Fully random transformations require exponential time for either classical or quantum systems, but in many cases pseudorandom operations can emulate certain properties of truly random ones. Indeed, in the classical realm there is by now a well-developed theory regarding such pseudorandom operations. However, the construction of such objects turns out to be much harder in the quantum case. Here, we show that random quantum unitary time evolutions ("circuits") are a powerful source of quantum pseudorandomness. This gives for the first time a polynomial-time construction of quantum unitary designs, which can replace fully random operations in most applications, and shows that generic quantum dynamics cannot be distinguished from truly random processes. We discuss applications of our result to quantum information science, cryptography, and understanding the self-equilibration of closed quantum dynamics.
NASA Astrophysics Data System (ADS)
Vanner, Michael R.; Pikovski, Igor; Cole, Garrett D.; Kim, Myungshik; Brukner, Caslav; Hammerer, Klemens; Milburn, Gerard J.; Aspelmeyer, Markus
2011-03-01
By combining quantum optics with mechanical resonators an avenue is opened to extend investigations of quantum behavior into unprecendented mass regimes. The field resulting from this combination - ``cavity quantum optomechanics'' -- is receiving a surge of interest for its potential to contribute to quantum measurement and control, studies of decoherence and non-classical state preparation of macroscopic objects. However, quantum state preparation and especially quantum state reconstruction of mechanical oscillators is currently a significant challenge. We are pursuing a scheme that employs short optical pulses to realize quantum state tomography, squeezing via measurement and state purifcation of a mechanical resonator. The pulsed scheme has considerable resilience to initial thermal occupation, provides a promising means to explore the quantum nature of massive oscillators and can be applied to other systems such as trapped ions. Our theoretical proposal and experimental results will be discussed.
Spring, William Joseph
2009-04-13
We consider quantum analogues of n-parameter stochastic processes, associated integrals and martingale properties extending classical results obtained in [1, 2, 3], and quantum results in [4, 5, 6, 7, 8, 9, 10].
Efficient Quantum Pseudorandomness.
Brandão, Fernando G S L; Harrow, Aram W; Horodecki, Michał
2016-04-29
Randomness is both a useful way to model natural systems and a useful tool for engineered systems, e.g., in computation, communication, and control. Fully random transformations require exponential time for either classical or quantum systems, but in many cases pseudorandom operations can emulate certain properties of truly random ones. Indeed, in the classical realm there is by now a well-developed theory regarding such pseudorandom operations. However, the construction of such objects turns out to be much harder in the quantum case. Here, we show that random quantum unitary time evolutions ("circuits") are a powerful source of quantum pseudorandomness. This gives for the first time a polynomial-time construction of quantum unitary designs, which can replace fully random operations in most applications, and shows that generic quantum dynamics cannot be distinguished from truly random processes. We discuss applications of our result to quantum information science, cryptography, and understanding the self-equilibration of closed quantum dynamics. PMID:27176509
NASA Astrophysics Data System (ADS)
Jennewein, Thomas; Higgins, Brendon
2013-03-01
Sending satellites equipped with quantum technologies into space will be the first step towards a global quantum-communication network. As Thomas Jennewein and Brendon Higgins explain, these systems will also enable physicists to test fundamental physics in new regimes.
Quantum information and computation
Bennett, C.H.
1995-10-01
A new quantum theory of communication and computation is emerging, in which the stuff transmitted or processed is not classical information, but arbitrary superpositions of quantum states. {copyright} 1995 {ital American} {ital Institute} {ital of} {ital Physics}.
Efficient Quantum Pseudorandomness.
Brandão, Fernando G S L; Harrow, Aram W; Horodecki, Michał
2016-04-29
Randomness is both a useful way to model natural systems and a useful tool for engineered systems, e.g., in computation, communication, and control. Fully random transformations require exponential time for either classical or quantum systems, but in many cases pseudorandom operations can emulate certain properties of truly random ones. Indeed, in the classical realm there is by now a well-developed theory regarding such pseudorandom operations. However, the construction of such objects turns out to be much harder in the quantum case. Here, we show that random quantum unitary time evolutions ("circuits") are a powerful source of quantum pseudorandomness. This gives for the first time a polynomial-time construction of quantum unitary designs, which can replace fully random operations in most applications, and shows that generic quantum dynamics cannot be distinguished from truly random processes. We discuss applications of our result to quantum information science, cryptography, and understanding the self-equilibration of closed quantum dynamics.
Quantum Spread Spectrum Communication
Humble, Travis S
2010-01-01
We demonstrate that spectral teleportation can coherently dilate the spectral probability amplitude of a single photon. In preserving the encoded quantum information, this variant of teleportation subsequently enables a form of quantum spread spectrum communication.
NASA Astrophysics Data System (ADS)
Goyal, Ketan; Kawai, Ryoichi
As nanotechnology advances, understanding of the thermodynamic properties of small systems becomes increasingly important. Such systems are found throughout physics, biology, and chemistry manifesting striking properties that are a direct result of their small dimensions where fluctuations become predominant. The standard theory of thermodynamics for macroscopic systems is powerless for such ever fluctuating systems. Furthermore, as small systems are inherently quantum mechanical, influence of quantum effects such as discreteness and quantum entanglement on their thermodynamic properties is of great interest. In particular, the quantum fluctuations due to quantum uncertainty principles may play a significant role. In this talk, we investigate thermodynamic properties of an autonomous quantum heat engine, resembling a quantum version of the Feynman Ratchet, in non-equilibrium condition based on the theory of open quantum systems. The heat engine consists of multiple subsystems individually contacted to different thermal environments.
Ferritin-Templated Quantum-Dots for Quantum Logic Gates
NASA Technical Reports Server (NTRS)
Choi, Sang H.; Kim, Jae-Woo; Chu, Sang-Hyon; Park, Yeonjoon; King, Glen C.; Lillehei, Peter T.; Kim, Seon-Jeong; Elliott, James R.
2005-01-01
Quantum logic gates (QLGs) or other logic systems are based on quantum-dots (QD) with a stringent requirement of size uniformity. The QD are widely known building units for QLGs. The size control of QD is a critical issue in quantum-dot fabrication. The work presented here offers a new method to develop quantum-dots using a bio-template, called ferritin, that ensures QD production in uniform size of nano-scale proportion. The bio-template for uniform yield of QD is based on a ferritin protein that allows reconstitution of core material through the reduction and chelation processes. One of the biggest challenges for developing QLG is the requirement of ordered and uniform size of QD for arrays on a substrate with nanometer precision. The QD development by bio-template includes the electrochemical/chemical reconsitution of ferritins with different core materials, such as iron, cobalt, manganese, platinum, and nickel. The other bio-template method used in our laboratory is dendrimers, precisely defined chemical structures. With ferritin-templated QD, we fabricated the heptagonshaped patterned array via direct nano manipulation of the ferritin molecules with a tip of atomic force microscope (AFM). We also designed various nanofabrication methods of QD arrays using a wide range manipulation techniques. The precise control of the ferritin-templated QD for a patterned arrangement are offered by various methods, such as a site-specific immobilization of thiolated ferritins through local oxidation using the AFM tip, ferritin arrays induced by gold nanoparticle manipulation, thiolated ferritin positioning by shaving method, etc. In the signal measurements, the current-voltage curve is obtained by measuring the current through the ferritin, between the tip and the substrate for potential sweeping or at constant potential. The measured resistance near zero bias was 1.8 teraohm for single holoferritin and 5.7 teraohm for single apoferritin, respectively.
Quantum dots as active material for quantum cascade lasers: comparison to quantum wells
NASA Astrophysics Data System (ADS)
Michael, Stephan; Chow, Weng W.; Schneider, Hans Christian
2016-03-01
We review a microscopic laser theory for quantum dots as active material for quantum cascade lasers, in which carrier collisions are treated at the level of quantum kinetic equations. The computed characteristics of such a quantum-dot active material are compared to a state-of-the-art quantum-well quantum cascade laser. We find that the current requirement to achieve a comparable gain-length product is reduced compared to that of the quantum-well quantum cascade laser.
NASA Astrophysics Data System (ADS)
Bengtsson, Ingemar; Zyczkowski, Karol
2007-12-01
Preface; 1. Convexity, colours and statistics; 2. Geometry of probability distributions; 3. Much ado about spheres; 4. Complex projective spaces; 5. Outline of quantum mechanics; 6. Coherent states and group actions; 7. The stellar representation; 8. The space of density matrices; 9. Purification of mixed quantum states; 10. Quantum operations; 11. Duality: maps versus states; 12. Density matrices and entropies; 13. Distinguishability measures; 14. Monotone metrics and measures; 15. Quantum entanglement; Epilogue; Appendices; References; Index.
Huang, Liang; Lai Yingcheng; Ferry, David K.; Goodnick, Stephen M.; Akis, Richard
2009-07-31
The concentrations of wave functions about classical periodic orbits, or quantum scars, are a fundamental phenomenon in physics. An open question is whether scarring can occur in relativistic quantum systems. To address this question, we investigate confinements made of graphene whose classical dynamics are chaotic and find unequivocal evidence of relativistic quantum scars. The scarred states can lead to strong conductance fluctuations in the corresponding open quantum dots via the mechanism of resonant transmission.
Introduction to Quantum Computation
NASA Astrophysics Data System (ADS)
Ekert, A.
A computation is a physical process. It may be performed by a piece of electronics or on an abacus, or in your brain, but it is a process that takes place in nature and as such it is subject to the laws of physics. Quantum computers are machines that rely on characteristically quantum phenomena, such as quantum interference and quantum entanglement in order to perform computation. In this series of lectures I want to elaborate on the computational power of such machines.
Quantum computing and probability.
Ferry, David K
2009-11-25
Over the past two decades, quantum computing has become a popular and promising approach to trying to solve computationally difficult problems. Missing in many descriptions of quantum computing is just how probability enters into the process. Here, we discuss some simple examples of how uncertainty and probability enter, and how this and the ideas of quantum computing challenge our interpretations of quantum mechanics. It is found that this uncertainty can lead to intrinsic decoherence, and this raises challenges for error correction.
Is quantum probability rational?
Houston, Alasdair I; Wiesner, Karoline
2013-06-01
We concentrate on two aspects of the article by Pothos & Busemeyer (P&B): the relationship between classical and quantum probability and quantum probability as a basis for rational decisions. We argue that the mathematical relationship between classical and quantum probability is not quite what the authors claim. Furthermore, it might be premature to regard quantum probability as the best practical rational scheme for decision making.
Correlations of the Time Dependent Signal and the State of a Continuously Monitored Quantum System
NASA Astrophysics Data System (ADS)
Foroozani, N.; Naghiloo, M.; Tan, D.; Mølmer, K.; Murch, K. W.
2016-03-01
In quantum physics, measurements give random results and yield a corresponding random backaction on the state of the system subject to measurement. If a quantum system is probed continuously over time, its state evolves along a stochastic quantum trajectory. To investigate the characteristic properties of such dynamics, we perform weak continuous measurements on a superconducting qubit that is driven to undergo Rabi oscillations. From the data we observe a number of striking temporal correlations within the time dependent signals and the quantum trajectories of the qubit, and we discuss their explanation in terms of quantum measurement and photodetection theory.
Interaction of Water-Soluble CdTe Quantum Dots with Bovine Serum Albumin
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
NASA Astrophysics Data System (ADS)
Salih, Hatim
2016-05-01
The phenomenon of quantum erasure has long intrigued physicists, but has surprisingly found limited practical application. Here, we propose a protocol for quantum key distribution (QKD) based on quantum erasure, promising inherent security against detector attacks. We particularly demonstrate its security against a powerful detector-blinding attack.
Eavesdropping without quantum memory
Bechmann-Pasquinucci, H.
2006-04-15
In quantum cryptography the optimal eavesdropping strategy requires that the eavesdropper uses ancillas and quantum memories in order to optimize her information. What happens if the eavesdropper has no quantum memory? It is shown that in this case the eavesdropper obtains a better information/disturbance trade-off by adopting the simple intercept/resend strategy.
Quantum phenomena in superconductors
Clarke, J.
1987-08-01
This paper contains remarks by the author on aspects of macroscopic quantum phenomena in superconductors. Some topics discussed are: Superconducting low-inductance undulatory galvanometer (SLUGS), charge imbalance, cylindrical dc superconducting quantum interference device (SQUIDS), Geophysics, noise theory, magnetic resonance with SQUIDS, and macroscopic quantum tunneling. 23 refs., 4 figs. (LSP)
NASA Astrophysics Data System (ADS)
Iqbal, A.; Toor, A. H.
2002-03-01
We investigate the role of quantum mechanical effects in the central stability concept of evolutionary game theory, i.e., an evolutionarily stable strategy (ESS). Using two and three-player symmetric quantum games we show how the presence of quantum phenomenon of entanglement can be crucial to decide the course of evolutionary dynamics in a population of interacting individuals.
Mesoscopic cavity quantum electrodynamics with quantum dots
Childress, L.; Soerensen, A.S.; Lukin, M.D.
2004-04-01
We describe an electrodynamic mechanism for coherent, quantum-mechanical coupling between spatially separated quantum dots on a microchip. The technique is based on capacitive interactions between the electron charge and a superconducting transmission line resonator, and is closely related to atomic cavity quantum electrodynamics. We investigate several potential applications of this technique which have varying degrees of complexity. In particular, we demonstrate that this mechanism allows design and investigation of an on-chip double-dot microscopic maser. Moreover, the interaction may be extended to couple spatially separated electron-spin states while only virtually populating fast-decaying superpositions of charge states. This represents an effective, controllable long-range interaction, which may facilitate implementation of quantum information processing with electron-spin qubits and potentially allow coupling to other quantum systems such as atomic or superconducting qubits.