Sample records for ir multiple-photon excitation

  1. Photo-Redox Activated Drug Delivery Systems Operating Under Two Photon Excitation in the Near-IR

    PubMed Central

    Guardado-Alvarez, Tania M.; Devi, Lekshmi Sudha; Vabre, Jean-Marie; Pecorelli, Travis; Schwartz, Benjamin J.; Durand, Jean-Olivier; Mongin, Olivier; Blanchard-Desce, Mireille; Zink, Jeffrey I.

    2014-01-01

    We report the design and synthesis of a nano-container consisting of mesoporous silica nanoparticles with the pore openings covered by “snap-top” caps that are opened by near-IR light. A photo transducer molecule that is a reducing agent in an excited electronic state is covalently attached to the system. Near IR two-photon excitation causes inter-molecular electron transfer that reduces a disulfide bond holding the cap in place, thus allowing the cargo molecules to escape. We describe the operation of the “snap-top” release mechanism by both one- and two-photon activation. This system presents a proof of concept of a near-IR photoredox-induced nanoparticle delivery system that may lead to a new type of photodynamic drug release therapy. PMID:24647752

  2. Photo-redox activated drug delivery systems operating under two photon excitation in the near-IR.

    PubMed

    Guardado-Alvarez, Tania M; Devi, Lekshmi Sudha; Vabre, Jean-Marie; Pecorelli, Travis A; Schwartz, Benjamin J; Durand, Jean-Olivier; Mongin, Olivier; Blanchard-Desce, Mireille; Zink, Jeffrey I

    2014-05-07

    We report the design and synthesis of a nano-container consisting of mesoporous silica nanoparticles with the pore openings covered by "snap-top" caps that are opened by near-IR light. A photo transducer molecule that is a reducing agent in an excited electronic state is covalently attached to the system. Near IR two-photon excitation causes inter-molecular electron transfer that reduces a disulfide bond holding the cap in place, thus allowing the cargo molecules to escape. We describe the operation of the "snap-top" release mechanism by both one- and two-photon activation. This system presents a proof of concept of a near-IR photoredox-induced nanoparticle delivery system that may lead to a new type of photodynamic drug release therapy.

  3. Multiple-photon excitation of nitrogen vacancy centers in diamond

    NASA Astrophysics Data System (ADS)

    Ji, Peng; Balili, R.; Beaumariage, J.; Mukherjee, S.; Snoke, D.; Dutt, M. V. Gurudev

    2018-04-01

    We report the observation of multiphoton photoluminescence excitation (PLE) below the resonant energies of nitrogen vacancy (NV) centers in diamond. The quadratic and cubic dependence of the integrated fluorescence intensity as a function of excitation power indicates a two-photon excitation pathway for the NV- charge state and a three-photon process involved for the neutral NV0 charge state, respectively. Comparing the total multiphoton energy with its single-photon equivalent, the PLE spectra follows the absorption spectrum of single photon excitation. We also observed that the efficiency of photoluminescence for different charge states, as well as the decay time constant, was dependent on the excitation wavelength and power.

  4. Single-photon and two-photon excited fluorescence behavior of a novel fluorene-based compound

    NASA Astrophysics Data System (ADS)

    Ma, Wenbo; Wu, Yiquan; Gu, Donghong; Gan, Fuxi

    2005-09-01

    A D-π-D type compound, 2,7-bis(4-methoxystyryl)-9,9-bis(2-ethylhexyl)-9H-fluorene (abbreviated as MO-Flu-MO), where electron-donor D is methoxy group andπis fluorene unit, has been synthesized. The molecular structures of the compound were characterized by elemental analyses, EI-MS and FT-IR spectra. UV-Vis spectra in the region 230--1000 nm and single-photon excited fluorescence in tetrahydrofuran (THF) of the compound were measured. It is found that the new compound exhibits strong two-photon excited fluorescence in the region 380--500 nm and moderate two-photon absorption (TPA) value in the femtoseconds regime (TPA cross-section as high as 55×10-50 cm4 s photon-1 with 13fs laser pulses). The results demonstrate that the compound is a promising candidate for two-photon three-dimensional (3D) optical data storage.

  5. Photofunctional triplet excited states of cyclometalated Ir(III) complexes: beyond electroluminescence.

    PubMed

    You, Youngmin; Nam, Wonwoo

    2012-11-07

    The development of cyclometalated Ir(III) complexes has enabled important breakthroughs in electroluminescence because such complexes permit the efficient population of triplet excited states that give rise to luminescent transitions. The triplet states of Ir(III) complexes are advantageous over those of other transition metal complexes in that their electronic transitions and charge-transfer characteristics are tunable over wide ranges. These favorable properties suggest that Ir(III) complexes have significant potential in a variety of photofunctions other than electroluminescence. In this critical review, we describe recent photonic applications of novel Ir(III) complexes. Ir(III) complexes have been shown to affect the exciton statistics in the active layers of organic photovoltaic cells, thereby improving the photon-to-current conversion efficiencies. Nonlinear optical applications that take advantage of the strong charge-transfer properties of triplet transitions are also discussed. The tunability of the electrochemical potentials facilitates the development of efficient photocatalysis in the context of water photolysis or organic syntheses. The photoredox reactivities of Ir(III) complexes have been employed in studies of charge migration along DNA chains. The photoinduced cytotoxicity of Ir(III) complexes on live cells suggests that the complexes may be useful in photodynamic therapy. Potential biological applications of the complexes include phosphorescence labeling and sensing. Intriguing platforms based on cyclometalated Ir(III) complexes potentially provide novel protein tagging and ratiometric detection. We envision that future research into the photofunctionality of Ir(III) complexes will provide important breakthroughs in a variety of photonic applications.

  6. Single photon infrared emission spectroscopy: a study of IR emission from UV laser excited PAHs between 3 and 15 micrometers

    NASA Technical Reports Server (NTRS)

    Cook, D. J.; Schlemmer, S.; Balucani, N.; Wagner, D. R.; Harrison, J. A.; Steiner, B.; Saykally, R. J.

    1998-01-01

    Single-photon infrared emission spectroscopy (SPIRES) has been used to measure emission spectra from polycyclic aromatic hydrocarbons (PAHs). A supersonic free-jet expansion has been used to provide emission spectra of rotationally cold and vibrationally excited naphthalene and benzene. Under these conditions, the observed width of the 3.3-micrometers (C-H stretch) band resembles the bandwidths observed in experiments in which emission is observed from naphthalene with higher rotational energy. To obtain complete coverage of IR wavelengths relevant to the unidentified infrared bands (UIRs), UV laser-induced desorption was used to generate gas-phase highly excited PAHs. Lorentzian band shapes were convoluted with the monochromator-slit function in order to determine the widths of PAH emission bands under astrophysically relevant conditions. Bandwidths were also extracted from bands consisting of multiple normal modes blended together. These parameters are grouped according to the functional groups mostly involved in the vibration, and mean bandwidths are obtained. These bandwidths are larger than the widths of the corresponding UIR bands. However, when the comparison is limited to the largest PAHs studied, the bandwidths are slightly smaller than the corresponding UIR bands. These parameters can be used to model emission spectra from PAH cations and cations of larger PAHs, which are better candidate carriers of the UIRs.

  7. Two-photon luminescence from polar bis-terpyridyl-stilbene derivatives of Ir(III) and Ru(II).

    PubMed

    Natrajan, Louise S; Toulmin, Anita; Chew, Alex; Magennis, Steven W

    2010-12-07

    Four structurally related iridium(III) and ruthenium(II) complexes bearing two polar terpyridyl-stilbene derived chromophores 4-(4-{2-[4-(methoxy)phenyl]ethenyl}phenyl)-2,2'-6',2''-terpyridine (ttpyeneanisole) and 4-(4-{2-[phenyl]ethenyl}phenyl)-2,2'-6',2''-terpyridine (tpystilbene) have been synthesised and characterised in the solid state and in solution. In the solid state, the dihedral angle subtending the pyridyl and tolyl groups of 27.1° in the Ir(III) complex [Ir(ttpyeneanisole)(2)]·3PF(6) is more acute than in the Ru(II) derivative [Ru(tpystilbene)(2)]·2PF(6) (35.5°), indicating the presence of a greater degree of π-delocalisation across the terpyridine unit in the former compound. Their luminescence properties in fluid solution have been investigated following both resonant and non-resonant excitation. We have shown that each of the complexes undergoes two-photon excitation when excited in the near infrared (740 to 820 nm), with two-photon absorption cross sections in the range 11-67 × 10(-50) cm(4) s photon(-1). The larger cross sections for the Ir(III) complexes reflect the differences observed in the solid state. This work therefore demonstrates that such complexes are promising as luminescent markers for 3D imaging and illustrates that simple functionalisation of the chromophores and the choice of metal can lead to marked enhancements in the two-photon cross sections (σ(2)) compared to those of simpler heteroleptic polypyridyl based derivatives.

  8. Direct two-photon excitation of Sm3+, Eu3+, Tb3+, Tb.DOTA-, and Tb.propargylDO3A in solution

    NASA Astrophysics Data System (ADS)

    Sørensen, Thomas Just; Blackburn, Octavia A.; Tropiano, Manuel; Faulkner, Stephen

    2012-07-01

    We have observed direct two-photon excitation of samarium, europium and terbium ions in solution upon near IR excitation using a tuneable pulsed light source, and have also studied two-photon processes in a pair of related terbium complexes, namely [Tb.DOTA]- and Tb.propargylDO3A. Direct two-photon excitation of lanthanides is observed in simple systems in the absence of sensitizing chromophores. Where even simple chromophores such as a triple bond are present in the complex, then single and two-photon excitation of chromophore excited states competes with direct two-photon excitation of the ions and is the dominant pathway for sensitizing formation of the lanthanide excited state.

  9. Time-resolved multicolor two-photon excitation fluorescence microscopy of cells and tissues

    NASA Astrophysics Data System (ADS)

    Zheng, Wei

    2014-11-01

    Multilabeling which maps the distribution of different targets is an indispensable technique in many biochemical and biophysical studies. Two-photon excitation fluorescence (TPEF) microscopy of endogenous fluorophores combining with conventional fluorescence labeling techniques such as genetically encoded fluorescent protein (FP) and fluorescent dyes staining could be a powerful tool for imaging living cells. However, the challenge is that the excitation and emission wavelength of these endogenous fluorophores and fluorescent labels are very different. A multi-color ultrafast source is required for the excitation of multiple fluorescence molecules. In this study, we developed a two-photon imaging system with excitations from the pump femtosecond laser and the selected supercontinuum generated from a photonic crystal fiber (PCF). Multiple endogenous fluorophores, fluorescent proteins and fluorescent dyes were excited in their optimal wavelengths simultaneously. A time- and spectral-resolved detection system was used to record the TPEF signals. This detection technique separated the TPEF signals from multiple sources in time and wavelength domains. Cellular organelles such as nucleus, mitochondria, microtubule and endoplasmic reticulum, were clearly revealed in the TPEF images. The simultaneous imaging of multiple fluorophores of cells will greatly aid the study of sub-cellular compartments and protein localization.

  10. Simultaneously exciting two atoms with photon-mediated Raman interactions

    NASA Astrophysics Data System (ADS)

    Zhao, Peng; Tan, Xinsheng; Yu, Haifeng; Zhu, Shi-Liang; Yu, Yang

    2017-06-01

    We propose an approach to simultaneously excite two atoms by using a cavity-assisted Raman process in combination with a cavity-photon-mediated interaction. The system consists of a two-level atom and a Λ -type or V -type three-level atom, which are coupled together with a cavity mode. Having derived the effective Hamiltonian, we find that under certain circumstances a single photon can simultaneously excite two atoms. In addition, multiple photons and even a classical field can also simultaneously excite two atoms. As an example, we show a scheme to realize our proposal in a circuit QED setup, which is artificial atoms coupled with a cavity. The dynamics and the quantum-statistical properties of the process are investigated with experimentally feasible parameters.

  11. Multi-photon excited coherent random laser emission in ZnO powders

    NASA Astrophysics Data System (ADS)

    Tolentino Dominguez, Christian; Gomes, Maria De A.; Macedo, Zélia S.; de Araújo, Cid B.; Gomes, Anderson S. L.

    2014-11-01

    We report the observation and analysis of anti-Stokes coherent random laser (RL) emission from zinc oxide (ZnO) powders excited by one-, two- or three-photon femtosecond laser radiation. The ZnO powders were produced via a novel proteic sol-gel, low-cost and environmentally friendly route using coconut water in the polymerization step of the metal precursor. One- and two-photon excitation at 354 nm and 710 nm, respectively, generated single-band emissions centred at about 387 nm. For three-photon excitation, the emission spectra showed a strong ultraviolet (UV) band (380-396 nm) attributed to direct three-photon absorption from the valence band to the conduction band. The presence of an intensity threshold and a bandwidth narrowing of the UV band from about 20 to 4 nm are clear evidence of RL action. The observation of multiple sub-nanometre narrow peaks in the emission spectra for excitation above the RL threshold is consistent with random lasing by coherent feedback.

  12. Selective two-photon excitation of a vibronic state by correlated photons.

    PubMed

    Oka, Hisaki

    2011-03-28

    We theoretically investigate the two-photon excitation of a molecular vibronic state by correlated photons with energy anticorrelation. A Morse oscillator having three sets of vibronic states is used, as an example, to evaluate the selectivity and efficiency of two-photon excitation. We show that a vibrational mode can be selectively excited with high efficiency by the correlated photons, without phase manipulation or pulse-shaping techniques. This can be achieved by controlling the quantum correlation so that the photon pair concurrently has two pulse widths, namely, a temporally narrow width and a spectrally narrow width. Though this concurrence is seemingly contradictory, we can create such a photon pair by tailoring the quantum correlation between two photons.

  13. Two-photon excitation fluorescence bioassays.

    PubMed

    Hänninen, Pekka; Soukka, Jori; Soini, Juhani T

    2008-01-01

    Application of two-photon excitation of fluorescence in microscopy is one of the major discoveries of the "renaissance" of light microscopy that started in the 1980s. The technique derives its advantages from the biologically "smooth" wavelength of the excitation light and the confinement of the excitation. Difficult, and seemingly nontransparent, samples may be imaged with the technique with good resolution. Although the bioresearch has been concentrating mostly on the positive properties of the technique for imaging, the same properties may be applied successfully to nonimaging bioassays. This article focuses on the development path of two-photon excitation-based assay system.

  14. Near-IR Two-Photon Fluorescent Sensor for K(+) Imaging in Live Cells.

    PubMed

    Sui, Binglin; Yue, Xiling; Kim, Bosung; Belfield, Kevin D

    2015-08-19

    A new two-photon excited fluorescent K(+) sensor is reported. The sensor comprises three moieties, a highly selective K(+) chelator as the K(+) recognition unit, a boron-dipyrromethene (BODIPY) derivative modified with phenylethynyl groups as the fluorophore, and two polyethylene glycol chains to afford water solubility. The sensor displays very high selectivity (>52-fold) in detecting K(+) over other physiological metal cations. Upon binding K(+), the sensor switches from nonfluorescent to highly fluorescent, emitting red to near-IR (NIR) fluorescence. The sensor exhibited a good two-photon absorption cross section, 500 GM at 940 nm. Moreover, it is not sensitive to pH in the physiological pH range. Time-dependent cell imaging studies via both one- and two-photon fluorescence microscopy demonstrate that the sensor is suitable for dynamic K(+) sensing in living cells.

  15. Wide-field three-photon excitation in biological samples

    PubMed Central

    Rowlands, Christopher J; Park, Demian; Bruns, Oliver T; Piatkevich, Kiryl D; Fukumura, Dai; Jain, Rakesh K; Bawendi, Moungi G; Boyden, Edward S; So, Peter TC

    2017-01-01

    Three-photon wide-field depth-resolved excitation is used to overcome some of the limitations in conventional point-scanning two- and three-photon microscopy. Excitation of chromophores as diverse as channelrhodopsins and quantum dots is shown, and a penetration depth of more than 700 μm into fixed scattering brain tissue is achieved, approximately twice as deep as that achieved using two-photon wide-field excitation. Compatibility with live animal experiments is confirmed by imaging the cerebral vasculature of an anesthetized mouse; a complete focal stack was obtained without any evidence of photodamage. As an additional validation of the utility of wide-field three-photon excitation, functional excitation is demonstrated by performing three-photon optogenetic stimulation of cultured mouse hippocampal neurons expressing a channelrhodopsin; action potentials could reliably be excited without causing photodamage. PMID:29152380

  16. Excitation Spectra and Brightness Optimization of Two-Photon Excited Probes

    PubMed Central

    Mütze, Jörg; Iyer, Vijay; Macklin, John J.; Colonell, Jennifer; Karsh, Bill; Petrášek, Zdeněk; Schwille, Petra; Looger, Loren L.; Lavis, Luke D.; Harris, Timothy D.

    2012-01-01

    Two-photon probe excitation data are commonly presented as absorption cross section or molecular brightness (the detected fluorescence rate per molecule). We report two-photon molecular brightness spectra for a diverse set of organic and genetically encoded probes with an automated spectroscopic system based on fluorescence correlation spectroscopy. The two-photon action cross section can be extracted from molecular brightness measurements at low excitation intensities, while peak molecular brightness (the maximum molecular brightness with increasing excitation intensity) is measured at higher intensities at which probe photophysical effects become significant. The spectral shape of these two parameters was similar across all dye families tested. Peak molecular brightness spectra, which can be obtained rapidly and with reduced experimental complexity, can thus serve as a first-order approximation to cross-section spectra in determining optimal wavelengths for two-photon excitation, while providing additional information pertaining to probe photostability. The data shown should assist in probe choice and experimental design for multiphoton microscopy studies. Further, we show that, by the addition of a passive pulse splitter, nonlinear bleaching can be reduced—resulting in an enhancement of the fluorescence signal in fluorescence correlation spectroscopy by a factor of two. This increase in fluorescence signal, together with the observed resemblance of action cross section and peak brightness spectra, suggests higher-order photobleaching pathways for two-photon excitation. PMID:22385865

  17. Highly sensitive detection of cancer cells using femtosecond dual-wavelength near-IR two-photon imaging.

    PubMed

    Starkey, Jean R; Makarov, Nikolay S; Drobizhev, Mikhail; Rebane, Aleksander

    2012-07-01

    We describe novel imaging protocols that allow detection of small cancer cell colonies deep inside tissue phantoms with high sensitivity and specificity. We compare fluorescence excited in Styryl-9M molecules by femtosecond pulses at near IR wavelengths, where Styryl-9M shows the largest dependence of the two-photon absorption (2PA) cross section on the local environment. We show that by calculating the normalized ratio of the two-photon excited fluorescence (2PEF) intensity at 1200 nm and 1100 nm excitation wavelengths we can achieve high sensitivity and specificity for determining the location of cancer cells surrounded by normal cells. The 2PEF results showed a positive correlation with the levels of MDR1 proteins expressed by the cells, and, for high MDR1 expressors, as few as ten cancer cells could be detected. Similar high sensitivity is also demonstrated for tumor colonies induced in mouse external ears. This technique could be useful in early cancer detection, and, perhaps, also in monitoring dormant cancer deposits.

  18. Apparatus for photon excited catalysis

    NASA Technical Reports Server (NTRS)

    Saffren, M. M. (Inventor)

    1977-01-01

    An apparatus is described for increasing the yield of photonically excited gas phase reactions by extracting excess energy from unstable, excited species by contacting the species with the surface of a finely divided solid.

  19. Strategic modulation of the photonic properties of conjugated organometallic Pt-Ir polymers exhibiting hybrid CT-excited states.

    PubMed

    Soliman, Ahmed M; Zysman-Colman, Eli; Harvey, Pierre D

    2015-04-01

    Polymer 6, ([trans-Pt(PBu3 )2 (C≡C)2 ]-[Ir(dFMeppy)2 (N^N)](PF6 ))n , (([Pt]-[Ir](PF6 ))n ; N^N = 5,5'-disubstituted-2,2'-bipyridyl; dFMeppy = 2-(2,4-difluoro-phenyl)-5-methylpyridine) is prepared along with model compounds. These complexes are investigated by absorption and emission spectroscopy and their photophysical and electrochemical properties are measured and compared with their corresponding non fluorinated complexes. Density functional theory (DFT) and time-dependent DFT computations corroborate the nature of the excited state as being a hybrid between the metal-to-ligand charge transfer ((1,3) MLCT) for the trans-Pt(PBu3 )2 (C≡CAr)2 unit, [Pt] and the metal-to-ligand/ligand-to-ligand' charge transfer ((1,3) ML'CT/LL'CT) for [Ir] with L = dFMeppy. Overall, the fluorination of the phenylpyridine group expectedly does not change the nature of the excited state but desirably induces a small blue shift of the absorption and emission bands along a slight decrease in emission quantum yields and lifetimes. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

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

    NASA Astrophysics Data System (ADS)

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

    2016-03-01

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

  1. Laser isotope separation by multiple photon absorption

    DOEpatents

    Robinson, C.P.; Rockwood, S.D.; Jensen, R.J.; Lyman, J.L.; Aldridge, J.P. III.

    1987-04-07

    Multiple photon absorption from an intense beam of infrared laser light may be used to induce selective chemical reactions in molecular species which result in isotope separation or enrichment. The molecular species must have a sufficient density of vibrational states in its vibrational manifold that, is the presence of sufficiently intense infrared laser light tuned to selectively excite only those molecules containing a particular isotope, multiple photon absorption can occur. By this technique, for example, intense CO[sub 2] laser light may be used to highly enrich [sup 34]S in natural SF[sub 6] and [sup 11]B in natural BCl[sub 3]. 8 figs.

  2. Laser isotope separation by multiple photon absorption

    DOEpatents

    Robinson, C. Paul; Rockwood, Stephen D.; Jensen, Reed J.; Lyman, John L.; Aldridge, III, Jack P.

    1987-01-01

    Multiple photon absorption from an intense beam of infrared laser light may be used to induce selective chemical reactions in molecular species which result in isotope separation or enrichment. The molecular species must have a sufficient density of vibrational states in its vibrational manifold that, is the presence of sufficiently intense infrared laser light tuned to selectively excite only those molecules containing a particular isotope, multiple photon absorption can occur. By this technique, for example, intense CO.sub.2 laser light may be used to highly enrich .sup.34 S in natural SF.sub.6 and .sup.11 B in natural BCl.sub.3.

  3. Laser isotope separation by multiple photon absorption

    DOEpatents

    Robinson, C. Paul; Rockwood, Stephen D.; Jensen, Reed J.; Lyman, John L.; Aldridge, III, Jack P.

    1977-01-01

    Multiple photon absorption from an intense beam of infrared laser light may be used to induce selective chemical reactions in molecular species which result in isotope separation or enrichment. The molecular species must have a sufficient density of vibrational states in its vibrational manifold that, in the presence of sufficiently intense infrared laser light tuned to selectively excite only those molecules containing a particular isotope, multiple photon absorption can occur. By this technique, for example, intense CO.sub.2 laser light may be used to highly enrich .sup.34 S in natural SF.sub.6 and .sup.11 B in natural BCl.sub.3.

  4. LASERS IN MEDICINE: Two-photon excitation of aluminium phthalocyanines

    NASA Astrophysics Data System (ADS)

    Meshalkin, Yu P.; Alfimov, E. E.; Vasil'ev, N. E.; Denisov, A. N.; Makukha, V. K.; Ogirenko, A. P.

    1999-12-01

    A demonstration is given of the feasibility of two-photon excitation of aluminium phthalocyanine and of the pharmaceutical preparation 'Fotosens', used in photodynamic therapy. The excitation source was an Nd:YAG laser emitting at the 1064 nm wavelength. The spectra of the two-photon-excited luminescence were obtained and the two-photon absorption cross sections were determined.

  5. Relaxation channels of multi-photon excited xenon clusters

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

    Serdobintsev, P. Yu.; Melnikov, A. S.; Department of Physics, St. Petersburg State University, Saint Petersburg 198904

    2015-09-21

    The relaxation processes of the xenon clusters subjected to multi-photon excitation by laser radiation with quantum energies significantly lower than the thresholds of excitation of atoms and ionization of clusters were studied. Results obtained by means of the photoelectron spectroscopy method showed that desorption processes of excited atoms play a significant role in the decay of two-photon excited xenon clusters. A number of excited states of xenon atoms formed during this process were discovered and identified.

  6. Investigation of infrared radiation in rubidium vapor upon two-photon and step-by-step excitations of the initial level

    NASA Astrophysics Data System (ADS)

    Bimagambetov, T. S.

    2011-12-01

    Stimulated infrared (IR) 5.231-μm line radiation is obtained upon two-photon and step-by-step excitations of the initial level. Dependences of the line power on the concentration of atoms and laser frequency are investigated. The mechanism of initial level occupation is explained.

  7. New two-photon excitation chromophores for cellular imaging

    NASA Astrophysics Data System (ADS)

    D'Alfonso, Laura; Chirico, Giuseppe; Collini, Maddalena; Baldini, Giancarlo; Diaspro, Alberto; Ramoino, Paola; Abbotto, Alessandro; Beverina, Luca; Pagani, Giorgio A.

    2003-10-01

    The one photon and two photon excitation spectral properties (absorption, emission spectra, singlet lifetime) of a very efficient two photon absorber, dimethyl-pepep, have been measured in solution. The one photon excitation peak lye near 525 nm and the emission falls at 600 nm, where autofluorescence of cells is weak. The value of the singlet-triplet conversion rate, obtained by two-photon excitation fluorescence correlation spectroscopy, has a quadratic dependence on the excitation power and is comparable to that shown by the dye rhodamine. Preliminary results on stained cells from yeast Saccaromices cerevisiae and Paramecium primaurelia show that the dye preferentially stains DNA in the cell. A direct comparison with a DNA stainer, Dapi, is also performed. Some measurements of the dye functionalized to react with lysine and n-terminal residues of protein are presented. Moreover, this dye can be employed in order to follow in detail some cellular processes such as nuclei division. In vitro fluorescence titration of dimethyl-pepep with calf thymus DNA allowed to estimate the values of the dye-DNA association constant versus ionic strength, and an affinity close to that of ethidium bromide is found.

  8. Indirect excitation of ultrafast demagnetization

    DOE PAGES

    Vodungbo, Boris; Tudu, Bahrati; Perron, Jonathan; ...

    2016-01-06

    Does the excitation of ultrafast magnetization require direct interaction between the photons of the optical pump pulse and the magnetic layer? Here, we demonstrate unambiguously that this is not the case. For this we have studied the magnetization dynamics of a ferromagnetic cobalt/palladium multilayer capped by an IR-opaque aluminum layer. Upon excitation with an intense femtosecond-short IR laser pulse, the film exhibits the classical ultrafast demagnetization phenomenon although only a negligible number of IR photons penetrate the aluminum layer. In comparison with an uncapped cobalt/palladium reference film, the initial demagnetization of the capped film occurs with a delayed onset andmore » at a slower rate. Both observations are qualitatively in line with energy transport from the aluminum layer into the underlying magnetic film by the excited, hot electrons of the aluminum film. As a result, our data thus confirm recent theoretical predictions.« less

  9. Indirect excitation of ultrafast demagnetization

    PubMed Central

    Vodungbo, Boris; Tudu, Bahrati; Perron, Jonathan; Delaunay, Renaud; Müller, Leonard; Berntsen, Magnus H.; Grübel, Gerhard; Malinowski, Grégory; Weier, Christian; Gautier, Julien; Lambert, Guillaume; Zeitoun, Philippe; Gutt, Christian; Jal, Emmanuelle; Reid, Alexander H.; Granitzka, Patrick W.; Jaouen, Nicolas; Dakovski, Georgi L.; Moeller, Stefan; Minitti, Michael P.; Mitra, Ankush; Carron, Sebastian; Pfau, Bastian; von Korff Schmising, Clemens; Schneider, Michael; Eisebitt, Stefan; Lüning, Jan

    2016-01-01

    Does the excitation of ultrafast magnetization require direct interaction between the photons of the optical pump pulse and the magnetic layer? Here, we demonstrate unambiguously that this is not the case. For this we have studied the magnetization dynamics of a ferromagnetic cobalt/palladium multilayer capped by an IR-opaque aluminum layer. Upon excitation with an intense femtosecond-short IR laser pulse, the film exhibits the classical ultrafast demagnetization phenomenon although only a negligible number of IR photons penetrate the aluminum layer. In comparison with an uncapped cobalt/palladium reference film, the initial demagnetization of the capped film occurs with a delayed onset and at a slower rate. Both observations are qualitatively in line with energy transport from the aluminum layer into the underlying magnetic film by the excited, hot electrons of the aluminum film. Our data thus confirm recent theoretical predictions. PMID:26733106

  10. Bright Photon Upconversion on Composite Organic Lanthanide Molecules through Localized Thermal Radiation.

    PubMed

    Ye, Huanqing; Bogdanov, Viktor; Liu, Sheng; Vajandar, Saumitra; Osipowicz, Thomas; Hernández, Ignacio; Xiong, Qihua

    2017-12-07

    Converting low-energy photons via thermal radiation can be a potential approach for utilizing infrared (IR) photons to improve photovoltaic efficiency. Lanthanide-containing materials have achieved great progress in IR-to-visible photon upconversion (UC). Herein, we first report bright photon, tunable wavelength UC through localized thermal radiation at the molecular scale with low excitation power density (<10 W/cm 2 ) realized on lanthanide complexes of perfluorinated organic ligands. This is enabled by engineering the pathways of nonradiative de-excitation and energy transfer in a composite of ytterbium and terbium perfluoroimidodiphosphinates. The IR-excited thermal UC and wavelength control is realized through the terbium activators sensitized by the ytterbium sensitizers having high luminescence efficiency. The metallic molecular composite thus can be a potential energy material in the use of the IR solar spectrum for thermal photovoltaic applications.

  11. Electronic excitations in γ -Li2IrO3

    NASA Astrophysics Data System (ADS)

    Li, Ying; Winter, Stephen M.; Jeschke, Harald O.; Valentí, Roser

    2017-01-01

    We investigate the electronic properties of the three-dimensional stripyhoneycomb γ -Li2IrO3 via relativistic density functional theory calculations as well as exact diagonalization of finite clusters and explore the details of the optical conductivity. Our analysis of this quantity reveals the microscopic origin of the experimentally observed (i) optical transitions and (ii) anisotropic behavior along the various polarization directions. In particular, we find that the optical excitations are overall dominated by transitions between jeff=1 /2 and 3/2 states and the weight of transitions between jeff=1 /2 states at low frequencies can be correlated to deviations from a pure Kitaev description. We furthermore reanalyze within this approach the electronic excitations in the known two-dimensional honeycomb systems α -Li2IrO3 and Na2IrO3 and discuss the results in comparison to γ -Li2IrO3 .

  12. Photonics of a conjugated organometallic Pt-Ir polymer and its model compounds exhibiting hybrid CT excited states.

    PubMed

    Soliman, Ahmed M; Fortin, Daniel; Zysman-Colman, Eli; Harvey, Pierre D

    2012-04-13

    Trans- dichlorobis(tri-n-butylphosphine)platinum(II) reacts with bis(2- phenylpyridinato)-(5,5'-diethynyl-2,2'-bipyridine)iridium(III) hexafluorophosphate to form the luminescent conjugated polymer poly[trans-[(5,5'-ethynyl-2,2'-bipyridine)bis(2- phenylpyridinato)-iridium(III)]bis(tri-n-butylphosphine)platinum(II)] hexafluorophosphate ([Pt]-[Ir])n. Gel permeation chromatography indicates a degree of polymerization of 9 inferring the presence of an oligomer. Comparison of the absorption and emission band positions and their temperature dependence, emission quantum yields, and lifetimes with those for models containing only the [Pt] or the [Ir] units indicates hybrid excited states including features from both chromophores. Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  13. Microwave-optical two-photon excitation of Rydberg states

    NASA Astrophysics Data System (ADS)

    Tate, D. A.; Gallagher, T. F.

    2018-03-01

    We report efficient microwave-optical two photon excitation of Rb Rydberg atoms in a magneto-optical trap. This approach allows the excitation of normally inaccessible states and provides a path toward excitation of high-angular-momentum states. The efficiency stems from the elimination of the Doppler width, the use of a narrow-band pulsed laser, and the enormous electric-dipole matrix element connecting the intermediate and final states of the transition. The excitation is efficient in spite of the low optical and microwave powers, of order 1 kW and 1 mW, respectively. This is an application of the large dipole coupling strengths between Rydberg states to achieve two-photon excitation of Rydberg atoms.

  14. Localised excitation of a single photon source by a nanowaveguide.

    PubMed

    Geng, Wei; Manceau, Mathieu; Rahbany, Nancy; Sallet, Vincent; De Vittorio, Massimo; Carbone, Luigi; Glorieux, Quentin; Bramati, Alberto; Couteau, Christophe

    2016-01-29

    Nowadays, integrated photonics is a key technology in quantum information processing (QIP) but achieving all-optical buses for quantum networks with efficient integration of single photon emitters remains a challenge. Photonic crystals and cavities are good candidates but do not tackle how to effectively address a nanoscale emitter. Using a nanowire nanowaveguide, we realise an hybrid nanodevice which locally excites a single photon source (SPS). The nanowire acts as a passive or active sub-wavelength waveguide to excite the quantum emitter. Our results show that localised excitation of a SPS is possible and is compared with free-space excitation. Our proof of principle experiment presents an absolute addressing efficiency ηa ~ 10(-4) only ~50% lower than the one using free-space optics. This important step demonstrates that sufficient guided light in a nanowaveguide made of a semiconductor nanowire is achievable to excite a single photon source. We accomplish a hybrid system offering great potentials for electrically driven SPSs and efficient single photon collection and detection, opening the way for optimum absorption/emission of nanoscale emitters. We also discuss how to improve the addressing efficiency of a dipolar nanoscale emitter with our system.

  15. Localised excitation of a single photon source by a nanowaveguide

    PubMed Central

    Geng, Wei; Manceau, Mathieu; Rahbany, Nancy; Sallet, Vincent; De Vittorio, Massimo; Carbone, Luigi; Glorieux, Quentin; Bramati, Alberto; Couteau, Christophe

    2016-01-01

    Nowadays, integrated photonics is a key technology in quantum information processing (QIP) but achieving all-optical buses for quantum networks with efficient integration of single photon emitters remains a challenge. Photonic crystals and cavities are good candidates but do not tackle how to effectively address a nanoscale emitter. Using a nanowire nanowaveguide, we realise an hybrid nanodevice which locally excites a single photon source (SPS). The nanowire acts as a passive or active sub-wavelength waveguide to excite the quantum emitter. Our results show that localised excitation of a SPS is possible and is compared with free-space excitation. Our proof of principle experiment presents an absolute addressing efficiency ηa ~ 10−4 only ~50% lower than the one using free-space optics. This important step demonstrates that sufficient guided light in a nanowaveguide made of a semiconductor nanowire is achievable to excite a single photon source. We accomplish a hybrid system offering great potentials for electrically driven SPSs and efficient single photon collection and detection, opening the way for optimum absorption/emission of nanoscale emitters. We also discuss how to improve the addressing efficiency of a dipolar nanoscale emitter with our system. PMID:26822999

  16. Melanin fluorescence spectra by step-wise three photon excitation

    NASA Astrophysics Data System (ADS)

    Lai, Zhenhua; Kerimo, Josef; DiMarzio, Charles A.

    2012-03-01

    Melanin is the characteristic chromophore of human skin with various potential biological functions. Kerimo discovered enhanced melanin fluorescence by stepwise three-photon excitation in 2011. In this article, step-wise three-photon excited fluorescence (STPEF) spectrum between 450 nm -700 nm of melanin is reported. The melanin STPEF spectrum exhibited an exponential increase with wavelength. However, there was a probability of about 33% that another kind of step-wise multi-photon excited fluorescence (SMPEF) that peaks at 525 nm, shown by previous research, could also be generated using the same process. Using an excitation source at 920 nm as opposed to 830 nm increased the potential for generating SMPEF peaks at 525 nm. The SMPEF spectrum peaks at 525 nm photo-bleached faster than STPEF spectrum.

  17. Crossed-coil detection of two-photon excited nuclear quadrupole resonance

    NASA Astrophysics Data System (ADS)

    Eles, Philip T.; Michal, Carl A.

    2005-08-01

    Applying a recently developed theoretical framework for determining two-photon excitation Hamiltonians using average Hamiltonian theory, we calculate the excitation produced by half-resonant irradiation of the pure quadrupole resonance of a spin-3/2 system. This formalism provides expressions for the single-quantum and double-quantum nutation frequencies as well as the Bloch-Siegert shift. The dependence of the excitation strength on RF field orientation and the appearance of the free-induction signal along an axis perpendicular to the excitation field provide an unmistakable signature of two-photon excitation. We demonstrate single- and double-quantum excitation in an axially symmetric system using 35Cl in a single crystal of potassium chlorate ( ωQ = 28 MHz) with crossed-coil detection. A rotation plot verifies the orientation dependence of the two-photon excitation, and double-quantum coherences are observed directly with the application of a static external magnetic field.

  18. Interferometric temporal focusing microscopy using three-photon excitation fluorescence.

    PubMed

    Toda, Keisuke; Isobe, Keisuke; Namiki, Kana; Kawano, Hiroyuki; Miyawaki, Atsushi; Midorikawa, Katsumi

    2018-04-01

    Super-resolution microscopy has become a powerful tool for biological research. However, its spatial resolution and imaging depth are limited, largely due to background light. Interferometric temporal focusing (ITF) microscopy, which combines structured illumination microscopy and three-photon excitation fluorescence microscopy, can overcome these limitations. Here, we demonstrate ITF microscopy using three-photon excitation fluorescence, which has a spatial resolution of 106 nm at an imaging depth of 100 µm with an excitation wavelength of 1060 nm.

  19. Two-photon excited fluorescence emission from hemoglobin

    NASA Astrophysics Data System (ADS)

    Sun, Qiqi; Zeng, Yan; Zhang, Wei; Zheng, Wei; Luo, Yi; Qu, Jianan Y.

    2015-03-01

    Hemoglobin, one of the most important proteins in blood, is responsible for oxygen transportation in almost all vertebrates. Recently, we discovered two-photon excited hemoglobin fluorescence and achieved label-free microvascular imaging based on the hemoglobin fluorescence. However, the mechanism of its fluorescence emission still remains unknown. In this work, we studied the two-photon excited fluorescence properties of the hemoglobin subunits, heme/hemin (iron (II)/(III) protoporphyrin IX) and globin. We first studied the properties of heme and the similar spectral and temporal characteristics of heme and hemoglobin fluorescence provide strong evidence that heme is the fluorophore in hemoglobin. Then we studied the fluorescence properties of hemin, globin and methemoglobin, and found that the hemin may have the main effect on the methemoglobin fluorescence and that globin has tryptophan fluorescence like other proteins. Finally, since heme is a centrosymmetric molecule, that the Soret band fluorescence of heme and hemoglobin was not observed in the single photon process in the previous study may be due to the parity selection rule. The discovery of heme two-photon excited fluorescence may open a new window for heme biology research, since heme as a cofactor of hemoprotein has many functions, including chemical catalysis, electron transfer and diatomic gases transportation.

  20. Peptide backbone orientation and dynamics in spider dragline silk and two-photon excitation in nuclear magnetic and quadrupole resonance

    NASA Astrophysics Data System (ADS)

    Eles, Philip Thomas

    2005-07-01

    In the first part of the dissertation, spider dragline silk is studied by solid state NMR techniques. The dependence of NMR frequency on molecular orientation is exploited using the DECODER experiment to determine the orientation of the protein backbone within the silk fibre. Practical experimental considerations require that the silk fibres be wound about a cylindrical axis perpendicular to the external magnetic field, complicating the reconstruction of the underlying orientation distribution and necess-itating the development of numerical techniques for this purpose. A two-component model of silk incorporating static b-sheets and polyglycine II helices adequately fits the NMR data and suggests that the b-sheets are well aligned along the silk axis (20 FWHM) while the helices are poorly aligned (68 FWHM). The effects of fibre strain, draw rate and hydration on orientation are measured. Measurements of the time-scale for peptide backbone motion indicate that when wet, a strain-dependent frac-tion of the poorly aligned component becomes mobile. This suggests a mechanism for the supercontraction of silk involving latent entropic springs that undergo a local strain-dependent phase transition, driving supercontraction. In the second part of this dissertation a novel method is developed for exciting NMR and nuclear quadrupole resonance (NQR) by rf irradiation at multiple frequencies that sum to (or differ by) the resonance frequency. This is fundamentally different than traditional NMR experiments where irradiation is applied on-resonance. With excitation outside the detection bandwidth, two-photon excitation allows for detection of free induction signals during excitation, completely eliminating receiver dead-time. A theoretical approach to describing two-photon excitation is developed based on average Hamiltonian theory. An intuition for two-photon excitation is gained by analogy to the coherent absorption of multiple photons requiring conservation of total energy and

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

    NASA Astrophysics Data System (ADS)

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

    2018-07-01

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

  2. Two-Photon Excitation of Launched Cold Atoms in Flight

    NASA Astrophysics Data System (ADS)

    Goodsell, Anne; Gonzalez, Rene; Alejandro, Eduardo; Erwin, Emma

    2017-04-01

    We demonstrate two-photon bi-chromatic excitation of cold rubidium atoms in flight, using the pathway 5S1 / 2 -> 5P3 / 2 -> 5D5 / 2 with two resonant photons. In our experiment, atoms are laser-cooled in a magneto-optical trap and launched upward in discrete clouds with a controllable vertical speed of 7.1 +/-0.6 m/s and a velocity spread that is less than 10% of the launch speed. Outside the cooling beams, as high as 14 mm above the original center of the trap, the launched cold atoms are illuminated simultaneously by spatially-localized horizontal excitation beams at 780 nm (5S1 / 2 -> 5P3 / 2) and 776 nm (5P3 / 2 -> 5D5 / 2). We monitor transmission of the 780-nm beam over a range of intensities of 780-nm and 776-nm light. As the center of the moving cloud passes the excitation beams, we observe as much as 97.9 +/-1.2% transmission when the rate of two-photon absorption is high and the 5S1 / 2 and 5P3 / 2 states are depopulated, compared to 87.6 +/-0.9% transmission if only the 780-nm beam is present. This demonstrates two-photon excitation of a launched cold-atom source with controllable launch velocity and narrow velocity spread, as a foundation for three-photon excitation to Rydberg states. Research supported by Middlebury College Bicentennial Fund, Palen Fund, and Gladstone Award.

  3. Individual bioaerosol particle discrimination by multi-photon excited fluorescence.

    PubMed

    Kiselev, Denis; Bonacina, Luigi; Wolf, Jean-Pierre

    2011-11-21

    Femtosecond laser induced multi-photon excited fluorescence (MPEF) from individual airborne particles is tested for the first time for discriminating bioaerosols. The fluorescence spectra, analysed in 32 channels, exhibit a composite character originating from simultaneous two-photon and three-photon excitation at 790 nm. Simulants of bacteria aggregates (clusters of dyed polystyrene microspheres) and different pollen particles (Ragweed, Pecan, Mulberry) are clearly discriminated by their MPEF spectra. This demonstration experiment opens the way to more sophisticated spectroscopic schemes like pump-probe and coherent control. © 2011 Optical Society of America

  4. Anomalous differential polarized phase angles for two-photon excitation with isotropic depolarizing rotations

    NASA Astrophysics Data System (ADS)

    Lakowicz, Joseph R.; Gryczynski, Ignacy; Danielsen, Eva

    1992-03-01

    We describe frequency-domain measurements of the anisotropy decay of 1,6-diphenylhexatriene resulting from one- and two-photon excitation. For two-photon excitation, the phase shifts (Δ) between the horizontally and vertically polarized components of the decay exceed the absolute maximum of 30° possible for one-photon excitation, and values of Δ as large as 37° were observed for 1,6-diphenylhexatriene in triacetin. These results are explained by the increased orientation of the photoselected population for two- as compared to one-photon excitation.

  5. High energy photons excited photodynamic cancer therapy in vitro

    NASA Astrophysics Data System (ADS)

    Guo, Yiping; Sheng, Shi; Zhang, Wei; Lun, Michael; Tsai, Shih-Ming; Chin, Wei-Chun; Hoglund, Roy; Li, Changqing

    2018-02-01

    Photodynamic therapy (PDT) is a noninvasive phototherapy method that has been clinically approved for many years. During this type of therapy, the photosensitizing agent will be excited by optical photons to generate reactive oxygen species which can kill nearby cancer cells. However, due to the strong optical scattering and absorption of tissue, optical photons can only penetrate tissues in few millimeters which result in the limited applications of PDT to superficial lesions like skin cancers. In this study, to overcome the penetration limitations, we used high-energy photons to excite photosensitizers directly by assuming that high-energy photons generate low-energy optical photons in tissues to excite photosensitizers. Cesium- 137 irradiator has been used as the high-energy photon source. A fiber pigtailed diode laser was used to validate the photosensitizer's efficacy. We used MPPa as the photosensitizer to treat A549 cancer cell line with different concentrations of drug (10μM/ ml, 5 μM/ml, 2.5 μM/ml, 1 μM/ml and 0 μM/ml). We have performed an irradiation experiment for different time durations of 30 min, 15 min, 7 min to 3 min, respectively, and we also compared different drug concentrations and different exposure durations. Our study not only proved the MPPa PDT method was effective, but also indicated that high-energy photons enhanced PDT could potentially overcome the penetration limitations thus making PDT feasible for deep tissue cancer.

  6. Two-photon excitation photodynamic therapy with Photofrin

    NASA Astrophysics Data System (ADS)

    Karotki, Aliaksandr; Khurana, Mamta; Lepock, James R.; Wilson, Brian C.

    2005-09-01

    Photodynamic therapy (PDT) based on simultaneous two-photon (2-γ) excitation has a potential advantage of highly targeted treatment by means of nonlinear localized photosensitizer excitation. One of the possible applications of 2-γ PDT is a treatment of exodus age-related macular degeneration where highly targeted excitation of photosensitizer in neovasculature is vital for reducing collateral damage to healthy surrounding tissue. To investigate effect of 2-γ PDT Photofrin was used as an archetypal photosensitizer. First, 2-γ absorption properties of Photofrin in the 750 - 900 nm excitation wavelength range were investigated. It was shown that above 800 nm 2-γ interaction was dominant mode of excitation. The 2-γ cross section of Photofrin was rather small and varied between 5 and 10 GM (1 GM = 10-50 cm4s/photon) in this wavelength range. Next, endothelial cells treated with Photofrin were used to model initial effect of 2-γ PDT on neovasculature. Ultrashort laser pulses provided by mode-locked Ti:sapphire laser (pulse duration at the sample 300 fs, repetition rate 90 MHz, mean laser power 10 mW, excitation wavelength 850 nm) were used for the excitation of the photosensitizer. Before 2-γ excitation of the Photofrin cells formed a single continuous sheet at the bottom of the well. The tightly focused laser light was scanned repeatedly over the cell layer. After irradiation the cell layer of the control cells stayed intact while cells treated with photofrin became clearly disrupted. The light doses required were high (6300 Jcm(-2) for ~ 50% killing), but 2-γ cytotoxicity was unequivocally demonstrated.

  7. Resonance-enhanced two-photon excitation of CaI

    NASA Astrophysics Data System (ADS)

    Casero-Junquera, Elena; Lawruszczuk, Rafal; Rostas, Joëlle; Taieb, Guy

    1994-07-01

    Induced fluorescence following visible (620-655 nm) laser excitation of the CaI radical has been detected not only in the same region (B, A-X transitions), but also in the UV (315-330 nm). The UV two-photon excitation spectrum consists of narrow bands appearing at laser frequencies located within certain bands of the Δ v = 1, 0 sequences of the B 2Σ +-X 2Σ + and A 2Π 1/2-X 2Σ + systems. The main peaks are tentatively assigned to resonance-enhanced excitation of a single vibrational level of the lowest Rydberg D 2Σ + state from successive vibrational levels of the ground state. The excitation process is a one-color two-photon optical—optical-double-resonance via B 2Σ + and A 2Π 1/2 intermediate levels. This analysis is supported by the absorption spectrum observed long ago by Walters and Barratt. The absorption and laser excitation complementary data have been used to derive approximate molecular constants for the D state.

  8. Two-photon-excited fluorescence spectroscopy of atomic fluorine at 170 nm

    NASA Technical Reports Server (NTRS)

    Herring, G. C.; Dyer, Mark J.; Jusinski, Leonard E.; Bischel, William K.

    1988-01-01

    Two-photon-excited fluorescence spectroscopy of atomic fluorine is reported. A doubled dye laser at 286-nm is Raman shifted in H2 to 170 nm (sixth anti-Stokes order) to excite ground-state 2P(0)J fluorine atoms to the 2D(0)J level. The fluorine atoms are detected by one of two methods: observing the fluorescence decay to the 2PJ level or observing F(+) production through the absorption of an additional photon by the excited atoms. Relative two-photon absorption cross sections to and the radiative lifetimes of the 2D(0)J states are measured.

  9. Absorption bleaching of squarylium dye J aggregates via a two-photon excitation process

    NASA Astrophysics Data System (ADS)

    Furuki, Makoto; Tian, Minquan; Sato, Yasuhiro; Pu, Lyong Sun; Tatsuura, Satoshi; Abe, Shuji

    2001-08-01

    Squarylium dye J aggregates exhibit ultrafast nonlinear optical response of absorption saturation at the resonant wavelength of 770 nm. We studied the two-photon excitation process of J aggregates. By fluorescence measurement, we found the two-photon absorption band at 1.3 μm, which was different from that of the dye solution at 1.2 μm. Absorption saturation at 770 nm via a two-photon excitation process was observed by two-photon resonant excitation at 1.3 μm and also by off-resonant excitation at 1.55 μm, suggesting the possibility of J aggregates for optical switching materials working at the wavelength used in optical communications.

  10. Multiple hot-carrier collection in photo-excited graphene Moiré superlattices

    PubMed Central

    Wu, Sanfeng; Wang, Lei; Lai, You; Shan, Wen-Yu; Aivazian, Grant; Zhang, Xian; Taniguchi, Takashi; Watanabe, Kenji; Xiao, Di; Dean, Cory; Hone, James; Li, Zhiqiang; Xu, Xiaodong

    2016-01-01

    In conventional light-harvesting devices, the absorption of a single photon only excites one electron, which sets the standard limit of power-conversion efficiency, such as the Shockley-Queisser limit. In principle, generating and harnessing multiple carriers per absorbed photon can improve efficiency and possibly overcome this limit. We report the observation of multiple hot-carrier collection in graphene/boron-nitride Moiré superlattice structures. A record-high zero-bias photoresponsivity of 0.3 A/W (equivalently, an external quantum efficiency exceeding 50%) is achieved using graphene’s photo-Nernst effect, which demonstrates a collection of at least five carriers per absorbed photon. We reveal that this effect arises from the enhanced Nernst coefficient through Lifshtiz transition at low-energy Van Hove singularities, which is an emergent phenomenon due to the formation of Moiré minibands. Our observation points to a new means for extremely efficient and flexible optoelectronics based on van der Waals heterostructures. PMID:27386538

  11. Two-photon excited fluorescence from a pseudoisocyanine-attached gold-coated tip via a thin tapered fiber under a weak continuous wave excitation.

    PubMed

    Ren, Fang; Takashima, Hideaki; Tanaka, Yoshito; Fujiwara, Hideki; Sasaki, Keiji

    2013-11-18

    A simple tapered fiber based photonic-plasmonic hybrid nanostructure composed of a thin tapered fiber and a pseudoisocyanine (PIC)-attached Au-coated tip was demonstrated. Using this simple hybrid nanostructure, we succeeded in observing two-photon excited fluorescence from the PIC dye molecules under a weak continuous wave excitation condition. From the results of the tip-fiber distance dependence and excitation polarization dependence, we found that using a thin tapered fiber and an Au-coated tip realized efficient coupling of the incident light (~95%) and LSP excitation at the Au-coated tip, suggesting the possibility of efficiently inducing two-photon excited fluorescence from the PIC dye molecules attached on the Au-coated tip. This simple photonic-plasmonic hybrid system is one of the promising tools for single photon sources, highly efficient plasmonic sensors, and integrated nonlinear plasmonic devices.

  12. One Photon Can Simultaneously Excite Two or More Atoms.

    PubMed

    Garziano, Luigi; Macrì, Vincenzo; Stassi, Roberto; Di Stefano, Omar; Nori, Franco; Savasta, Salvatore

    2016-07-22

    We consider two separate atoms interacting with a single-mode optical or microwave resonator. When the frequency of the resonator field is twice the atomic transition frequency, we show that there exists a resonant coupling between one photon and two atoms, via intermediate virtual states connected by counterrotating processes. If the resonator is prepared in its one-photon state, the photon can be jointly absorbed by the two atoms in their ground state which will both reach their excited state with a probability close to one. Like ordinary quantum Rabi oscillations, this process is coherent and reversible, so that two atoms in their excited state will undergo a downward transition jointly emitting a single cavity photon. This joint absorption and emission process can also occur with three atoms. The parameters used to investigate this process correspond to experimentally demonstrated values in circuit quantum electrodynamics systems.

  13. Mitochondrial Dynamics Tracking with Two-Photon Phosphorescent Terpyridyl Iridium(III) Complexes

    NASA Astrophysics Data System (ADS)

    Huang, Huaiyi; Zhang, Pingyu; Qiu, Kangqiang; Huang, Juanjuan; Chen, Yu; Ji, Liangnian; Chao, Hui

    2016-02-01

    Mitochondrial dynamics, including fission and fusion, control the morphology and function of mitochondria, and disruption of mitochondrial dynamics leads to Parkinson’s disease, Alzheimer’s disease, metabolic diseases, and cancers. Currently, many types of commercial mitochondria probes are available, but high excitation energy and low photo-stability render them unsuitable for tracking mitochondrial dynamics in living cells. Therefore, mitochondrial targeting agents that exhibit superior anti-photo-bleaching ability, deep tissue penetration and intrinsically high three-dimensional resolutions are urgently needed. Two-photon-excited compounds that use low-energy near-infrared excitation lasers have emerged as non-invasive tools for cell imaging. In this work, terpyridyl cyclometalated Ir(III) complexes (Ir1-Ir3) are demonstrated as one- and two-photon phosphorescent probes for real-time imaging and tracking of mitochondrial morphology changes in living cells.

  14. Broadband Doppler-limited two-photon and stepwise excitation spectroscopy with laser frequency combs

    NASA Astrophysics Data System (ADS)

    Hipke, Arthur; Meek, Samuel A.; Ideguchi, Takuro; Hänsch, Theodor W.; Picqué, Nathalie

    2014-07-01

    Multiplex two-photon excitation spectroscopy is demonstrated at Doppler-limited resolution. We describe first Fourier-transform two-photon spectroscopy of an atomic sample with two mode-locked laser oscillators in a dual-comb technique. Each transition is uniquely identified by the modulation imparted by the interfering comb excitations. The temporal modulation of the spontaneous two-photon fluorescence is monitored with a single photodetector, and the spectrum of all excited transitions is revealed by a Fourier transform.

  15. Two-photon excitation of 2,5-diphenyloxazole using a low power green solid state laser

    NASA Astrophysics Data System (ADS)

    Luchowski, Rafal

    2011-01-01

    This Letter concerns two-photon excitation of 2,5-diphenyloxazole (PPO) upon illumination from a pulsed 532 nm solid state laser, with an average power of 30 mW, and a repetition rate of 20 MHz. A very agreeable emission spectrum position and shape has been achieved for PPO receiving one- and two-photon excitation, which suggests that the same excited state is involved for both excitation modes. Also, a perfect quadratic dependence of laser power in the emission intensity function has been recorded. We tested the application of a small solid state green laser to two-photon induced time-resolved fluorescence, revealing the emission anisotropy of PPO to be considerably higher for two-photon than for one-photon excitation.

  16. Polarized two-photon fluorescence excitation spectra of indole and benzimidazole

    NASA Astrophysics Data System (ADS)

    Anderson, Bruce E.; Jones, Richard D.; Rehms, Aden A.; Ilich, Predrag; Callis, Patrik R.

    1986-03-01

    Polarized two-photon fluorescence excitation spectra of indole in hexane, benzimidazole in isopropanol, and benzimidazole cation in methanol-H 2SO 4, all at 0.2 M and 25°C are reported for the excitation range 470-600 nm, the region of their L b, and L a bands. Relative two-photon absorptivities are deduced by correcting for different fluorescence response and are compared to toluene's L b band. The indole integrated absorptivity is about 10 times greater than that of toluene. The L a band of indole appears less dominant than in one-photon but still outweighs the L b band by a factor of 4. The two-photon polarization spectrum for indole indicates that the L a origin lies ≈500-1000 cm -1 above the L b origin in hexane. The benzimidazoles absorb only about twice as strongly as toluene and show strong vibronic peaks; the L a, bands are only faintly seen. Two-photon properties calculated from INDO/S CI wavefunctions with doubly excited configurations are in good agreement with those of indole, but predict the benzimidazole TPA to be several times stronger than observed. For the cation, the predicted results are nearly two orders of magnitude too high.

  17. Two-photon excited autofluorescence imaging of freshly isolated frog retinas.

    PubMed

    Lu, Rong-Wen; Li, Yi-Chao; Ye, Tong; Strang, Christianne; Keyser, Kent; Curcio, Christine A; Yao, Xin-Cheng

    2011-06-01

    The purpose of this study was to investigate cellular sources of autofluorescence signals in freshly isolated frog (Rana pipiens) retinas. Equipped with an ultrafast laser, a laser scanning two-photon excitation fluorescence microscope was employed for sub-cellular resolution examination of both sliced and flat-mounted retinas. Two-photon imaging of retinal slices revealed autofluorescence signals over multiple functional layers, including the photoreceptor layer (PRL), outer nuclear layer (ONL), outer plexiform layer (OPL), inner nuclear layer (INL), inner plexiform layer (IPL), and ganglion cell layer (GCL). Using flat-mounted retinas, depth-resolved imaging of individual retinal layers further confirmed multiple sources of autofluorescence signals. Cellular structures were clearly observed at the PRL, ONL, INL, and GCL. At the PRL, the autofluorescence was dominantly recorded from the intracellular compartment of the photoreceptors; while mixed intracellular and extracellular autofluorescence signals were observed at the ONL, INL, and GCL. High resolution autofluorescence imaging clearly revealed mosaic organization of rod and cone photoreceptors; and sub-cellular bright autofluorescence spots, which might relate to connecting cilium, was observed in the cone photoreceptors only. Moreover, single-cone and double-cone outer segments could be directly differentiated.

  18. Two-photon excitation spectroscopy of carotenoid-containing and carotenoid-depleted LH2 complexes from purple bacteria.

    PubMed

    Stepanenko, Ilya; Kompanetz, Viktor; Makhneva, Zoya; Chekalin, Sergey; Moskalenko, Andrei; Razjivin, Andrei

    2009-08-27

    We applied two-photon fluorescence excitation spectroscopy to LH2 complex from purple bacteria Allochromatium minutissimum and Rhodobacter sphaeroides . Bacteriochlorophyll fluorescence was measured under two-photon excitation of the samples within the 1200-1500 nm region. Spectra were obtained for both carotenoid-containing and -depleted complexes of each bacterium to allow their direct comparison. The depletion of carotenoids did not alter the two-photon excitation spectra of either bacteria. The spectra featured a wide excitation band around 1350 nm (2x675 nm, 14,800 cm(-1)) which strongly resembled two-photon fluorescence excitation spectra of similar complexes published by other authors. We consider obtained experimental data to be evidence of direct two-photon excitation of bacteriochlorophyll excitonic states in this spectral region.

  19. Three-photon excitation of 2,5-bis(4-biphenyl)oxazole: steady-state and time-resolved intensities and anisotropies

    NASA Astrophysics Data System (ADS)

    Gryczynski, Ignacy; Malak, Henryk; Hell, Stefan W.; Lakowicz, Joseph R.

    1996-10-01

    Three-photon excitation of 2,5-bis(4-biphenyl) oxazole (BBO) was observed when it was excited with the fundamental output of a femtosecond Ti:sapphire laser above 820 nm. The emission spectrum of BBO was identical for one-, two-, and three-photon excitation at 320, 640, and 960 nm, respectively. In toluene and triacetin, the emission intensity of BBO depended on the square of the laser power for wavelengths below 820 nm and displayed a sharp transition to a cubic dependence at longer wavelengths. The spatial distribution of the emission of BBO with three- photon excitation was more strongly localized than for two- photon excitation of a coumarin fluorophore at the same wavelength. The same single exponential intensity decay was observed for one-, two-, and three-photon excitation. However, the frequency domain anisotropy decay with three- photon excitation at 960 nm revealed a larger time-zero anisotropy, larger differential polarized phase angle, and larger modulated anisotropy than is possible for two-photon excitation with colinear oscillators. In triacetin, the anisotropy is not constant for three-photon excitation at different wavelengths. Surprisingly, the fluorescence intensities for three-photon excitation were only about 100- fold less than for two-photon excitation. The increasing availability of Ti:sapphire lasers suggests that multiphoton excitation can become a common tool in fluorescence spectroscopy.

  20. Non-Poissonian photon statistics from macroscopic photon cutting materials.

    PubMed

    de Jong, Mathijs; Meijerink, Andries; Rabouw, Freddy T

    2017-05-24

    In optical materials energy is usually extracted only from the lowest excited state, resulting in fundamental energy-efficiency limits such as the Shockley-Queisser limit for single-junction solar cells. Photon-cutting materials provide a way around such limits by absorbing high-energy photons and 'cutting' them into multiple low-energy excitations that can subsequently be extracted. The occurrence of photon cutting or quantum cutting has been demonstrated in a variety of materials, including semiconductor quantum dots, lanthanides and organic dyes. Here we show that photon cutting results in bunched photon emission on the timescale of the excited-state lifetime, even when observing a macroscopic number of optical centres. Our theoretical derivation matches well with experimental data on NaLaF 4 :Pr 3+ , a material that can cut deep-ultraviolet photons into two visible photons. This signature of photon cutting can be used to identify and characterize new photon-cutting materials unambiguously.

  1. Highly Efficient and Excitation Tunable Two-Photon Luminescence Platform For Targeted Multi-Color MDRB Imaging Using Graphene Oxide

    NASA Astrophysics Data System (ADS)

    Pramanik, Avijit; Fan, Zhen; Chavva, Suhash Reddy; Sinha, Sudarson Sekhar; Ray, Paresh Chandra

    2014-08-01

    Multiple drug-resistance bacteria (MDRB) infection is one of the top three threats to human health according to the World Health Organization (WHO). Due to the large penetration depth and reduced photodamage, two-photon imaging is an highly promising technique for clinical MDRB diagnostics. Since most commercially available water-soluble organic dyes have low two-photon absorption cross-section and rapid photobleaching tendency, their applications in two-photon imaging is highly limited. Driven by the need, in this article we report extremely high two-photon absorption from aptamer conjugated graphene oxide (σ2PA = 50800 GM) which can be used for highly efficient two-photon fluorescent probe for MDRB imaging. Reported experimental data show that two-photon photoluminescence imaging color, as well as luminescence peak position can be tuned from deep blue to red, just by varying the excitation wavelength without changing its chemical composition and size. We have demonstrated that graphene oxide (GO) based two-photon fluorescence probe is capable of imaging of multiple antibiotics resistance MRSA in the first and second biological transparency windows using 760-1120 nm wavelength range.

  2. Determination of band offset using continuous-wave two-photon excitation in a ZnSe quantum-well waveguide structure

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

    Wagner, H. P.; Kuhnelt, M.; Wenisch, H.

    2001-06-15

    We investigate exciton subband transitions in a ZnSe/Zn{sub 1{minus}x}Mg{sub x}S{sub y}Se{sub 1{minus}y} multiple-quantum-well grown by molecular beam epitaxy waveguide structure by photoluminescence excitation and two-photon excitation spectroscopy. A continuous-wave two-photon absorption is realized by an efficient waveguide coupling scheme within the cryostat. From the energetic position of the 1s and 2p exciton transitions exciton binding energies of 33 and 38 meV are deduced for heavy and light-hole excitons, respectively. With these values we are able to determine the strain free and dimensionless conduction-band-offset parameter to Q{sub c}=0.3{+-}0.1.

  3. Multi-photon excited luminescence of magnetic FePt core-shell nanoparticles.

    PubMed

    Seemann, K M; Kuhn, B

    2014-07-01

    We present magnetic FePt nanoparticles with a hydrophilic, inert, and biocompatible silico-tungsten oxide shell. The particles can be functionalized, optically detected, and optically manipulated. To show the functionalization the fluorescent dye NOPS was bound to the FePt core-shell nanoparticles with propyl-triethoxy-silane linkers and fluorescence of the labeled particles were observed in ethanol (EtOH). In aqueous dispersion the NOPS fluorescence is quenched making them invisible using 1-photon excitation. However, we observe bright luminescence of labeled and even unlabeled magnetic core-shell nanoparticles with multi-photon excitation. Luminescence can be detected in the near ultraviolet and the full visible spectral range by near infrared multi-photon excitation. For optical manipulation, we were able to drag clusters of particles, and maybe also single particles, by a focused laser beam that acts as optical tweezers by inducing an electric dipole in the insulated metal nanoparticles. In a first application, we show that the luminescence of the core-shell nanoparticles is bright enough for in vivo multi-photon imaging in the mouse neocortex down to cortical layer 5.

  4. Fluorescence anisotropy of tyrosinate anion using one-, two- and three-photon excitation: tyrosinate anion fluorescence.

    PubMed

    Kierdaszuk, Borys

    2013-03-01

    We examined the emission spectra and steady-state anisotropy of tyrosinate anion fluorescence with one-photon (250-310 nm), two-photon (570-620 nm) and three-photon (750-930 nm) excitation. Similar emission spectra of the neutral (pH 7.2) and anionic (pH 13) forms of N-acetyl-L-tyrosinamide (NATyrA) (pKa 10.6) were observed for all modes of excitation, with the maxima at 302 and 352 nm, respectively. Two-photon excitation (2PE) and three-photon excitation (3PE) spectra of the anionic form were the same as that for one-photon excitation (1PE). In contrast, 2PE spectrum from the neutral form showed ~30-nm shift to shorter wavelengths relative to 1PE spectrum (λmax 275 nm) at two-photon energy (550 nm), the latter being overlapped with 3PE spectrum, both at two-photon energy (550 nm). Two-photon cross-sections for NATyrA anion at 565-580 nm were 10 % of that for N-acetyl-L-tryptophanamide (NATrpA), and increased to 90 % at 610 nm, while for the neutral form of NATyrA decreased from 2 % of that for NATrpA at 570 nm to near zero at 585 nm. Surprisingly, the fundamental anisotropy of NATyrA anion in vitrified solution at -60 °C was ~0.05 for 2PE at 610 nm as compared to near 0.3 for 1PE at 305 nm, and wavelength-dependence appears to be a basic feature of its anisotropy. In contrast, the 3PE anisotropy at 900 nm was about 0.5, and 3PE and 1PE anisotropy values appear to be related by the cos(6) θ to cos(2) θ photoselection factor (approx. 10/6) independently of excitation wavelength. Attention is drawn to the possible effect of tyrosinate anions in proteins on their multi-photon induced fluorescence emission and excitation spectra as well as excitation anisotropy spectra.

  5. Two-Photon Excitation Microscopy for the Study of Living Cells and Tissues

    PubMed Central

    Benninger, Richard K.P.; Piston, David W.

    2013-01-01

    Two-photon excitation microscopy is an alternative to confocal microscopy that provides advantages for three-dimensional and deep tissue imaging. This unit will describe the basic physical principles behind two-photon excitation and discuss the advantages and limitations of its use in laser-scanning microscopy. The principal advantages of two-photon microscopy are reduced phototoxicity, increased imaging depth, and the ability to initiate highly localized photochemistry in thick samples. Practical considerations for the application of two-photon microscopy will then be discussed, including recent technological advances. This unit will conclude with some recent applications of two-photon microscopy that highlight the key advantages over confocal microscopy and the types of experiments which would benefit most from its application. PMID:23728746

  6. Coherent Terahertz Radiation from Multiple Electron Beams Excitation within a Plasmonic Crystal-like structure.

    PubMed

    Zhang, Yaxin; Zhou, Yucong; Gang, Yin; Jiang, Guili; Yang, Ziqiang

    2017-01-23

    Coherent terahertz radiation from multiple electron beams excitation within a plasmonic crystal-like structure (a three-dimensional holes array) which is composed of multiple stacked layers with 3 × 3 subwavelength holes array has been proposed in this paper. It has been found that in the structure the electromagnetic fields in each hole can be coupled with one another to construct a composite mode with strong field intensity. Therefore, the multiple electron beams injection can excite and efficiently interact with such mode. Meanwhile, the coupling among the electron beams is taken place during the interaction so that a very strong coherent terahertz radiation with high electron conversion efficiency can be generated. Furthermore, due to the coupling, the starting current density of this mechanism is much lower than that of traditional electron beam-driven terahertz sources. This multi-beam radiation system may provide a favorable way to combine photonics structure with electronics excitation to generate middle, high power terahertz radiation.

  7. Coherent Terahertz Radiation from Multiple Electron Beams Excitation within a Plasmonic Crystal-like structure

    PubMed Central

    Zhang, Yaxin; Zhou, Yucong; Gang, Yin; Jiang, Guili; Yang, Ziqiang

    2017-01-01

    Coherent terahertz radiation from multiple electron beams excitation within a plasmonic crystal-like structure (a three-dimensional holes array) which is composed of multiple stacked layers with 3 × 3 subwavelength holes array has been proposed in this paper. It has been found that in the structure the electromagnetic fields in each hole can be coupled with one another to construct a composite mode with strong field intensity. Therefore, the multiple electron beams injection can excite and efficiently interact with such mode. Meanwhile, the coupling among the electron beams is taken place during the interaction so that a very strong coherent terahertz radiation with high electron conversion efficiency can be generated. Furthermore, due to the coupling, the starting current density of this mechanism is much lower than that of traditional electron beam-driven terahertz sources. This multi-beam radiation system may provide a favorable way to combine photonics structure with electronics excitation to generate middle, high power terahertz radiation. PMID:28112234

  8. Two-color two-photon excited fluorescence of indole: Determination of wavelength-dependent molecular parameters

    NASA Astrophysics Data System (ADS)

    Herbrich, Sebastian; Al-Hadhuri, Tawfik; Gericke, Karl-Heinz; Shternin, Peter S.; Smolin, Andrey G.; Vasyutinskii, Oleg S.

    2015-01-01

    We present a detailed study of two-color two-photon excited fluorescence in indole dissolved in propylene glycol. Femtosecond excitation pulses at effective wavelengths from 268 to 293.33 nm were used to populate the two lowest indole excited states 1La and 1Lb and polarized fluorescence was then detected. All seven molecular parameters and the two-photon polarization ratio Ω containing information on two-photon absorption dynamics, molecular lifetime τf, and rotation correlation time τrot have been determined from experiment and analyzed as a function of the excitation wavelength. The analysis of the experimental data has shown that 1Lb-1La inversion occurred under the conditions of our experiment. The two-photon absorption predominantly populated the 1La state at all excitation wavelengths but in the 287-289 nm area which contained an absorption hump of the 1Lb state 0-0 origin. The components of the two-photon excitation tensor S were analyzed giving important information on the principal tensor axes and absorption symmetry. The results obtained are in a good agreement with the results reported by other groups. The lifetime τf and the rotation correlation time τrot showed no explicit dependence on the effective excitation wavelength. Their calculated weighted average values were found to be τf = 3.83 ± 0.14 ns and τrot = 0.74 ± 0.06 ns.

  9. Arduino Due based tool to facilitate in vivo two-photon excitation microscopy

    PubMed Central

    Artoni, Pietro; Landi, Silvia; Sato, Sebastian Sulis; Luin, Stefano; Ratto, Gian Michele

    2016-01-01

    Two-photon excitation spectroscopy is a powerful technique for the characterization of the optical properties of genetically encoded and synthetic fluorescent molecules. Excitation spectroscopy requires tuning the wavelength of the Ti:sapphire laser while carefully monitoring the delivered power. To assist laser tuning and the control of delivered power, we developed an Arduino Due based tool for the automatic acquisition of high quality spectra. This tool is portable, fast, affordable and precise. It allowed studying the impact of scattering and of blood absorption on two-photon excitation light. In this way, we determined the wavelength-dependent deformation of excitation spectra occurring in deep tissues in vivo. PMID:27446677

  10. Arduino Due based tool to facilitate in vivo two-photon excitation microscopy.

    PubMed

    Artoni, Pietro; Landi, Silvia; Sato, Sebastian Sulis; Luin, Stefano; Ratto, Gian Michele

    2016-04-01

    Two-photon excitation spectroscopy is a powerful technique for the characterization of the optical properties of genetically encoded and synthetic fluorescent molecules. Excitation spectroscopy requires tuning the wavelength of the Ti:sapphire laser while carefully monitoring the delivered power. To assist laser tuning and the control of delivered power, we developed an Arduino Due based tool for the automatic acquisition of high quality spectra. This tool is portable, fast, affordable and precise. It allowed studying the impact of scattering and of blood absorption on two-photon excitation light. In this way, we determined the wavelength-dependent deformation of excitation spectra occurring in deep tissues in vivo.

  11. Nascent PO(X 2Π) E,V,R,T excitations from collision-free IR laser photolysis: Specificity toward the PO(X 2Pi 1/2) spin-orbit statea)

    NASA Astrophysics Data System (ADS)

    Chou, Jim-Son; Sumida, David S.; Wittig, C.

    1985-02-01

    PO (X 2Π) is produced via the collision-free infrared multiple photon dissociation (IRMPD) of volatile organophosphorous molecules, and is detected by two-frequency two-photon ionization, using the B 2Σ+ state to provide a spectral signature from which X 2Π populations are obtained. Sequential dissociations occur during the IR laser photolysis, in which nascent fragments continue to undergo IRMPD, and PO (X 2Π) accrues from a series of bond fission reactions. Nascent vibrational, rotational, and translational excitations are in sensible accord with this mechanism, except for a few rotational states near J=19.5. Unlike the nuclear degrees of freedom, the PO (X 2Π) spin-orbit states are populated quite selectively. The 2Π3/2 state, lying only 224 cm-1 above the 2Π1/2 ground state, contains only ˜11% of the population, compared to 34% for a 300 K sample. This result is unambiguous; it persists with all precursors, laser fluences, etc., and is verified by comparisons to spectra obtained using a microwave discharge, a flame, and when thermalizing nascent excitations with an inert diluent. This result underscores the importance of the separate potential surfaces which correlate to the product spin-orbit states, and the small amount of 2Π3/2 population can be accounted for by nonadiabatic coupling during dissociation, and/or ``freezing'' the amount of S1 character in an excited precursor in which S0 and S1 are coupled nonradiatively. We note that such electronic specificity should be dealt with in the analogous recombination reactions.

  12. Vibrational excitation of hydrogen molecules by two-photon absorption and third-harmonic generation

    NASA Astrophysics Data System (ADS)

    Miyamoto, Yuki; Hara, Hideaki; Hiraki, Takahiro; Masuda, Takahiko; Sasao, Noboru; Uetake, Satoshi; Yoshimi, Akihiro; Yoshimura, Koji; Yoshimura, Motohiko

    2018-01-01

    We report the coherent excitation of the vibrational state of hydrogen molecules by two-photon absorption and the resultant third-harmonic generation (THG). Parahydrogen molecules cooled by liquid nitrogen are irradiated by mid-infrared nanosecond pulses at 4.8 μm with a nearly Fourier-transform-limited linewidth. The first excited vibrational state of parahydrogen is populated by two-photon absorption of the mid-infrared photons. Because of the narrow linewidth of the mid-infrared pulses, coherence between the ground and excited states is sufficient to induce higher-order processes. Near-infrared photons from the THG are observed at 1.6 μm. The dependence of the intensity of the near-infrared radiation on mid-infrared pulse energy, target pressure, and cell length is determined. We used a simple formula for THG with consideration of realistic experimental conditions to explain the observed results.

  13. Direct slow-light excitation in photonic crystal waveguides forming ultra-compact splitters.

    PubMed

    Zhang, Min; Groothoff, Nathaniel; Krüger, Asger Christian; Shi, Peixing; Kristensen, Martin

    2011-04-11

    Based on a series of 1x2 beam splitters, novel direct excitation of slow-light from input- to output-region in photonic crystal waveguides is investigated theoretically and experimentally. The study shows that the slow-light excitation provides over 50 nm bandwidth for TE-polarized light splitting between two output ports, and co-exists together with self-imaging leading to ~20 nm extra bandwidth. The intensity of the direct excitation is qualitatively explained by the overlap integral of the magnetic fields between the ground input- and excited output-modes. The direct excitation of slow light is practically lossless compared with transmission in a W1 photonic crystal waveguides, which broadens the application-field for slow-light and further minimizes the size of a 1x2 splitter. © 2011 Optical Society of America

  14. Two-color two-photon excited fluorescence of indole: Determination of wavelength-dependent molecular parameters

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

    Herbrich, Sebastian; Al-Hadhuri, Tawfik; Gericke, Karl-Heinz, E-mail: k.Gericke@tu-bs.de

    2015-01-14

    We present a detailed study of two-color two-photon excited fluorescence in indole dissolved in propylene glycol. Femtosecond excitation pulses at effective wavelengths from 268 to 293.33 nm were used to populate the two lowest indole excited states {sup 1}L{sub a} and {sup 1}L{sub b} and polarized fluorescence was then detected. All seven molecular parameters and the two-photon polarization ratio Ω containing information on two-photon absorption dynamics, molecular lifetime τ{sub f}, and rotation correlation time τ{sub rot} have been determined from experiment and analyzed as a function of the excitation wavelength. The analysis of the experimental data has shown that {supmore » 1}L{sub b}–{sup 1}L{sub a} inversion occurred under the conditions of our experiment. The two-photon absorption predominantly populated the {sup 1}L{sub a} state at all excitation wavelengths but in the 287–289 nm area which contained an absorption hump of the {sup 1}L{sub b} state 0-0 origin. The components of the two-photon excitation tensor S were analyzed giving important information on the principal tensor axes and absorption symmetry. The results obtained are in a good agreement with the results reported by other groups. The lifetime τ{sub f} and the rotation correlation time τ{sub rot} showed no explicit dependence on the effective excitation wavelength. Their calculated weighted average values were found to be τ{sub f} = 3.83 ± 0.14 ns and τ{sub rot} = 0.74 ± 0.06 ns.« less

  15. Tuning Ag29 nanocluster light emission from red to blue with one and two-photon excitation.

    PubMed

    Russier-Antoine, Isabelle; Bertorelle, Franck; Hamouda, Ramzi; Rayane, Driss; Dugourd, Philippe; Sanader, Željka; Bonačić-Koutecký, Vlasta; Brevet, Pierre-François; Antoine, Rodolphe

    2016-02-07

    We demonstrate that the tuning of the light emission from red to blue in dihydrolipoic acid (DHLA) capped Ag29 nanoclusters can be trigged with one and two photon excitations. The cluster stoichiometry was determined with mass spectrometry and found to be Ag29(DHLA)12. In a detailed optical investigation, we show that these silver nanoclusters exhibit a strong red photoluminescence visible to the naked eye and characterized by a quantum yield of nearly ∼2% upon one-photon excitation. In the nonlinear optical (NLO) study of the properties of the clusters, the two-photon excited fluorescence spectra were recorded and their first hyperpolarizability obtained. The two-photon absorption cross-section at ∼800 nm for Ag29(DHLA)12 is higher than 10(4) GM and the hyperpolarizability is 106 × 10(-30) esu at the same excitation wavelength. The two-photon excited fluorescence spectrum appears strongly blue-shifted as compared to the one-photon excited spectrum, displaying a broad band between 400 and 700 nm. The density functional theory (DFT) provides insight into the structural and electronic properties of Ag29(DHLA)12 as well as into interplay between metallic subunit or core and ligands which is responsible for unique optical properties.

  16. Single-molecule detection by two-photon excitation of fluorescence

    NASA Astrophysics Data System (ADS)

    Zander, Christoph; Brand, Leif; Eggeling, C.; Drexhage, Karl-Heinz; Seidel, Claus A. M.

    1997-05-01

    Using a mode-locked titanium: sapphire laser at 700 nm for two-photon excitation we studied fluorescence bursts from individual coumarin 120 molecules in water and triacetin. Fluorescence lifetimes and multichannel scaler traces have been measured simultaneously. Due to the fact that scattered excitation light as well as Raman scattered photons can be suppressed by a short-pass filter a very low background level was achieved. To identify the fluorophore by its characteristic fluorescence lifetime the time-resolved fluorescence signals were analyzed by a maximum likelihood estimator. The obtained average fluorescence lifetimes (tau) av equals 4.8 +/- 1.2 ns for coumarin 120 in water and (tau) av equals 3.3 +/- 0.6 for coumarin 120 in triacetin are in good agreement with results obtained from separate measurements at higher concentrations.

  17. Resonantly enhanced multiple exciton generation through below-band-gap multi-photon absorption in perovskite nanocrystals.

    PubMed

    Manzi, Aurora; Tong, Yu; Feucht, Julius; Yao, En-Ping; Polavarapu, Lakshminarayana; Urban, Alexander S; Feldmann, Jochen

    2018-04-17

    Multi-photon absorption and multiple exciton generation represent two separate strategies for enhancing the conversion efficiency of light into usable electric power. Targeting below-band-gap and above-band-gap energies, respectively, to date these processes have only been demonstrated independently. Here we report the combined interaction of both nonlinear processes in CsPbBr 3 perovskite nanocrystals. We demonstrate nonlinear absorption over a wide range of below-band-gap excitation energies (0.5-0.8 E g ). Interestingly, we discover high-order absorption processes, deviating from the typical two-photon absorption, at specific energetic positions. These energies are associated with a strong enhancement of the photoluminescence intensity by up to 10 5 . The analysis of the corresponding energy levels reveals that the observed phenomena can be ascribed to the resonant creation of multiple excitons via the absorption of multiple below-band-gap photons. This effect may open new pathways for the efficient conversion of optical energy, potentially also in other semiconducting materials.

  18. Quasiperiodic one-dimensional photonic crystals with adjustable multiple photonic bandgaps.

    PubMed

    Vyunishev, Andrey M; Pankin, Pavel S; Svyakhovskiy, Sergey E; Timofeev, Ivan V; Vetrov, Stepan Ya

    2017-09-15

    We propose an elegant approach to produce photonic bandgap (PBG) structures with multiple photonic bandgaps by constructing quasiperiodic photonic crystals (QPPCs) composed of a superposition of photonic lattices with different periods. Generally, QPPC structures exhibit both aperiodicity and multiple PBGs due to their long-range order. They are described by a simple analytical expression, instead of quasiperiodic tiling approaches based on substitution rules. Here we describe the optical properties of QPPCs exhibiting two PBGs that can be tuned independently. PBG interband spacing and its depth can be varied by choosing appropriate reciprocal lattice vectors and their amplitudes. These effects are confirmed by the proof-of-concept measurements made for the porous silicon-based QPPC of the appropriate design.

  19. Observation of localized ground and excited orbitals in graphene photonic ribbons

    NASA Astrophysics Data System (ADS)

    Cantillano, C.; Mukherjee, S.; Morales-Inostroza, L.; Real, B.; Cáceres-Aravena, G.; Hermann-Avigliano, C.; Thomson, R. R.; Vicencio, R. A.

    2018-03-01

    We report on the experimental realization of a quasi-one-dimensional photonic graphene ribbon supporting four flat-bands (FBs). We study the dynamics of fundamental and dipolar modes, which are analogous to the s and p orbitals, respectively. In the experiment, both modes (orbitals) are effectively decoupled from each other, implying two sets of six bands, where two of them are completely flat (dispersionless). Using an image generator setup, we excite the s and p FB modes and demonstrate their non-diffracting propagation for the first time. Our results open an exciting route towards photonic emulation of higher orbital dynamics.

  20. Harvesting multiple electron-hole pairs generated through plasmonic excitation of Au nanoparticles.

    PubMed

    Kim, Youngsoo; Smith, Jeremy G; Jain, Prashant K

    2018-05-07

    Multi-electron redox reactions, although central to artificial photosynthesis, are kinetically sluggish. Amidst the search for synthetic catalysts for such processes, plasmonic nanoparticles have been found to catalyse multi-electron reduction of CO 2 under visible light. This example motivates the need for a general, insight-driven framework for plasmonic catalysis of such multi-electron chemistry. Here, we elucidate the principles underlying the extraction of multiple redox equivalents from a plasmonic photocatalyst. We measure the kinetics of electron harvesting from a gold nanoparticle photocatalyst as a function of photon flux. Our measurements, supported by theoretical modelling, reveal a regime where two-electron transfer from the excited gold nanoparticle becomes prevalent. Multiple electron harvesting becomes possible under continuous-wave, visible-light excitation of moderate intensity due to strong interband transitions in gold and electron-hole separation accomplished using a hole scavenger. These insights will help expand the utility of plasmonic photocatalysis beyond CO 2 reduction to other challenging multi-electron, multi-proton transformations such as N 2 fixation.

  1. Investigation of electron-loss and photon scattering correction factors for FAC-IR-300 ionization chamber

    NASA Astrophysics Data System (ADS)

    Mohammadi, S. M.; Tavakoli-Anbaran, H.; Zeinali, H. Z.

    2017-02-01

    The parallel-plate free-air ionization chamber termed FAC-IR-300 was designed at the Atomic Energy Organization of Iran, AEOI. This chamber is used for low and medium X-ray dosimetry on the primary standard level. In order to evaluate the air-kerma, some correction factors such as electron-loss correction factor (ke) and photon scattering correction factor (ksc) are needed. ke factor corrects the charge loss from the collecting volume and ksc factor corrects the scattering of photons into collecting volume. In this work ke and ksc were estimated by Monte Carlo simulation. These correction factors are calculated for mono-energy photon. As a result of the simulation data, the ke and ksc values for FAC-IR-300 ionization chamber are 1.0704 and 0.9982, respectively.

  2. The excitation mechanism of btp2 Ir(acac) in CBP host.

    PubMed

    Xiao-Bo, Zhang; Fu-Xiang, Wei

    2017-05-01

    Whether bis(2-(2'-benzo[4,5-α]thienyl)pyridinato-N,C3')iridium(acetylacetonate) (btp 2 Ir(acac)) emission comes from carrier trapping and/or energy transfer, when doped in the 4,4'-bis(N-carbazolyl)biphenyl (CBP) host in organic light-emitting devices, is not clear; therefore, the btp 2 Ir(acac) emission in CBP hosts was studied. In the red-doped device, both N,N'-bis(1-naphthyl)-N,N'-diphenyl-1.1'-bipheny1-4-4'-diamine (NPB) and (1,1'-biphenyl-4'-oxy)bis(8-hydroxy-2-methylquinolinato)-aluminum (BAlq) emission appeared, which illustrated that CBP excitons cannot be formed at two emissive layer (EML) interfaces in the device. In the co-doped devices, NPB and BAlq emissions disappear and 1,4-bis[2-(3-N-ethylcarbazoryl)vinyl]benzene (BCzVB) emission appears, illustrating the formation of CBP excitons at two EML interfaces in these devices. The reason for this difference was analyzed and it was found that holes in the NPB layer could be made directly into the CBP host in the EML interface of the red-doped device. In contrast, holes were injected into CBP host via the btp 2 Ir(acac)/BCzVB dopants in the co-doped devices, which facilitated hole injection from the NPB layer to the EML, leading to the formation of CBP excitons at two EML interfaces in the co-doped devices. Therefore, btp 2 Ir(acac) emission was caused by carrier trapping in the red-doped device, while, in the co-doped devices, it resulted from both carrier trapping and energy transfer from the CBP. Furthermore, it was revealed that the carrier trapping mechanism is less efficient than the energy transfer mechanism for btp 2 Ir(acac) excitation in co-doped devices. In summary, our results clarified the excitation mechanism of btp 2 Ir(acac) in the CBP host. Copyright © 2016 John Wiley & Sons, Ltd.

  3. Intravital autofluorescence 2-photon microscopy of murine intestinal mucosa with ultra-broadband femtosecond laser pulse excitation: image quality, photodamage, and inflammation

    NASA Astrophysics Data System (ADS)

    Klinger, Antje; Krapf, Lisa; Orzekowsky-Schroeder, Regina; Koop, Norbert; Vogel, Alfred; Hüttmann, Gereon

    2015-11-01

    Ultra-broadband excitation with ultrashort pulses may enable simultaneous excitation of multiple endogenous fluorophores in vital tissue. Imaging living gut mucosa by autofluorescence 2-photon microscopy with more than 150 nm broad excitation at an 800-nm central wavelength from a sub-10 fs titanium-sapphire (Ti:sapphire) laser with a dielectric mirror based prechirp was compared to the excitation with 220 fs pulses of a tunable Ti:sapphire laser at 730 and 800 nm wavelengths. Excitation efficiency, image quality, and photochemical damage were evaluated. At similar excitation fluxes, the same image brightness was achieved with both lasers. As expected, with ultra-broadband pulses, fluorescence from NAD(P)H, flavines, and lipoproteins was observed simultaneously. However, nonlinear photodamage apparent as hyperfluorescence with functional and structural alterations of the tissue occurred earlier when the laser power was adjusted to the same image brightness. After only a few minutes, the immigration of polymorphonuclear leucocytes into the epithelium and degranulation of these cells, a sign of inflammation, was observed. Photodamage is promoted by the higher peak irradiances and/or by nonoptimal excitation of autofluorescence at the longer wavelength. We conclude that excitation with a tunable narrow bandwidth laser is preferable to ultra-broadband excitation for autofluorescence-based 2-photon microscopy, unless the spectral phase can be controlled to optimize excitation conditions.

  4. Fabrication of 3D polymer photonic crystals for near-IR applications

    NASA Astrophysics Data System (ADS)

    Yao, Peng; Qiu, Liang; Shi, Shouyuan; Schneider, Garrett J.; Prather, Dennis W.; Sharkawy, Ahmed; Kelmelis, Eric

    2008-02-01

    Photonic crystals[1, 2] have stirred enormous research interest and became a growing enterprise in the last 15 years. Generally, PhCs consist of periodic structures that possess periodicity comparable with the wavelength that the PhCs are designed to modulate. If material and periodic pattern are properly selected, PhCs can be applied to many applications based on their unique properties, including photonic band gaps (PBG)[3], self-collimation[4], super prism[5], etc. Strictly speaking, PhCs need to possess periodicity in three dimensions to maximize their advantageous capabilities. However, many current research is based on scaled two-dimensional PhCs, mainly due to the difficulty of fabrication such three-dimensional PhCs. Many approaches have been explored for the fabrication of 3D photonic crystals, including layer-by-layer surface micromachining[6], glancing angle deposition[7], 3D micro-sculpture method[8], self-assembly[9] and lithographical methods[10-12]. Among them, lithographic methods became increasingly accepted due to low costs and precise control over the photonic crystal structure. There are three mostly developed lithographical methods, namely X-ray lithography[10], holographic lithography[11] and two-photon polymerization[12]. Although significant progress has been made in developing these lithography-based technologies, these approaches still suffer from significant disadvantages. X-ray lithography relies on an expensive radiation source. Holographic lithography lacks the flexibility to create engineered defects, and multi-photon polymerization is not suitable for parallel fabrication. In our previous work, we developed a multi-layer photolithography processes[13, 14] that is based on multiple resist application and enhanced absorption upon exposure. Using a negative lift-off resist (LOR) and 254nm DUV source, we have demonstrated fabrication of 3D arbitrary structures with feature size of several microns. However, severe intermixing problem

  5. Hydricity, electrochemistry, and excited-state chemistry of Ir complexes for CO 2 reduction

    DOE PAGES

    Manbeck, Gerald F.; Garg, Komal; Shimoda, Tomoe; ...

    2016-12-01

    Here, we prepared electron-rich derivatives of [Ir(tpy)(ppy)Cl] + with modification of the bidentate (ppy) or tridentate (tpy) ligands in attempt to increase the reactivity for CO 2 reduction and the ability to transfer hydrides (hydricity). Density functional theory (DFT) calculations reveal that complexes with dimethyl-substituted ppy have similar hydricities to the non-substituted parent complex, and photocatalytic CO 2 reduction studies show selective CO formation. Substitution of tpy for bis(benzimidazole)-phenyl or -pyridine (L3 and L4, respectively) induces changes in the physical properties much more pronounced than addition of methyl groups to ppy. Theoretical data predict [Ir(L3)(ppy)(H)] is the strongest hydride donormore » among complexes studied in this work, but [Ir(L3)(ppy)(NCCH 3)] + cannot be reduced photochemically because the excited state reduction potential is only 0.52 V due to the negative ground state potential of –1.91 V. The excited state [Ir(L4)(ppy)(NCCH 3)] 2+ is the strongest oxidant among complexes studied in this work and the singly reduced species is formed readily upon photolysis in the presence of tertiary amines. Both [Ir(L3)(ppy)(NCCH 3)] + and [Ir(L4)(ppy)(NCCH 3)] 2+ exhibit electrocatalytic current for CO 2 reduction. While a significantly greater overpotential is needed for the L3 complex, a small amount of formate (5-10 %) generation in addition to CO was observed as predicted by the DFT calculations.« less

  6. Visible-to-visible four-photon ultrahigh resolution microscopic imaging with 730-nm diode laser excited nanocrystals.

    PubMed

    Wang, Baoju; Zhan, Qiuqiang; Zhao, Yuxiang; Wu, Ruitao; Liu, Jing; He, Sailing

    2016-01-25

    Further development of multiphoton microscopic imaging is confronted with a number of limitations, including high-cost, high complexity and relatively low spatial resolution due to the long excitation wavelength. To overcome these problems, for the first time, we propose visible-to-visible four-photon ultrahigh resolution microscopic imaging by using a common cost-effective 730-nm laser diode to excite the prepared Nd(3+)-sensitized upconversion nanoparticles (Nd(3+)-UCNPs). An ordinary multiphoton scanning microscope system was built using a visible CW diode laser and the lateral imaging resolution as high as 161-nm was achieved via the four-photon upconversion process. The demonstrated large saturation excitation power for Nd(3+)-UCNPs would be more practical and facilitate the four-photon imaging in the application. A sample with fine structure was imaged to demonstrate the advantages of visible-to-visible four-photon ultrahigh resolution microscopic imaging with 730-nm diode laser excited nanocrystals. Combining the uniqueness of UCNPs, the proposed visible-to-visible four-photon imaging would be highly promising and attractive in the field of multiphoton imaging.

  7. The mid-IR silicon photonics sensor platform (Conference Presentation)

    NASA Astrophysics Data System (ADS)

    Kimerling, Lionel; Hu, Juejun; Agarwal, Anuradha M.

    2017-02-01

    Advances in integrated silicon photonics are enabling highly connected sensor networks that offer sensitivity, selectivity and pattern recognition. Cost, performance and the evolution path of the so-called `Internet of Things' will gate the proliferation of these networks. The wavelength spectral range of 3-8um, commonly known as the mid-IR, is critical to specificity for sensors that identify materials by detection of local vibrational modes, reflectivity and thermal emission. For ubiquitous sensing applications in this regime, the sensors must move from premium to commodity level manufacturing volumes and cost. Scaling performance/cost is critically dependent on establishing a minimum set of platform attributes for point, wearable, and physical sensing. Optical sensors are ideal for non-invasive applications. Optical sensor device physics involves evanescent or intra-cavity structures for applied to concentration, interrogation and photo-catalysis functions. The ultimate utility of a platform is dependent on sample delivery/presentation modalities; system reset, recalibration and maintenance capabilities; and sensitivity and selectivity performance. The attributes and performance of a unified Glass-on-Silicon platform has shown good prospects for heterogeneous integration on materials and devices using a low cost process flow. Integrated, single mode, silicon photonic platforms offer significant performance and cost advantages, but they require discovery and qualification of new materials and process integration schemes for the mid-IR. Waveguide integrated light sources based on rare earth dopants and Ge-pumped frequency combs have promise. Optical resonators and waveguide spirals can enhance sensitivity. PbTe materials are among the best choices for a standard, waveguide integrated photodetector. Chalcogenide glasses are capable of transmitting mid-IR signals with high transparency. Integrated sensor case studies of i) high sensitivity analyte detection in

  8. Towards two-photon excited endogenous fluorescence lifetime imaging microendoscopy

    PubMed Central

    Hage, C. H.; Leclerc, P.; Brevier, J.; Fabert, M.; Le Nézet, C.; Kudlinski, A.; Héliot, L.; Louradour, F.

    2017-01-01

    In situ fluorescence lifetime imaging microscopy (FLIM) in an endoscopic configuration of the endogenous biomarker nicotinamide adenine dinucleotide (NADH) has a great potential for malignant tissue diagnosis. Moreover, two-photon nonlinear excitation provides intrinsic optical sectioning along with enhanced imaging depth. We demonstrate, for the first time to our knowledge, nonlinear endogenous FLIM in a fibered microscope with proximal detection, applied to NADH in cultured cells, as a first step to a nonlinear endomicroscope, using a double-clad microstructured fiber with convenient fiber length (> 3 m) and excitation pulse duration (≈50 fs). Fluorescence photons are collected by the fiber inner cladding and we show that its contribution to the impulse response function (IRF), which originates from its intermodal and chromatic dispersions, is small (< 600 ps) and stable for lengths up to 8 m and allows for short lifetime measurements. We use the phasor representation as a quick visualization tool adapted to the endoscopy speed requirements. PMID:29359093

  9. Cardiovascular Imaging Using Two-Photon Microscopy

    PubMed Central

    Scherschel, John A.; Rubart, Michael

    2008-01-01

    Two-photon excitation microscopy has become the standard technique for high resolution deep tissue and intravital imaging. It provides intrinsic three-dimensional resolution in combination with increased penetration depth compared to single-photon confocal microscopy. This article will describe the basic physical principles of two-photon excitation and will review its multiple applications to cardiovascular imaging, including second harmonic generation and fluorescence laser scanning microscopy. In particular, the capability and limitations of multiphoton microscopy to assess functional heterogeneity on a cellular scale deep within intact, Langendorff-perfused hearts are demonstrated. It will also discuss the use of two-photon excitation-induced release of caged compounds for the study of intracellular calcium signaling and intercellular dye transfer. PMID:18986603

  10. Fragmentation mechanism of UV-excited peptides in the gas phase

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

    Zabuga, Aleksandra V., E-mail: aleksandra.zabuga@epfl.ch; Kamrath, Michael Z.; Boyarkin, Oleg V.

    We present evidence that following near-UV excitation, protonated tyrosine- or phenylalanine–containing peptides undergo intersystem crossing to produce a triplet species. This pathway competes with direct dissociation from the excited electronic state and with dissociation from the electronic ground state subsequent to internal conversion. We employ UV-IR double-resonance photofragment spectroscopy to record conformer-specific vibrational spectra of cold peptides pre-excited to their S{sub 1} electronic state. The absorption of tunable IR light by these electronically excited peptides leads to a drastic increase in fragmentation, selectively enhancing the loss of neutral phenylalanine or tyrosine side-chain, which are not the lowest dissociation channels inmore » the ground electronic state. The recorded IR spectra evolve upon increasing the time delay between the UV and IR pulses, reflecting the dynamics of the intersystem crossing on a timescale of ∼80 ns and <10 ns for phenylalanine- and tyrosine-containing peptides, respectively. Once in the triplet state, phenylalanine-containing peptides may live for more than 100 ms, unless they absorb IR photons and undergo dissociation by the loss of an aromatic side-chain. We discuss the mechanism of this fragmentation channel and its possible implications for photofragment spectroscopy and peptide photostability.« less

  11. Two-photon excitation spectrum of light-harvesting complex II and fluorescence upconversion after one- and two-photon excitation of the carotenoids

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

    Walla, P.J.; Yom, J.; Krueger, B.P.

    2000-05-18

    The two-photon excitation (TPE) spectrum of light-harvesting complex II (LHC II) has been measured in the spectral region of 1,000--1,600 nm, corresponding to one-photon wavelengths of 500--800 nm. The authors observed a band with an origin at {approximately}2 x 660 nm (ca. 15,100 {+-} 300 cm{sup {minus}1}) and a maximum at {approximately}2 x 600 nm. The line shape and origin of this band strongly suggest that the observed signal is due to the two-photon-allowed S{sub 1} state of the energy-transferring carotenoids (Car ) in LHC II. The authors also report the time dependence of the upconverted chlorophyll (Chl) fluorescence aftermore » TPE at the maximum of the observed band. Surprisingly, a fast rise of 250 {+-} 50 fs followed by a multiexponential decay on the picosecond time scale was observed. This result provides strong indication that there is a fast energy transfer even from the dipole-forbidden Car S{sub 1} state to the Chl's. The sub picosecond energy transfer from the Car S{sub 1} state is likely a consequence of the large number of energy-accepting Chls in van der Waals contact with the central Car's in LHC II. They also present upconversion data of the Car S{sub 2}, Chl a, and Chl b fluorescence observed after one-photon excitation into the dipole-allowed Car S{sub 2} state. The lifetime of the Car S{sub 2} state is {approximately}120 {+-} 30 fs. With the observed time constants they are able to calculate quantum yields for the different possible pathways contributing to the overall Car to Chl energy transfer in LHC II.« less

  12. Two photon excitation of atomic oxygen

    NASA Technical Reports Server (NTRS)

    Pindzola, M. S.

    1977-01-01

    A standard perturbation expansion in the atom-radiation field interaction is used to calculate the two photon excitation cross section for 1s(2) 2s(2) 2p(4) p3 to 1s(2) 2s(2) 2p(3) (s4) 3p p3 transition in atomic oxygen. The summation over bound and continuum intermediate states is handled by solving the equivalent inhomogeneous differential equation. Exact summation results differ by a factor of 2 from a rough estimate obtained by limiting the intermediate state summation to one bound state. Higher order electron correlation effects are also examined.

  13. Thermal bleaching in single fluorescent molecules under two-photon excitation regime

    NASA Astrophysics Data System (ADS)

    Chirico, Giuseppe; Cannone, Fabio; Baldini, Giancarlo; Diaspro, Alberto

    2003-07-01

    Single molecule spectroscopy often requires the immobilization of the molecules onto solid or quasi-solid substrates and the use of relatively high excitation intensity We have studied the fluorescence emission of four common dyes used for bio-imaging studies, rhodamine 6G, fluorescein, pyrene and indo-1 at the single molecule level under two-photon excitation regime. We focus on two-photon excitation thermal effects on the stability of the single molecules, influencing the internal photo-dynamics and the total duration of the fluorescent emission. Single dye molecules, spread on a glass substrate by spin coating, show a constant fluorescence output till a sudden transition to a dark state very close to the background. The bleaching time that is found to vary in the series pyrene, Indo-1, fluorescein and rhodamine 6G from the fastest to the slowest one respectively, has a Gaussian distribution suggesting that bleaching is not due to photo-bleaching. Moreover it shows a correlation to the amount of absorbed power not re-irradiated as fluorescence and to the complexity of the molecule. These observations are interpreted as thermal bleaching where the temperature increase is induced by the two-photon excitation process. This study should be extended to different trapping media of interest in single molecule basic research and applications, such as silica and polyacrylamide gels or nanosctructured polyelectrolyte matrices. We think that the observed behavior and the correlations found to the molecular chemical and physical parameters, may be of some help for the design of molecules with switching on-off behavior of longer duration.

  14. Hyperspectral imaging of microalgae using two-photon excitation.

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

    Sinclair, Michael B.; Melgaard, David Kennett; Reichardt, Thomas A.

    2010-10-01

    A considerable amount research is being conducted on microalgae, since microalgae are becoming a promising source of renewable energy. Most of this research is centered on lipid production in microalgae because microalgae produce triacylglycerol which is ideal for biodiesel fuels. Although we are interested in research to increase lipid production in algae, we are also interested in research to sustain healthy algal cultures in large scale biomass production farms or facilities. The early detection of fluctuations in algal health, productivity, and invasive predators must be developed to ensure that algae are an efficient and cost-effective source of biofuel. Therefore wemore » are developing technologies to monitor the health of algae using spectroscopic measurements in the field. To do this, we have proposed to spectroscopically monitor large algal cultivations using LIDAR (Light Detection And Ranging) remote sensing technology. Before we can deploy this type of technology, we must first characterize the spectral bio-signatures that are related to algal health. Recently, we have adapted our confocal hyperspectral imaging microscope at Sandia to have two-photon excitation capabilities using a chameleon tunable laser. We are using this microscope to understand the spectroscopic signatures necessary to characterize microalgae at the cellular level prior to using these signatures to classify the health of bulk samples, with the eventual goal of using of LIDAR to monitor large scale ponds and raceways. By imaging algal cultures using a tunable laser to excite at several different wavelengths we will be able to select the optimal excitation/emission wavelengths needed to characterize algal cultures. To analyze the hyperspectral images generated from this two-photon microscope, we are using Multivariate Curve Resolution (MCR) algorithms to extract the spectral signatures and their associated relative intensities from the data. For this presentation, I will show our

  15. Excitation enhancement and extraction enhancement with photonic crystals

    DOEpatents

    Shapira, Ofer; Soljacic, Marin; Zhen, Bo; Chua, Song-Liang; Lee, Jeongwon; Joannopoulos, John

    2015-03-03

    Disclosed herein is a system for stimulating emission from at least one an emitter, such as a quantum dot or organic molecule, on the surface of a photonic crystal comprising a patterned dielectric substrate. Embodiments of this system include a laser or other source that illuminates the emitter and the photonic crystal, which is characterized by an energy band structure exhibiting a Fano resonance, from a first angle so as to stimulate the emission from the emitter at a second angle. The coupling between the photonic crystal and the emitter may result in spectral and angular enhancement of the emission through excitation and extraction enhancement. These enhancement mechanisms also reduce the emitter's lasing threshold. For instance, these enhancement mechanisms enable lasing of a 100 nm thick layer of diluted organic molecules solution with reduced threshold intensity. This reduction in lasing threshold enables more efficient organic light emitting devices and more sensitive molecular sensing.

  16. Entanglement between a Photonic Time-Bin Qubit and a Collective Atomic Spin Excitation.

    PubMed

    Farrera, Pau; Heinze, Georg; de Riedmatten, Hugues

    2018-03-09

    Entanglement between light and matter combines the advantage of long distance transmission of photonic qubits with the storage and processing capabilities of atomic qubits. To distribute photonic states efficiently over long distances several schemes to encode qubits have been investigated-time-bin encoding being particularly promising due to its robustness against decoherence in optical fibers. Here, we demonstrate the generation of entanglement between a photonic time-bin qubit and a single collective atomic spin excitation (spin wave) in a cold atomic ensemble, followed by the mapping of the atomic qubit onto another photonic qubit. A magnetic field that induces a periodic dephasing and rephasing of the atomic excitation ensures the temporal distinguishability of the two time bins and plays a central role in the entanglement generation. To analyze the generated quantum state, we use largely imbalanced Mach-Zehnder interferometers to perform projective measurements in different qubit bases and verify the entanglement by violating a Clauser-Horne-Shimony-Holt Bell inequality.

  17. Entanglement between a Photonic Time-Bin Qubit and a Collective Atomic Spin Excitation

    NASA Astrophysics Data System (ADS)

    Farrera, Pau; Heinze, Georg; de Riedmatten, Hugues

    2018-03-01

    Entanglement between light and matter combines the advantage of long distance transmission of photonic qubits with the storage and processing capabilities of atomic qubits. To distribute photonic states efficiently over long distances several schemes to encode qubits have been investigated—time-bin encoding being particularly promising due to its robustness against decoherence in optical fibers. Here, we demonstrate the generation of entanglement between a photonic time-bin qubit and a single collective atomic spin excitation (spin wave) in a cold atomic ensemble, followed by the mapping of the atomic qubit onto another photonic qubit. A magnetic field that induces a periodic dephasing and rephasing of the atomic excitation ensures the temporal distinguishability of the two time bins and plays a central role in the entanglement generation. To analyze the generated quantum state, we use largely imbalanced Mach-Zehnder interferometers to perform projective measurements in different qubit bases and verify the entanglement by violating a Clauser-Horne-Shimony-Holt Bell inequality.

  18. Dual-color multiple-particle tracking at 50-nm localization and over 100-µm range in 3D with temporal focusing two-photon microscopy

    PubMed Central

    Ding, Yu; Li, Chunqiang

    2016-01-01

    Nanoscale particle tracking in three dimensions is crucial to directly observe dynamics of molecules and nanoparticles in living cells. Here we present a three-dimensional particle tracking method based on temporally focused two-photon excitation. Multiple particles are imaged at 30 frames/s in volume up to 180 × 180 × 100 µm3. The spatial localization precision can reach 50 nm. We demonstrate its capability of tracking fast swimming microbes at speed of ~200 µm/s. Two-photon dual-color tracking is achieved by simultaneously exciting two kinds of fluorescent beads at 800 nm to demonstrate its potential in molecular interaction studies. Our method provides a simple wide-field fluorescence imaging approach for deep multiple-particle tracking. PMID:27867724

  19. Watching the coherence of multiple vibrational states in organic dye molecules by using supercontinuum probing photon echo spectroscopy

    NASA Astrophysics Data System (ADS)

    Yu, Guoyang; Song, Yunfei; Wang, Yang; He, Xing; Liu, Yuqiang; Liu, Weilong; Yang, Yanqiang

    2011-12-01

    A modified photon echo (PE) technique, the supercontinuum probing photon echo (SCPPE), is introduced and performed to investigate the vibrational coherence in organic dye IR780 perchlorate doped polyvinyl alcohol (PVA) film. The coherences of multiple vibrational states which belong to four vibrational modes create complex oscillations in SCPPE signal. The frequencies of vibrational modes are confirmed from the results of Raman calculation which accord fairly well with the results of Raman scattering experiment. Compared with conventional one-color PE, the SCPPE technique can realize broadband detection and make the experiment about vibrational coherence more efficient.

  20. Light-induced damage and its diagnosis in two-photon excited autofluorescence imaging of retinal pigment epithelium cells

    NASA Astrophysics Data System (ADS)

    Chen, Danni; Qu, Junle; Xu, Gaixia; Zhao, Lingling; Niu, Hanben

    2007-05-01

    In this paper, a novel method for the differentiation of the retinal pigment epithelium (RPE) cells after light-induced damage by two-photon excitation is presented. Fresh samples of RPE cells of pig eyes are obtained from local slaughterhouse. Light-induced damage is produced by the output from Ti: sapphire laser which is focused onto the RPE layer. We study the change of the autofluorescence properties of RPE after two-photon excitation with the same wavelength. Preliminary results show that after two-photon excitation, there are two clear changes in the emission spectrum. The first change is the blue-shift of the emission peak. The emission peak of the intact RPE is located at 592nm, and after excitation, it shifts to 540nm. It is supposed that the excitation has led to the increased autofluorescence of flavin whose emission peak is located at 540nm. The second change is the increased intensity of the emission peak, which might be caused by the accelerated aging because the autofluorescence of RPE would increase during aging process. Experimental results indicate that two-photon excitation could not only lead to the damage of the RPE cells in multiphoton RPE imaging, but also provide an evaluation of the light-induced damage.

  1. Improved reference standards for femtosecond three-photon excitation of fluorescence in the wavelength range 950 - 1750 nm

    NASA Astrophysics Data System (ADS)

    Rebane, Aleksander; Mikhaylov, Alexander

    2018-02-01

    Fluorescence excited by instantaneous three-photon absorption (3PA) in organic fluorophores is gaining importance as a versatile modality for deep-tissue microscopy and imaging. However, due to technical difficulty of quantifying the higher-order nonlinear absorption cross-section, reliable 3PA cross section values, σ3PA, covering a broad spectral range have been so far not available. This lack of experimental data hinders us from gaining quantitative understanding of relevant structure-property relationships as well as impedes progress towards developing 3-photon fluorophores optimized for various applications. We report on measurement of the absolute 3PA cross section spectra in the 950 - 1750 nm range in a series of common organic fluorophores in various solvents: (a) Rhodamine 6G in deuterated methanol, (b) Coumarin 153 in DMSO and toluene, (c) Prodan in DMSO and toluene, (d) Fluorescein in pH11 buffer, (e) AF455 in toluene, (f) BDPAS in deuterated methylene chloride. In these experiments, we employ femtosecond wavelength-tunable optical parametric amplifier to excite fluorescence signal that has cubic dependence on the incident photon flux. Absolute values of σ3PA are determined using two complementary methods: (i) calibrating the fluorescence signal relative to one-photon (linear) excitation combined with accurate measurement of the pulse temporal- and spatial profile to determine the excitation photon flux and (ii) calibration of the cubic fluorescence signal relative to quadratic florescence excited in fluorophores with known two-photon absorption cross section. Depending on the method utilized, the peak σ3PA values have estimated accuracy 50% and vary in the range, σ3PA = 10-81 - 10-79 cm6 s2 photon-2 , depending on the system studied, with AF455 showing the most enhanced 3PA efficiency. The 3PA spectral shapes have estimated accuracy of 20% and show some unexpected deviations from corresponding one-photon spectral profiles.

  2. Sonic IR crack detection of aircraft turbine engine blades with multi-frequency ultrasound excitations

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

    Zhang, Ding; Han, Xiaoyan; Newaz, Golam

    Effectively and accurately detecting cracks or defects in critical engine components, such as turbine engine blades, is very important for aircraft safety. Sonic Infrared (IR) Imaging is such a technology with great potential for these applications. This technology combines ultrasound excitation and IR imaging to identify cracks and flaws in targets. In general, failure of engine components, such as blades, begins with tiny cracks. Since the attenuation of the ultrasound wave propagation in turbine engine blades is small, the efficiency of crack detection in turbine engine blades can be quite high. The authors at Wayne State University have been developingmore » the technology as a reliable tool for the future field use in aircraft engines and engine parts. One part of the development is to use finite element modeling to assist our understanding of effects of different parameters on crack heating while experimentally hard to achieve. The development has been focused with single frequency ultrasound excitation and some results have been presented in a previous conference. We are currently working on multi-frequency excitation models. The study will provide results and insights of the efficiency of different frequency excitation sources to foster the development of the technology for crack detection in aircraft engine components.« less

  3. Multimodal wide-field two-photon excitation imaging: characterization of the technique for in vivo applications

    PubMed Central

    Hwang, Jae Youn; Wachsmann-Hogiu, Sebastian; Ramanujan, V Krishnan; Nowatzyk, Andreas G.; Koronyo, Yosef; Medina-Kauwe, Lali K.; Gross, Zeev; Gray, Harry B.; Farkas, Daniel L.

    2011-01-01

    We report fast, non-scanning, wide-field two-photon fluorescence excitation with spectral and lifetime detection for in vivo biomedical applications. We determined the optical characteristics of the technique, developed a Gaussian flat-field correction method to reduce artifacts resulting from non-uniform excitation such that contrast is enhanced, and showed that it can be used for ex vivo and in vivo cellular-level imaging. Two applications were demonstrated: (i) ex vivo measurements of beta-amyloid plaques in retinas of transgenic mice, and (ii) in vivo imaging of sulfonated gallium(III) corroles injected into tumors. We demonstrate that wide-field two photon fluorescence excitation with flat-field correction provides more penetration depth as well as better contrast and axial resolution than the corresponding one-photon wide field excitation for the same dye. Importantly, when this technique is used together with spectral and fluorescence lifetime detection modules, it offers improved discrimination between fluorescence from molecules of interest and autofluorescence, with higher sensitivity and specificity for in vivo applications. PMID:21339880

  4. Fluorescence anisotropy of indole molecules under two-photon excitation in the spectral range of 485-510 nm

    NASA Astrophysics Data System (ADS)

    Sasin, M. E.; Tushkanov, V. I.; Smolin, A. G.; Vasyutinskii, O. S.

    2017-10-01

    Decay of polarized fluorescence in indole dissolved in propylene glycol under two-photon excitation by femtosecond laser pulses in the wavelength range of 485-510 nm has been studied. It is shown that under the experimental conditions used the fluorescence decay signal can be well described by a single excited state lifetime τf and a single rotation diffusion time τrot. By processing the data obtained, the times τf and τrot as well as anisotropy parameter r 0 characterizing the symmetry of two-photon excitation of indole molecules have been determined. Decreasing of the anisotropy parameter r0 down to zero under two-photon excitation energy higher than 5.1 eV has been observed. Interpretation of the obtained results have been done on the basis of ab initio quantum-mechanical computations. A model of energy relaxation under the condition of twophoton excitation of indole in a polar solvent has been discussed.

  5. Mapping and controlling ultrafast dynamics of highly excited H 2 molecules by VUV-IR pump-probe schemes

    DOE PAGES

    Sturm, F. P.; Tong, X. M.; Palacios, A.; ...

    2017-01-09

    Here, we used ultrashort femtosecond vacuum ultraviolet (VUV) and infrared (IR) pulses in a pump-probe scheme to map the dynamics and nonequilibrium dissociation channels of excited neutral H 2 molecules. A nuclear wave packet is created in the B 1Σmore » $$+\\atop{u}$$ state of the neutral H 2 molecule by absorption of the ninth harmonic of the driving infrared laser field. Due to the large stretching amplitude of the molecule excited in the B 1Σ$$+\\atop{u}$$ electronic state, the effective H 2 + ionization potential changes significantly as the nuclear wave packet vibrates in the bound, highly electronically and vibrationally excited B potential-energy curve. We probed such dynamics by ionizing the excited neutral molecule using time-delayed VUV-or-IR radiation. We identified the nonequilibrium dissociation channels by utilizing three-dimensional momentum imaging of the ion fragments. We also found that different dissociation channels can be controlled, to some extent, by changing the IR laser intensity and by choosing the wavelength of the probe laser light. Furthermore, we concluded that even in a benchmark molecular system such as H 2*, the interpretation of the nonequilibrium multiphoton and multicolor ionization processes is still a challenging task, requiring intricate theoretical analysis.« less

  6. Two-photon absorption by spectrally shaped entangled photons

    NASA Astrophysics Data System (ADS)

    Oka, Hisaki

    2018-03-01

    We theoretically investigate two-photon excitation by spectrally shaped entangled photons with energy anticorrelation in terms of how the real excitation of an intermediate state affects two-photon absorption by entangled photons. Spectral holes are introduced in the entangled photons around the energy levels of an intermediate state so that two-step excitation via the real excitation of the intermediated state can be suppressed. Using a three-level atomic system as an example, we show that the spectral holes well suppress the real excitation of the intermediate state and recover two-photon absorption via a virtual state. Furthermore, for a short pulse close to a monocycle, we show that the excitation efficiency by the spectrally shaped entangled photons can be enhanced a thousand times as large as that by uncorrelated photons.

  7. Transient absorption study of two-photon excitation mechanism in the LH2 complex from purple bacterium Rhodobacter sphaeroides.

    PubMed

    Stepanenko, Ilya; Kompanetz, Viktor; Makhneva, Zoya; Chekalin, Sergey; Moskalenko, Andrei; Razjivin, Andrei

    2012-03-08

    The mechanism of two-photon excitation of a peripheral light-harvesting complex LH2 (B800-850) from purple bacterium Rhodobacter sphaeroides was explained on the basis of femtosecond transient absorption data. Fast bleaching of the B850 absorption band was measured under two-photon excitation by 1350 nm femtosecond pulses, showing fast subpicosecond arrival of excitation energy to B850 circular aggregates. Any spectral changes connected with the B800 absorption band of B800-BChl molecules were absent. A similar picture was observed under one-photon excitation of the LH2 complex by 675 nm femtosecond pulses. We believe these effects may be attributed to direct excitation of high-energy excitonic states of a B850 circular aggregate or its vibrational manifold in accordance with the model of Abe [Chem. Phys. 2001, 264, 355-363].

  8. Two-Photon Excitation, Fluorescence Microscopy, and Quantitative Measurement of Two-Photon Absorption Cross Sections

    NASA Astrophysics Data System (ADS)

    DeArmond, Fredrick Michael

    As optical microscopy techniques continue to improve, most notably the development of super-resolution optical microscopy which garnered the Nobel Prize in Chemistry in 2014, renewed emphasis has been placed on the development and use of fluorescence microscopy techniques. Of particular note is a renewed interest in multiphoton excitation due to a number of inherent properties of the technique including simplified optical filtering, increased sample penetration, and inherently confocal operation. With this renewed interest in multiphoton fluorescence microscopy, comes an increased demand for robust non-linear fluorescent markers, and characterization of the associated tool set. These factors have led to an experimental setup to allow a systematized approach for identifying and characterizing properties of fluorescent probes in the hopes that the tool set will provide researchers with additional information to guide their efforts in developing novel fluorophores suitable for use in advanced optical microscopy techniques as well as identifying trends for their synthesis. Hardware was setup around a software control system previously developed. Three experimental tool sets were set up, characterized, and applied over the course of this work. These tools include scanning multiphoton fluorescence microscope with single molecule sensitivity, an interferometric autocorrelator for precise determination of the bandwidth and pulse width of the ultrafast Titanium Sapphire excitation source, and a simplified fluorescence microscope for the measurement of two-photon absorption cross sections. Resulting values for two-photon absorption cross sections and two-photon absorption action cross sections for two standardized fluorophores, four commercially available fluorophores, and ten novel fluorophores are presented as well as absorption and emission spectra.

  9. High resolution multiple excitation spot optical microscopy

    NASA Astrophysics Data System (ADS)

    Dilipkumar, Shilpa; Mondal, Partha Pratim

    2011-06-01

    We propose fundamental improvements in three-dimensional (3D) resolution of multiple excitation spot optical microscopy. The excitation point spread function (PSF) is generated by two interfering counter-propagating depth-of-focus beams along the optical axis. Detection PSF is obtained by coherently interfering the emitted fluorescent light (collected by both the objectives) at the detector. System PSF shows upto 14-fold reduction in focal volume as compared to confocal, and almost 2-fold improvement in lateral resolution. Proposed PSF has the ability to simultaneously excite multiple 3D-spots of sub-femtoliter volume. Potential applications are in fluorescence microscopy and nanobioimaging.

  10. Three-photon-excited luminescence from unsymmetrical cyanostilbene aggregates: morphology tuning and targeted bioimaging.

    PubMed

    Mandal, Amal Kumar; Sreejith, Sivaramapanicker; He, Tingchao; Maji, Swarup Kumar; Wang, Xiao-Jun; Ong, Shi Li; Joseph, James; Sun, Handong; Zhao, Yanli

    2015-05-26

    We report an experimental observation of aggregation-induced enhanced luminescence upon three-photon excitation in aggregates formed from a class of unsymmetrical cyanostilbene derivatives. Changing side chains (-CH3, -C6H13, -C7H15O3, and folic acid) attached to the cyanostilbene core leads to instantaneous formation of aggregates with sizes ranging from micrometer to nanometer scale in aqueous conditions. The crystal structure of a derivative with a methyl side chain reveals the planarization in the unsymmetrical cyanostilbene core, causing luminescence from corresponding aggregates upon three-photon excitation. Furthermore, folic acid attached cyanostilbene forms well-dispersed spherical nanoaggregates that show a high three-photon cross-section of 6.0 × 10(-80) cm(6) s(2) photon(-2) and high luminescence quantum yield in water. In order to demonstrate the targeted bioimaging capability of the nanoaggregates, three cell lines (HEK293 healthy cell line, MCF7 cancerous cell line, and HeLa cancerous cell line) were employed for the investigations on the basis of their different folate receptor expression level. Two kinds of nanoaggregates with and without the folic acid targeting ligand were chosen for three-photon bioimaging studies. The cell viability of three types of cells incubated with high concentration of nanoaggregates still remained above 70% after 24 h. It was observed that the nanoaggregates without the folic acid unit could not undergo the endocytosis by both healthy and cancerous cell lines. No obvious endocytosis of folic acid attached nanoaggregates was observed from the HEK293 and MCF7 cell lines having a low expression of the folate receptor. Interestingly, a significant amount of endocytosis and internalization of folic acid attached nanoaggregates was observed from HeLa cells with a high expression of the folate receptor under three-photon excitation, indicating targeted bioimaging of folic acid attached nanoaggregates to the cancer cell line

  11. Magnetic Excitations across the Metal-Insulator Transition in the Pyrochlore Iridate Eu2Ir2O7

    NASA Astrophysics Data System (ADS)

    Chun, Sae Hwan; Yuan, Bo; Casa, Diego; Kim, Jungho; Kim, Chang-Yong; Tian, Zhaoming; Qiu, Yang; Nakatsuji, Satoru; Kim, Young-June

    2018-04-01

    We report a resonant inelastic x-ray scattering study of the magnetic excitation spectrum in a highly insulating Eu2 Ir2 O7 single crystal that exhibits a metal-insulator transition at TMI=111 (7 ) K . A propagating magnon mode with a 20 meV bandwidth and a 28 meV magnon gap is found in the excitation spectrum at 7 K, which is expected in the all-in-all-out magnetically ordered state. This magnetic excitation exhibits substantial softening as the temperature is raised towards TMI and turns into a highly damped excitation in the paramagnetic phase. Remarkably, the softening occurs throughout the whole Brillouin zone including the zone boundary. This observation is inconsistent with the magnon renormalization expected in a local moment system and indicates that the strength of the electron correlation in Eu2 Ir2 O7 is only moderate, so that electron itinerancy should be taken into account in describing its magnetism.

  12. Mid-IR Plasmonics, Cavity Coupled Excitations, and IR Spectra of Individual Airborne Particulate Matter

    NASA Astrophysics Data System (ADS)

    Luthra, Antriksh

    With the advances in plasmonics, new fields have evolved involving the mixing of light with various states like Surface Plasmons (SPs), Surface Phonons (SPh), molecular emitters or resonators, and wavelength scale cavities. This work concentrates on the interaction of infrared (IR) light with SPs, cavity modes, and molecular vibrations. In the first chapter, the field of Plasmonics is introduced from a classical and a quantum mechanical perspective and a comparison of both is presented. In Chapter 2, the interaction of cavity modes with vibrations is discussed. Briefly, when IR light is illuminated upon an etalon, its fringes disperse as function of angle. If there is a dielectric in a cavity having a vibrational transition in the fringe region, it leads to a strong interaction that gives rise to a Rabi splitting. Data was obtained from collaborators at the U.S. Naval Research Laboratory (NRL) and a derivation for the dispersion of etalon cavity modes was carried out to model the peak positions of the fringes. In Chapter 3, the excitation of Surface Plasmons Polaritons (SPPs) on metal bi-gratings is discussed. The resonance condition occurs when the momentum of the IR light parallel to the surface plus the grating vector match the momentum of the SPP. Experiments were performed in the GammaX space (ky=0) and the resonance peak positions were modeled with SPP momentum matching equations. In Chapter 4, the application of plasmonics in the mid-IR frequency range that overlaps with the frequencies of molecular vibrations is explored. The plasmonic mesh has interesting optical properties, it focuses more light in the holes and that leads to an enhancement of the IR spectra of a particle trapped in the mesh hole. In this work, plasmonic mesh is used to study airborne particles that are usually difficult to study using FTIR spectroscopy due to strong Mie scattering effect. Respiring dust particles of 4 microns size has significant negative health consequences. Different

  13. Photonic crystal fiber modal interferometer based on thin-core-fiber mode exciter.

    PubMed

    Miao, Yinping; Ma, Xixi; Wu, Jixuan; Song, Binbin; Zhang, Hao; Liu, Bo; Yao, Jianquan

    2015-11-10

    A thin-core-fiber excited photonic crystal fiber modal interferometer has been proposed and experimentally demonstrated. By employing a thin-core fiber as the mode exciter, both of the core and cladding modes propagate in the photonic crystal fiber and interfere with each other. The experimental results show that the transmission dips corresponding to different-order modes have various strain responses with opposite shift directions. The strain sensitivity could be improved to 58.57  pm/με for the applied strain from 0 to 491 με by utilizing the wavelength interval between the dips with opposite shift directions. Moreover, due to the pure silica property of the employed photonic crystal fiber, the proposed fiber modal interferometer exhibits a low-temperature sensitivity of about 0.56  pm/°C within a temperature range from 26.4°C (room temperature) to 70°C. Additionally, the proposed fiber modal interferometer has several advantages, such as good stability, compact structure, and simple fabrication. Therefore, it is more applicable for strain measurement with reducing temperature cross-sensitivity.

  14. Competition between second harmonic generation and two-photon-induced luminescence in single, double and multiple ZnO nanorods.

    PubMed

    Dai, Jun; Zeng, Jian-Hua; Lan, Sheng; Wan, Xia; Tie, Shao-Long

    2013-04-22

    The nonlinear optical properties of single, double and multiple ZnO nanorods (NRs) were investigated by using a focused femtosecond (fs) laser beam. The excitation wavelength of the fs laser was intentionally chosen to be 754 nm at which the energy of two photons is slightly larger than that of the exciton ground state but smaller than the bandgap energy of ZnO. Second harmonic generation (SHG) or/and two-photon-induced luminescence (TPL) were observed and their dependences on excitation density were examined. For single ZnO NRs, only SHG was observed even at the highest excitation density we used in the experiments. The situation was changed when the joint point of two ZnO NRs perpendicular to each other was excited. In this case, TPL could be detected at low excitation densities and it increased rapidly with increasing excitation density. At the highest excitation density of ~15 MW/cm(2), the intensity of the TPL became comparable to that of the SHG. For an ensemble of ZnO NRs packed closely, a rapid increase of TPL with a slope of more than 7.0 and a gradual saturation of SHG with a slope of ~0.34 were found at high excitation densities. Consequently, the nonlinear response spectrum was eventually dominated by the TPL at high excitation densities and the SHG appeared to be very weak. We interpret this phenomenon by considering both the difference in electric field distribution and the effect of heat accumulation. It is suggested that the electric field enhancement in double and multiple NRs plays a crucial role in determining the nonlinear response of the NRs. In addition, the reduction in the bandgap energy induced by the heat accumulation effect also leads to the significant change in nonlinear response. This explanation is supported by the calculation of the electric field distribution using the discrete dipole approximation method and the simulation of temperature rise in different ZnO NRs based on the finite element method.

  15. Multicolor fluorescence enhancement from a photonics crystal surface

    NASA Astrophysics Data System (ADS)

    Pokhriyal, A.; Lu, M.; Huang, C. S.; Schulz, S.; Cunningham, B. T.

    2010-09-01

    A photonic crystal substrate exhibiting resonant enhancement of multiple fluorophores has been demonstrated. The device, fabricated uniformly from plastic materials over a ˜3×5 in.2 surface area by nanoreplica molding, utilizes two distinct resonant modes to enhance electric field stimulation of a dye excited by a λ =632.8 nm laser (cyanine-5) and a dye excited by a λ =532 nm laser (cyanine-3). Resonant coupling of the laser excitation to the photonic crystal surface is obtained for each wavelength at a distinct incident angle. Compared to detection of a dye-labeled protein on an ordinary glass surface, the photonic crystal surface exhibited a 32× increase in fluorescent signal intensity for cyanine-5 conjugated streptavidin labeling, while a 25× increase was obtained for cyanine-3 conjugated streptavidin labeling. The photonic crystal is capable of amplifying the output of any fluorescent dye with an excitation wavelength in the 532 nm<λ<633 nm range by selection of an appropriate incident angle. The device is designed for biological assays that utilize multiple fluorescent dyes within a single imaged area, such as gene expression microarrays.

  16. Multicolor fluorescence enhancement from a photonics crystal surface

    PubMed Central

    Pokhriyal, A.; Lu, M.; Huang, C. S.; Schulz, S.; Cunningham, B. T.

    2010-01-01

    A photonic crystal substrate exhibiting resonant enhancement of multiple fluorophores has been demonstrated. The device, fabricated uniformly from plastic materials over a ∼3×5 in.2 surface area by nanoreplica molding, utilizes two distinct resonant modes to enhance electric field stimulation of a dye excited by a λ=632.8 nm laser (cyanine-5) and a dye excited by a λ=532 nm laser (cyanine-3). Resonant coupling of the laser excitation to the photonic crystal surface is obtained for each wavelength at a distinct incident angle. Compared to detection of a dye-labeled protein on an ordinary glass surface, the photonic crystal surface exhibited a 32× increase in fluorescent signal intensity for cyanine-5 conjugated streptavidin labeling, while a 25× increase was obtained for cyanine-3 conjugated streptavidin labeling. The photonic crystal is capable of amplifying the output of any fluorescent dye with an excitation wavelength in the 532 nm<λ<633 nm range by selection of an appropriate incident angle. The device is designed for biological assays that utilize multiple fluorescent dyes within a single imaged area, such as gene expression microarrays. PMID:20957067

  17. Two-photon excitation of porphyrin-functionalized porous silicon nanoparticles for photodynamic therapy.

    PubMed

    Secret, Emilie; Maynadier, Marie; Gallud, Audrey; Chaix, Arnaud; Bouffard, Elise; Gary-Bobo, Magali; Marcotte, Nathalie; Mongin, Olivier; El Cheikh, Khaled; Hugues, Vincent; Auffan, Mélanie; Frochot, Céline; Morère, Alain; Maillard, Philippe; Blanchard-Desce, Mireille; Sailor, Michael J; Garcia, Marcel; Durand, Jean-Olivier; Cunin, Frédérique

    2014-12-03

    Porous silicon nanoparticles (pSiNPs) act as a sensitizer for the 2-photon excitation of a pendant porphyrin using NIR laser light, for imaging and photodynamic therapy. Mannose-functionalized pSiNPs can be vectorized to MCF-7 human breast cancer cells through a mannose receptor-mediated endocytosis mechanism to provide a 3-fold enhancement of the 2-photon PDT effect. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  18. Polarized fluorescence in NADH under two-photon excitation with femtosecond laser pulses

    NASA Astrophysics Data System (ADS)

    Vasyutinskii, O. S.; Smolin, A. G.; Oswald, C.; Gericke, K. H.

    2017-04-01

    Polarized fluorescence decay in NADH molecules in aqueous solution under two-photon excitation by femtosecond laser pulses has been studied. The excitation was carried out by linear and circularly polarized radiation at four wavelengths: 720, 730, 740, and 750 nm. Time-dependent polarized fluorescence signals were recorded as a function of the excitation light polarization and used for determination of a set of molecular parameters, two lifetimes characterizing the molecular excited states, and the rotation correlation time τrot. The results obtained can be used to create and prove theoretical models describing the intensity and polarization of fluorescence in NADH involved in the regulation of the redox reactions in cells and tissues of living organisms.

  19. Ge-rich graded-index Si1-xGex devices for MID-IR integrated photonics

    NASA Astrophysics Data System (ADS)

    Ramirez, J. M.; Vakarin, V.; Liu, Q.; Frigerio, J.; Ballabio, A.; Le Roux, X.; Benedikovic, D.; Alonso-Ramos, C.; Isella, G.; Vivien, L.; Marris-Morini, D.

    2018-02-01

    Mid-infrared (mid-IR) silicon photonics is becoming a prominent research with remarkable potential in several applications such as in early medical diagnosis, safe communications, imaging, food safety and many more. In the quest for the best material platform to develop new photonic systems, Si and Ge depart with a notable advantage over other materials due to the high processing maturity accomplished during the last part of the 20th century through the deployment of the CMOS technology. From an optical viewpoint, combining Si with Ge to obtain SiGe alloys with controlled stoichiometry is also of interest for the photonic community since permits to increase the effective refractive index and the nonlinear parameter, providing a fascinating playground to exploit nonlinear effects. Furthermore, using Ge-rich SiGe gives access to a range of deep mid-IR wavelengths otherwise inaccessible (λ 2-20 μm). In this paper, we explore for the first time the limits of this approach by measuring the spectral loss characteristic over a broadband wavelength range spanning from λ = 5.5 μm to 8.5 μm. Three different SiGe waveguide platforms are compared, each one showing higher compactness than the preceding through the engineering of the vertical Ge profile, giving rise to different confinement characteristics to the propagating modes. A flat propagation loss characteristic of 2-3 dB/cm over the entire wavelength span is demonstrated in Ge-rich graded-index SiGe waveguides of only 6 μm thick. Also, the role of the overlap fraction of the confined optical mode with the Si-rich area at the bottom side of the epitaxial SiGe waveguide is put in perspective, revealing a lossy characteristic compared to the other designs were the optical mode is located in the Ge-rich area at the top of the waveguide uniquely. These Ge-rich graded-index SiGe waveguides may pave the way towards a new generation of photonic integrated circuits operating at deep mid-IR wavelengths.

  20. Two-photon microscopy using fiber-based nanosecond excitation.

    PubMed

    Karpf, Sebastian; Eibl, Matthias; Sauer, Benjamin; Reinholz, Fred; Hüttmann, Gereon; Huber, Robert

    2016-07-01

    Two-photon excitation fluorescence (TPEF) microscopy is a powerful technique for sensitive tissue imaging at depths of up to 1000 micrometers. However, due to the shallow penetration, for in vivo imaging of internal organs in patients beam delivery by an endoscope is crucial. Until today, this is hindered by linear and non-linear pulse broadening of the femtosecond pulses in the optical fibers of the endoscopes. Here we present an endoscope-ready, fiber-based TPEF microscope, using nanosecond pulses at low repetition rates instead of femtosecond pulses. These nanosecond pulses lack most of the problems connected with femtosecond pulses but are equally suited for TPEF imaging. We derive and demonstrate that at given cw-power the TPEF signal only depends on the duty cycle of the laser source. Due to the higher pulse energy at the same peak power we can also demonstrate single shot two-photon fluorescence lifetime measurements.

  1. Adapting a compact confocal microscope system to a two-photon excitation fluorescence imaging architecture.

    PubMed

    Diaspro, A; Corosu, M; Ramoino, P; Robello, M

    1999-11-01

    Within the framework of a national National Institute of Physics of Matter (INFM) project, we have realised a two-photon excitation (TPE) fluorescence microscope based on a new generation commercial confocal scanning head. The core of the architecture is a mode-locked Ti:Sapphire laser (Tsunami 3960, Spectra Physics Inc., Mountain View, CA) pumped by a high-power (5 W, 532 nm) laser (Millennia V, Spectra Physics Inc.) and an ultracompact confocal scanning head, Nikon PCM2000 (Nikon Instruments, Florence, Italy) using a single-pinhole design. Three-dimensional point-spread function has been measured to define spatial resolution performances. The TPE microscope has been used with a wide range of excitable fluorescent molecules (DAPI, Fura-2, Indo-1, DiOC(6)(3), fluoresceine, Texas red) covering a single photon spectral range from UV to green. An example is reported on 3D imaging of the helical structure of the sperm head of the Octopus Eledone cirrhosa labelled with an UV excitable dye, i.e., DAPI. The system can be easily switched for operating both in conventional and two-photon mode. Copyright 1999 Wiley-Liss, Inc.

  2. LETTER TO THE EDITOR: Green emission and bandgap narrowing due to two-photon excitation in thin film CdS formed by spray pyrolysis

    NASA Astrophysics Data System (ADS)

    Ullrich, B.; Schroeder, R.

    2001-08-01

    Thin (10 µm) film CdS on Pyrex® formed by spray pyrolysis is excited below the gap at 804 nm with 200 fs laser pulses at room temperature. Excitation intensities up to 250 GW cm-2 evoke green bandgap emission due to two-photon transitions. This two-photon photoluminescence does not show a red emission contribution in contrast to the single-photon excited emission, which is dominated by broad emission in the red spectral range. It is demonstrated that two-photon excitation causes photo-induced bandgap narrowing due to Debye screening. At 250 GW cm-2 bandgap narrowing of 47 meV is observed, which corresponds to an excited electron density of 1.6×1018 cm-3.

  3. Concept for polychromatic laser guide stars: one-photon excitation of the 4P3/2 level of a sodium atom.

    PubMed

    Pique, Jean-Paul; Moldovan, Ioana Cristina; Fesquet, Vincent

    2006-11-01

    One challenge for polychromatic laser guide stars is to create a sufficiently intense source in the UV. The flux required for the measurement of differential tip-tilt is the main issue that we address. We describe a model that has been validated using on-sky data. We present a method that excites the 4P3/2 sodium level using a one-photon excitation at 330 nm. It is more efficient than the two-photon excitation previously suggested since its power slope flux is 3 x 10(4) photons/s/m2/W instead of 1.3 x 10(3) photons/s/m2/W. This method is very promising both in terms of flux and system simplicity.

  4. Memory-assisted quantum key distribution resilient against multiple-excitation effects

    NASA Astrophysics Data System (ADS)

    Lo Piparo, Nicolò; Sinclair, Neil; Razavi, Mohsen

    2018-01-01

    Memory-assisted measurement-device-independent quantum key distribution (MA-MDI-QKD) has recently been proposed as a technique to improve the rate-versus-distance behavior of QKD systems by using existing, or nearly-achievable, quantum technologies. The promise is that MA-MDI-QKD would require less demanding quantum memories than the ones needed for probabilistic quantum repeaters. Nevertheless, early investigations suggest that, in order to beat the conventional memory-less QKD schemes, the quantum memories used in the MA-MDI-QKD protocols must have high bandwidth-storage products and short interaction times. Among different types of quantum memories, ensemble-based memories offer some of the required specifications, but they typically suffer from multiple excitation effects. To avoid the latter issue, in this paper, we propose two new variants of MA-MDI-QKD both relying on single-photon sources for entangling purposes. One is based on known techniques for entanglement distribution in quantum repeaters. This scheme turns out to offer no advantage even if one uses ideal single-photon sources. By finding the root cause of the problem, we then propose another setup, which can outperform single memory-less setups even if we allow for some imperfections in our single-photon sources. For such a scheme, we compare the key rate for different types of ensemble-based memories and show that certain classes of atomic ensembles can improve the rate-versus-distance behavior.

  5. Micromanipulation and physiological monitoring of cells using two-photon excited fluorescence in cw laser tweezers

    NASA Astrophysics Data System (ADS)

    Sonek, Gregory J.; Liu, Yagang; Berns, Michael W.; Tromberg, Bruce J.

    1996-05-01

    We report the observation of two-photon fluorescence excitation and cell confinement, simultaneously, in a continuous-wave (cw) single-beam gradient force optical trap, and demonstrate its use as an in-situ probe to study the physiological state of an optically confined cell sample. At the wavelength of 1064 nm, a single focused gaussian laser beam is used to simultaneously confine, and excite visible fluorescence from, a human sperm cell that has been tagged with propidium iodide, a exogenous fluorescent dye that functions as a viability assay of cellular physiological state. The intensity at the dye peak emission wavelength of 620 nm exhibits a near-square-law dependence on incident trapping beam photon laser power, a behavior consistent with a two-photon absorption process. In addition, for a sperm cell held stationary in the optical tweezers for a period of several minutes at a constant trapping power, red fluorescence emission was observed to increase the time, indicating that the cell has gradually transitioned between a live and dead state. Two-photon excited fluorescence was also observed in chinese hamster ovary cells that were confined by cw laser tweezers and stained with either propidium iodide or Snarf, a pH-sensitive dye probe. These results suggest that, for samples suitably tagged with fluorescent probes and vital stains, optical tweezers can be used to generate their own in-situ diagnostic optical probes of cellular viability or induced photodamage, via two-photon processes.

  6. Broadband transient absorption spectroscopy with 1- and 2-photon excitations: Relaxation paths and cross sections of a triphenylamine dye in solution

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

    Moreno, J.; Dobryakov, A. L.; Hecht, S., E-mail: sh@chemie.hu-berlin.de, E-mail: skovale@chemie.hu-berlin.de

    2015-07-14

    1-photon (382 nm) and 2-photon (752 nm) excitations to the S{sub 1} state are applied to record and compare transient absorption spectra of a push-pull triphenylamine (TrP) dye in solution. After 1-photon excitation, ultrafast vibrational and structural molecular relaxations are detected on a 0.1 ps time scale in nonpolar hexane, while in polar acetonitrile, the spectral evolution is dominated by dipolar solvation. Upon 2-photon excitation, transient spectra in hexane reveal an unexpected growth of stimulated emission (SE) and excited-state absorption (ESA) bands. The behavior is explained by strong population transfer S{sub 1} → S{sub n} due to resonant absorption ofmore » a third pump photon. Subsequent S{sub n} → S{sub 1} internal conversion (with τ{sub 1} = 1 ps) prepares a very hot S{sub 1} state which cools down with τ{sub 2} = 13 ps. The pump pulse energy dependence proves the 2-photon origin of the bleach signal. At the same time, SE and ESA are strongly affected by higher-order pump absorptions that should be taken into account in nonlinear fluorescence applications. The 2-photon excitation cross sections σ{sup (2)} = 32 ⋅ 10{sup −50} cm{sup 4} s at 752 nm are evaluated from the bleach signal.« less

  7. One-dimensional photonic crystals for eliminating cross-talk in mid-IR photonics-based respiratory gas sensing

    NASA Astrophysics Data System (ADS)

    Fleming, L.; Gibson, D.; Song, S.; Hutson, D.; Reid, S.; MacGregor, C.; Clark, C.

    2017-02-01

    Mid-IR carbon dioxide (CO2) gas sensing is critical for monitoring in respiratory care, and is finding increasing importance in surgical anaesthetics where nitrous oxide (N2O) induced cross-talk is a major obstacle to accurate CO2 monitoring. In this work, a novel, solid state mid-IR photonics based CO2 gas sensor is described, and the role that 1- dimensional photonic crystals, often referred to as multilayer thin film optical coatings [1], play in boosting the sensor's capability of gas discrimination is discussed. Filter performance in isolating CO2 IR absorption is tested on an optical filter test bed and a theoretical gas sensor model is developed, with the inclusion of a modelled multilayer optical filter to analyse the efficacy of optical filtering on eliminating N2O induced cross-talk for this particular gas sensor architecture. Future possible in-house optical filter fabrication techniques are discussed. As the actual gas sensor configuration is small, it would be challenging to manufacture a filter of the correct size; dismantling the sensor and mounting a new filter for different optical coating designs each time would prove to be laborious. For this reason, an optical filter testbed set-up is described and, using a commercial optical filter, it is demonstrated that cross-talk can be considerably reduced; cross-talk is minimal even for very high concentrations of N2O, which are unlikely to be encountered in exhaled surgical anaesthetic patient breath profiles. A completely new and versatile system for breath emulation is described and the capability it has for producing realistic human exhaled CO2 vs. time waveforms is shown. The cross-talk inducing effect that N2O has on realistic emulated CO2 vs. time waveforms as measured using the NDIR gas sensing technique is demonstrated and the effect that optical filtering will have on said cross-talk is discussed.

  8. Multiple-Event, Single-Photon Counting Imaging Sensor

    NASA Technical Reports Server (NTRS)

    Zheng, Xinyu; Cunningham, Thomas J.; Sun, Chao; Wang, Kang L.

    2011-01-01

    The single-photon counting imaging sensor is typically an array of silicon Geiger-mode avalanche photodiodes that are monolithically integrated with CMOS (complementary metal oxide semiconductor) readout, signal processing, and addressing circuits located in each pixel and the peripheral area of the chip. The major problem is its single-event method for photon count number registration. A single-event single-photon counting imaging array only allows registration of up to one photon count in each of its pixels during a frame time, i.e., the interval between two successive pixel reset operations. Since the frame time can t be too short, this will lead to very low dynamic range and make the sensor merely useful for very low flux environments. The second problem of the prior technique is a limited fill factor resulting from consumption of chip area by the monolithically integrated CMOS readout in pixels. The resulting low photon collection efficiency will substantially ruin any benefit gained from the very sensitive single-photon counting detection. The single-photon counting imaging sensor developed in this work has a novel multiple-event architecture, which allows each of its pixels to register as more than one million (or more) photon-counting events during a frame time. Because of a consequently boosted dynamic range, the imaging array of the invention is capable of performing single-photon counting under ultra-low light through high-flux environments. On the other hand, since the multiple-event architecture is implemented in a hybrid structure, back-illumination and close-to-unity fill factor can be realized, and maximized quantum efficiency can also be achieved in the detector array.

  9. Video-rate scanning two-photon excitation fluorescence microscopy and ratio imaging with cameleons.

    PubMed Central

    Fan, G Y; Fujisaki, H; Miyawaki, A; Tsay, R K; Tsien, R Y; Ellisman, M H

    1999-01-01

    A video-rate (30 frames/s) scanning two-photon excitation microscope has been successfully tested. The microscope, based on a Nikon RCM 8000, incorporates a femtosecond pulsed laser with wavelength tunable from 690 to 1050 nm, prechirper optics for laser pulse-width compression, resonant galvanometer for video-rate point scanning, and a pair of nonconfocal detectors for fast emission ratioing. An increase in fluorescent emission of 1.75-fold is consistently obtained with the use of the prechirper optics. The nonconfocal detectors provide another 2.25-fold increase in detection efficiency. Ratio imaging and optical sectioning can therefore be performed more efficiently without confocal optics. Faster frame rates, at 60, 120, and 240 frames/s, can be achieved with proportionally reduced scan lines per frame. Useful two-photon images can be acquired at video rate with a laser power as low as 2.7 mW at specimen with the genetically modified green fluorescent proteins. Preliminary results obtained using this system confirm that the yellow "cameleons" exhibit similar optical properties as under one-photon excitation conditions. Dynamic two-photon images of cardiac myocytes and ratio images of yellow cameleon-2.1, -3.1, and -3.1nu are also presented. PMID:10233058

  10. Constraining nuclear photon strength functions by the decay properties of photo-excited states

    NASA Astrophysics Data System (ADS)

    Isaak, J.; Savran, D.; Krtička, M.; Ahmed, M. W.; Beller, J.; Fiori, E.; Glorius, J.; Kelley, J. H.; Löher, B.; Pietralla, N.; Romig, C.; Rusev, G.; Scheck, M.; Schnorrenberger, L.; Silva, J.; Sonnabend, K.; Tonchev, A. P.; Tornow, W.; Weller, H. R.; Zweidinger, M.

    2013-12-01

    A new approach for constraining the low-energy part of the electric dipole Photon Strength Function (E1-PSF) is presented. Experiments at the Darmstadt High-Intensity Photon Setup and the High Intensity γ→-Ray Source have been performed to investigate the decay properties of 130Te between 5.50 and 8.15 MeV excitation energy. In particular, the average γ-ray branching ratio to the ground state and the population intensity of low-lying excited states have been studied. A comparison to the statistical model shows that the latter is sensitive to the low-energy behavior of the E1-PSF, while the average ground state branching ratio cannot be described by the statistical model in the energy range between 5.5 and 6.5 MeV.

  11. Two-Photon Flow Cytometry

    NASA Technical Reports Server (NTRS)

    Zhog, Cheng Frank; Ye, Jing Yong; Norris, Theodore B.; Myc, Andrzej; Cao, Zhengyl; Bielinska, Anna; Thomas, Thommey; Baker, James R., Jr.

    2004-01-01

    Flow cytometry is a powerful technique for obtaining quantitative information from fluorescence in cells. Quantitation is achieved by assuring a high degree of uniformity in the optical excitation and detection, generally by using a highly controlled flow such as is obtained via hydrodynamic focusing. In this work, we demonstrate a two-beam, two- channel detection and two-photon excitation flow cytometry (T(sup 3)FC) system that enables multi-dye analysis to be performed very simply, with greatly relaxed requirements on the fluid flow. Two-photon excitation using a femtosecond near-infrared (NIR) laser has the advantages that it enables simultaneous excitation of multiple dyes and achieves very high signal-to-noise ratio through simplified filtering and fluorescence background reduction. By matching the excitation volume to the size of a cell, single-cell detection is ensured. Labeling of cells by targeted nanoparticles with multiple fluorophores enables normalization of the fluorescence signal and thus ratiometric measurements under nonuniform excitation. Quantitative size measurements can also be done even under conditions of nonuniform flow via a two-beam layout. This innovative detection scheme not only considerably simplifies the fluid flow system and the excitation and collection optics, it opens the way to quantitative cytometry in simple and compact microfluidics systems, or in vivo. Real-time detection of fluorescent microbeads in the vasculature of mouse ear demonstrates the ability to do flow cytometry in vivo. The conditions required to perform quantitative in vivo cytometry on labeled cells will be presented.

  12. Monte Carlo wave-packet approach to trace nuclear dynamics in molecular excited states by XUV-pump-IR-probe spectroscopy

    NASA Astrophysics Data System (ADS)

    Jing, Qingli; Bello, Roger Y.; Martín, Fernando; Palacios, Alicia; Madsen, Lars Bojer

    2018-04-01

    Recent research interests have been raised in uncovering and controlling ultrafast dynamics in excited neutral molecules. In this work we generalize the Monte Carlo wave packet (MCWP) approach to XUV-pump-IR-probe schemes to simulate the process of dissociative double ionization of H2 where singly excited states in H2 are involved. The XUV pulse is chosen to resonantly excite the initial ground state of H2 to the lowest excited electronic state of 1Σu + symmetry in H2 within the Franck-Condon region. The delayed intense IR pulse couples the excited states of 1Σu + symmetry with the nearby excited states of 1Σg + symmetry. It also induces the first ionization from H2 to H2 + and the second ionization from H2 + to H++H+. To reduce the computational costs in the MCWP approach, a sampling method is proposed to determine in time the dominant ionization events from H2 to H2+. By conducting a trajectory analysis, which is a unique possibility within the MCWP approach, the origins of the characteristic features in the nuclear kinetic energy release spectra are identified for delays ranging from 0 to 140 fs and the nuclear dynamics in the singly excited states in H2 is mapped out.

  13. Brominated 7-hydroxycoumarin-4-ylmethyls: Photolabile protecting groups with biologically useful cross-sections for two photon photolysis

    PubMed Central

    Furuta, Toshiaki; Wang, Samuel S.-H.; Dantzker, Jami L.; Dore, Timothy M.; Bybee, Wendy J.; Callaway, Edward M.; Denk, Winfried; Tsien, Roger Y.

    1999-01-01

    Photochemical release (uncaging) of bioactive messengers with three-dimensional spatial resolution in light-scattering media would be greatly facilitated if the photolysis could be powered by pairs of IR photons rather than the customary single UV photons. The quadratic dependence on light intensity would confine the photolysis to the focus point of the laser, and the longer wavelengths would be much less affected by scattering. However, previous caged messengers have had very small cross sections for two-photon excitation in the IR region. We now show that brominated 7-hydroxycoumarin-4-ylmethyl esters and carbamates efficiently release carboxylates and amines on photolysis, with one- and two-photon cross sections up to one or two orders of magnitude better than previously available. These advantages are demonstrated on neurons in brain slices from rat cortex and hippocampus excited by glutamate uncaged from N-(6-bromo-7-hydroxycoumarin-4-ylmethoxycarbonyl)-l-glutamate (Bhc-glu). Conventional UV photolysis of Bhc-glu requires less than one-fifth the intensities needed by one of the best previous caged glutamates, γ-(α-carboxy-2-nitrobenzyl)-l-glutamate (CNB-glu). Two-photon photolysis with raster-scanned femtosecond IR pulses gives the first three-dimensionally resolved maps of the glutamate sensitivity of neurons in intact slices. Bhc-glu and analogs should allow more efficient and three-dimensionally localized uncaging and photocleavage, not only in cell biology and neurobiology but also in many technological applications. PMID:9990000

  14. Infrared (IR) photon-sensitive spectromicroscopy in a cryogenic environment

    DOEpatents

    Pereverzev, Sergey

    2016-06-14

    A system designed to suppress thermal radiation background and to allow IR single-photon sensitive spectromicroscopy of small samples by using both absorption, reflection, and emission/luminescence measurements. The system in one embodiment includes: a light source; a plurality of cold mirrors configured to direct light along a beam path; a cold or warm sample holder in the beam path; windows of sample holder (or whole sample holder) are transparent in a spectral region of interest, so they do not emit thermal radiation in the same spectral region of interest; a cold monochromator or other cold spectral device configured to direct a selected fraction of light onto a cold detector; a system of cold apertures and shields positioned along the beam path to prevent unwanted thermal radiation from arriving at the cold monochromator and/or the detector; a plurality of optical, IR and microwave filters positioned along the beam path and configured to adjust a spectral composition of light incident upon the sample under investigation and/or on the detector; a refrigerator configured to maintain the detector at a temperature below 1.0K; and an enclosure configured to: thermally insulate the light source, the plurality of mirrors, the sample holder, the cold monochromator and the refrigerator.

  15. Ultrafast coherent excitation of a trapped ion qubit for fast gates and photon frequency qubits.

    PubMed

    Madsen, M J; Moehring, D L; Maunz, P; Kohn, R N; Duan, L-M; Monroe, C

    2006-07-28

    We demonstrate ultrafast coherent excitation of an atomic qubit stored in the hyperfine levels of a single trapped cadmium ion. Such ultrafast excitation is crucial for entangling networks of remotely located trapped ions through the interference of photon frequency qubits, and is also a key component for realizing ultrafast quantum gates between Coulomb-coupled ions.

  16. Ligand-core NLO-phores: a combined experimental and theoretical approach to the two-photon absorption and two-photon excited emission properties of small-ligated silver nanoclusters.

    PubMed

    Russier-Antoine, Isabelle; Bertorelle, Franck; Calin, Nathalie; Sanader, Željka; Krstić, Marjan; Comby-Zerbino, Clothilde; Dugourd, Philippe; Brevet, Pierre-François; Bonačić-Koutecký, Vlasta; Antoine, Rodolphe

    2017-01-19

    We report a combined experimental and theoretical study of the two-photon absorption and excited emission properties of monodisperse ligand stabilized Ag 11 , Ag 15 and Ag 31 nanoclusters in aqueous solutions. The nanoclusters were synthesized using a cyclic reduction under oxidative conditions and separated by vertical gel electrophoresis. The two-photon absorption cross-sections of these protected noble metal nanoclusters measured within the biologically attractive 750-900 nm window are several orders of magnitude larger than that reported for commercially available standard organic dyes. The two-photon excited fluorescence spectra are also presented for excitation wavelengths within the same excitation spectral window. They exhibit size-tunability. Because the fundamental photophysical mechanisms underlying these multiphoton processes in ligand protected clusters with only a few metal atoms are not fully understood yet, a theoretical model is proposed to identify the key driving elements. Elements that regulate the dipole moments and the nonlinear optical properties are the nanocluster size, its structure and the charge distribution on both the metal core and the bound ligands. We coined this new class of NLO materials as "Ligand-Core" NLO-phores.

  17. Two-Photon Study on the Electronic Interactions between the First Excited Singlet States in Carotenoid-Tetrapyrrole Dyads

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

    Liao, Pen-Nan; Pillai, Smitha; Gust, Devens

    Electronic interactions between the first excited states (S 1) of carotenoids (Car) of different conjugation lengths (8-11 double bonds) and phthalocyanines (Pc) in different Car-Pc dyad molecules were investigated by two-photon spectroscopy and compared with Car S 1-chlorophyll (Chl) interactions in photosynthetic light harvesting complexes (LHCs). The observation of Chl/Pc fluorescence after selective two-photon excitation of the Car S 1 state allowed sensitive monitoring of the flow of energy between Car S 1 and Pc or Chl. It is found that two-photon excitation excites to about 80% to 100% exclusively the carotenoid state Car S 1 and that only amore » small fraction of direct tetrapyrrole two-photon excitation occurs. Amide-linked Car-Pc dyads in tetrahydrofuran demonstrate a molecular gear shift mechanism in that effective Car S 1 → Pc energy transfer is observed in a dyad with 9 double bonds in the carotenoid, whereas in similar dyads with 11 double bonds in the carotenoid, the Pc fluorescence is strongly quenched by Pc → Car S 1 energy transfer. In phenylamino-linked Car-Pc dyads in toluene extremely large electronic interactions between the Car S 1 state and Pc were observed, particularly in the case of a dyad in which the carotenoid contained 10 double bonds. This observation together with previous findings in the same system provides strong evidence for excitonic Car S 1-Pc Q y interactions. Very similar results were observed with photosynthetic LHC II complexes in the past, supporting an important role of such interactions in photosynthetic down-regulation.« less

  18. Two-color temporal focusing multiphoton excitation imaging with tunable-wavelength excitation

    NASA Astrophysics Data System (ADS)

    Lien, Chi-Hsiang; Abrigo, Gerald; Chen, Pei-Hsuan; Chien, Fan-Ching

    2017-02-01

    Wavelength tunable temporal focusing multiphoton excitation microscopy (TFMPEM) is conducted to visualize optical sectioning images of multiple fluorophore-labeled specimens through the optimal two-photon excitation (TPE) of each type of fluorophore. The tunable range of excitation wavelength was determined by the groove density of the grating, the diffraction angle, the focal length of lenses, and the shifting distance of the first lens in the beam expander. Based on a consideration of the trade-off between the tunable-wavelength range and axial resolution of temporal focusing multiphoton excitation imaging, the presented system demonstrated a tunable-wavelength range from 770 to 920 nm using a diffraction grating with groove density of 830 lines/mm. TPE fluorescence imaging examination of a fluorescent thin film indicated that the width of the axial confined excitation was 3.0±0.7 μm and the shifting distance of the temporal focal plane was less than 0.95 μm within the presented wavelength tunable range. Fast different wavelength excitation and three-dimensionally rendered imaging of Hela cell mitochondria and cytoskeletons and mouse muscle fibers were demonstrated. Significantly, the proposed system can improve the quality of two-color TFMPEM images through different excitation wavelengths to obtain higher-quality fluorescent signals in multiple-fluorophore measurements.

  19. Details of the Collagen and Elastin Architecture in the Human Limbal Conjunctiva, Tenon's Capsule and Sclera Revealed by Two-Photon Excited Fluorescence Microscopy.

    PubMed

    Park, Choul Yong; Marando, Catherine M; Liao, Jason A; Lee, Jimmy K; Kwon, Jiwon; Chuck, Roy S

    2016-10-01

    To investigate the architecture and distribution of collagen and elastin in human limbal conjunctiva, Tenon's capsule, and sclera. The limbal conjunctiva, Tenon's capsule, and sclera of human donor corneal buttons were imaged with an inverted two-photon excited fluorescence microscope. No fixation process was necessary. The laser (Ti:sapphire) was tuned at 850 nm for two-photon excitation. Backscatter signals of second harmonic generation (SHG) and autofluorescence (AF) were collected through a 425/30-nm and a 525/45-nm emission filter, respectively. Multiple, consecutive, and overlapping (z-stack) images were acquired. Collagen signals were collected with SHG, whereas elastin signals were collected with AF. The size and density of collagen bundles varied widely depending on depth: increasing from conjunctiva to sclera. In superficial image planes, collagen bundles were <10 μm in width, in a loose, disorganized arrangement. In deeper image planes (episclera and superficial sclera), collagen bundles were thicker (near 100 μm in width) and densely packed. Comparatively, elastin fibers were thinner and sparse. The orientation of elastin fibers was independent of collagen fibers in superficial layers; but in deep sclera, elastin fibers wove through collagen interbundle gaps. At the limbus, both collagen and elastin fibers were relatively compact and were distributed perpendicular to the limbal annulus. Two-photon excited fluorescence microscopy has enabled us to understand in greater detail the collagen and elastin architecture of the human limbal conjunctiva, Tenon's capsule, and sclera.

  20. Spectroscopy of the three-photon laser excitation of cold Rubidium Rydberg atoms in a magneto-optical trap

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

    Entin, V. M.; Yakshina, E. A.; Tretyakov, D. B.

    2013-05-15

    The spectra of the three-photon laser excitation 5S{sub 1/2} {yields} 5P{sub 3/2} {yields} 6S{sub 1/2}nP of cold Rb Rydberg atoms in an operating magneto-optical trap based on continuous single-frequency lasers at each stage are studied. These spectra contain two partly overlapping peaks of different amplitudes, which correspond to coherent three-photon excitation and incoherent three-step excitation due to the presence of two different ways of excitation through the dressed states of intermediate levels. A four-level theoretical model based on optical Bloch equations is developed to analyze these spectra. Good agreement between the experimental and calculated data is achieved by introducing additionalmore » decay of optical coherence induced by a finite laser line width and other broadening sources (stray electromagnetic fields, residual Doppler broadening, interatomic interactions) into the model.« less

  1. Raman spectroscopic signature of fractionalized excitations in the harmonic-honeycomb iridates β- and γ-Li2IrO3

    PubMed Central

    Glamazda, A.; Lemmens, P.; Do, S. -H.; Choi, Y. S.; Choi, K. -Y.

    2016-01-01

    The fractionalization of elementary excitations in quantum spin systems is a central theme in current condensed matter physics. The Kitaev honeycomb spin model provides a prominent example of exotic fractionalized quasiparticles, composed of itinerant Majorana fermions and gapped gauge fluxes. However, identification of the Majorana fermions in a three-dimensional honeycomb lattice remains elusive. Here we report spectroscopic signatures of fractional excitations in the harmonic-honeycomb iridates β- and γ-Li2IrO3. Using polarization-resolved Raman spectroscopy, we find that the dynamical Raman response of β- and γ-Li2IrO3 features a broad scattering continuum with distinct polarization and composition dependence. The temperature dependence of the Raman spectral weight is dominated by the thermal damping of fermionic excitations. These results suggest the emergence of Majorana fermions from spin fractionalization in a three-dimensional Kitaev–Heisenberg system. PMID:27457278

  2. Two-photon excited microscale colour centre patterns in Ag-activated phosphate glass written using a focused proton beam

    NASA Astrophysics Data System (ADS)

    Kurobori, Toshio; Kada, Wataru; Shirao, Taichi; Satoh, Takahiro

    2018-02-01

    We report a demonstration of microscale patterns in Ag-activated phosphate glass fabricated using a focused proton beam with an energy range of 1-3 MeV. Various microscale patterns are based on blue and orange radiophotoluminescent (RPL) centres. Two- and three-dimensional (2D and 3D) microstructures are visualised by combining two-photon confocal microscopy with femtosecond (fs) laser pulses generated from a mode-locked Ti:sapphire laser operating at 700 nm. The reconstructed images are analytically evaluated using lateral/axial dose mapping and RPL spectra. In addition, the advantages of two-photon excitation applied to Ag-activated phosphate glass are discussed, and this method is compared with single-photon excitation.

  3. On-chip beamsplitter operation on single photons from quasi-resonantly excited quantum dots embedded in GaAs rib waveguides

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

    Rengstl, U.; Schwartz, M.; Herzog, T.

    2015-07-13

    We present an on-chip beamsplitter operating on a single-photon level by means of a quasi-resonantly driven InGaAs/GaAs quantum dot. The single photons are guided by rib waveguides and split into two arms by an evanescent field coupler. Although the waveguides themselves support the fundamental TE and TM modes, the measured degree of polarization (∼90%) reveals the main excitation and propagation of the TE mode. We observe the preserved single-photon nature of a quasi-resonantly excited quantum dot by performing a cross-correlation measurement on the two output arms of the beamsplitter. Additionally, the same quantum dot is investigated under resonant excitation, wheremore » the same splitting ratio is observed. An autocorrelation measurement with an off-chip beamsplitter on a single output arm reveal the single-photon nature after evanescent coupling inside the on-chip splitter. Due to their robustness, adjustable splitting ratio, and their easy implementation, rib waveguide beamsplitters with embedded quantum dots provide a promising step towards fully integrated quantum circuits.« less

  4. Excited-state lifetime measurement of silicon vacancy centers in diamond by single-photon frequency upconversion

    NASA Astrophysics Data System (ADS)

    Rong, Youying; Ma, Jianhui; Chen, Lingxiao; Liu, Yan; Siyushev, Petr; Wu, Botao; Pan, Haifeng; Jelezko, Fedor; Wu, E.; Zeng, Heping

    2018-05-01

    We report a method with high time resolution to measure the excited-state lifetime of silicon vacancy centers in bulk diamond avoiding timing jitter from the single-photon detectors. Frequency upconversion of the fluorescence emitted from silicon vacancy centers was achieved from 738 nm to 436 nm via sum frequency generation with a short pump pulse. The excited-state lifetime can be obtained by measuring the intensity of upconverted light while the pump delay changes. As a probe, a pump laser with pulse duration of 11 ps provided a high temporal resolution of the measurement. The lifetime extracted from the pump–probe curve was 0.755 ns, which was comparable to the timing jitter of the single-photon detectors.

  5. Widefield Two-Photon Excitation without Scanning: Live Cell Microscopy with High Time Resolution and Low Photo-Bleaching

    PubMed Central

    Amor, Rumelo; McDonald, Alison; Trägårdh, Johanna; Robb, Gillian; Wilson, Louise; Abdul Rahman, Nor Zaihana; Dempster, John; Amos, William Bradshaw; Bushell, Trevor J.; McConnell, Gail

    2016-01-01

    We demonstrate fluorescence imaging by two-photon excitation without scanning in biological specimens as previously described by Hwang and co-workers, but with an increased field size and with framing rates of up to 100 Hz. During recordings of synaptically-driven Ca2+ events in primary rat hippocampal neurone cultures loaded with the fluorescent Ca2+ indicator Fluo-4 AM, we have observed greatly reduced photo-bleaching in comparison with single-photon excitation. This method, which requires no costly additions to the microscope, promises to be useful for work where high time-resolution is required. PMID:26824845

  6. How does a planet excite multiple spiral arms?

    NASA Astrophysics Data System (ADS)

    Bae, Jaehan; Zhu, Zhaohuan

    2018-01-01

    Protoplanetary disk simulations show that a single planet excites multiple spiral arms in the background disk, potentially supported by the multi-armed spirals revealed with recent high-resolution observations in some disks. The existence of multiple spiral arms is of importance in many aspects. It is empirically found that the arm-to-arm separation increases as a function of the planetary mass, so one can use the morphology of observed spiral arms to infer the mass of unseen planets. In addition, a spiral arm opens a radial gap as it steepens into a shock, so when a planet excites multiple spiral arms it can open multiple gaps in the disk. Despite the important implications, however, the formation mechanism of multiple spiral arms has not been fully understood by far.In this talk, we explain how a planet excites multiple spiral arms. The gravitational potential of a planet can be decomposed into a Fourier series, a sum of individual azimuthal modes having different azimuthal wavenumbers. Using a linear wave theory, we first demonstrate that appropriate sets of Fourier decomposed waves can be in phase, raising a possibility that constructive interference among the waves can produce coherent structures - spiral arms. More than one spiral arm can form since such constructive interference can occur at different positions in the disk for different sets of waves. We then verify this hypothesis using a suite of two-dimensional hydrodynamic simulations. Finally, we present non-linear behavior in the formation of multiple spiral arms.

  7. Method and apparatus for producing laser radiation following two-photon excitation of a gaseous medium

    DOEpatents

    Bischel, William K. [Menlo Park, CA; Jacobs, Ralph R. [Livermore, CA; Prosnitz, Donald [Hamden, CT; Rhodes, Charles K. [Palo Alto, CA; Kelly, Patrick J. [Fort Lewis, WA

    1979-02-20

    Method and apparatus for producing laser radiation by two-photon optical pumping of an atomic or molecular gaseous medium and subsequent lasing action. A population inversion is created as a result of two-photon absorption of the gaseous species. Stark tuning is utilized, if necessary, in order to tune the two-photon transition into exact resonance. In particular, gaseous ammonia (NH.sub.3) or methyl fluoride (CH.sub.3 F) is optically pumped by a pair of CO.sub.2 lasers to create a population inversion resulting from simultaneous two-photon excitation of a high-lying vibrational state, and laser radiation is produced by stimulated emission of coherent radiation from the inverted level.

  8. Method and apparatus for producing laser radiation following two-photon excitation of a gaseous medium

    DOEpatents

    Bischel, W.K.; Jacobs, R.R.; Prosnitz, D.P.; Rhodes, C.K.; Kelly, P.J.

    1979-02-20

    Method and apparatus are disclosed for producing laser radiation by two-photon optical pumping of an atomic or molecular gaseous medium and subsequent lasing action. A population inversion is created as a result of two-photon absorption of the gaseous species. Stark tuning is utilized, if necessary, in order to tune the two-photon transition into exact resonance. In particular, gaseous ammonia (NH[sub 3]) or methyl fluoride (CH[sub 3]F) is optically pumped by a pair of CO[sub 2] lasers to create a population inversion resulting from simultaneous two-photon excitation of a high-lying vibrational state, and laser radiation is produced by stimulated emission of coherent radiation from the inverted level. 3 figs.

  9. Simulation of multi-photon emission isotopes using time-resolved SimSET multiple photon history generator

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

    Chiang, Chih-Chieh; Lin, Hsin-Hon; Lin, Chang-Shiun

    Abstract-Multiple-photon emitters, such as In-111 or Se-75, have enormous potential in the field of nuclear medicine imaging. For example, Se-75 can be used to investigate the bile acid malabsorption and measure the bile acid pool loss. The simulation system for emission tomography (SimSET) is a well-known Monte Carlo simulation (MCS) code in nuclear medicine for its high computational efficiency. However, current SimSET cannot simulate these isotopes due to the lack of modeling of complex decay scheme and the time-dependent decay process. To extend the versatility of SimSET for simulation of those multi-photon emission isotopes, a time-resolved multiple photon history generatormore » based on SimSET codes is developed in present study. For developing the time-resolved SimSET (trSimSET) with radionuclide decay process, the new MCS model introduce new features, including decay time information and photon time-of-flight information, into this new code. The half-life of energy states were tabulated from the Evaluated Nuclear Structure Data File (ENSDF) database. The MCS results indicate that the overall percent difference is less than 8.5% for all simulation trials as compared to GATE. To sum up, we demonstrated that time-resolved SimSET multiple photon history generator can have comparable accuracy with GATE and keeping better computational efficiency. The new MCS code is very useful to study the multi-photon imaging of novel isotopes that needs the simulation of lifetime and the time-of-fight measurements. (authors)« less

  10. White-Light Supercontinuum Laser-Based Multiple Wavelength Excitation for TCSPC-FLIM of Cutaneous Nanocarrier Uptake

    NASA Astrophysics Data System (ADS)

    Volz, Pierre; Brodwolf, Robert; Zoschke, Christian; Haag, Rainer; Schäfer-Korting, Monika; Alexiev, Ulrike

    2018-05-01

    We report here on a custom-built time-correlated single photon-counting (TCSPC)-based fluorescence lifetime imaging microscopy (FLIM) setup with a continuously tunable white-light supercontinuum laser combined with acousto-optical tunable filters (AOTF) as an excitation source for simultaneous excitation of multiple spectrally separated fluorophores. We characterized the wavelength dependence of the white-light supercontinuum laser pulse properties and demonstrated the performance of the FLIM setup, aiming to show the experimental setup in depth together with a biomedical application. We herein summarize the physical-technical parameters as well as our approach to map the skin uptake of nanocarriers using FLIM with a resolution compared to spectroscopy. As an example, we focus on the penetration study of indocarbocyanine-labeled dendritic core-multishell nanocarriers (CMS-ICC) into reconstructed human epidermis. Unique fluorescence lifetime signatures of indocarbocyanine-labeled nanocarriers indicate nanocarrier-tissue interactions within reconstructed human epidermis, bringing FLIM close to spectroscopic analysis.

  11. Three-photon excitation source at 1250 nm generated in a dual zero dispersion wavelength nonlinear fiber

    DOE PAGES

    Domingue, Scott R.; Bartels, Randy A.

    2014-12-04

    Here, we demonstrate 1250 nm pulses generated in dual-zero dispersion photonic crystal fiber capable of three-photon excitation fluorescence microscopy. The total power conversion efficiency from the 28 fs seed pulse centered at 1075 nm to pulses at 1250 nm, including coupling losses from the nonlinear fiber, is 35%, with up to 67% power conversion efficiency of the fiber coupled light. Frequency-resolved optical gating measurements characterize 1250 nm pulses at 0.6 nJ and 2 nJ, illustrating the change in nonlinear spectral phase accumulation with pulse energy even for nonlinear fiber lengths < 50 mm. The 0.6 nJ pulse has a 26more » fs duration and is the shortest nonlinear fiber derived 1250 nm pulse yet reported (to the best of our knowledge). The short pulse durations and energies make these pulses a viable route to producing light at 1250 nm for multiphoton microscopy, which we we demonstrate here, via a three-photon excitation fluorescence microscope.« less

  12. Multiple excitation nano-spot generation and confocal detection for far-field microscopy.

    PubMed

    Mondal, Partha Pratim

    2010-03-01

    An imaging technique is developed for the controlled generation of multiple excitation nano-spots for far-field microscopy. The system point spread function (PSF) is obtained by interfering two counter-propagating extended depth-of-focus PSF (DoF-PSF), resulting in highly localized multiple excitation spots along the optical axis. The technique permits (1) simultaneous excitation of multiple planes in the specimen; (2) control of the number of spots by confocal detection; and (3) overcoming the point-by-point based excitation. Fluorescence detection from the excitation spots can be efficiently achieved by Z-scanning the detector/pinhole assembly. The technique complements most of the bioimaging techniques and may find potential application in high resolution fluorescence microscopy and nanoscale imaging.

  13. Multiple excitation nano-spot generation and confocal detection for far-field microscopy

    NASA Astrophysics Data System (ADS)

    Mondal, Partha Pratim

    2010-03-01

    An imaging technique is developed for the controlled generation of multiple excitation nano-spots for far-field microscopy. The system point spread function (PSF) is obtained by interfering two counter-propagating extended depth-of-focus PSF (DoF-PSF), resulting in highly localized multiple excitation spots along the optical axis. The technique permits (1) simultaneous excitation of multiple planes in the specimen; (2) control of the number of spots by confocal detection; and (3) overcoming the point-by-point based excitation. Fluorescence detection from the excitation spots can be efficiently achieved by Z-scanning the detector/pinhole assembly. The technique complements most of the bioimaging techniques and may find potential application in high resolution fluorescence microscopy and nanoscale imaging.

  14. Photonic structures in diamond based on femtosecond UV laser induced periodic surface structuring (LIPSS).

    PubMed

    Granados, Eduardo; Martinez-Calderon, Miguel; Gomez, Mikel; Rodriguez, Ainara; Olaizola, Santiago M

    2017-06-26

    We study the fabrication of photonic surface structures in single crystal diamond by means of highly controllable direct femtosecond UV laser induced periodic surface structuring. By appropriately selecting the excitation wavelength, intensity, number of impinging pulses and their polarization state, we demonstrate emerging high quality and fidelity diamond grating structures with surface roughness below 1.4 nm. We characterize their optical properties and study their potential for the fabrication of photonic structure anti-reflection coatings for diamond Raman lasers in the near-IR.

  15. Single photon detection with self-quenching multiplication

    NASA Technical Reports Server (NTRS)

    Zheng, Xinyu (Inventor); Cunningham, Thomas J. (Inventor); Pain, Bedabrata (Inventor)

    2011-01-01

    A photoelectronic device and an avalanche self-quenching process for a photoelectronic device are described. The photoelectronic device comprises a nanoscale semiconductor multiplication region and a nanoscale doped semiconductor quenching structure including a depletion region and an undepletion region. The photoelectronic device can act as a single photon detector or a single carrier multiplier. The avalanche self-quenching process allows electrical field reduction in the multiplication region by movement of the multiplication carriers, thus quenching the avalanche.

  16. Two-Photon Excitation STED Microscopy with Time-Gated Detection

    PubMed Central

    Coto Hernández, Iván; Castello, Marco; Lanzanò, Luca; d’Amora, Marta; Bianchini, Paolo; Diaspro, Alberto; Vicidomini, Giuseppe

    2016-01-01

    We report on a novel two-photon excitation stimulated emission depletion (2PE-STED) microscope based on time-gated detection. The time-gated detection allows for the effective silencing of the fluorophores using moderate stimulated emission beam intensity. This opens the possibility of implementing an efficient 2PE-STED microscope with a stimulated emission beam running in a continuous-wave. The continuous-wave stimulated emission beam tempers the laser architecture’s complexity and cost, but the time-gated detection degrades the signal-to-noise ratio (SNR) and signal-to-background ratio (SBR) of the image. We recover the SNR and the SBR through a multi-image deconvolution algorithm. Indeed, the algorithm simultaneously reassigns early-photons (normally discarded by the time-gated detection) to their original positions and removes the background induced by the stimulated emission beam. We exemplify the benefits of this implementation by imaging sub-cellular structures. Finally, we discuss of the extension of this algorithm to future all-pulsed 2PE-STED implementationd based on time-gated detection and a nanosecond laser source. PMID:26757892

  17. Doping Evolution of Magnetic Order and Magnetic Excitations in (Sr1 -xLax)3Ir2O7

    NASA Astrophysics Data System (ADS)

    Lu, Xingye; McNally, D. E.; Moretti Sala, M.; Terzic, J.; Upton, M. H.; Casa, D.; Ingold, G.; Cao, G.; Schmitt, T.

    2017-01-01

    We use resonant elastic and inelastic x-ray scattering at the Ir-L3 edge to study the doping-dependent magnetic order, magnetic excitations, and spin-orbit excitons in the electron-doped bilayer iridate (Sr1 -xLax )3Ir2 O7 (0 ≤x ≤0.065 ). With increasing doping x , the three-dimensional long range antiferromagnetic order is gradually suppressed and evolves into a three-dimensional short range order across the insulator-to-metal transition from x =0 to 0.05, followed by a transition to two-dimensional short range order between x =0.05 and 0.065. Because of the interactions between the Jeff=1/2 pseudospins and the emergent itinerant electrons, magnetic excitations undergo damping, anisotropic softening, and gap collapse, accompanied by weakly doping-dependent spin-orbit excitons. Therefore, we conclude that electron doping suppresses the magnetic anisotropy and interlayer couplings and drives (Sr1 -xLax )3Ir2 O7 into a correlated metallic state with two-dimensional short range antiferromagnetic order. Strong antiferromagnetic fluctuations of the Jeff=1/2 moments persist deep in this correlated metallic state, with the magnon gap strongly suppressed.

  18. Multimode theory of plasmon excitation at a metal - photonic crystal interface

    NASA Astrophysics Data System (ADS)

    Kuznetsova, T. I.; Raspopov, N. A.

    2017-12-01

    Surface plasmon excitation at a photonic crystal - metal interface is studied taking into account multiple scattering of an initial light wave on a periodical crystal structure. The analysis is focused on calculating characteristics of the eigenwaves in a one-dimensional crystal, which comprise a set of harmonics with the wavevectors separated from each other by the value of the crystal lattice wavevector. Reflection from the crystal - metal interface binds the amplitudes of propagating and evanescent modes. Calculations show that for the dielectric characteristics of a synthetic opal and a substrate made of a real metal with a ruby laser radiation used as the initial wave, the fulfilment of plasmon resonance conditions leads to a local increase in the surface plasmon amplitude by a factor of 6.4 - 9 as compared to the average amplitude of the initial wave. As a rule, the effect can only be obtained for a single surface wave, all other waves being substantially weaker than the main plasmon. There is a specific case where the resonance condition holds for two modes simultaneously. In this case, two oppositely directed fluxes of equal intensity are generated at the interface. The resonance condition breaks at a small deviation of the incident angle of the initial wave θ from the normal direction (|θ| ⩾ 10-4 rad). In the latter case, the picture is asymmetric: at angles |θ| ⩾ 5 × 10-3 rad, only one plasmon remains intensive. The local density of electromagnetic energy at the photonic crystal - metal interface may exceed the corresponding value of the initial wave by a factor of 40 - 80.

  19. Infrared Multiple Photon Dissociation Spectroscopy Of Metal Cluster-Adducts

    NASA Astrophysics Data System (ADS)

    Cox, D. M.; Kaldor, A.; Zakin, M. R.

    1987-01-01

    Recent development of the laser vaporization technique combined with mass-selective detection has made possible new studies of the fundamental chemical and physical properties of unsupported transition metal clusters as a function of the number of constituent atoms. A variety of experimental techniques have been developed in our laboratory to measure ionization threshold energies, magnetic moments, and gas phase reactivity of clusters. However, studies have so far been unable to determine the cluster structure or the chemical state of chemisorbed species on gas phase clusters. The application of infrared multiple photon dissociation IRMPD to obtain the IR absorption properties of metal cluster-adsorbate species in a molecular beam is described here. Specifically using a high power, pulsed CO2 laser as the infrared source, the IRMPD spectrum for methanol chemisorbed on small iron clusters is measured as a function of the number of both iron atoms and methanols in the complex for different methanol isotopes. Both the feasibility and potential utility of IRMPD for characterizing metal cluster-adsorbate interactions are demonstrated. The method is generally applicable to any cluster or cluster-adsorbate system dependent only upon the availability of appropriate high power infrared sources.

  20. Multiple nonlinear Bragg diffraction of femtosecond laser pulses in a {\\chi^{(2)}} photonic lattice with hexagonal domains

    NASA Astrophysics Data System (ADS)

    Vyunishev, A. M.; Arkhipkin, V. G.; Baturin, I. S.; Akhmatkhanov, A. R.; Shur, V. Ya; Chirkin, A. S.

    2018-04-01

    The frequency doubling of femtosecond laser pulses in a two-dimensional (2D) rectangular nonlinear photonic lattice with hexagonal domains is studied experimentally and theoretically. The broad fundamental spectrum enables frequency conversion under nonlinear Bragg diffraction for a series of transverse orders at a fixed longitudinal quasi-phase-matching order. The consistent nonstationary theory of the frequency doubling of femtosecond laser pulses is developed using the representation based on the reciprocal lattice of the structure. The calculated spatial distribution of the second-harmonic spectral intensity agrees well with the experimental data. The condition for multiple nonlinear Bragg diffraction in a 2D nonlinear photonic lattice is offered. The hexagonal shape of the domains contributes to multibeam second harmonic excitation. The maximum conversion efficiency for a series of transverse orders in the range 0.01%-0.03% is obtained.

  1. Two-photon excited autofluorescence imaging of human retinal pigment epithelial cells

    NASA Astrophysics Data System (ADS)

    Han, Meng; Blindewald-Wittich, Almut; Holz, Frank G.; Giese, Günter; Niemz, Markolf H.; Snyder, Sarah; Sun, Hui; Yu, Jiayi; Agopov, Michael; La Schiazza, Olivier; Bille, Josef F.

    2006-01-01

    Degeneration of retinal pigment epithelial (RPE) cells severely impairs the visual function of retina photoreceptors. However, little is known about the events that trigger the death of RPE cells at the subcellular level. Two-photon excited autofluorescence (TPEF) imaging of RPE cells proves to be well suited to investigate both the morphological and the spectral characteristics of the human RPE cells. The dominant fluorophores of autofluorescence derive from lipofuscin (LF) granules that accumulate in the cytoplasm of the RPE cells with increasing age. Spectral TPEF imaging reveals the existence of abnormal LF granules with blue shifted autofluorescence in RPE cells of aging patients and brings new insights into the complicated composition of the LF granules. Based on a proposed two-photon laser scanning ophthalmoscope, TPEF imaging of the living retina may be valuable for diagnostic and pathological studies of age related eye diseases.

  2. On the optimization, and the intensity dependence, of the excitation rate for the absorption of two-photons due to the direct permanent dipole moment excitation mechanism

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

    Meath, William J., E-mail: wmeath@uwo.ca

    2016-07-15

    A model two-level dipolar molecule, and the rotating wave approximation and perturbation theory, are used to investigate the optimization and the laser intensity dependence of the two-photon excitation rate via the direct permanent dipole mechanism. The rate is proportional to the square of the laser intensity I only for small intensities and times when perturbation theory is applicable. An improvement on perturbation theory is provided by a small time RWA result for the rate which is not proportional to I{sup 2}; rather it is proportional to the square of an effective intensity I{sub eff}. For each laser intensity the optimummore » RWA excitation rate as a function of time, for low intensities, is proportional to I, not I{sup 2}, and for high intensities it is proportional to I{sub eff}. For a given two-photon transition the laser-molecule coupling optimizes for an intensity I{sub max} which, for example, leads to a maximum possible excitation rate as a function of time. The validity of the RWA results of this paper, and the importance of including the effects of virtual excited states, are also discussed briefly.« less

  3. Ultrafast Silicon Photonics with Visible to Mid-Infrared Pumping of Silicon Nanocrystals.

    PubMed

    Diroll, Benjamin T; Schramke, Katelyn S; Guo, Peijun; Kortshagen, Uwe R; Schaller, Richard D

    2017-10-11

    Dynamic optical control of infrared (IR) transparency and refractive index is achieved using boron-doped silicon nanocrystals excited with mid-IR optical pulses. Unlike previous silicon-based optical switches, large changes in transmittance are achieved without a fabricated structure by exploiting strong light coupling of the localized surface plasmon resonance (LSPR) produced from free holes of p-type silicon nanocrystals. The choice of optical excitation wavelength allows for selectivity between hole heating and carrier generation through intraband or interband photoexcitation, respectively. Mid-IR optical pumping heats the free holes of p-Si nanocrystals to effective temperatures greater than 3500 K. Increases of the hole effective mass at high effective hole temperatures lead to a subpicosecond change of the dielectric function, resulting in a redshift of the LSPR, modulating mid-IR transmission by as much as 27%, and increasing the index of refraction by more than 0.1 in the mid-IR. Low hole heat capacity dictates subpicosecond hole cooling, substantially faster than carrier recombination, and negligible heating of the Si lattice, permitting mid-IR optical switching at terahertz repetition frequencies. Further, the energetic distribution of holes at high effective temperatures partially reverses the Burstein-Moss effect, permitting the modulation of transmittance at telecommunications wavelengths. The results presented here show that doped silicon, particularly in micro- or nanostructures, is a promising dynamic metamaterial for ultrafast IR photonics.

  4. Probing single magnon excitations in Sr₂IrO₄ using O K-edge resonant inelastic x-ray scattering.

    PubMed

    Liu, X; Dean, M P M; Liu, J; Chiuzbăian, S G; Jaouen, N; Nicolaou, A; Yin, W G; Rayan Serrao, C; Ramesh, R; Ding, H; Hill, J P

    2015-05-27

    Resonant inelastic x-ray scattering (RIXS) at the L-edge of transition metal elements is now commonly used to probe single magnon excitations. Here we show that single magnon excitations can also be measured with RIXS at the K-edge of the surrounding ligand atoms when the center heavy metal elements have strong spin-orbit coupling. This is demonstrated with oxygen K-edge RIXS experiments on the perovskite Sr2IrO4, where low energy peaks from single magnon excitations were observed. This new application of RIXS has excellent potential to be applied to a wide range of magnetic systems based on heavy elements, for which the L-edge RIXS energy resolution in the hard x-ray region is usually poor.

  5. Selective bond breaking mediated by state specific vibrational excitation in model HOD molecule through optimized femtosecond IR pulse: a simulated annealing based approach.

    PubMed

    Shandilya, Bhavesh K; Sen, Shrabani; Sahoo, Tapas; Talukder, Srijeeta; Chaudhury, Pinaki; Adhikari, Satrajit

    2013-07-21

    The selective control of O-H/O-D bond dissociation in reduced dimensionality model of HOD molecule has been explored through IR+UV femtosecond pulses. The IR pulse has been optimized using simulated annealing stochastic approach to maximize population of a desired low quanta vibrational state. Since those vibrational wavefunctions of the ground electronic states are preferentially localized either along the O-H or O-D mode, the femtosecond UV pulse is used only to transfer vibrationally excited molecule to the repulsive upper surface to cleave specific bond, O-H or O-D. While transferring from the ground electronic state to the repulsive one, the optimization of the UV pulse is not necessarily required except specific case. The results so obtained are analyzed with respect to time integrated flux along with contours of time evolution of probability density on excited potential energy surface. After preferential excitation from [line]0, 0> ([line]m, n> stands for the state having m and n quanta of excitations in O-H and O-D mode, respectively) vibrational level of the ground electronic state to its specific low quanta vibrational state ([line]1, 0> or [line]0, 1> or [line]2, 0> or [line]0, 2>) by using optimized IR pulse, the dissociation of O-D or O-H bond through the excited potential energy surface by UV laser pulse appears quite high namely, 88% (O-H ; [line]1, 0>) or 58% (O-D ; [line]0, 1>) or 85% (O-H ; [line]2, 0>) or 59% (O-D ; [line]0, 2>). Such selectivity of the bond breaking by UV pulse (if required, optimized) together with optimized IR one is encouraging compared to the normal pulses.

  6. Photon excitation enabled large aperture space-charge-controlled potassium tantalate niobate (KTN) beam deflector

    NASA Astrophysics Data System (ADS)

    Zhu, Wenbin; Chao, Ju-Hung; Chen, Chang-Jiang; Shang, Annan; Lee, Yun Goo; Yin, Shizhuo; Dubinskii, Mark; Hoffman, Robert C.

    2018-03-01

    To overcome the depth limitation of the space-charge-controlled (SCC) potassium tantalate niobate (KTN) deflectors, we report in this paper a method of increasing the aperture of SCC-KTN deflectors by harnessing the physical mechanism of blue light photon excitation. The experimental results show that the deflection angle can be increased from 0.7 mrad without the blue light excitation to 2.5 mrad with the blue light excitation at a penetration depth of 5 mm under the same external applied voltage, which is consistent with the theoretical analysis. This represents a substantial increase in the deflection angle at a much deeper penetration depth, which can be very useful for applications such as high speed 3D printings and displays.

  7. Soft pair excitations and double-log divergences due to carrier interactions in graphene

    NASA Astrophysics Data System (ADS)

    Lewandowski, Cyprian; Levitov, L. S.

    2018-03-01

    Interactions between charge carriers in graphene lead to logarithmic renormalization of observables mimicking the behavior known in (3+1)-dimensional quantum electrodynamics (QED). Here we analyze soft electron-hole (e -h ) excitations generated as a result of fast charge dynamics, a direct analog of the signature QED effect—multiple soft photons produced by the QED vacuum shakeup. We show that such excitations are generated in photon absorption, when a photogenerated high-energy e -h pair cascades down in energy and gives rise to multiple soft e -h excitations. This fundamental process is manifested in a double-log divergence in the emission rate of soft pairs and a characteristic power-law divergence in their energy spectrum of the form 1/ω ln(ω/Δ ) . Strong carrier-carrier interactions make pair production a prominent pathway in the photoexcitation cascade.

  8. Photonic Shape Memory Polymer with Stable Multiple Colors

    PubMed Central

    2017-01-01

    A photonic shape memory polymer film that shows large color response (∼155 nm) in a wide temperature range has been fabricated from a semi-interpenetrating network of a cholesteric polymer and poly(benzyl acrylate). The large color response is achieved by mechanical embossing of the photonic film above its broad glass transition temperature. The embossed film, as it recovers to its original shape on heating through the broad thermal transition, exhibits multiple structural colors ranging from blue to orange. The relaxation behavior of the embossed film can be fully described using a Kelvin–Voigt model, which reveals that the influence of temperature on the generation of colors is much stronger than that of time, thereby producing stable multiple colors. PMID:28840717

  9. Mechanism for the Excited-State Multiple Proton Transfer Process of Dihydroxyanthraquinone Chromophores.

    PubMed

    Zhou, Qiao; Du, Can; Yang, Li; Zhao, Meiyu; Dai, Yumei; Song, Peng

    2017-06-22

    The single and dual cooperated proton transfer dynamic process in the excited state of 1,5-dihydroxyanthraquinone (1,5-DHAQ) was theoretically investigated, taking solvent effects (ethanol) into account. The absorption and fluorescence spectra were simulated, and dual fluorescence exhibited, which is consistent with previous experiments. Analysis of the calculated IR and Raman vibration spectra reveals that the intramolecular hydrogen bonding interactions (O 20 -H 21 ···O 24 and O 22 -H 23 ···O 25 ) are strengthened following the excited proton transfer process. Finally, by constructing the potential energy surfaces of the ground state, first excited singlet state, and triplet state, the mechanism of the intramolecular proton transfer of 1,5-DHAQ can be revealed.

  10. Structural elucidation of direct analysis in real time ionized nerve agent simulants with infrared multiple photon dissociation spectroscopy.

    PubMed

    Rummel, Julia L; Steill, Jeffrey D; Oomens, Jos; Contreras, Cesar S; Pearson, Wright L; Szczepanski, Jan; Powell, David H; Eyler, John R

    2011-06-01

    Infrared multiple photon dissociation (IRMPD) was used to generate vibrational spectra of ions produced with a direct analysis in real time (DART) ionization source coupled to a 4.7 T Fourier transform ion cyclotron resonance (FT-ICR) mass spectrometer. The location of protonation on the nerve agent simulants diisopropyl methylphosphonate (DIMP) and dimethyl methylphosphonate (DMMP) was studied while solutions of the compounds were introduced for extended periods of time with a syringe pump. Theoretical vibrational spectra were generated with density functional theory calculations. Visual comparison of experimental mid-IR IRMPD spectra and theoretical spectra could not establish definitively if a single structure or a mixture of conformations was present for the protonated parent of each compound. However, theoretical calculations, near-ir IRMPD spectra, and frequency-to-frequency and statistical comparisons indicated that the protonation site for both DIMP and DMMP was predominantly, if not exclusively, the phosphonyl oxygen instead of one of the oxygen atoms with only single bonds.

  11. Long-lived room-temperature deep-red-emissive intraligand triplet excited state of naphthalimide in cyclometalated Ir(III) complexes and its application in triplet-triplet annihilation-based upconversion.

    PubMed

    Sun, Jifu; Wu, Wanhua; Zhao, Jianzhang

    2012-06-25

    Cyclometalated Ir(III) complexes with acetylide ppy and bpy ligands were prepared (ppy = 2-phenylpyridine, bpy = 2,2'-bipyridine) in which naphthal (Ir-2) and naphthalimide (NI) were attached onto the ppy (Ir-3) and bpy ligands (Ir-4) through acetylide bonds. [Ir(ppy)(3)] (Ir-1) was also prepared as a model complex. Room-temperature phosphorescence was observed for the complexes; both neutral and cationic complexes Ir-3 and Ir-4 showed strong absorption in the visible range (ε=39,600  M(-1)  cm(-1) at 402 nm and ε=25,100  M(-1)  cm(-1) at 404 nm, respectively), long-lived triplet excited states (τ(T)=9.30 μs and 16.45 μs) and room-temperature red emission (λ(em)=640 nm, Φ(p)=1.4 % and λ(em)=627 nm, Φ(p)=0.3 %; cf. Ir-1: ε=16,600  M(-1)  cm(-1) at 382 nm, τ(em)=1.16 μs, Φ(p)=72.6 %). Ir-3 was strongly phosphorescent in non-polar solvent (i.e., toluene), but the emission was completely quenched in polar solvents (MeCN). Ir-4 gave an opposite response to the solvent polarity, that is, stronger phosphorescence in polar solvents than in non-polar solvents. Emission of Ir-1 and Ir-2 was not solvent-polarity-dependent. The T(1) excited states of Ir-2, Ir-3, and Ir-4 were identified as mainly intraligand triplet excited states ((3)IL) by their small thermally induced Stokes shifts (ΔE(s)), nanosecond time-resolved transient difference absorption spectroscopy, and spin-density analysis. The complexes were used as triplet photosensitizers for triplet-triplet annihilation (TTA) upconversion and quantum yields of 7.1 % and 14.4 % were observed for Ir-2 and Ir-3, respectively, whereas the upconversion was negligible for Ir-1 and Ir-4. These results will be useful for designing visible-light-harvesting transition-metal complexes and for their applications as triplet photosensitizers for photocatalysis, photovoltaics, TTA upconversion, etc. Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  12. Infrared Multiple Photon Dissociation Spectroscopy of Sodium and Potassium Chlorate Anions

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

    Ryan P. Dain; Christopher M. Leavitt; Jos Oomens

    2010-01-01

    The structures of gas-phase, metal chlorate anions with the formula [M(ClO3)2]-, M=Na and K, were determined using tandem mass spectrometry and infrared multiple photon dissociation (IRMPD) spectroscopy. Structural assignments for both anions are based on comparisons of the experimental vibrational spectra for the two species to those predicted by density functional theory and involve conformations that feature either bidentate or tridentate coordination of the cation by chlorate. Our results strongly suggest that a structure in which both chlorate anions are bidentate ligands is preferred for [Na(ClO3)2]-. However, for [K(ClO3)2]- the best agreement between experimental and theoretical spectra is obtained frommore » a composite of predicted spectra for which the chlorate anions are either both bidentate or both tridentate ligands. In general, we find that the overall accuracy of DFT calculations for prediction of IR spectra is dependent on both functional and basis set, with best agreement achieved using frequencies generated at the B3LYP/6-311+g(3df) level of theory.« less

  13. Infrared multiple photon dissociation spectroscopy of sodium and potassium chlorate anions.

    PubMed

    Dain, Ryan P; Leavitt, Christopher M; Oomens, Jos; Steill, Jeffrey D; Groenewold, Gary S; Van Stipdonk, Michael J

    2010-01-01

    The structures of gas-phase, metal chlorate anions with the formula [M(ClO(3))(2)](-), M = Na and K, were determined using tandem mass spectrometry and infrared multiple photon dissociation (IRMPD) spectroscopy. Structural assignments for both anions are based on comparisons of the experimental vibrational spectra for the two species with those predicted by density functional theory (DFT) and involve conformations that feature either bidentate or tridentate coordination of the cation by chlorate. Our results strongly suggest that a structure in which both chlorate anions are bidentate ligands is preferred for [Na(ClO(3))(2)](-). However, for [K(ClO(3))(2)](-) the best agreement between experimental and theoretical spectra is obtained from a composite of predicted spectra for which the chlorate anions are either both bidentate or both tridentate ligands. In general, we find that the overall accuracy of DFT calculations for prediction of IR spectra is dependent on both functional and basis set, with best agreement achieved using frequencies generated at the B3LYP/6-311+g(3df) level of theory. Copyright 2009 John Wiley & Sons, Ltd.

  14. Integrated photonics for infrared spectroscopic sensing

    NASA Astrophysics Data System (ADS)

    Lin, Hongtao; Kita, Derek; Han, Zhaohong; Su, Peter; Agarwal, Anu; Yadav, Anupama; Richardson, Kathleen; Gu, Tian; Hu, Juejun

    2017-05-01

    Infrared (IR) spectroscopy is widely recognized as a gold standard technique for chemical analysis. Traditional IR spectroscopy relies on fragile bench-top instruments located in dedicated laboratory settings, and is thus not suitable for emerging field-deployed applications such as in-line industrial process control, environmental monitoring, and point-ofcare diagnosis. Recent strides in photonic integration technologies provide a promising route towards enabling miniaturized, rugged platforms for IR spectroscopic analysis. Chalcogenide glasses, the amorphous compounds containing S, Se or Te, have stand out as a promising material for infrared photonic integration given their broadband infrared transparency and compatibility with silicon photonic integration. In this paper, we discuss our recent work exploring integrated chalcogenide glass based photonic devices for IR spectroscopic chemical analysis, including on-chip cavityenhanced chemical sensing and monolithic integration of mid-IR waveguides with photodetectors.

  15. Time-resolved stimulated emission depletion and energy transfer dynamics in two-photon excited EGFP.

    PubMed

    Masters, T A; Robinson, N A; Marsh, R J; Blacker, T S; Armoogum, D A; Larijani, B; Bain, A J

    2018-04-07

    Time and polarization-resolved stimulated emission depletion (STED) measurements are used to investigate excited state evolution following the two-photon excitation of enhanced green fluorescent protein (EGFP). We employ a new approach for the accurate STED measurement of the hitherto unmeasured degree of hexadecapolar transition dipole moment alignment α 40 present at a given excitation-depletion (pump-dump) pulse separation. Time-resolved polarized fluorescence measurements as a function of pump-dump delay reveal the time evolution of α 40 to be considerably more rapid than predicted for isotropic rotational diffusion in EGFP. Additional depolarization by homo-Förster resonance energy transfer is investigated for both α 20 (quadrupolar) and α 40 transition dipole alignments. These results point to the utility of higher order dipole correlation measurements in the investigation of resonance energy transfer processes.

  16. LANTHANIDE ENHANCE LUMINESCENCE (LEL) WITH ONE AND TWO PHOTON EXCITATION OF QUANTUM DYES LANTHANIDE (III) - MACROCYCLES

    EPA Science Inventory

    Title: Lanthanide Enhance Luminescence (LEL) with one and two photon excitation of Quantum Dyes? Lanthanide(III)-Macrocycles
    Principal Author:
    Robert C. Leif, Newport Instruments
    Secondary Authors:
    Margie C. Becker, Phoenix Flow Systems
    Al Bromm, Virginia Commonw...

  17. IR multiphoton absorption of SF6 in flow with Ar at moderate energy fluences

    NASA Astrophysics Data System (ADS)

    Makarov, G. N.; Ronander, E.; van Heerden, S. P.; Gouws, M.; van der Merwe, K.

    1997-10-01

    IR multiple photon absorption (MPA) of SF6 in flow with Ar (SF6: Ar=1:100) in conditions of a large vibrational/rotational temperature difference (TV𪒮 K, TR䏐 K) was studied at moderate energy fluences from ۂ.1 to 𪐬 mJ/cm2, which are of interest for isotope selective two-step dissociation of molecules. A 50 cm Laval-type slit nozzle for the flow cooling, and a TEA CO2-laser for excitation of molecules were used in the experiments. The laser energy fluence dependences of the SF6 MPA were studied for several CO2-laser lines which are in a good resonance with the linear absorption spectrum of the Ƚ vibration of SF6 at low temperature. The effect of the laser pulse duration (intensity) on MPA of flow cooled SF6 with Ar was also studied. The results are compared with those obtained in earlier studies.

  18. In-vivo multi-nonlinear optical imaging of a living cell using a supercontinuum light source generated from a photonic crystal fiber

    NASA Astrophysics Data System (ADS)

    Kano, Hideaki; Hamaguchi, Hiro-O.

    2006-04-01

    A supercontinuum light source generated with a femtosecond Ti:Sapphire oscillator has been used to obtain both vibrational and two-photon excitation fluorescence (TPEF) images of a living cell simultaneously at different wavelengths. Owing to an ultrabroadband spectral profile of the supercontinuum, multiple vibrational resonances have been detected through coherent anti-Stokes Raman scattering (CARS) process. In addition to the multiplex CARS process, multiple electronic states can be excited due to the broadband electronic two-photon excitation using the supercontinuum, giving rise to a two-photon excitation fluorescence (TPEF) signal. Using a living yeast cell whose nucleus is labeled by green fluorescent protein (GFP), we have succeeded in visualizing organelles such as mitochondria, septum, and nucleus through the CARS and the TPEF processes. The supercontinuum enables us to perform unique multi-nonlinear optical imaging through two different nonlinear optical processes.

  19. Research in Electronics - JSEP.

    DTIC Science & Technology

    1981-03-01

    17. H . Helvajian and C. Wittig, "Collisional Quenching of HgBr(B 2 4i/2), Opt. Commun. 30, 189 (1979). 18. H . Reisler and C. Wittig, "Electronic...Luminescence Resulting from IR Multiple Photon Excitation, " in ’Photoselective Chemistry, Part I,’ J. Jortner ed., Wiley, 1981. 19. H . Helvajian , M...to Intramolecular V E coupling in IR Laser Excited Polyatomics, " J. Chem. Phys., in press. 22. H . Helvajian and C. Wittig, "Vibrational Quenching of

  20. Ultrafast Silicon Photonics with Visible to Mid-Infrared Pumping of Silicon Nanocrystals

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

    Diroll, Benjamin T.; Schramke, Katelyn S.; Guo, Peijun

    Dynamic optical control of infrared (IR) transparency and refractive index is achieved using boron-doped silicon nanocrystals excited with mid-IR optical pulses. Also, unlike previous silicon-based optical switches, large changes in transmittance are achieved without a fabricated structure by exploiting strong light coupling of the localized surface plasmon resonance (LSPR) produced from free holes of p-type silicon nanocrystals. The choice of optical excitation wavelength allows selectivity between hole heating and carrier generation through intraband or interband photoexcitation, respectively. Mid-IR optical pumping heats the free holes of p-Si nanocrystals to effective temperatures greater than 3500 K. Increases of the hole effective massmore » at high effective hole temperatures lead to a sub-picosecond change of the dielectric function resulting in a redshift of the LSPR, modulating mid-IR transmission by as much as 27% and increasing the index of refraction by more than 0.1 in the mid-IR. Low hole heat capacity dictates sub-picosecond hole cooling, substantially faster than carrier recombination, and negligible heating of the Si lattice, permitting mid-IR optical switching at terahertz repetition frequencies. Further, the energetic distribution of holes at high effective temperatures partially reverses the Burstein-Moss effect, permitting modulation of transmittance at telecommunications wavelengths. Lastly, the results presented here show that doped silicon, particularly in micro- or nanostructures, is a promising dynamic metamaterial for ultrafast IR photonics.« less

  1. Ultrafast Silicon Photonics with Visible to Mid-Infrared Pumping of Silicon Nanocrystals

    DOE PAGES

    Diroll, Benjamin T.; Schramke, Katelyn S.; Guo, Peijun; ...

    2017-09-11

    Dynamic optical control of infrared (IR) transparency and refractive index is achieved using boron-doped silicon nanocrystals excited with mid-IR optical pulses. Also, unlike previous silicon-based optical switches, large changes in transmittance are achieved without a fabricated structure by exploiting strong light coupling of the localized surface plasmon resonance (LSPR) produced from free holes of p-type silicon nanocrystals. The choice of optical excitation wavelength allows selectivity between hole heating and carrier generation through intraband or interband photoexcitation, respectively. Mid-IR optical pumping heats the free holes of p-Si nanocrystals to effective temperatures greater than 3500 K. Increases of the hole effective massmore » at high effective hole temperatures lead to a sub-picosecond change of the dielectric function resulting in a redshift of the LSPR, modulating mid-IR transmission by as much as 27% and increasing the index of refraction by more than 0.1 in the mid-IR. Low hole heat capacity dictates sub-picosecond hole cooling, substantially faster than carrier recombination, and negligible heating of the Si lattice, permitting mid-IR optical switching at terahertz repetition frequencies. Further, the energetic distribution of holes at high effective temperatures partially reverses the Burstein-Moss effect, permitting modulation of transmittance at telecommunications wavelengths. Lastly, the results presented here show that doped silicon, particularly in micro- or nanostructures, is a promising dynamic metamaterial for ultrafast IR photonics.« less

  2. Mid-infrared integrated photonics on silicon: a perspective

    NASA Astrophysics Data System (ADS)

    Lin, Hongtao; Luo, Zhengqian; Gu, Tian; Kimerling, Lionel C.; Wada, Kazumi; Agarwal, Anu; Hu, Juejun

    2017-12-01

    The emergence of silicon photonics over the past two decades has established silicon as a preferred substrate platform for photonic integration. While most silicon-based photonic components have so far been realized in the near-infrared (near-IR) telecommunication bands, the mid-infrared (mid-IR, 2-20-μm wavelength) band presents a significant growth opportunity for integrated photonics. In this review, we offer our perspective on the burgeoning field of mid-IR integrated photonics on silicon. A comprehensive survey on the state-of-the-art of key photonic devices such as waveguides, light sources, modulators, and detectors is presented. Furthermore, on-chip spectroscopic chemical sensing is quantitatively analyzed as an example of mid-IR photonic system integration based on these basic building blocks, and the constituent component choices are discussed and contrasted in the context of system performance and integration technologies.

  3. Two-Photon Optical Properties of Near-Infrared Dyes at 1.55 microns Excitation

    PubMed Central

    Berezin, Mikhail; Zhan, Chun; Lee, Hyeran; Joo, Chulmin; Akers, Walter; Yazdanfar, Siavash; Achilefu, Samuel

    2011-01-01

    Two-photon (2P) optical properties of cyanine dyes were evaluated using a 2P fluorescence spectrophotometer with 1.55 μm excitation. We report the 2P characteristics of common NIR polymethine dyes, including their 2P action cross-sections and the 2P excited fluorescence lifetime. One of the dyes, DTTC showed the highest 2P action cross-section (~103 ± 19 GM) and relatively high 2P excited fluorescence lifetime and can be used as a scaffold for the synthesis of 2P molecular imaging probes. The 2P action cross-section of DTTC and the lifetime were also highly sensitive to the solvent polarity, providing other additional parameters for its use in optical imaging and the mechanism for probing environmental factors Overall, this study demonstrated the quantitative measurement of 2P properties of NIR dyes and established the foundation for designing molecular probes for 2P imaging applications in the NIR region. PMID:21866928

  4. Time-resolved stimulated emission depletion and energy transfer dynamics in two-photon excited EGFP

    NASA Astrophysics Data System (ADS)

    Masters, T. A.; Robinson, N. A.; Marsh, R. J.; Blacker, T. S.; Armoogum, D. A.; Larijani, B.; Bain, A. J.

    2018-04-01

    Time and polarization-resolved stimulated emission depletion (STED) measurements are used to investigate excited state evolution following the two-photon excitation of enhanced green fluorescent protein (EGFP). We employ a new approach for the accurate STED measurement of the hitherto unmeasured degree of hexadecapolar transition dipole moment alignment ⟨α40 ⟩ present at a given excitation-depletion (pump-dump) pulse separation. Time-resolved polarized fluorescence measurements as a function of pump-dump delay reveal the time evolution of ⟨α40 ⟩ to be considerably more rapid than predicted for isotropic rotational diffusion in EGFP. Additional depolarization by homo-Förster resonance energy transfer is investigated for both ⟨α20 ⟩ (quadrupolar) and ⟨α40 ⟩ transition dipole alignments. These results point to the utility of higher order dipole correlation measurements in the investigation of resonance energy transfer processes.

  5. Two-Photon Excitation in Biological Material for Conventional and Long Working-Distance Objectives.

    NASA Astrophysics Data System (ADS)

    Keeler, W. J.; McGhee, P.

    2000-03-01

    The application of laser two-photon excitation or nonlinear second-harmonic generation to imaging, spectroscopy, and light activated medical therapies, is an expanding field of research. When small feature sizes such as cells and their components are to be studied, high numerical aperture (NA) lenses are required to obtain the necessary lateral and axial resolutions. If one wishes to increase the depth of sample penetration, factors such as scattering and absorption quickly degrade the quality of the focused beam. The problem is further exacerbated by the short working distance of conventional high NA microscope objectives if they are used for light delivery and pickup. These lenses and their accompanying eyepieces, are designed to produce an exit pupil that can be accomodated by the human eye. Such a design will underfil detectors such as large CCD arrays. To simultaneously increase the working distance at the sample and the system exit pupil, larger scale objectives can be used. We will report the results of two-photon excitation and fluorescence investigations of several feature sizes as a function of penetration depth in homogeneous media and tissue samples, for conventional and long working distance objectives. The possible implications of these results to imaging and therapeutic dose delivery will also be presented.

  6. Automatic cytometric device using multiple wavelength excitations

    NASA Astrophysics Data System (ADS)

    Rongeat, Nelly; Ledroit, Sylvain; Chauvet, Laurence; Cremien, Didier; Urankar, Alexandra; Couderc, Vincent; Nérin, Philippe

    2011-05-01

    Precise identification of eosinophils, basophils, and specific subpopulations of blood cells (B lymphocytes) in an unconventional automatic hematology analyzer is demonstrated. Our specific apparatus mixes two excitation radiations by means of an acousto-optics tunable filter to properly control fluorescence emission of phycoerythrin cyanin 5 (PC5) conjugated to antibodies (anti-CD20 or anti-CRTH2) and Thiazole Orange. This way our analyzer combining techniques of hematology analysis and flow cytometry based on multiple fluorescence detection, drastically improves the signal to noise ratio and decreases the spectral overlaps impact coming from multiple fluorescence emissions.

  7. Two-photon excited fluorescence microscopy application for ex vivo investigation of ocular fundus samples

    NASA Astrophysics Data System (ADS)

    Peters, Sven; Hammer, Martin; Schweitzer, Dietrich

    2011-07-01

    Two-photon excited fluorescence (TPEF) imaging of ocular tissue has recently become a promising tool in ophthalmology for diagnostic and research purposes. The feasibility and the advantages of TPEF imaging, namely deeper tissue penetration and improved high-resolution imaging of microstructures, have been demonstrated lately using human ocular samples. The autofluorescence properties of endogenous fluorophores in ocular fundus tissue are well known from spectrophotometric analysis. But fluorophores, especially when it comes to fluorescence lifetime, typically display a dependence of their fluorescence properties on local environmental parameters. Hence, a more detailed investigation of ocular fundus autofluorescence ideally in vivo is of utmost interest. The aim of this study is to determine space-resolved the stationary and time-resolved fluorescence properties of endogenous fluorophores in ex vivo porcine ocular fundus samples by means of two-photon excited fluorescence spectrum and lifetime imaging microscopy (FSIM/FLIM). By our first results, we characterized the autofluorescence of individual anatomical structures of porcine retina samples excited at 760 nm. The fluorescence properties of almost all investigated retinal layers are relatively homogenous. But as previously unknown, ganglion cell bodies show a significantly shorter fluorescence lifetime compared to the adjacent mueller cells. Since all retinal layers exhibit bi-exponential autofluorescence decays, we were able to achieve a more precise characterization of fluorescence properties of endogenous fluorophores compared to a present in vivo FLIM approach by confocal scanning laser ophthalmoscope (cSLO).

  8. Large-area, near-infrared (IR) photonic crystals with colloidal gold nanoparticles embedding.

    PubMed

    Shukla, Shobha; Baev, Alexander; Jee, Hongsub; Hu, Rui; Burzynski, Ryszard; Yoon, Yong-Kyu; Prasad, Paras N

    2010-04-01

    A polymeric composite material composed of colloidal gold nanoparticles (<10 nm) and SU8 has been utilized for the fabrication of large-area, high-definition photonic crystal. We have successfully fabricated near-infrared photonic crystal slabs from composite materials using a combination of multiple beam interference lithography and reactive ion etching processes. Doping of colloidal gold nanoparticles into the SU8 photopolymer results in a better definition of structural features and hence in the enhancement of the optical properties of the fabricated photonic crystals. A 2D air hole array of triangular symmetry with a hole-to-hole pitch of approximately 500 nm has been successfully fabricated in a large circular area of 1 cm diameter. Resonant features observed in reflectance spectra of our slabs are found to depend on the exposure time, and can be tuned over a range of near-infrared frequencies.

  9. Spectroscopic study on the iodine molecule by a sequential three-photon excitation

    NASA Astrophysics Data System (ADS)

    Ishiwata, Takashi; Ohtoshi, Hirokazu; Sakaki, Mamoru; Tanaka, Ikuzo

    1984-02-01

    A three-photon absorption technique which utilizes a visible B 3Π0+u-X 1Σ+g transition followed by a simultaneous two-photon absorption was applied to study an ion-pair state of molecular iodine. The derived molecular parameters were Te=51 707 cm-1, ωe=131 cm-1, and Be=0.021 90 cm-1 for the F'(0+u) ion-pair state, which dissociates to I-(1S)+I+(1D). The excitation of I2 to a single rovibronic level of the F' state was achieved and its fluorescence spectrum showed two discrete band systems corresponding to the transitions to: (1) the ground state at higher vibrational levels; and (2) the weakly bound state (Te=19 286 cm-1, ωe=64 cm-1, and re=3.65 Å) converging to the I(2P3/2)+I(2P1/2) products.

  10. FPGA-based photon-counting phase-modulation fluorometer and a brief comparison with that operated in a pulsed-excitation mode

    NASA Astrophysics Data System (ADS)

    Iwata, Tetsuo; Taga, Takanori; Mizuno, Takahiko

    2018-02-01

    We have constructed a high-efficiency, photon-counting phase-modulation fluorometer (PC-PMF) using a field-programmable gate array, which is a modified version of the photon-counting fluorometer (PCF) that works in a pulsed-excitation mode (Iwata and Mizuno in Meas Sci Technol 28:075501, 2017). The common working principle for both is the simultaneous detection of the photoelectron pulse train, which covers 64 ns with a 1.0-ns resolution time (1.0 ns/channel). The signal-gathering efficiency was improved more than 100 times over that of conventional time-correlated single-photon-counting at the expense of resolution time depending on the number of channels. The system dead time for building a histogram was eliminated, markedly shortening the measurement time for fluorescent samples with moderately high quantum yields. We describe the PC-PMF and make a brief comparison with the pulsed-excitation PCF in precision, demonstrating the potential advantage of PC-PMF.

  11. Discrete Chromatic Aberrations Arising from Photoinduced Electron-Photon Interactions in Ultrafast Electron Microscopy.

    PubMed

    Plemmons, Dayne A; Flannigan, David J

    2016-05-26

    In femtosecond ultrafast electron microscopy (UEM) experiments, the initial excitation period is composed of spatiotemporal overlap of the temporally commensurate pump photon pulse and probe photoelectron packet. Generation of evanescent near-fields at the nanostructure specimens produces a dispersion relation that enables coupling of the photons (ℏω = 2.4 eV, for example) and freely propagating electrons (200 keV, for example) in the near-field. Typically, this manifests as discrete peaks occurring at integer multiples (n) of the photon energy in the low-loss/gain region of electron-energy spectra (i.e., at 200 keV ± nℏω eV). Here, we examine the UEM imaging resolution implications of the strong inelastic near-field interactions between the photons employed in optical excitation and the probe photoelectrons. We find that the additional photoinduced energy dispersion occurring when swift electrons pass through intense evanescent near-fields results in a discrete chromatic aberration that limits the spatial resolving power to several angstroms during the excitation period.

  12. Diagnosis of basal cell carcinoma by two photon excited fluorescence combined with lifetime imaging

    NASA Astrophysics Data System (ADS)

    Fan, Shunping; Peng, Xiao; Liu, Lixin; Liu, Shaoxiong; Lu, Yuan; Qu, Junle

    2014-02-01

    Basal cell carcinoma (BCC) is the most common type of human skin cancer. The traditional diagnostic procedure of BCC is histological examination with haematoxylin and eosin staining of the tissue biopsy. In order to reduce complexity of the diagnosis procedure, a number of noninvasive optical methods have been applied in skin examination, for example, multiphoton tomography (MPT) and fluorescence lifetime imaging microscopy (FLIM). In this study, we explored two-photon optical tomography of human skin specimens using two-photon excited autofluorescence imaging and FLIM. There are a number of naturally endogenous fluorophores in skin sample, such as keratin, melanin, collagen, elastin, flavin and porphyrin. Confocal microscopy was used to obtain structures of the sample. Properties of epidermic and cancer cells were characterized by fluorescence emission spectra, as well as fluorescence lifetime imaging. Our results show that two-photon autofluorescence lifetime imaging can provide accurate optical biopsies with subcellular resolution and is potentially a quantitative optical diagnostic method in skin cancer diagnosis.

  13. Two-Photon-Excited Silica and Organosilica Nanoparticles for Spatiotemporal Cancer Treatment.

    PubMed

    Croissant, Jonas G; Zink, Jeffrey I; Raehm, Laurence; Durand, Jean-Olivier

    2018-04-01

    Coherent two-photon-excited (TPE) therapy in the near-infrared (NIR) provides safer cancer treatments than current therapies lacking spatial and temporal selectivities because it is characterized by a 3D spatial resolution of 1 µm 3 and very low scattering. In this review, the principle of TPE and its significance in combination with organosilica nanoparticles (NPs) are introduced and then studies involving the design of pioneering TPE-NIR organosilica nanomaterials are discussed for bioimaging, drug delivery, and photodynamic therapy. Organosilica nanoparticles and their rich and well-established chemistry, tunable composition, porosity, size, and morphology provide ideal platforms for minimal side-effect therapies via TPE-NIR. Mesoporous silica and organosilica nanoparticles endowed with high surface areas can be functionalized to carry hydrophobic and biologically unstable two-photon absorbers for drug delivery and diagnosis. Currently, most light-actuated clinical therapeutic applications with NPs involve photodynamic therapy by singlet oxygen generation, but low photosensitizing efficiencies, tumor resistance, and lack of spatial resolution limit their applicability. On the contrary, higher photosensitizing yields, versatile therapies, and a unique spatial resolution are available with engineered two-photon-sensitive organosilica particles that selectively impact tumors while healthy tissues remain untouched. Patients suffering pathologies such as retinoblastoma, breast, and skin cancers will greatly benefit from TPE-NIR ultrasensitive diagnosis and therapy. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  14. Means and method for calibrating a photon detector utilizing electron-photon coincidence

    NASA Technical Reports Server (NTRS)

    Srivastava, S. K. (Inventor)

    1984-01-01

    An arrangement for calibrating a photon detector particularly applicable for the ultraviolet and vacuum ultraviolet regions is based on electron photon coincidence utilizing crossed electron beam atom beam collisions. Atoms are excited by electrons which lose a known amount of energy and scatter with a known remaining energy, while the excited atoms emit photons of known radiation. Electrons of the known remaining energy are separated from other electrons and are counted. Photons emitted in a direction related to the particular direction of scattered electrons are detected to serve as a standard. Each of the electrons is used to initiate the measurements of a time interval which terminates with the arrival of a photon exciting the photon detector. Only the number of time intervals related to the coincidence correlation and of electrons scattered in the particular direction with the known remaining energy and photons of a particular radiation level emitted due to the collisions of such scattered electrons are counted. The detector calibration is related to the number of counted electrons and photons.

  15. Tunable optical coherence tomography in the infrared range using visible photons

    NASA Astrophysics Data System (ADS)

    Paterova, Anna V.; Yang, Hongzhi; An, Chengwu; Kalashnikov, Dmitry A.; Krivitsky, Leonid A.

    2018-04-01

    Optical coherence tomography (OCT) is an appealing technique for bio-imaging, medicine, and material analysis. For many applications, OCT in mid- and far-infrared (IR) leads to significantly more accurate results. Reported mid-IR OCT systems require light sources and photodetectors which operate in mid-IR range. These devices are expensive and need cryogenic cooling. Here, we report a proof-of-concept demonstration of a wavelength tunable IR OCT technique with detection of only visible range photons. Our method is based on the nonlinear interference of frequency correlated photon pairs. The nonlinear crystal, introduced in the Michelson-type interferometer, generates photon pairs with one photon in the visible and another in the IR range. The intensity of detected visible photons depends on the phase and loss of IR photons, which interact with the sample under study. This enables us to characterize sample properties and perform imaging in the IR range by detecting visible photons. The technique possesses broad wavelength tunability and yields a fair axial and lateral resolution, which can be tailored to the specific application. The work contributes to the development of versatile 3D imaging and material characterization systems working in a broad range of IR wavelengths, which do not require the use of IR-range light sources and photodetectors.

  16. Uncooled infrared photon detection concepts and devices

    NASA Astrophysics Data System (ADS)

    Piyankarage, Viraj Vishwakantha Jayaweera

    This work describes infrared (IR) photon detector techniques based on novel semiconductor device concepts and detector designs. The aim of the investigation was to examine alternative IR detection concepts with a view to resolve some of the issues of existing IR detectors such as operating temperature and response range. Systems were fabricated to demonstrate the following IR detection concepts and determine detector parameters: (i) Near-infrared (NIR) detection based on dye-sensitization of nanostructured semiconductors, (ii) Displacement currents in semiconductor quantum dots (QDs) embedded dielectric media, (iii) Split-off band transitions in GaAs/AlGaAs heterojunction interfacial workfunction internal photoemission (HEIWIP) detectors. A far-infrared detector based on GaSb homojunction interfacial workfunction internal photoemission (HIWIP) structure is also discussed. Device concepts, detector structures, and experimental results discussed in the text are summarized below. Dye-sensitized (DS) detector structures consisting of n-TiO 2/Dye/p-CuSCN heterostructures with several IR-sensitive dyes showed response peaks at 808, 812, 858, 866, 876, and 1056 nm at room temperature. The peak specific-detectivity (D*) was 9.5x1010 cm Hz-1/2 W-1 at 812 nm at room temperature. Radiation induced carrier generation alters the electronic polarizability of QDs provided the quenching of excitation is suppressed by separation of the QDs. A device constructed to illustrate this concept by embedding PbS QDs in paraffin wax showed a peak D* of 3x108 cm Hz 1/2 W-1 at ˜540 nm at ambient temperature. A typical HEIWIP/HIWIP detector structures consist of single (or multiple) period(s) of doped emitter(s) and undoped barrier(s) which are sandwiched between two highly doped contact layers. A p-GaAs/AlGaAs HEIWIP structure showed enhanced absorption in NIR range due to heavy/light-hole band to split-off band transitions and leading to the development of GaAs based uncooled sensors for IR

  17. Interplay of Zero-Field Splitting and Excited State Geometry Relaxation in fac-Ir(ppy)3.

    PubMed

    Gonzalez-Vazquez, José P; Burn, Paul L; Powell, Benjamin J

    2015-11-02

    The lowest energy triplet state, T1, of organometallic complexes based on iridium(III) is of fundamental interest, as the behavior of molecules in this state determines the suitability of the complex for use in many applications, e.g., organic light-emitting diodes. Previous characterization of T1 in fac-Ir(ppy)3 suggests that the trigonal symmetry of the complex is weakly broken in the excited state. Here we report relativistic time dependent density functional calculations of the zero-field splitting (ZFS) of fac-Ir(ppy)3 in the ground state (S0) and lowest energy triplet (T1) geometries and at intermediate geometries. We show that the energy scale of the geometry relaxation in the T1 state is large compared to the ZFS. Thus, the natural analysis of the ZFS and the radiative decay rates, based on the assumption that the structural distortion is a small perturbation, fails dramatically. In contrast, our calculations of these quantities are in good agreement with experiment.

  18. Nonlinear optical and multiphoton processes for in situ manipulation and conversion of photons: applications to energy and healthcare (Conference Presentation)

    NASA Astrophysics Data System (ADS)

    Prasad, Paras N.

    2017-02-01

    Chiral control of nonlinear optical functions holds a great promise for a wide range of applications including optical signal processing, bio-sensing and chiral bio-imaging. In chiral polyfluorene thin films, we demonstrated extremely large chiral nonlinearity. The physics of manipulating excitation dynamics for photon transformation will be discussed, along with nanochemistry control of upconversion in hierarchically built organic chromophore coupled-core-multiple shell nanostructures which enable introduce new, organic-inorganic energy transfer routes for broadband light harvesting and increased upconversion efficiency via multistep cascaded energy transfer. We are pursuing the applications of photon conversion technology in IR harvesting for photovoltaics, high contrast bioimaging, photoacoustic imaging, photodynamic therapy, and optogenetics. An important application is in Brain research and Neurophotonics for functional mapping and modulation of brain activities. Another new direction pursued is magnetic field control of light in in a chiral polymer nanocomposite to achieve large magneto-optic coefficient which can enable sensing of extremely weak magnetic field due to brain waves. Finally, we will consider the thought provoking concept of utilizing photons to quantify, through magneto-optics, and augment - through nanoptogenetics, the cognitive states, thus paving the path way to a quantified human paradigm.

  19. Entanglement of Two Superconducting Qubits in a Waveguide Cavity via Monochromatic Two-Photon Excitation

    NASA Astrophysics Data System (ADS)

    Poletto, S.; Gambetta, Jay M.; Merkel, Seth T.; Smolin, John A.; Chow, Jerry M.; Córcoles, A. D.; Keefe, George A.; Rothwell, Mary B.; Rozen, J. R.; Abraham, D. W.; Rigetti, Chad; Steffen, M.

    2012-12-01

    We report a system where fixed interactions between noncomputational levels make bright the otherwise forbidden two-photon |00⟩→|11⟩ transition. The system is formed by hand selection and assembly of two discrete component transmon-style superconducting qubits inside a rectangular microwave cavity. The application of a monochromatic drive tuned to this transition induces two-photon Rabi-like oscillations between the ground and doubly excited states via the Bell basis. The system therefore allows all-microwave two-qubit universal control with the same techniques and hardware required for single qubit control. We report Ramsey-like and spin echo sequences with the generated Bell states, and measure a two-qubit gate fidelity of Fg=90% (unconstrained) and 86% (maximum likelihood estimator).

  20. Entanglement of two superconducting qubits in a waveguide cavity via monochromatic two-photon excitation.

    PubMed

    Poletto, S; Gambetta, Jay M; Merkel, Seth T; Smolin, John A; Chow, Jerry M; Córcoles, A D; Keefe, George A; Rothwell, Mary B; Rozen, J R; Abraham, D W; Rigetti, Chad; Steffen, M

    2012-12-14

    We report a system where fixed interactions between noncomputational levels make bright the otherwise forbidden two-photon |00}→|11} transition. The system is formed by hand selection and assembly of two discrete component transmon-style superconducting qubits inside a rectangular microwave cavity. The application of a monochromatic drive tuned to this transition induces two-photon Rabi-like oscillations between the ground and doubly excited states via the Bell basis. The system therefore allows all-microwave two-qubit universal control with the same techniques and hardware required for single qubit control. We report Ramsey-like and spin echo sequences with the generated Bell states, and measure a two-qubit gate fidelity of F(g)=90% (unconstrained) and 86% (maximum likelihood estimator).

  1. Semi-active control of a cable-stayed bridge under multiple-support excitations.

    PubMed

    Dai, Ze-Bing; Huang, Jin-Zhi; Wang, Hong-Xia

    2004-03-01

    This paper presents a semi-active strategy for seismic protection of a benchmark cable-stayed bridge with consideration of multiple-support excitations. In this control strategy, Magnetorheological (MR) dampers are proposed as control devices, a LQG-clipped-optimal control algorithm is employed. An active control strategy, shown in previous researches to perform well at controlling the benchmark bridge when uniform earthquake motion was assumed, is also used in this study to control this benchmark bridge with consideration of multiple-support excitations. The performance of active control system is compared to that of the presented semi-active control strategy. Because the MR fluid damper is a controllable energy- dissipation device that cannot add mechanical energy to the structural system, the proposed control strategy is fail-safe in that bounded-input, bounded-output stability of the controlled structure is guaranteed. The numerical results demonstrated that the performance of the presented control design is nearly the same as that of the active control system; and that the MR dampers can effectively be used to control seismically excited cable-stayed bridges with multiple-support excitations.

  2. Electron dynamics and prompt ablation of aluminum surface excited by intense femtosecond laser pulse

    NASA Astrophysics Data System (ADS)

    Ionin, A. A.; Kudryashov, S. I.; Makarov, S. V.; Seleznev, L. V.; Sinitsyn, D. V.

    2014-12-01

    Thin aluminum film homogeneously heated by intense IR femtosecond laser pulses exhibits on the excitation timescale consequent fluence-dependent rise and drop of the IR-pump self-reflectivity, followed by its final saturation at higher fluences F > 0.3 J/cm2. This prompt optical dynamics correlates with the initial monotonic increase in the accompanying laser-induced electron emission, which is succeeded by its non-linear (three-photon) increase for F > 0.3 J/cm2. The underlying electronic dynamics is related to the initial saturation of IR resonant interband transitions in this material, followed by its strong instantaneous electronic heating via intraband transitions during the pump pulse resulting in thermionic emission. Above the threshold fluence of 0.3 J/cm2, the surface electronic heating is balanced during the pump pulse by simultaneous cooling via intense plasma removal (prompt ablation). The relationship between the deposited volume energy density in the film and its prompt electronic temperature derived from the self-reflection measurements using a Drude model, demonstrates a kind of electron "liquid-vapor" phase transition, driven by strong cubic optical non-linearity of the photo-excited aluminum.

  3. Bulky Counterions: Enhancing the Two-Photon Excited Fluorescence of Gold Nanoclusters.

    PubMed

    Bertorelle, Franck; Moulin, Christophe; Soleilhac, Antonin; Comby-Zerbino, Clothilde; Dugourd, Philippe; Russier-Antoine, Isabelle; Brevet, Pierre-François; Antoine, Rodolphe

    2018-01-19

    Increasing fluorescence quantum yields of ligand-protected gold nanoclusters has attracted wide research interest. The strategy consisting in using bulky counterions has been found to dramatically enhance the fluorescence. In this Communication, we push forward this concept to the nonlinear optical regime. We show that by an appropriate choice of bulky counterions and of solvent, a 30-fold increase in two-photon excited fluorescence (TPEF) signal at ≈600 nm for gold nanoclusters can be obtained. This would correspond to a TPEF cross-section in the range of 0.1 to 1 GM. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  4. Ultrafast studies of the excited-state dynamics of copper and nickel phthalocyanine tetrasulfonates: potential sensitizers for the two-photon photodynamic therapy of tumors.

    PubMed

    Fournier, Michel; Pépin, Claude; Houde, Daniel; Ouellet, René; van Lier, Johan E

    2004-01-01

    In order to evaluate the potential of copper and nickel phthalocyanine tetrasulfonates as sensitizers for two-photon photodynamic therapy, we conducted kinetic femtosecond measurements of transient absorption and bleaching of their excited state dynamics in aqueous solution. Samples were pumped with 620 nm and 310 nm laser light, which allowed us to study relaxation processes from both the first and second singlet (or doublet for the copper phthalocyanine) excited states. A second excitation from the first excited triplet state, approximately 685 and 105 ps after the first excitation for copper and nickel phthalocyanine tetrasulfonate respectively, was the most efficient way to bring the molecules to an upper triplet state. Presumably this highest triplet state can inflict molecular damage on adjacent biomolecules int eh absence of oxygen, resulting in the desired cytotoxic cellular response. Transient absorption spectra at different fixed delays indicate that optimum efficiency would require that the second photon has a wavelength of approximately 750 nm.

  5. Coherent blue emission generated by Rb two-photon excitation using diode and femtosecond lasers

    NASA Astrophysics Data System (ADS)

    Lopez, Jesus P.; Moreno, Marco P.; de Miranda, Marcio H. G.; Vianna, Sandra S.

    2017-04-01

    The coherent blue light generated in rubidium vapor due to the combined action of an ultrashort pulse train and a continuous wave diode laser is investigated. Each step of the two-photon transition 5S-5P{}3/2-5D is excited by one of the lasers, and the induced coherence between the 5S and 6P{}3/2 states is responsible for generating the blue beam. Measurements of the excitation spectrum reveal the frequency comb structure and allow us to identify the resonant modes responsible for inducing the nonlinear process. Further, each resonant mode excites a different group of atoms, making the process selective in atomic velocity. The signal dependency on the atomic density is characterized by a sharp growth and a rapid saturation. We also show that for high intensity of the diode laser, the Stark shift at resonance causes the signal suppression observed at low atomic density.

  6. Optical Anisotropy of Photonic Crystals of Cubic Symmetry Induced by Multiple Diffraction of Light

    NASA Astrophysics Data System (ADS)

    Ukleev, T. A.; Shevchenko, N. N.; Iurasova, D. I.; Sel'kin, A. V.

    2018-05-01

    The optical spectra of Bragg reflection from opal-like photonic crystals under conditions of the resonant enhancement of the multiple diffraction of light have been studied experimentally and theoretically using the photonic crystal structures prepared of monodisperse polystyrene globules. It is shown that the reflection signal registered in mutually orthogonal configurations of the polarizer and analyzer is related to the intrinsic optical anisotropy of the crystals and is a specific manifestation of the multiple Bragg diffraction in three-dimensional photonic crystals.

  7. Optical nonlinearities of colloidal InP@ZnS core-shell quantum dots probed by Z-scan and two-photon excited emission

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

    Wawrzynczyk, Dominika; Szeremeta, Janusz; Samoc, Marek

    Spectrally resolved nonlinear optical properties of colloidal InP@ZnS core-shell quantum dots of various sizes were investigated with the Z-scan technique and two-photon fluorescence excitation method using a femtosecond laser system tunable in the range from 750 nm to 1600 nm. In principle, both techniques should provide comparable results and can be interchangeably used for determination of the nonlinear optical absorption parameters, finding maximal values of the cross sections and optimizing them. We have observed slight differences between the two-photon absorption cross sections measured by the two techniques and attributed them to the presence of non-radiative paths of absorption or relaxation.more » The most significant value of two-photon absorption cross section σ{sub 2} for 4.3 nm size InP@ZnS quantum dot was equal to 2200 GM, while the two-photon excitation action cross section σ{sub 2}Φ was found to be 682 GM at 880 nm. The properties of these cadmium-free colloidal quantum dots can be potentially useful for nonlinear bioimaging.« less

  8. Optical nonlinearities of colloidal InP@ZnS core-shell quantum dots probed by Z-scan and two-photon excited emission

    NASA Astrophysics Data System (ADS)

    Wawrzynczyk, Dominika; Szeremeta, Janusz; Samoc, Marek; Nyk, Marcin

    2015-11-01

    Spectrally resolved nonlinear optical properties of colloidal InP@ZnS core-shell quantum dots of various sizes were investigated with the Z-scan technique and two-photon fluorescence excitation method using a femtosecond laser system tunable in the range from 750 nm to 1600 nm. In principle, both techniques should provide comparable results and can be interchangeably used for determination of the nonlinear optical absorption parameters, finding maximal values of the cross sections and optimizing them. We have observed slight differences between the two-photon absorption cross sections measured by the two techniques and attributed them to the presence of non-radiative paths of absorption or relaxation. The most significant value of two-photon absorption cross section σ2 for 4.3 nm size InP@ZnS quantum dot was equal to 2200 GM, while the two-photon excitation action cross section σ2Φ was found to be 682 GM at 880 nm. The properties of these cadmium-free colloidal quantum dots can be potentially useful for nonlinear bioimaging.

  9. Multiple Weyl points and the sign change of their topological charges in woodpile photonic crystals

    NASA Astrophysics Data System (ADS)

    Chang, Ming-Li; Xiao, Meng; Chen, Wen-Jie; Chan, C. T.

    2017-03-01

    We show that Weyl points with topological charges 1 and 2 can be found in very simple chiral woodpile photonic crystals and the distribution of the charges can be changed by changing the material parameters without altering space-group symmetry. The underlying physics can be understood through a tight-binding model. Gapless surface states and their backscattering immune properties also are demonstrated in these systems. Obtaining Weyl points in these easily fabricated woodpile photonic crystals will facilitate the realization of Weyl point physics in optical and IR frequencies.

  10. Electronic absorption and MCD spectra of M sub 2 (TMB) sub 4 sup 2+ , M = Rh and Ir. A valence-bond description of the upper electronic excited states

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

    Smith, D.C.; Miskowski, V.M.; Gray, H.B.

    1990-05-09

    Electronic absorption and magnetic circular dichroism (MCD) spectra of Rh{sub 2}(TMB){sub 4}{sup 2+} and Ir{sub 2}(TMB){sub 4}{sup 2+} are reported along with polarized single-crystal absorption spectra of (Ir{sub 2}(TMB){sub 4})(B(C{sub 6}H{sub 5}){sub 4}){sub 2} {times} CH{sub 3}C{sub 6}H{sub 5} (TMB = 2,5-diisocyano-2,5-dimethylhexane). Interpretation of the spectra is based on a valence-bond model that accommodates highly perturbed dimer transitions as well as monomer-like dimer excitations. In this model, half of the dimer electronic excited states possess ionic character; these states involve metal-to-metal charge transfer (MMCT). The most prominent of the weak features ({approximately} 430 nm) is assigned to the transition tomore » {sup 1}A{sub 1g} (a single-center d{sub z{sup 2}} {yields} p{sub z} excitation). High-energy features ({lambda} < 300 nm) in the spectra of Rh{sub 2}(TMB){sub 4}{sup 2+} and Ir{sub 2}(TMB){sub 4}{sup 2+} are assigned to MMCT arising from d{sub xzyz} {yields} p{sub z} excitations.« less

  11. Photolysis of caged calcium in femtoliter volumes using two-photon excitation.

    PubMed Central

    Brown, E B; Shear, J B; Adams, S R; Tsien, R Y; Webb, W W

    1999-01-01

    A new technique for the determination of the two-photon uncaging action cross section (deltau) of photolyzable calcium cages is described. This technique is potentially applicable to other caged species that can be chelated by a fluorescent indicator dye, as well as caged fluorescent compounds. The two-photon action cross sections of three calcium cages, DM-nitrophen, NP-EGTA, and azid-1, are studied in the range of excitation wavelengths between 700 and 800 nm. Azid-1 has a maximum deltau of approximately 1.4 GM at 700 nm, DM-nitrophen has a maximum deltau of approximately 0.013 GM at 730 nm, and NP-EGTA has no measurable uncaging yield. The equations necessary to predict the amount of cage photolyzed and the temporal behavior of the liberated calcium distribution under a variety of conditions are derived. These equations predict that by using 700-nm light from a Ti:sapphire laser focused with a 1.3-NA objective, essentially all of the azid-1 within the two-photon focal volume would be photolyzed with a 10-micros pulse train of approximately 7 mW average power. The initially localized distributions of free calcium will dissipate rapidly because of diffusion of free calcium and uptake by buffers. In buffer-free cytoplasm, the elevation of the calcium concentration at the center of the focal volume is expected to last for approximately 165 micros. PMID:9876162

  12. Search for Excited or Exotic Electron Production Using the Dielectron + Photon Signature at CDF in Run II

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

    Gerberich, Heather Kay

    The author presents a search for excited or exotic electrons decaying to an electron and a photon with high transverse momentum. An oppositely charged electron is produced in association with the excited electron, yielding a final state dielectron + photon signature. The discovery of excited electrons would be a first indication of lepton compositeness. They use ~ 202 pb -1 of data collected in pmore » $$\\bar{p}$$ collisions at √s = 1.96 TeV with the Collider Detector at Fermilab during March 2001 through September 2003. The data are consistent with standard model expectations. Upper limits are set on the experimental cross-section σ($$\\bar{p}$$p → ee* → eeγ) at the 95% confidence level in a contact-interaction model and a gauge-mediated interaction model. Limits are also presented as exclusion regions in the parameter space of the excited electron mass (M e*) and the compositeness energy scale (Λ). In the contact-interaction model, for which there are no previously published limits, they find M e* < 906 GeV is excluded for M e* = Λ. In the gauge-mediated model, the exclusion region in the M e* versus the phenomenological coupling f/Λ parameter space is extended to M{sub e*} < 430 GeV for f/Λ ~ 10 -2 GeV -1. In comparison, other experiments have excluded M e* < 280 GeV for f/Λ ~ 10 -2 GeV -1.« less

  13. Optimizing ultrafast wide field-of-view illumination for high-throughput multi-photon imaging and screening of mutant fluorescent proteins

    NASA Astrophysics Data System (ADS)

    Stoltzfus, Caleb; Mikhailov, Alexandr; Rebane, Aleksander

    2017-02-01

    Fluorescence induced by 1wo-photon absorption (2PA) and three-photon absorption (3PA) is becoming an increasingly important tool for deep-tissue microscopy, especially in conjunction with genetically-encoded functional probes such as fluorescent proteins (FPs). Unfortunately, the efficacy of the multi-photon excitation of FPs is notoriously low, and because relations between a biological fluorophore's nonlinear-optical properties and its molecular structure are inherently complex, there are no practical avenues available that would allow boosting the performance of current FPs. Here we describe a novel method, where we apply directed evolution to optimize the 2PA properties of EGFP. Key to the success of this approach consists in high-throughput screening of mutants that would allow selection of variants with promising 2PA and 3PA properties in a broad near-IR excitation range of wavelength. For this purpose, we construct and test a wide field-of-view (FOV), femtosecond imaging system that we then use to quantify the multi-photon excited fluorescence in the 550- 1600 nm range of tens of thousands of E. coli colonies expressing randomly mutated FPs in a standard 10 cm diameter Petri dish configuration. We present a quantitative analysis of different factors that are currently limiting the maximum throughput of the femtosecond multi-photon screening techniques and also report on quantitative measurement of absolute 2PA and 3PA cross sections spectra.

  14. Imaging-guided two-photon excitation-emission-matrix measurements of human skin tissues

    NASA Astrophysics Data System (ADS)

    Yu, Yingqiu; Lee, Anthony M. D.; Wang, Hequn; Tang, Shuo; Zhao, Jianhua; Lui, Harvey; Zeng, Haishan

    2012-07-01

    There are increased interests on using multiphoton imaging and spectroscopy for skin tissue characterization and diagnosis. However, most studies have been done with just a few excitation wavelengths. Our objective is to perform a systematic study of the two-photon fluorescence (TPF) properties of skin fluorophores, normal skin, and diseased skin tissues. A nonlinear excitation-emission-matrix (EEM) spectroscopy system with multiphoton imaging guidance was constructed. A tunable femtosecond laser was used to vary excitation wavelengths from 730 to 920 nm for EEM data acquisition. EEM measurements were performed on excised fresh normal skin tissues, seborrheic keratosis tissue samples, and skin fluorophores including: NADH, FAD, keratin, melanin, collagen, and elastin. We found that in the stratum corneum and upper epidermis of normal skin, the cells have large sizes and the TPF originates from keratin. In the lower epidermis, cells are smaller and TPF is dominated by NADH contributions. In the dermis, TPF is dominated by elastin components. The depth resolved EEM measurements also demonstrated that keratin structure has intruded into the middle sublayers of the epidermal part of the seborrheic keratosis lesion. These results suggest that the imaging guided TPF EEM spectroscopy provides useful information for the development of multiphoton clinical devices for skin disease diagnosis.

  15. Comparison of the hypothetical 57Co brachytherapy source with the 192Ir source

    PubMed Central

    Toossi, Mohammad Taghi Bahreyni; Rostami, Atefeh; Khosroabadi, Mohsen; Khademi, Sara; Knaup, Courtney

    2016-01-01

    Aim of the study The 57Co radioisotope has recently been proposed as a hypothetical brachytherapy source due to its high specific activity, appropriate half-life (272 days) and medium energy photons (114.17 keV on average). In this study, Task Group No. 43 dosimetric parameters were calculated and reported for a hypothetical 57Co source. Material and methods A hypothetical 57Co source was simulated in MCNPX, consisting of an active cylinder with 3.5 mm length and 0.6 mm radius encapsulated in a stainless steel capsule. Three photon energies were utilized (136 keV [10.68%], 122 keV [85.60%], 14 keV [9.16%]) for the 57Co source. Air kerma strength, dose rate constant, radial dose function, anisotropy function, and isodose curves for the source were calculated and compared to the corresponding data for a 192Ir source. Results The results are presented as tables and figures. Air kerma strength per 1 mCi activity for the 57Co source was 0.46 cGyh–1 cm 2 mCi–1. The dose rate constant for the 57Co source was determined to be 1.215 cGyh–1U–1. The radial dose function for the 57Co source has an increasing trend due to multiple scattering of low energy photons. The anisotropy function for the 57Co source at various distances from the source is more isotropic than the 192Ir source. Conclusions The 57Co source has advantages over 192Ir due to its lower energy photons, longer half-life, higher dose rate constant and more isotropic anisotropic function. However, the 192Ir source has a higher initial air kerma strength and more uniform radial dose function. These properties make 57Co a suitable source for use in brachytherapy applications. PMID:27688731

  16. Analysis of deterministic swapping of photonic and atomic states through single-photon Raman interaction

    NASA Astrophysics Data System (ADS)

    Rosenblum, Serge; Borne, Adrien; Dayan, Barak

    2017-03-01

    The long-standing goal of deterministic quantum interactions between single photons and single atoms was recently realized in various experiments. Among these, an appealing demonstration relied on single-photon Raman interaction (SPRINT) in a three-level atom coupled to a single-mode waveguide. In essence, the interference-based process of SPRINT deterministically swaps the qubits encoded in a single photon and a single atom, without the need for additional control pulses. It can also be harnessed to construct passive entangling quantum gates, and can therefore form the basis for scalable quantum networks in which communication between the nodes is carried out only by single-photon pulses. Here we present an analytical and numerical study of SPRINT, characterizing its limitations and defining parameters for its optimal operation. Specifically, we study the effect of losses, imperfect polarization, and the presence of multiple excited states. In all cases we discuss strategies for restoring the operation of SPRINT.

  17. Two-photon excitation of nitric oxide fluorescence as a temperature indicator in unsteady gas-dynamic processes

    NASA Technical Reports Server (NTRS)

    Mckenzie, R. L.; Gross, K. P.

    1980-01-01

    A laser induced fluorescence technique, suitable for measuring fluctuating temperatures in cold turbulent flows containing very low concentrations of nitric oxide is described. Temperatures below 300 K may be resolved with signal to noise ratios greater than 50 to 1 using high peak power, tunable dye lasers. The method relies on the two photon excitation of selected ro-vibronic transitions. The analysis includes the effects of fluorescence quenching and shows the technique to be effective at all densities below ambient. Signal to noise ratio estimates are based on a preliminary measurement of the two photon absorptivity for a selected rotational transition in the NO gamma (0,0) band.

  18. Two-photon excited photoconversion of cyanine-based dyes

    NASA Astrophysics Data System (ADS)

    Kwok, Sheldon J. J.; Choi, Myunghwan; Bhayana, Brijesh; Zhang, Xueli; Ran, Chongzhao; Yun, Seok-Hyun

    2016-03-01

    The advent of phototransformable fluorescent proteins has led to significant advances in optical imaging, including the unambiguous tracking of cells over large spatiotemporal scales. However, these proteins typically require activating light in the UV-blue spectrum, which limits their in vivo applicability due to poor light penetration and associated phototoxicity on cells and tissue. We report that cyanine-based, organic dyes can be efficiently photoconverted by nonlinear excitation at the near infrared (NIR) window. Photoconversion likely involves singlet-oxygen mediated photochemical cleavage, yielding blue-shifted fluorescent products. Using SYTO62, a biocompatible and cell-permeable dye, we demonstrate photoconversion in a variety of cell lines, including depth-resolved labeling of cells in 3D culture. Two-photon photoconversion of cyanine-based dyes offer several advantages over existing photoconvertible proteins, including use of minimally toxic NIR light, labeling without need for genetic intervention, rapid kinetics, remote subsurface targeting, and long persistence of photoconverted signal. These findings are expected to be useful for applications involving rapid labeling of cells deep in tissue.

  19. Magnetic structure and excitation spectrum of the hyperhoneycomb Kitaev magnet β -Li2IrO3

    NASA Astrophysics Data System (ADS)

    Ducatman, Samuel; Rousochatzakis, Ioannis; Perkins, Natalia B.

    2018-03-01

    We present a theoretical study of the static and dynamical properties of the three-dimensional, hyperhoneycomb Kitaev magnet β -Li2IrO3 . We argue that the observed incommensurate order can be understood in terms of a long-wavelength twisting of a nearby commensurate period-3 state, with the same key qualitatively features. The period-3 state shows very different structure when either the Kitaev interaction K or the off-diagonal exchange anisotropy Γ is dominant. A comparison of the associated static spin structure factors with reported scattering experiments in zero and finite fields gives strong evidence that β -Li2IrO3 lies in the regime of dominant Kitaev coupling, and that the Heisenberg exchange J is much weaker than both K and Γ . Our predictions for the magnon excitation spectra, the dynamical spin structure factors, and their polarization dependence provide additional distinctive fingerprints that can be checked experimentally.

  20. Simulations of the infrared, Raman, and 2D-IR photon echo spectra of water in nanoscale silica pores

    DOE PAGES

    Burris, Paul C.; Laage, Damien; Thompson, Ward H.

    2016-05-20

    Vibrational spectroscopy is frequently used to characterize nanoconfined liquids and probe the effect of the confining framework on the liquid structure and dynamics relative to the corresponding bulk fluid. However, it is still unclear what molecular-level information can be obtained from such measurements. In this Paper, we address this question by using molecular dynamics (MD) simulations to reproduce the linear infrared (IR), Raman, and two-dimensional IR (2D-IR) photon echo spectra for water confined within hydrophilic (hydroxyl-terminated) silica mesopores. To simplify the spectra the OH stretching region of isotopically dilute HOD in D 2O is considered. An empirical mapping approach ismore » used to obtain the OH vibrational frequencies, transition dipoles, and transition polarizabilities from the MD simulations. The simulated linear IR and Raman spectra are in good general agreement with measured spectra of water in mesoporous silica reported in the literature. The key effect of confinement on the water spectrum is a vibrational blueshift for OH groups that are closest to the pore interface. The blueshift can be attributed to the weaker hydrogen bonds (H-bonds) formed between the OH groups and silica oxygen acceptors. Non-Condon effects greatly diminish the contribution of these OH moieties to the linear IR spectrum, but these weaker H-bonds are readily apparent in the Raman spectrum. The 2D-IR spectra have not yet been measured and thus the present results represent a prediction. Lastly, the simulated spectra indicate that it should be possible to probe the slower spectral diffusion of confined water compared to the bulk liquid by analysis of the 2D-IR spectra.« less

  1. Simulations of the infrared, Raman, and 2D-IR photon echo spectra of water in nanoscale silica pores.

    PubMed

    Burris, Paul C; Laage, Damien; Thompson, Ward H

    2016-05-21

    Vibrational spectroscopy is frequently used to characterize nanoconfined liquids and probe the effect of the confining framework on the liquid structure and dynamics relative to the corresponding bulk fluid. However, it is still unclear what molecular-level information can be obtained from such measurements. In this paper, we address this question by using molecular dynamics (MD) simulations to reproduce the linear infrared (IR), Raman, and two-dimensional IR (2D-IR) photon echo spectra for water confined within hydrophilic (hydroxyl-terminated) silica mesopores. To simplify the spectra the OH stretching region of isotopically dilute HOD in D2O is considered. An empirical mapping approach is used to obtain the OH vibrational frequencies, transition dipoles, and transition polarizabilities from the MD simulations. The simulated linear IR and Raman spectra are in good general agreement with measured spectra of water in mesoporous silica reported in the literature. The key effect of confinement on the water spectrum is a vibrational blueshift for OH groups that are closest to the pore interface. The blueshift can be attributed to the weaker hydrogen bonds (H-bonds) formed between the OH groups and silica oxygen acceptors. Non-Condon effects greatly diminish the contribution of these OH moieties to the linear IR spectrum, but these weaker H-bonds are readily apparent in the Raman spectrum. The 2D-IR spectra have not yet been measured and thus the present results represent a prediction. The simulated spectra indicates that it should be possible to probe the slower spectral diffusion of confined water compared to the bulk liquid by analysis of the 2D-IR spectra.

  2. Simulations of the infrared, Raman, and 2D-IR photon echo spectra of water in nanoscale silica pores

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

    Burris, Paul C.; Thompson, Ward H., E-mail: wthompson@ku.edu; Laage, Damien, E-mail: damien.laage@ens.fr

    2016-05-21

    Vibrational spectroscopy is frequently used to characterize nanoconfined liquids and probe the effect of the confining framework on the liquid structure and dynamics relative to the corresponding bulk fluid. However, it is still unclear what molecular-level information can be obtained from such measurements. In this paper, we address this question by using molecular dynamics (MD) simulations to reproduce the linear infrared (IR), Raman, and two-dimensional IR (2D-IR) photon echo spectra for water confined within hydrophilic (hydroxyl-terminated) silica mesopores. To simplify the spectra the OH stretching region of isotopically dilute HOD in D{sub 2}O is considered. An empirical mapping approach ismore » used to obtain the OH vibrational frequencies, transition dipoles, and transition polarizabilities from the MD simulations. The simulated linear IR and Raman spectra are in good general agreement with measured spectra of water in mesoporous silica reported in the literature. The key effect of confinement on the water spectrum is a vibrational blueshift for OH groups that are closest to the pore interface. The blueshift can be attributed to the weaker hydrogen bonds (H-bonds) formed between the OH groups and silica oxygen acceptors. Non-Condon effects greatly diminish the contribution of these OH moieties to the linear IR spectrum, but these weaker H-bonds are readily apparent in the Raman spectrum. The 2D-IR spectra have not yet been measured and thus the present results represent a prediction. The simulated spectra indicates that it should be possible to probe the slower spectral diffusion of confined water compared to the bulk liquid by analysis of the 2D-IR spectra.« less

  3. Holographic 3D multi-spot two-photon excitation for fast optical stimulation in brain

    NASA Astrophysics Data System (ADS)

    Takiguchi, Yu; Toyoda, Haruyoshi

    2017-04-01

    We report here a holographic high speed accessing microscope of sensory-driven synaptic activity across all inputs to single living neurons in the context of the intact cerebral cortex. This system is based on holographic multiple beam generation with spatial light modulator, we have demonstrated performance of the holographic excitation efficiency in several in vitro prototype system. 3D weighted iterative Fourier Transform method using the Ewald sphere in consideration of calculation speed has been adopted; multiple locations can be patterned in 3D with single hologram. Standard deviation of intensities of spots are still large due to the aberration of the system and/or hologram calculation, we successfully excited multiple locations of neurons in living mouse brain to monitor the calcium signals.

  4. Nitric oxide excited under auroral conditions: Excited state densities and band emissions

    NASA Astrophysics Data System (ADS)

    Cartwright, D. C.; Brunger, M. J.; Campbell, L.; Mojarrabi, B.; Teubner, P. J. O.

    2000-09-01

    Electron impact excitation of vibrational levels in the ground electronic state and nine excited electronic states in NO has been simulated for an IBC II aurora (i.e., ˜10 kR in 3914 Å radiation) in order to predict NO excited state number densities and band emission intensities. New integral electron impact excitation cross sections for NO were combined with a measured IBC II auroral secondary electron distribution, and the vibrational populations of 10 NO electronic states were determined under conditions of statistical equilibrium. This model predicts an extended vibrational distribution in the NO ground electronic state produced by radiative cascade from the seven higher-lying doublet excited electronic states populated by electron impact. In addition to significant energy storage in vibrational excitation of the ground electronic state, both the a 4Π and L2 Φ excited electronic states are predicted to have relatively high number densities because they are only weakly connected to lower electronic states by radiative decay. Fundamental mode radiative transitions involving the lowest nine excited vibrational levels in the ground electronic state are predicted to produce infrared (IR) radiation from 5.33 to 6.05 μm with greater intensity than any single NO electronic emission band. Fundamental mode radiative transitions within the a 4Π electronic state, in the 10.08-11.37 μm region, are predicted to have IR intensities comparable to individual electronic emission bands in the Heath and ɛ band systems. Results from this model quantitatively predict the vibrational quantum number dependence of the NO IR measurements of Espy et al. [1988].

  5. A single-photon fluorescence and multi-photon spectroscopic study of atherosclerotic lesions

    NASA Astrophysics Data System (ADS)

    Smith, Michael S. D.; Ko, Alex C. T.; Ridsdale, Andrew; Schattka, Bernie; Pegoraro, Adrian; Hewko, Mark D.; Shiomi, Masashi; Stolow, Albert; Sowa, Michael G.

    2009-06-01

    In this study we compare the single-photon autofluorescence and multi-photon emission spectra obtained from the luminal surface of healthy segments of artery with segments where there are early atherosclerotic lesions. Arterial tissue was harvested from atherosclerosis-prone WHHL-MI rabbits (Watanabe heritable hyperlipidemic rabbit-myocardial infarction), an animal model which mimics spontaneous myocardial infarction in humans. Single photon fluorescence emission spectra of samples were acquired using a simple spectrofluorometer set-up with 400 nm excitation. Samples were also investigated using a home built multi-photon microscope based on a Ti:sapphire femto-second oscillator. The excitation wavelength was set at 800 nm with a ~100 femto-second pulse width. Epi-multi-photon spectroscopic signals were collected through a fibre-optics coupled spectrometer. While the single-photon fluorescence spectra of atherosclerotic lesions show minimal spectroscopic difference from those of healthy arterial tissue, the multi-photon spectra collected from atherosclerotic lesions show marked changes in the relative intensity of two-photon excited fluorescence (TPEF) and second-harmonic generation (SHG) signals when compared with those from healthy arterial tissue. The observed sharp increase of the relative SHG signal intensity in a plaque is in agreement with the known pathology of early lesions which have increased collagen content.

  6. Differentiation of ocular fundus fluorophores by fluorescence lifetime imaging using multiple excitation and emission wavelengths

    NASA Astrophysics Data System (ADS)

    Hammer, M.; Schweitzer, D.; Schenke, S.; Becker, W.; Bergmann, A.

    2006-10-01

    Ocular fundus autofluorescence imaging has been introduced into clinical diagnostics recently. It is in use for the observation of the age pigment lipofuscin, a precursor of age - related macular degeneration (AMD). But other fluorophores may be of interest too: The redox pair FAD - FADH II provides information on the retinal energy metabolism, advanced glycation end products (AGE) indicate protein glycation associated with pathologic processes in diabetes as well as AMD, and alterations in the fluorescence of collagen and elastin in connective tissue give us the opportunity to observe fibrosis by fluorescence imaging. This, however, needs techniques able to differentiate particular fluorophores despite limited permissible ocular exposure as well as excitation wavelength (limited by the transmission of the human ocular lens to >400 nm). We present an ophthalmic laser scanning system (SLO), equipped with picosecond laser diodes (FWHM 100 ps, 446 nm or 468 nm respectively) and time correlated single photon counting (TCSPC) in two emission bands (500 - 560 nm and 560 - 700 nm). The decays were fitted by a bi-exponential model. Fluorescence spectra were measured by a fluorescence spectrometer fluorolog. Upon excitation at 446 nm, the fluorescence of AGE, FAD, and lipofuscin were found to peak at 503 nm, 525 nm, and 600 nm respectively. Accordingly, the statistical distribution of the fluorescence decay times was found to depend on the different excitation wavelengths and emission bands used. The use of multiple excitation and emission wavelengths in conjunction with fluorescence lifetime imaging allows us to discriminate between intrinsic fluorophores of the ocular fundus. Taken together with our knowledge on the anatomical structure of the fundus, these findings suggest an association of the short, middle and long fluorescence decay time to the retinal pigment epithelium, the retina, and connective tissue respectively.

  7. Ultrafast Spectroscopic Studies of Two-Photon States in Third Order Optical Processes of Dye Chromophores.

    NASA Astrophysics Data System (ADS)

    Yu, Yi-Zhong

    1995-01-01

    Conjugated organic and polymeric materials usually have large, nonresonant third order optical nonlinearity due to correlations of their delocalized pi -electrons. Most materials studied so far show positive values of third order nonlinear susceptibility when all frequencies that generate the third order effect are below any optical transition. A new class of organic molecules, namely indole squarylium (ISQ) and anilinium squarylium (BSQ), exhibit negative < gamma(-omega_4;omega_1, omega_2,omega_3)> when all three frequencies, omega_1, omega_2 and omega_3, lie below the first electronic transition. Although quantum many-electron calculations based on multiple-excitation configuration interaction have shown that the negative third order coefficient is essentially due to the contribution from high-lying two-photon states, the field of experimental studies exploring the microscopic origins of the negative squaraines remains uncultivated. The work presented in this thesis involves extensive experimental investigation of squaraines using techniques such as time-resolved transit absorption spectroscopy and saturable absorption. Theoretical simulations studying nonlinear absorption behavior of a simplified two-level system with ultrashort pulses are also presented. Part of the thesis is dedicated to the development, fabrication and characterization of our ultrafast laser system which offers tunable femtosecond pulses at wavelengths from UV to IR and served as a major tool in the experimental measurements. The dynamics of the population inversion between the ground state and the first excited state was also investigated through time-resolved experiments. The experiment results agree well with the theoretical predictions. Strong couplings between the gateway state and high-lying two-photon states were observed in BSQ squarylium molecules, which suggested a complete quantum calculation with multiple energy levels is required to

  8. Pulse-shaping based two-photon FRET stoichiometry

    PubMed Central

    Flynn, Daniel C.; Bhagwat, Amar R.; Brenner, Meredith H.; Núñez, Marcos F.; Mork, Briana E.; Cai, Dawen; Swanson, Joel A.; Ogilvie, Jennifer P.

    2015-01-01

    Förster Resonance Energy Transfer (FRET) based measurements that calculate the stoichiometry of intermolecular interactions in living cells have recently been demonstrated, where the technique utilizes selective one-photon excitation of donor and acceptor fluorophores to isolate the pure FRET signal. Here, we present work towards extending this FRET stoichiometry method to employ two-photon excitation using a pulse-shaping methodology. In pulse-shaping, frequency-dependent phases are applied to a broadband femtosecond laser pulse to tailor the two-photon excitation conditions to preferentially excite donor and acceptor fluorophores. We have also generalized the existing stoichiometry theory to account for additional cross-talk terms that are non-vanishing under two-photon excitation conditions. Using the generalized theory we demonstrate two-photon FRET stoichiometry in live COS-7 cells expressing fluorescent proteins mAmetrine as the donor and tdTomato as the acceptor. PMID:25836193

  9. Excitation of Bloch surface wave on tapered fiber coated with one-dimensional photonic crystal for refractive index sensing.

    PubMed

    Tu, Tianyu; Pang, Fufei; Zhu, Shan; Cheng, Jiajing; Liu, Huanhuan; Wen, Jianxiang; Wang, Tingyun

    2017-04-17

    We have theoretically and experimentally demonstrated a novel approach to excite Bloch surface wave (BSW) on tapered optical fibers, which are coated with one-dimensional photonic crystal (1DPC) consisting of periodic TiO2 and Al2O3 by atomic layer deposition technology. Two resonant dips are found in transmission spectra that are originated from the excitation of BSW for p-polarized light and s-polarized light, respectively. For the first time, we have demonstrated the developed device for refractive index (RI) sensing.

  10. Two-photon microscopy and spectroscopy based on a compact confocal scanning head

    NASA Astrophysics Data System (ADS)

    Diaspro, Alberto; Chirico, Giberto; Federici, Federico; Cannone, Fabio; Beretta, Sabrina; Robello, Mauro; Olivini, Francesca; Ramoino, Paola

    2001-07-01

    We have combined a confocal laser scanning head modified for TPE (two-photon excitation) microscopy with some spectroscopic modules to study single molecules and molecular aggregates. The behavior of the TPE microscope unit has been characterized by means of point spread function measurements and of the demonstration of its micropatterning abilities. One-photon and two-photon mode can be simply accomplished by switching from a mono-mode optical fiber (one-photon) coupled to conventional laser sources to an optical module that allows IR laser beam (two- photon/TPE) delivery to the confocal laser scanning head. We have then described the characterization of the two-photon microscope for spectroscopic applications: fluorescence correlation, lifetime and fluorescence polarization anisotropy measurements. We describe the measurement of the response of the two-photon microscope to the light polarization and discuss fluorescence polarization anisotropy measurements on Rhodamine 6G as a function of the viscosity and on a globular protein, the Beta-lactoglobulin B labeled with Alexa 532 at very high dilutions. The average rotational and translational diffusion coefficients measured with fluorescence polarization anisotropy and fluorescence correlation methods are in good agreement with the protein size, therefore validating the use of the microscope for two-photon spectroscopy on biomolecules.

  11. Two-photon interference and coherent control of single InAs quantum dot emissions in an Ag-embedded structure

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

    Liu, X., E-mail: iu.xiangming@nims.go.jp; National Institute for Materials Science, 1-1 Namiki, Tsukuba 305-0044; Kumano, H.

    2014-07-28

    We have recently reported the successful fabrication of bright single-photon sources based on Ag-embedded nanocone structures that incorporate InAs quantum dots. The source had a photon collection efficiency as high as 24.6%. Here, we show the results of various types of photonic characterizations of the Ag-embedded nanocone structures that confirm their versatility as regards a broad range of quantum optical applications. We measure the first-order autocorrelation function to evaluate the coherence time of emitted photons, and the second-order correlation function, which reveals the strong suppression of multiple photon generation. The high indistinguishability of emitted photons is shown by the Hong-Ou-Mandel-typemore » two-photon interference. With quasi-resonant excitation, coherent population flopping is demonstrated through Rabi oscillations. Extremely high single-photon purity with a g{sup (2)}(0) value of 0.008 is achieved with π-pulse quasi-resonant excitation.« less

  12. Molecular photosensitisers for two-photon photodynamic therapy.

    PubMed

    Bolze, F; Jenni, S; Sour, A; Heitz, V

    2017-11-30

    Two-photon excitation has attracted the attention of biologists, especially after the development of two-photon excited microscopy in the nineties. Since then, new applications have rapidly emerged such as the release of biologically active molecules and photodynamic therapy (PDT) using two-photon excitation. PDT, which requires a light-activated drug (photosensitiser), is a clinically approved and minimally invasive treatment for cancer and for non-malignant diseases. This feature article focuses on the engineering of molecular two-photon photosensitisers for PDT, which should bring important benefits to the treatment, increase the treatment penetration depth with near-infrared light excitation, improve the spatial selectivity and reduce the photodamage to healthy tissues. After an overview of the two-photon absorption phenomenon and the methods to evaluate two-photon induced phototoxicity on cell cultures, the different classes of photosensitisers described in the literature are discussed. The two-photon PDT performed with historical one-photon sensitisers are briefly presented, followed by specifically engineered cyclic tetrapyrrole photosensitisers, purely organic photosensitisers and transition metal complexes. Finally, targeted two-photon photosensitisers and theranostic agents that should enhance the selectivity and efficiency of the treatment are discussed.

  13. Measurement of wavefront aberrations in cortex and peripheral nerve using a two-photon excitation guidestar

    NASA Astrophysics Data System (ADS)

    Futia, Gregory L.; Fontaine, Arjun; McCullough, Connor; Ozbay, Baris N.; George, Nickolas M.; Caldwell, John; Restrepo, Diego; Weir, Richard; Gibson, Emily A.

    2018-02-01

    Neural-machine interfaces using optogenetics are of interest due to their minimal invasiveness and potential for parallel read in and read out of activity. One possible biological target for such an interface is the peripheral nerve, where axonlevel imaging or stimulation could greatly improve interfacing with artificial limbs or enable neuron/fascicle level neuromodulation in the vagus nerve. Two-photon imaging has been successful in imaging brain activity using genetically encoded calcium or voltage indicators, but in the peripheral nerve, this is severely limited by scattering and aberrations from myelin. We employ a Shack-Hartman wavefront sensor and two-photon excitation guidestar to quantify optical scattering and aberrations in peripheral nerves and cortex. The sciatic and vagus nerves, and cortex from a ChAT-Cre ChR-eYFP transgenic mouse were excised and imaged directly. In peripheral nerves, defocus was the strongest aberration followed by astigmatism and coma. Peripheral nerve had orders of magnitude higher aberration compared with cortex. These results point to the potential of adaptive optics for increasing the depth of two-photon access into peripheral nerves.

  14. Multiple spatially localized dynamical states in friction-excited oscillator chains

    NASA Astrophysics Data System (ADS)

    Papangelo, A.; Hoffmann, N.; Grolet, A.; Stender, M.; Ciavarella, M.

    2018-03-01

    Friction-induced vibrations are known to affect many engineering applications. Here, we study a chain of friction-excited oscillators with nearest neighbor elastic coupling. The excitation is provided by a moving belt which moves at a certain velocity vd while friction is modelled with an exponentially decaying friction law. It is shown that in a certain range of driving velocities, multiple stable spatially localized solutions exist whose dynamical behavior (i.e. regular or irregular) depends on the number of oscillators involved in the vibration. The classical non-repeatability of friction-induced vibration problems can be interpreted in light of those multiple stable dynamical states. These states are found within a "snaking-like" bifurcation pattern. Contrary to the classical Anderson localization phenomenon, here the underlying linear system is perfectly homogeneous and localization is solely triggered by the friction nonlinearity.

  15. IGRINS NEAR-IR HIGH-RESOLUTION SPECTROSCOPY OF MULTIPLE JETS AROUND LkHα 234

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

    Oh, Heeyoung; Yuk, In-Soo; Park, Byeong-Gon

    2016-02-01

    We present the results of high-resolution near-IR spectroscopy toward the multiple outflows around the Herbig Be star LkHα 234 using the Immersion Grating Infrared Spectrograph. Previous studies indicate that the region around LkHα 234 is complex, with several embedded young stellar objects and the outflows associated with them. In simultaneous H- and K-band spectra from HH 167, we detected 5 [Fe ii] and 14 H{sub 2} emission lines. We revealed a new [Fe ii] jet driven by radio continuum source VLA 3B. Position–velocity diagrams of the H{sub 2} 1−0 S(1) λ2.122 μm line show multiple velocity peaks. The kinematics maymore » be explained by a geometrical bow shock model. We detected a component of H{sub 2} emission at the systemic velocity (V{sub LSR} = −10.2 km s{sup −1}) along the whole slit in all slit positions, which may arise from the ambient photodissociation region. Low-velocity gas dominates the molecular hydrogen emission from knots A and B in HH 167, which is close to the systemic velocity; [Fe ii] emission lines are detected farther from the systemic velocity, at V{sub LSR} = −100–−130 km s{sup −1}. We infer that the H{sub 2} emission arises from shocked gas entrained by a high-velocity outflow. Population diagrams of H{sub 2} lines imply that the gas is thermalized at a temperature of 2500–3000 K and the emission results from shock excitation.« less

  16. Probing the Adsorption of Carbon Monoxide on Transition Metal Clusters Using IR Action Spectroscopy

    NASA Astrophysics Data System (ADS)

    Lapoutre, Vivike J. F.; Oomens, Jos; Bakker, Joost M.

    2012-06-01

    The discovery of enhanced catalytic activity of small gold clusters has led to a great interest in size-dependent catalytic properties of metal clusters. To obtain a better understanding of the catalytic mechanisms it is essential to know the structures of these clusters and the nature of their interaction with reactant molecules. We have studied the structure of gas-phase niobium clusters with a carbon monoxide adsorbed using IR action spectroscopy. We present size-selective IR spectra obtained via IR multiple photon spectroscopy monitoring either photodetachment or photodissociation depending on the charge state. The combination of these spectra with DFT calculations allows for the structural determination of the adsorption product. M. Haruta et al., Journal of Catalysis 115 301-309 (1989). M. Haertelt et al., The Journal of Physical Chemistry Letters 2 1720-1724 (2011)

  17. Multi-dimensional photonic states from a quantum dot

    NASA Astrophysics Data System (ADS)

    Lee, J. P.; Bennett, A. J.; Stevenson, R. M.; Ellis, D. J. P.; Farrer, I.; Ritchie, D. A.; Shields, A. J.

    2018-04-01

    Quantum states superposed across multiple particles or degrees of freedom offer an advantage in the development of quantum technologies. Creating these states deterministically and with high efficiency is an ongoing challenge. A promising approach is the repeated excitation of multi-level quantum emitters, which have been shown to naturally generate light with quantum statistics. Here we describe how to create one class of higher dimensional quantum state, a so called W-state, which is superposed across multiple time bins. We do this by repeated Raman scattering of photons from a charged quantum dot in a pillar microcavity. We show this method can be scaled to larger dimensions with no reduction in coherence or single-photon character. We explain how to extend this work to enable the deterministic creation of arbitrary time-bin encoded qudits.

  18. Femtosecond two-photon Rabi oscillations in excited He driven by ultrashort intense laser fields

    NASA Astrophysics Data System (ADS)

    Fushitani, M.; Liu, C.-N.; Matsuda, A.; Endo, T.; Toida, Y.; Nagasono, M.; Togashi, T.; Yabashi, M.; Ishikawa, T.; Hikosaka, Y.; Morishita, T.; Hishikawa, A.

    2016-02-01

    Coherent light-matter interaction provides powerful methods for manipulating quantum systems. Rabi oscillation is one such process. As it enables complete population transfer to a target state, it is thus routinely exploited in a variety of applications in photonics, notably quantum information processing. The extension of coherent control techniques to the multiphoton regime offers wider applicability, and access to highly excited or dipole-forbidden transition states. However, the multiphoton Rabi process is often disrupted by other competing nonlinear effects such as the a.c. Stark shift, especially at the high laser-field intensities necessary to achieve ultrafast Rabi oscillations. Here we demonstrate a new route to drive two-photon Rabi oscillations on timescales as short as tens of femtoseconds, by utilizing the strong-field phenomenon known as Freeman resonance. The scenario is not specific to atomic helium as investigated in the present study, but broadly applicable to other systems, thus opening new prospects for the ultrafast manipulation of Rydberg states.

  19. Excitation of photonic atoms (dielectric microspheres) on optical fibers: application to room-temperature persistent spectral hole burning

    NASA Astrophysics Data System (ADS)

    Serpenguzel, Ali; Arnold, Stephen; Griffel, Giora

    1995-05-01

    Recently, photonic atoms (dielectric microspheres) have enjoyed the attention of the optical spectroscopy community. A variety of linear and nonlinear optical processes have been observed in liquid microdroplets. But solid state photonic devices using these properties are scarce. A first of these applications is the room temperature microparticle hole-burning memory. New applications can be envisioned if microparticle resonances can be coupled to traveling waves in optical fibers. In this paper we demonstrate the excitation of narrow morphology dependent resonances of microparticles placed on an optical fiber. Furthermore we reveal a model for this process which describes the coupling efficiency in terms of the geometrical and material properties of the microparticle-fiber system.

  20. Two-photon speckle illumination for super-resolution microscopy.

    PubMed

    Negash, Awoke; Labouesse, Simon; Chaumet, Patrick C; Belkebir, Kamal; Giovannini, Hugues; Allain, Marc; Idier, Jérôme; Sentenac, Anne

    2018-06-01

    We present a numerical study of a microscopy setup in which the sample is illuminated with uncontrolled speckle patterns and the two-photon excitation fluorescence is collected on a camera. We show that, using a simple deconvolution algorithm for processing the speckle low-resolution images, this wide-field imaging technique exhibits resolution significantly better than that of two-photon excitation scanning microscopy or one-photon excitation bright-field microscopy.

  1. Toward two-photon excited fluorescence lifetime endomicroscopy (Conference Presentation)

    NASA Astrophysics Data System (ADS)

    Hage, Charles-Henri; Leclerc, Pierre; Fabert, Marc; Brevier, Julien; Habert, Rémi; Braud, Flavie; Kudlinski, Alexandre; Louradour, Frédéric

    2017-02-01

    Fluorescence lifetime imaging microscopy (FLIM) represents a powerful tool for biological studies. Endoscopic FLIM applied to the intracellular native biomarker NADH and FAD represents a promising mean for in vivo in situ malignant tissue diagnosis in the medical field. Else, 2-photon-excited fluorescence (2PEF) provides increased 3D resolution and imaging depth. But very few demonstrations about 2PEF lifetime measurement through a fiber have been reported and none about endoscopic 2P-FLIM through a practical fiber length (< 3m). Our group has recently demonstrated the possibility to efficiently deliver through a very long optical fiber the short and intense excitation pulses required for 2P-FLIM. Our goal is now to check that collecting fluorescence through the same endoscopic fiber does not deteriorate the lifetime measurement. Relying on the basis previously published in case of 1PEF by P. French and co-workers (J. Biophotonics, 2015), we have experimentally quantitatively evaluated the influence on the lifetime measurement of the fiber chromatic and intermodal dispersions. The main result is that the fiber contribution to the system impulse response function, even in the case of a 3-meter long double-clad optical fiber, does not hinder the separation between free and bound NADH states using FLIM. Related calibrations and measurements will be detailed. Ongoing experiments about the development of a 2P-FLIM endomicroscope on the basis of an previously reported 2P-endomicroscope (Ducourthial et al., Sc. Reports, 2015), used under various configurations (i.e. point measurement in the center of the 2P-endomicroscope image, averaged lifetime, binned endoscopic 2P-FLIM image), will be also presented.

  2. Raman signal enhancement by multiple beam excitation and its application for the detection of chemicals

    NASA Astrophysics Data System (ADS)

    Gupta, Sakshi; Ahmad, Azeem; Gambhir, Vijayeta; Reddy, Martha N.; Mehta, Dalip S.

    2015-08-01

    In a typical Raman based sensor, a single laser beam is used for exciting the sample and the backscattered or forward scattered light is collected using collection optics and is analyzed by a spectrometer. We have investigated that by means of exciting the sample with multiple beams, i.e., by dividing the same input power of the single beam into two or three or more beams and exciting the sample from different angles, the Raman signal enhances significantly. Due to the presence of multiple beams passing through the same volume of the sample, an interference pattern is formed and the volume of interaction of excitation beams with the sample increases. By means of this geometry, the enhancement in the Raman signal is observed and it was found that the signal strength increases linearly with the increase in number of excitation beams. Experimental results of this scheme for excitation of the samples are reported for explosive detection at a standoff distance.

  3. Two-Photon/Laser-Induced Fluorescence (TP/LIF) sensor

    NASA Technical Reports Server (NTRS)

    Bradshaw, John D.

    1994-01-01

    The Two-Photon/Laser-Induced Fluorescence (TP/LIF) technique is based on the stepwise excitation of the OH transitions, X(exp 2)II, v(exp '') = 0 yields X(exp 2)II, v(exp '') = 1 (lambda = 2.9 microns) and X(exp 2)II v(exp '') = 1 yields A(exp2)Sigma, v' = 0 (lambda = 345 nm) with background free fluorescence monitoring of the A(exp 2)Sigma, v' = 0 yields X(exp 2)II, v(exp '') = 0 transition near 309 nm. This technique has awaited the advent of a suitable mid-infrared (2.9 microns) laser source. Turnable mid-IR lasers now exist that are capable of meeting the specifications required of a high sensitivity TP/LIF OH sensor.

  4. Long-depth imaging of specific gene expressions in whole-mount mouse embryos with single-photon excitation confocal fluorescence microscopy and FISH.

    PubMed

    Palmes-Saloma, C; Saloma, C

    2000-07-01

    Long-depth imaging of specific gene expression in the midgestation whole-mount mouse embryo (WME) is demonstrated with single-photon excitation (1PE) confocal fluorescence microscopy and fluorescence in situ hybridization. Expression domains of Pax-6 mRNA transcripts were labeled with an in situ hybridization probe that is a RNA sequence complementary to the cloned gene fragment and were rendered visible using two fluorochrome-conjugated antibodies that fluoresce at peak wavelengths of lambda(F) = 0.525 microm and lambda(F) = 0. 580 microm, respectively. Distributions of Pax-6 mRNA domains as deep as 1000 microm in the day 9.5 WME were imaged with a long-working-distance (13.6 mm) objective lens (magnification 5x). The scattering problem posed by the optically thick WME sample is alleviated by careful control of the detector pinhole size and the application of simple but fast postdetection image enhancement techniques, such as space and wavelength averaging to produce high-quality fluorescence images. A three-dimensional reconstruction that clearly shows the Pax-6 mRNA expression domains in the forebrain, diencephalon, optic cup, and spinal cord of the day 9.5 WME is obtained. The advantages of 1PE confocal fluorescence imaging over two-photon excitation fluorescence imaging are discussed for the case of long-depth imaging in highly scattering media. Imaging in midgestation WMEs at optical depths of more than 350 microm has not yet been realized with two-photon fluorescence excitation. Copyright 2000 Academic Press.

  5. RGD-conjugated two-photon absorbing near-IR emitting fluorescent probes for tumor vascular imaging (Conference Presentation)

    NASA Astrophysics Data System (ADS)

    Belfield, Kevin D.; Yue, Xiling; Morales, Alma R.; Githaiga, Grace W.; Woodward, Adam W.; Tang, Simon; Sawada, Junko; Komatsu, Masanobu; Liu, Xuan

    2016-03-01

    Observation of the activation and inhibition of angiogenesis processes is important in the progression of cancer. Application of targeting peptides, such as a small peptide that contains adjacent L-arginine (R), glycine (G) and L-aspartic acid (D) residues can afford high selectivity and deep penetration in vessel imaging. To facilitate deep tissue vasculature imaging, probes that can be excited via two-photon absorption (2PA) in the near-infrared (NIR) and subsequently emit in the NIR are essential. In this study, the enhancement of tissue image quality with RGD conjugates was investigated with new NIR-emitting pyranyl fluorophore derivatives in two-photon fluorescence microscopy. Linear and nonlinear photophysical properties of the new probes were comprehensively characterized; significantly the probes exhibited good 2PA over a broad spectral range from 700-1100 nm. Cell and tissue images were then acquired and examined, revealing deep penetration and high contrast with the new pyranyl RGD-conjugates up to 350 μm in tumor tissue.

  6. Wave excitation at Lindblad resonances using the method of multiple scales

    NASA Astrophysics Data System (ADS)

    Horák, Jiří

    2017-12-01

    In this note, the method of multiple scales is adopted to the problem of excitation of non–axisymmetric acoustic waves in vertically integrated disk by tidal gravitational fields. We derive a formula describing a waveform of exited wave that is uniformly valid in a whole disk as long as only a single Lindblad resonance is present. Our formalism is subsequently applied to two classical problems: trapped p–mode oscillations in relativistic accretion disks and the excitation of waves in infinite disks.

  7. Two-photon excitation based photochemistry and neural imaging

    NASA Astrophysics Data System (ADS)

    Hatch, Kevin Andrew

    Two-photon microscopy is a fluorescence imaging technique which provides distinct advantages in three-dimensional cellular and molecular imaging. The benefits of this technology may extend beyond imaging capabilities through exploitation of the quantum processes responsible for fluorescent events. This study utilized a two-photon microscope to investigate a synthetic photoreactive collagen peptidomimetic, which may serve as a potential material for tissue engineering using the techniques of two-photon photolysis and two-photon polymerization. The combination of these techniques could potentially be used to produce a scaffold for the vascularization of engineered three-dimensional tissues in vitro to address the current limitations of tissue engineering. Additionally, two-photon microscopy was used to observe the effects of the application of the neurotransmitter dopamine to the mushroom body neural structures of Drosophila melanogaster to investigate dopamine's connection to cognitive degeneration.

  8. Real-time synchronized multiple-sensor IR/EO scene generation utilizing the SGI Onyx2

    NASA Astrophysics Data System (ADS)

    Makar, Robert J.; O'Toole, Brian E.

    1998-07-01

    An approach to utilize the symmetric multiprocessing environment of the Silicon Graphics Inc.R (SGI) Onyx2TM has been developed to support the generation of IR/EO scenes in real-time. This development, supported by the Naval Air Warfare Center Aircraft Division (NAWC/AD), focuses on high frame rate hardware-in-the-loop testing of multiple sensor avionics systems. In the past, real-time IR/EO scene generators have been developed as custom architectures that were often expensive and difficult to maintain. Previous COTS scene generation systems, designed and optimized for visual simulation, could not be adapted for accurate IR/EO sensor stimulation. The new Onyx2 connection mesh architecture made it possible to develop a more economical system while maintaining the fidelity needed to stimulate actual sensors. An SGI based Real-time IR/EO Scene Simulator (RISS) system was developed to utilize the Onyx2's fast multiprocessing hardware to perform real-time IR/EO scene radiance calculations. During real-time scene simulation, the multiprocessors are used to update polygon vertex locations and compute radiometrically accurate floating point radiance values. The output of this process can be utilized to drive a variety of scene rendering engines. Recent advancements in COTS graphics systems, such as the Silicon Graphics InfiniteRealityR make a total COTS solution possible for some classes of sensors. This paper will discuss the critical technologies that apply to infrared scene generation and hardware-in-the-loop testing using SGI compatible hardware. Specifically, the application of RISS high-fidelity real-time radiance algorithms on the SGI Onyx2's multiprocessing hardware will be discussed. Also, issues relating to external real-time control of multiple synchronized scene generation channels will be addressed.

  9. Multifrequency Gap Solitons in Nonlinear Photonic Crystals

    NASA Astrophysics Data System (ADS)

    Xie, Ping; Zhang, Zhao-Qing

    2003-11-01

    We predict the existence of multifrequency gap solitons (MFGSs) in both one- and two-dimensional nonlinear photonic crystals. A MFGS is a single intrinsic mode possessing multiple frequencies inside the gap. Its existence is a result of synergic nonlinear coupling among solitons or soliton trains at different frequencies. Its formation can either lower the threshold fields of the respective frequency components or stabilize their excitations. These MFGSs form a new class of stable gap solitons.

  10. Upconversion luminescent logic gates and turn-on sensing of glutathione based on two-photon excited quantum dots conjugated with dopamine.

    PubMed

    Gui, Rijun; Jin, Hui; Liu, Xifeng; Wang, Zonghua; Zhang, Feifei; Xia, Jianfei; Yang, Min; Bi, Sai

    2014-12-07

    Under the two-photon excitation, upconversion luminescent "INHIBIT" and "OR" logic gates of water-dispersed CdTe quantum dots (QDs) were constituted by conjugating the QDs with dopamine. This facilitated the development of a novel QDs-based upconversion luminescent probe for efficient turn-on sensing of glutathione.

  11. Electron-impact excitation of He: Dependence of electron-photon coherence parameters on the principal quantum number

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

    Hammond, P.; Khakoo, M.A.; McConkey, J.W.

    1987-12-01

    Measurements are presented representing a complete set of electron-photon polarization correlation parameters for the excitation of n /sup 1/P states of He at an incident energy of 80 eV and an electron scattering angle of 20/sup 0/. The data support the predictions of a recent theoretical paper that these parameters should exhibit little variation with n. However, disagreement in absolute values between experiment and theory indicates the need for additional theoretical input into the problem.

  12. Multiphoton-Excited Fluorescence of Silicon-Vacancy Color Centers in Diamond

    NASA Astrophysics Data System (ADS)

    Higbie, J. M.; Perreault, J. D.; Acosta, V. M.; Belthangady, C.; Lebel, P.; Kim, M. H.; Nguyen, K.; Demas, V.; Bajaj, V.; Santori, C.

    2017-05-01

    Silicon-vacancy color centers in nanodiamonds are promising as fluorescent labels for biological applications, with a narrow, nonbleaching emission line at 738 nm. Two-photon excitation of this fluorescence offers the possibility of low-background detection at significant tissue depth with high three-dimensional spatial resolution. We measure the two-photon fluorescence cross section of a negatively charged silicon vacancy (Si -V- ) in ion-implanted bulk diamond to be 0.74 (19 )×10-50 cm4 s /photon at an excitation wavelength of 1040 nm. Compared to the diamond nitrogen-vacancy center, the expected detection threshold of a two-photon excited Si -V center is more than an order of magnitude lower, largely due to its much narrower linewidth. We also present measurements of two- and three-photon excitation spectra, finding an increase in the two-photon cross section with decreasing wavelength, and we discuss the physical interpretation of the spectra in the context of existing models of the Si -V energy-level structure.

  13. Strong lattice correlation of non-equilibrium quasiparticles in a pseudospin-1/2 Mott insulator Sr 2IrO 4

    DOE PAGES

    Li, Yuelin; Schaller, Richard D.; Zhu, Mengze; ...

    2016-01-20

    In correlated oxides the coupling of quasiparticles to other degrees of freedom such as spin and lattice plays critical roles in the emergence of symmetry-breaking quantum ordered states such as high temperature superconductivity. We report a strong lattice coupling of photon-induced quasiparticles in spin-orbital coupling Mott insulator Sr 2IrO 4 probed via optical excitation. Combining time-resolved x-ray diffraction and optical spectroscopy techniques, we reconstruct a spatiotemporal map of the diffusion of these quasiparticles. Lastly, due to the unique electronic configuration of the quasiparticles, the strong lattice correlation is unexpected but extends the similarity between Sr 2IrO 4 and cuprates tomore » a new dimension of electron-phonon coupling which persists under highly non-equilibrium conditions.« less

  14. Multiplicity of transmission coefficients in photonic crystal and split ring resonator waveguides with Kerr nonlinear impurities

    NASA Astrophysics Data System (ADS)

    Rai, Buddhi; McGurn, Arthur R.

    2015-02-01

    Photonic crystal and split ring resonator (SRR) metamaterial waveguides with Kerr nonlinear dielectric impurities are studied. The transmission coefficients for two guided modes of different frequencies scattering from the Kerr impurities are computed. The systems are shown to exhibit multiple transmission coefficient solutions arising from the Kerr nonlinearity. Multiple transmission coefficients occur when different input intensities into a waveguide result in the same transmitted output intensities past its nonlinear impurities. (In the case of a single incident guided mode the multiplicity of transmission coefficients is known as optical bistability.) The analytical conditions under which the transmission coefficients are single and multiple valued are determined, and specific examples of both single and multiple valued transmission coefficient scattering are presented. Both photonic crystal and split ring resonator systems are studied as the Kerr nonlinearity enters the photonic crystal and SRR systems in different ways. This allows for an interesting comparison of the differences in behaviors of these two types of system which are described by distinctly different mathematical structures. Both the photonic crystal and SRR models used in the calculations are based on a difference equation approach to the system dynamics. The difference equation approach has been extensively employed in previous papers to model the basic properties of these systems. The paper is a continuation of work on the optical bistability of single guided modes interacting with Kerr impurities in photonic crystals originally considered by McGurn [Chaos 13, 754 (2003), 10.1063/1.1568691] and work on the resonant scattering from Kerr impurities in photonic crystal waveguides considered by McGurn [J. Phys.: Condens. Matter 16, S5243 (2004), 10.1088/0953-8984/16/44/021]. It generalizes this work making the extension to the more complex interaction of two guided modes at different frequencies

  15. Hyperspectral Probing of Exciton dynamics and Multiplication in PbSe Nanocrystals

    NASA Astrophysics Data System (ADS)

    Gdor, I.; Sachs, H.; Roitblat, A.; Strasfeld, D.; Bawendi, M. G.; Ruhman, S.

    2013-03-01

    Height time hyperspectral near IR probing providing broad-band coverage is employed on PbSe nanocrystals, uncovering spectral evolution following high energy photo-excitation due to hot exciton relaxation and recombination. Separation of single, double and triple exciton state contributions to these spectra is demonstrated, and the mechanisms underlying the course of spectral evolution are investigated. In addition no sign of MEG was detected in this sample up to a photon energy 3.7 times that of the band gap.

  16. Induced structural defects in Ti-doped ZnO and its two-photon-excitation

    NASA Astrophysics Data System (ADS)

    Martínez Julca, Milton A.; Rivera, Ivonnemary; Santillan Mercado, Jaime; Sierra, Heidy; Perales-Pérez, Oscar

    2016-03-01

    ZnO is a well-known luminescent material that reacts with light to generate free radicals enabling its use in cancer treatment by Photodynamic Therapy (PDT). Unfortunately, up to know, the photo-excitation of ZnO-based materials' requires excitation with ultraviolet light, which limits their biomedical applications. In this regard, this work investigates the effect of Ti species incorporation into the lattice of ZnO nanoparticles (NPs) with the aim of improving the corresponding optical properties and enabling the two-photoexcitation with 690nm-light (near infrared light). A modified polyol-based route was used to synthesize pure and Ti-doped (9% at.) ZnO NPs. X-ray diffraction confirmed the formation of ZnO-wurtzite whereas Scanning Electron Microscopy confirmed the formation of monodispersed 100-nm NPs. Raman Spectroscopy measurements evidenced the presence of zinc interstitials (Zni) and oxygen vacancies (VO) in the host oxide strcuture. Asynthesized NPs were excited using the technique of two-photon fluorescence microscopy (TPFM). The photoluminescence (PL) spectra generated from the analysis of TPFM images revealed a high emission peak presence in the green region (555 nm) that was assigned to VO. Also, a weak but noticeable band at 420 nm was detected, which is attributed to electron transition from the shallow donor level of Zni to the valence band. These PL transitions will favor triplet states formation necessary to yield cytotoxic reactive oxygen species. Furthermore, the presence of the PL peaks confirmed the Ti-ZnO NPs capacity to be excited by 690-nm light, thus, opening new possibilities for this NPs to be used in lightinduced bio-medical applications.

  17. Photonic crystal geometry for organic solar cells.

    PubMed

    Ko, Doo-Hyun; Tumbleston, John R; Zhang, Lei; Williams, Stuart; DeSimone, Joseph M; Lopez, Rene; Samulski, Edward T

    2009-07-01

    We report organic solar cells with a photonic crystal nanostructure embossed in the photoactive bulk heterojunction layer, a topography that exhibits a 3-fold enhancement of the absorption in specific regions of the solar spectrum in part through multiple excitation resonances. The photonic crystal geometry is fabricated using a materials-agnostic process called PRINT wherein highly ordered arrays of nanoscale features are readily made in a single processing step over wide areas (approximately 4 cm(2)) that is scalable. We show efficiency improvements of approximately 70% that result not only from greater absorption, but also from electrical enhancements. The methodology is generally applicable to organic solar cells and the experimental findings reported in our manuscript corroborate theoretical expectations.

  18. Synthesis, prodigious two-photon absorption cross sections and electrochemical properties of a series of triphenylamine-based chromophores

    NASA Astrophysics Data System (ADS)

    Li, Rui; Li, Dandan; Fei, Wenwen; Tan, Jingyun; Li, Shengli; Zhou, Hongping; Zhang, Shengyi; Wu, Jieying; Tian, Yupeng

    2014-06-01

    A series of triphenylamine-based chromophores (L1-3) with donor-π-donor (D-π-D) model have been designed and synthesized via solid phase Wittig reaction. Their one/two-photon fluorescence and electrochemical properties have been investigated. The results show that L2 and L3 exhibited strong and wide-dispersed two-photon-excited fluorescence (TPEF) in different solvents. Chromophore L3 displays the strongest intensity two-photon absorption activity and large cross-sections (>3600 GM) in the range of 680-840 nm in THF, the largest δ up to 8899 GM in the near-IR range, and the measured maximum TPA cross-sections per molecular weight (δmax/MW) is 8.64 GM/g (L3) in THF. Significantly, it also exhibits good solubility in common organic solvents when the chromophore was modified by polyether units as peripheral groups.

  19. Single-photon cesium Rydberg excitation spectroscopy using 318.6-nm UV laser and room-temperature vapor cell.

    PubMed

    Wang, Jieying; Bai, Jiandong; He, Jun; Wang, Junmin

    2017-09-18

    We demonstrate a single-photon Rydberg excitation spectroscopy of cesium (Cs) atoms in a room-temperature vapor cell. Cs atoms are excited directly from 6S 1/2 ground state to nP 3/2 (n = 70 - 100) Rydberg states with a 318.6 nm ultraviolet (UV) laser, and Rydberg excitation spectra are obtained by transmission enhancement of a probe beam resonant to Cs 6S 1/2 , F = 4 - 6P 3/2 , F' = 5 transition as partial population on F = 4 ground state are transferred to Rydberg state. Analysis reveals that the observed spectra are velocity-selective spectroscopy of Rydberg state, from which the amplitude and linewidth influenced by lasers' Rabi frequency have been investigated. Fitting to energies of Cs nP 3/2 (n = 70 -100) states, the determined quantum defect is 3.56671(42). The demodulated spectra can also be employed as frequency references to stabilize the UV laser frequency to specific Cs Rydberg transition.

  20. Pressure Dependence of Excitation Cross Sections for Resonant Levels of Rare Gases

    NASA Astrophysics Data System (ADS)

    Stewart, Michael D.; Chilton, J. Ethan; Lin, Chun C.

    2000-06-01

    In the rare gases, the excited n'p^5ns and n'p^5nd levels with J = 1 are optically coupled to ground as well as lower lying p levels. Resonant photons emitted when the atom decays to ground can be reabsorbed by another ground-state atom. At low gas pressures this reabsorption occurs infrequently, but at higher pressures becomes increasingly likely until the resonant transition is completely suppressed. This enhances the cascade transitions into lower p levels, resulting in pressure dependent optical emission cross sections. This reabsorption process can be understood quantitatively with a model developed by Heddle et al(D. W. O. Heddle and N. J. Samuel, J. Phys. B 3), 1593 (1970).. The radiation from transitions into the nonresonant levels often lie in the ir, while the resonant radiation is always in the uv spectral region. Using a Fourier-transform spectrometer, one can measure the cross sections for the ir transitions as a function of pressure. The Heddle model can be fit to these data with the use of theoretical values for the Einstein A coefficients. This provides a test of the accuracy of calculated A values. Discussion will include cross section measurements for Ne, Ar, and Kr excited by electron impact over a range of gas pressures.

  1. Measurement of two-photon-absorption spectra through nonlinear fluorescence produced by a line-shaped excitation beam.

    PubMed

    Hasani, E; Parravicini, J; Tartara, L; Tomaselli, A; Tomassini, D

    2018-05-01

    We propose an innovative experimental approach to estimate the two-photon absorption (TPA) spectrum of a fluorescent material. Our method develops the standard indirect fluorescence-based method for the TPA measurement by employing a line-shaped excitation beam, generating a line-shaped fluorescence emission. Such a configuration, which requires a relatively high amount of optical power, permits to have a greatly increased fluorescence signal, thus avoiding the photon counterdetection devices usually used in these measurements, and allowing to employ detectors such as charge-coupled device (CCD) cameras. The method is finally tested on a fluorescent isothiocyanate sample, whose TPA spectrum, which is measured with the proposed technique, is compared with the TPA spectra reported in the literature, confirming the validity of our experimental approach. © 2018 The Authors Journal of Microscopy © 2018 Royal Microscopical Society.

  2. Broadband photon-photon interactions mediated by cold atoms in a photonic crystal fiber

    PubMed Central

    Litinskaya, Marina; Tignone, Edoardo; Pupillo, Guido

    2016-01-01

    We demonstrate theoretically that photon-photon attraction can be engineered in the continuum of scattering states for pairs of photons propagating in a hollow-core photonic crystal fiber filled with cold atoms. The atoms are regularly spaced in an optical lattice configuration and the photons are resonantly tuned to an internal atomic transition. We show that the hard-core repulsion resulting from saturation of the atomic transitions induces bunching in the photonic component of the collective atom-photon modes (polaritons). Bunching is obtained in a frequency range as large as tens of GHz, and can be controlled by the inter-atomic separation. We provide a fully analytical explanation for this phenomenon by proving that correlations result from a mismatch of the quantization volumes for atomic excitations and photons in the continuum. Even stronger correlations can be observed for in-gap two-polariton bound states. Our theoretical results use parameters relevant for current experiments and suggest a simple and feasible way to induce interactions between photons. PMID:27170160

  3. Up-conversion fluorescence: noncoherent excitation by sunlight.

    PubMed

    Baluschev, S; Miteva, T; Yakutkin, V; Nelles, G; Yasuda, A; Wegner, G

    2006-10-06

    We demonstrate up-conversion of noncoherent sunlight realized by ultralow excitation intensity. The bimolecular up-conversion process in our systems relies on the presence of a metastable triplet excited state, and thus has dramatically different photophysical characteristics relative to the other known methods for photon up-conversion (two-photon absorption, parametric processes, second harmonic generation, sequential multiphoton absorption, etc.).

  4. REVIEW: Optics of globular photonic crystals

    NASA Astrophysics Data System (ADS)

    Gorelik, V. S.

    2007-05-01

    The results of experimental and theoretical studies of the optical properties of globular photonic crystals - new physical objects having a crystal structure with the lattice period exceeding considerably the atomic size, are presented. As globular photonic crystals, artificial opal matrices consisting of close-packed silica globules of diameter ~200 nm were used. The reflection spectra of these objects characterising the parameters of photonic bands existing in these crystals in the visible spectral region are presented. The idealised models of the energy band structure of photonic crystals investigated in the review give analytic dispersion dependences for the group velocity and the effective photon mass in a globular photonic crystal. The characteristics of secondary emission excited in globular photonic crystals by monochromatic and broadband radiation are presented. The results of investigations of single-photon-excited delayed scattering of light observed in globular photonic crystals exposed to cw UV radiation and radiation from a repetitively pulsed copper vapour laser are presented. The possibilities of using globular photonic crystals as active media for lasing in different spectral regions are considered. It is proposed to use globular photonic crystals as sensitive sensors in optoelectronic devices for molecular analysis of organic and inorganic materials by the modern methods of laser spectroscopy. The results of experimental studies of spontaneous and stimulated globular scattering of light are discussed. The conditions for observing resonance and two-photon-excited delayed scattering of light are found. The possibility of accumulation and localisation of the laser radiation energy inside a globular photonic crystal is reported.

  5. L i ( i=1,2,3) subshell X-ray production cross-sections and fluorescence yields for Ir, Pt, Pb and Bi

    NASA Astrophysics Data System (ADS)

    Singh, P.; Sharma, M.; Shahi, J. S.; Mehta, D.; Singh, N.

    2003-09-01

    The L i ( i=1,2,3) subshell X-ray production (XRP) cross-sections were measured for 77Ir, 78Pt, 82Pb and 83Bi following direct ionization in the L i ( i=1,2,3) subshells by the 59.54 keV γ-rays and the L 3 subshell by the Br/Rb/Sr/Y K X-rays. The photon sources consisting of an 241Am source in (i) the direct excitation mode and (ii) the secondary excitation mode together with the KBr/RbNO 3/SrCO 3 /Y secondary exciter and an Si(Li) detector were used. The L i ( i=1,2,3) subshell fluorescence yields ( ωi) for these elements were deduced using the measured XRP cross-sections and the L i subshell photoionization cross-sections based on the Hartree-Fock-Slater model. The measured ω1 values are found to be higher upto 50% than those based on the relativistic Dirac-Hartree-Slater (RDHS) calculations, while the ω2 and ω3 values exhibit good agreement. The predicted jump in the RDHS based ω1 values from 77Ir to 78Pt due to onset of intense L 1-L 3M 4 CK transition is not observed.

  6. Quantum nonlinear optics without photons

    NASA Astrophysics Data System (ADS)

    Stassi, Roberto; Macrı, Vincenzo; Kockum, Anton Frisk; Di Stefano, Omar; Miranowicz, Adam; Savasta, Salvatore; Nori, Franco

    2017-08-01

    Spontaneous parametric down-conversion is a well-known process in quantum nonlinear optics in which a photon incident on a nonlinear crystal spontaneously splits into two photons. Here we propose an analogous physical process where one excited atom directly transfers its excitation to a pair of spatially separated atoms with probability approaching 1. The interaction is mediated by the exchange of virtual rather than real photons. This nonlinear atomic process is coherent and reversible, so the pair of excited atoms can transfer the excitation back to the first one: the atomic analog of sum-frequency generation of light. The parameters used to investigate this process correspond to experimentally demonstrated values in ultrastrong circuit quantum electrodynamics. This approach can be extended to realize other nonlinear interatomic processes, such as four-atom mixing, and is an attractive architecture for the realization of quantum devices on a chip. We show that four-qubit mixing can efficiently implement quantum repetition codes and, thus, can be used for error-correction codes.

  7. Photon upconversion using InAs-based quantum structures and the control of intermediate states (Conference Presentation)

    NASA Astrophysics Data System (ADS)

    Kamiya, Itaru; Tex, David M.; Zhang, Yuwei; Kanemitsu, Yoshihiko

    2017-04-01

    We have reported that a novel quantum structure which we term quantum well island (QWI), a few monolayer thick and sub-micron wide structure, is effective in confining the carriers and enhancing multi-exciton interactions. By embedding InAs-based QWIs in AlGaAs barrier layers, we demonstrated that upconverted photoluminescence (PL) in the visible regime can be obtained by impinging near infrared (IR) photons, which may potentially be applied for intermediate band (IB) solar cells [1]. Further investigation has revealed that the dominant upconversion mechanism is most likely Auger, while two-step excitation may also take place under selected conditions [2]. The upconverted carriers generated by IR irradiation may also be detected as photocurrents. Through a series of studies using this structure, we note the importance of the carrier trapping involved during the upconversion processes. For instance, multiple laser-beam excitation measurements have shown that trapping and re-trapping processes reduce the photocurrents [3]. However, recently, using a structure that consists of InAs quantum dots embedded in InAs/GaAs multi-quantum wells (MQWs), we find that efficient carrier trapping can enhance upconverted PL [4]. We show the preparation and the control of this structure by molecular beam epitaxy (MBE), and the possible mechanisms of the upconversion. We also discuss how the conversion efficiency may be improved using device structures based on this concept. [1] D. M. Tex and I. Kamiya, Phys. Rev. B 83 (2011) 081309. [2] D. M. Tex, I. Kamiya, and Y. Kanemitsu, Sci. Rep. 4 (2014) 4125. [3] D. M. Tex, T. Ihara, I. Kamiya, and Y. Kanemitsu, to be published. [4] Y. Zhang and I. Kamiya, JSAP Spring Meeting, 2016.

  8. Synthesis of Photoresponsive Dual NIR Two-Photon Absorptive [60]Fullerene Triads and Tetrads

    PubMed Central

    Jeon, Seaho; Wang, Min; Tan, Loon-Seng; Cooper, Thomas; Hamblin, Michael R.; Chiang, Long Y.

    2013-01-01

    Broadband nonlinear optical (NLO) organic nanostructures exhibiting both ultrafast photoresponse and a large cross-section of two-photon absorption throughout a wide NIR spectrum may make them suitable for use as nonlinear biophotonic materials. We report here the synthesis and characterization of two C60-(antenna)x analogous compounds as branched triad C60(>DPAF-C18)(>CPAF-C2M) and tetrad C60(>DPAF-C18)(>CPAF-C2M)2 nanostructures. These compounds showed approximately equal extinction coefficients of optical absorption over 400–550 nm that corresponds to near-IR two-photon based excitation wavelengths at 780–1,100 nm. Accordingly, they may be utilized as potential precursor candidates to the active-core structures of photosensitizing nanodrugs for 2γ-PDT in the biological optical window of 800–1,050 nm. PMID:23941881

  9. An integrated single- and two-photon non-diffracting light-sheet microscope

    NASA Astrophysics Data System (ADS)

    Lau, Sze Cheung; Chiu, Hoi Chun; Zhao, Luwei; Zhao, Teng; Loy, M. M. T.; Du, Shengwang

    2018-04-01

    We describe a fluorescence optical microscope with both single-photon and two-photon non-diffracting light-sheet excitations for large volume imaging. With a special design to accommodate two different wavelength ranges (visible: 400-700 nm and near infrared: 800-1200 nm), we combine the line-Bessel sheet (LBS, for single-photon excitation) and the scanning Bessel beam (SBB, for two-photon excitation) light sheet together in a single microscope setup. For a transparent thin sample where the scattering can be ignored, the LBS single-photon excitation is the optimal imaging solution. When the light scattering becomes significant for a deep-cell or deep-tissue imaging, we use SBB light-sheet two-photon excitation with a longer wavelength. We achieved nearly identical lateral/axial resolution of about 350/270 nm for both imagings. This integrated light-sheet microscope may have a wide application for live-cell and live-tissue three-dimensional high-speed imaging.

  10. Resonance Enhanced Multi-Photon Ionization and Uv-Uv Hole-Burning Spectroscopic Studies of Jet-Cooled Acetanilide Derivatives

    NASA Astrophysics Data System (ADS)

    Moon, Ceol Joo; Min, Ahreum; Ahn, Ahreum; Lee, Seung Jun; Choi, Myong Yong; Kim, Seong Keun

    2013-06-01

    Conformational investigations and photochemistry of jet-cooled methacetine (MA) and phenacetine (PA) using one color resonant two-photon ionization (REMPI), UV-UV hole-burning and IR-dip spectroscopy are presented. MA and PA are derivatives of acetanilide, substituted by methoxyl, ethoxyl group in the para position of acetanilide, respectively. Moreover, we have investigated conformational information of the acetanilide derivatives (AAP, MA and PA)-water. In this work, we will present and discuss the solvent effects of the hydroxyl group of acetanilide derivatives in the excited state.

  11. Water-Soluble Triarylborane Chromophores for One- and Two-Photon Excited Fluorescence Imaging of Mitochondria in Cells.

    PubMed

    Griesbeck, Stefanie; Zhang, Zuolun; Gutmann, Marcus; Lühmann, Tessa; Edkins, Robert M; Clermont, Guillaume; Lazar, Adina N; Haehnel, Martin; Edkins, Katharina; Eichhorn, Antonius; Blanchard-Desce, Mireille; Meinel, Lorenz; Marder, Todd B

    2016-10-04

    Three water-soluble tetracationic quadrupolar chromophores comprising two three-coordinate boron π-acceptor groups bridged by thiophene-containing moieties were synthesised for biological imaging applications. Compound 3 containing the bulkier 5-(3,5-Me2 C6 H2 )-2,2'-(C4 H2 S)2 -5'-(3,5-Me2 C6 H2 ) bridge is stable over a long period of time, exhibits a high fluorescence quantum yield and strong one- and two-photon absorption (TPA), and has a TPA cross section of 268 GM at 800 nm in water. Confocal laser scanning fluorescence microscopy studies in live cells indicated localisation of the chromophore at the mitochondria; moreover, cytotoxicity measurements proved biocompatibility. Thus, chromophore 3 has excellent potential for one- and two-photon-excited fluorescence imaging of mitochondrial function in cells. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  12. Excitation of photosystem I by 760 nm femtosecond laser pulses: transient absorption spectra and intermediates

    NASA Astrophysics Data System (ADS)

    Cherepanov, Dmitry A.; Shelaev, Ivan V.; Gostev, Fedor E.; Mamedov, Mahir D.; Petrova, Anastasia A.; Aybush, Arseniy V.; Shuvalov, Vladimir A.; Semenov, Alexey Yu; Nadtochenko, Victor A.

    2017-09-01

    Excitation of photosystem I (PS I) by a femtosecond 760 nm pump leads to one- and two-photon absorption. The one-photon excitation produces intermediates with transient absorption spectra similar to the spectra of the primary [{{{P}}700}+{{{A}}0}-{{A}}1] and secondary [{{{P}}700}+{{A}}0{{{A}}1}-] ion-radical pairs in the PS I reaction center. The two-photon absorption generates the upper level excited states of chlorophyll (Chl) and carotenoid molecules in the antenna. These excited states are converted into the long-lived intermediates and can be tentatively attributed to the excited and charge-transfer ion-radical states of Chl molecules and to the excited states of carotenoids in the antenna. The transient spectra of intermediates generated by two-photon excitation differ from the transient one-photon spectra of the primary and secondary ion-radical pairs.

  13. Efficient quantum computing using coherent photon conversion.

    PubMed

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

    2011-10-12

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

  14. Multiple period s-p hybridization in nano-strip embedded photonic crystal.

    PubMed

    Han, Seunghoon; Lee, Il-Min; Kim, Hwi; Lee, Byoungho

    2005-04-04

    We report and analyze hybridization of s-state and p-state modes in photonic crystal one-dimensional defect cavity array. When embedding a nano-strip into a dielectric rod photonic crystal, an effective cavity array is made, where each cavity possesses two cavity modes: s-state and p-state. The two modes are laterally even versus the nano-strip direction, and interact with each other, producing defect bands, of which the group velocity becomes zero within the first Brillouin zone. We could model and describe the phenomena by using the tight-binding method, well agreeing with the plane-wave expansion method analysis. We note that the reported s- and p-state mode interaction corresponds to the hybridization of atomic orbital in solid-state physics. The concept of multiple period s-p hybridization and the proposed model can be useful for analyzing and developing novel photonic crystal waveguides and devices.

  15. Storage of multiple single-photon pulses emitted from a quantum dot in a solid-state quantum memory.

    PubMed

    Tang, Jian-Shun; Zhou, Zong-Quan; Wang, Yi-Tao; Li, Yu-Long; Liu, Xiao; Hua, Yi-Lin; Zou, Yang; Wang, Shuang; He, De-Yong; Chen, Geng; Sun, Yong-Nan; Yu, Ying; Li, Mi-Feng; Zha, Guo-Wei; Ni, Hai-Qiao; Niu, Zhi-Chuan; Li, Chuan-Feng; Guo, Guang-Can

    2015-10-15

    Quantum repeaters are critical components for distributing entanglement over long distances in presence of unavoidable optical losses during transmission. Stimulated by the Duan-Lukin-Cirac-Zoller protocol, many improved quantum repeater protocols based on quantum memories have been proposed, which commonly focus on the entanglement-distribution rate. Among these protocols, the elimination of multiple photons (or multiple photon-pairs) and the use of multimode quantum memory are demonstrated to have the ability to greatly improve the entanglement-distribution rate. Here, we demonstrate the storage of deterministic single photons emitted from a quantum dot in a polarization-maintaining solid-state quantum memory; in addition, multi-temporal-mode memory with 1, 20 and 100 narrow single-photon pulses is also demonstrated. Multi-photons are eliminated, and only one photon at most is contained in each pulse. Moreover, the solid-state properties of both sub-systems make this configuration more stable and easier to be scalable. Our work will be helpful in the construction of efficient quantum repeaters based on all-solid-state devices.

  16. Storage of multiple single-photon pulses emitted from a quantum dot in a solid-state quantum memory

    PubMed Central

    Tang, Jian-Shun; Zhou, Zong-Quan; Wang, Yi-Tao; Li, Yu-Long; Liu, Xiao; Hua, Yi-Lin; Zou, Yang; Wang, Shuang; He, De-Yong; Chen, Geng; Sun, Yong-Nan; Yu, Ying; Li, Mi-Feng; Zha, Guo-Wei; Ni, Hai-Qiao; Niu, Zhi-Chuan; Li, Chuan-Feng; Guo, Guang-Can

    2015-01-01

    Quantum repeaters are critical components for distributing entanglement over long distances in presence of unavoidable optical losses during transmission. Stimulated by the Duan–Lukin–Cirac–Zoller protocol, many improved quantum repeater protocols based on quantum memories have been proposed, which commonly focus on the entanglement-distribution rate. Among these protocols, the elimination of multiple photons (or multiple photon-pairs) and the use of multimode quantum memory are demonstrated to have the ability to greatly improve the entanglement-distribution rate. Here, we demonstrate the storage of deterministic single photons emitted from a quantum dot in a polarization-maintaining solid-state quantum memory; in addition, multi-temporal-mode memory with 1, 20 and 100 narrow single-photon pulses is also demonstrated. Multi-photons are eliminated, and only one photon at most is contained in each pulse. Moreover, the solid-state properties of both sub-systems make this configuration more stable and easier to be scalable. Our work will be helpful in the construction of efficient quantum repeaters based on all-solid-state devices. PMID:26468996

  17. Selective Two-Photon Absorptive Resonance Femtosecond-Laser Electronic-Excitation Tagging (STARFLEET) Velocimetry in Flow and Combustion Diagnostics

    NASA Technical Reports Server (NTRS)

    Jiang, Naibo; Halls, Benjamin R.; Stauffer, Hans U.; Roy, Sukesh; Danehy, Paul M.; Gord, James R.

    2016-01-01

    Selective Two-Photon Absorptive Resonance Femtosecond-Laser Electronic-Excitation Tagging (STARFLEET), a non-seeded ultrafast-laser-based velocimetry technique, is demonstrated in reactive and non-reactive flows. STARFLEET is pumped via a two-photon resonance in N2 using 202.25-nm 100-fs light. STARFLEET greatly reduces the per-pulse energy required (30 µJ/pulse) to generate the signature FLEET emission compared to the conventional FLEET technique (1.1 mJ/pulse). This reduction in laser energy results in less energy deposited in the flow, which allows for reduced flow perturbations (reactive and non-reactive), increased thermometric accuracy, and less severe damage to materials. Velocity measurements conducted in a free jet of N2 and in a premixed flame show good agreement with theoretical velocities and further demonstrate the significantly less-intrusive nature of STARFLEET.

  18. X-ray scattering study of pyrochlore iridates: Crystal structure, electronic, and magnetic excitations

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

    Clancy, J. P.; Gretarsson, H.; Lee, E. K. H.

    2016-07-06

    We have investigated the structural, electronic, and magnetic properties of the pyrochlore iridates Eu 2Ir 2O 7 and Pr 2Ir 2O 7 using a combination of resonant elastic x-ray scattering, x-ray powder diffraction, and resonant inelastic x-ray scattering (RIXS). The structural parameters of Eu 2Ir 2O 7 have been examined as a function of temperature and applied pressure, with a particular emphasis on regions of the phase diagram where electronic and magnetic phase transitions have been reported. We find no evidence of crystal symmetry change over the range of temperatures (~6 to 300 K) and pressures (~0.1 to 17 GPa)more » studied. We have also investigated the electronic and magnetic excitations in single-crystal samples of Eu 2Ir 2O 7 and Pr 2Ir 2O 7 using high-resolution Ir L- 3-edge RIXS. In spite of very different ground state properties, we find that these materials exhibit qualitatively similar excitation spectra, with crystal field excitations at ~3-5 eV, spin-orbit excitations at ~ 0.5-1 eV, and broad low-lying excitations below ~0.15 eV. In single-crystal samples of "Eu-rich" Eu 2Ir 2O 7 (found to possess an actual stoichiometry of Eu 2.18Ir 1.82O 7.06) we observe highly damped magnetic excitations at ~45 meV, which display significant momentum dependence. Here, we compare these results with recent dynamical structure factor calculations« less

  19. IR-IR Conformation Specific Spectroscopy of Na+(Glucose) Adducts

    NASA Astrophysics Data System (ADS)

    Voss, Jonathan M.; Kregel, Steven J.; Fischer, Kaitlyn C.; Garand, Etienne

    2018-01-01

    We report an IR-IR double resonance study of the structural landscape present in the Na+(glucose) complex. Our experimental approach involves minimal modifications to a typical IR predissociation setup, and can be carried out via ion-dip or isomer-burning methods, providing additional flexibility to suit different experimental needs. In the current study, the single-laser IR predissociation spectrum of Na+(glucose), which clearly indicates contributions from multiple structures, was experimentally disentangled to reveal the presence of three α-conformers and five β-conformers. Comparisons with calculations show that these eight conformations correspond to the lowest energy gas-phase structures with distinctive Na+ coordination. [Figure not available: see fulltext.

  20. Visualization of deep ultraviolet photons based on Förster resonance energy transfer and cascade photon reabsorption in diphenylalanine-carbon nitrides composite film

    NASA Astrophysics Data System (ADS)

    Gan, Zhixing; Zhou, Weiping; Chen, Zhihui; Wang, Huan; Di, Yunsong; Huang, Shisong

    2016-11-01

    A diphenylalanine (L-Phe-L-Phe, FF)-carbon nitride composite film is designed and fabricated to visualize the deep ultraviolet (DUV, 245-290 nm) photons. The FF film, composed of diphenylalanine molecules, doped with carbon nitrides shows blue emission under excitation of DUV light, which makes the DUV beam observable. Both Förster resonance energy transfer and cascade photon reabsorption contribute to the conversion of photon energy. First, the FF is excited by the DUV photons. On one hand, the energy transfers to the embedded carbon nitrides through nonradiative dipole-dipole couplings. On the other hand, the 284 nm photons emitted from the FF would further excite the carbon nitrides, which will finally convert to blue fluorescence. Herein, the experimental demonstration of a simple device for the visualization of high DUV fluxes is reported.

  1. Laser scanning stereomicroscopy for fast volumetric imaging with two-photon excitation and scanned Bessel beams

    NASA Astrophysics Data System (ADS)

    Yang, Yanlong; Zhou, Xing; Li, Runze; Van Horn, Mark; Peng, Tong; Lei, Ming; Wu, Di; Chen, Xun; Yao, Baoli; Ye, Tong

    2015-03-01

    Bessel beams have been used in many applications due to their unique optical properties of maintaining their intensity profiles unchanged during propagation. In imaging applications, Bessel beams have been successfully used to provide extended focuses for volumetric imaging and uniformed illumination plane in light-sheet microscopy. Coupled with two-photon excitation, Bessel beams have been successfully used in realizing fluorescence projected volumetric imaging. We demonstrated previously a stereoscopic solution-two-photon fluorescence stereomicroscopy (TPFSM)-for recovering the depth information in volumetric imaging with Bessel beams. In TPFSM, tilted Bessel beams were used to generate stereoscopic images on a laser scanning two-photon fluorescence microscope; upon post image processing we could successfully provide 3D perception of acquired volume images by wearing anaglyph 3D glasses. However, tilted Bessel beams were generated by shifting either an axicon or an objective laterally; the slow imaging speed and severe aberrations made it hard to use in real-time volume imaging. In this article, we report recent improvements of TPFSM with newly designed scanner and imaging software, which allows 3D stereoscopic imaging without moving any of the optical components on the setup. This improvement has dramatically improved focusing qualities and imaging speed so that the TPFSM can be performed potentially in real-time to provide 3D visualization in scattering media without post image processing.

  2. Aberration correction considering curved sample surface shape for non-contact two-photon excitation microscopy with spatial light modulator.

    PubMed

    Matsumoto, Naoya; Konno, Alu; Inoue, Takashi; Okazaki, Shigetoshi

    2018-06-18

    In this paper, excitation light wavefront modulation is performed considering the curved sample surface shape to demonstrate high-quality deep observation using two-photon excitation microscopy (TPM) with a dry objective lens. A large spherical aberration typically occurs when the refractive index (RI) interface between air and the sample is a plane perpendicular to the optical axis. Moreover, the curved sample surface shape and the RI mismatch cause various aberrations, including spherical ones. Consequently, the fluorescence intensity and resolution of the obtained image are degraded in the deep regions. To improve them, we designed a pre-distortion wavefront for correcting the aberration caused by the curved sample surface shape by using a novel, simple optical path length difference calculation method. The excitation light wavefront is modulated to the pre-distortion wavefront by a spatial light modulator incorporated in the TPM system before passing through the interface, where the RI mismatch occurs. Thus, the excitation light is condensed without aberrations. Blood vessels were thereby observed up to an optical depth of 2,000 μm in a cleared mouse brain by using a dry objective lens.

  3. Controllably releasing long-lived quantum memory for photonic polarization qubit into multiple spatially-separate photonic channels.

    PubMed

    Chen, Lirong; Xu, Zhongxiao; Zeng, Weiqing; Wen, Yafei; Li, Shujing; Wang, Hai

    2016-09-26

    We report an experiment in which long-lived quantum memories for photonic polarization qubits (PPQs) are controllably released into any one of multiple spatially-separate channels. The PPQs are implemented with an arbitrarily-polarized coherent signal light pulses at the single-photon level and are stored in cold atoms by means of electromagnetic-induced-transparency scheme. Reading laser pulses propagating along the direction at a small angle relative to quantum axis are applied to release the stored PPQs into an output channel. By changing the propagating directions of the read laser beam, we controllably release the retrieved PPQs into 7 different photonic output channels, respectively. At a storage time of δt = 5 μs, the least quantum-process fidelity in 7 different output channels is ~89%. At one of the output channels, the measured maximum quantum-process fidelity for the PPQs is 94.2% at storage time of δt = 0.85 ms. At storage time of 6 ms, the quantum-process fidelity is still beyond the bound of 78% to violate the Bell's inequality. The demonstrated controllable release of the stored PPQs may extend the capabilities of the quantum information storage technique.

  4. Theoretical investigation of the hyper-Raman scattering in hexagonal semiconductors under two-photon excitation near resonance with the An=2 exciton level

    NASA Astrophysics Data System (ADS)

    Semenova, L. E.

    2018-04-01

    The hyper-Raman scattering of light by LO-phonons under two-photon excitation near resonance with the An=2 exciton level in the wurtzite semiconductors A2B6 was theoretically investigated, taking into account the influence of the complex structure of the top valence band.

  5. Stokes parameter studies of spontaneous emission from chiral nematic liquid crystals as a one-dimensional photonic stopband crystal: experiment and theory.

    PubMed

    Woon, Kai L; O'Neill, Mary; Richards, Gary J; Aldred, Matthew P; Kelly, Stephen M

    2005-04-01

    The helical structure of uniformly aligned chiral nematic liquid crystals results in a photonic stopband for only one sense of circular polarization. The spectroscopic Stokes polarimeter is used to analyze spontaneous emission in the stopband. Highly polarized photoluminescence is found and the polarization properties vary with the excitation wavelength. Spontaneous emission is enhanced at the stopband edge and this Purcell effect is greater on excitation at wavelengths where the absorption coefficient is low. This is interpreted as greater overlap between the excited molecules and the electrical modal field of the resonant modes at the stopband edge. Photoluminescence detected from the excitation face of the liquid crystal cell is less polarized because of photon tunneling. Fermi's golden rule in conjunction with Stokes vectors is used to model the polarization of emission taking multiple reflections at the interfaces of the cell into account. The discrepancy between the experiment and the theoretical model is interpreted as direct experimental evidence that virtual photons, which originate from zero point fluctuations of quantum space, are randomly polarized.

  6. Excitability and optical pulse generation in semiconductor lasers driven by resonant tunneling diode photo-detectors.

    PubMed

    Romeira, Bruno; Javaloyes, Julien; Ironside, Charles N; Figueiredo, José M L; Balle, Salvador; Piro, Oreste

    2013-09-09

    We demonstrate, experimentally and theoretically, excitable nanosecond optical pulses in optoelectronic integrated circuits operating at telecommunication wavelengths (1550 nm) comprising a nanoscale double barrier quantum well resonant tunneling diode (RTD) photo-detector driving a laser diode (LD). When perturbed either electrically or optically by an input signal above a certain threshold, the optoelectronic circuit generates short electrical and optical excitable pulses mimicking the spiking behavior of biological neurons. Interestingly, the asymmetric nonlinear characteristic of the RTD-LD allows for two different regimes where one obtain either single pulses or a burst of multiple pulses. The high-speed excitable response capabilities are promising for neurally inspired information applications in photonics.

  7. Multiple-frame IR photo-recorder KIT-3M

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

    Roos, E; Wilkins, P; Nebeker, N

    2006-05-15

    This paper reports the experimental results of a high-speed multi-frame infrared camera which has been developed in Sarov at VNIIEF. Earlier [1] we discussed the possibility of creation of the multi-frame infrared radiation photo-recorder with framing frequency about 1 MHz. The basis of the photo-recorder is a semiconductor ionization camera [2, 3], which converts IR radiation of spectral range 1-10 micrometers into a visible image. Several sequential thermal images are registered by using the IR converter in conjunction with a multi-frame electron-optical camera. In the present report we discuss the performance characteristics of a prototype commercial 9-frame high-speed IR photo-recorder.more » The image converter records infrared images of thermal fields corresponding to temperatures ranging from 300 C to 2000 C with an exposure time of 1-20 {micro}s at a frame frequency up to 500 KHz. The IR-photo-recorder camera is useful for recording the time evolution of thermal fields in fast processes such as gas dynamics, ballistics, pulsed welding, thermal processing, automotive industry, aircraft construction, in pulsed-power electric experiments, and for the measurement of spatial mode characteristics of IR-laser radiation.« less

  8. Application of Excitation from Multiple Locations on a Simplified High-Lift System

    NASA Technical Reports Server (NTRS)

    Melton, LaTunia Pack; Yao, Chung-Sheng; Seifert, Avi

    2004-01-01

    A series of active flow control experiments were recently conducted on a simplified high-lift system. The purpose of the experiments was to explore the prospects of eliminating all but simply hinged leading and trailing edge flaps, while controlling separation on the supercritical airfoil using multiple periodic excitation slots. Excitation was provided by three. independently controlled, self-contained, piezoelectric actuators. Low frequency excitation was generated through amplitude modulation of the high frequency carrier wave, the actuators' resonant frequencies. It was demonstrated, for the first time, that pulsed modulated signal from two neighboring slots interact favorably to increase lift. Phase sensitivity at the low frequency was measured, even though the excitation was synthesized from the high-frequency carrier wave. The measurements were performed at low Reynolds numbers and included mean and unsteady surface pressures, surface hot-films, wake pressures and particle image velocimetry. A modest (6%) increase in maximum lift (compared to the optimal baseline) was obtained due t o the activation of two of the three actuators.

  9. Ultra-compact fiber-optic two-photon microscope for functional fluorescence imaging in vivo.

    PubMed

    Engelbrecht, Christoph J; Johnston, Richard S; Seibel, Eric J; Helmchen, Fritjof

    2008-04-14

    We present a small, lightweight two-photon fiberscope and demonstrate its suitability for functional imaging in the intact brain. Our device consists of a hollow-core photonic crystal fiber for efficient delivery of near-IR femtosecond laser pulses, a spiral fiber-scanner for resonant beam steering, and a gradient-index lens system for fluorescence excitation, dichroic beam splitting, and signal collection. Fluorescence light is remotely detected using a standard photomultiplier tube. All optical components have 1 mm dimensions and the microscope's headpiece weighs only 0.6 grams. The instrument achieves micrometer resolution at frame rates of typically 25 Hz with a field-of-view of up to 200 microns. We demonstrate functional imaging of calcium signals in Purkinje cell dendrites in the cerebellum of anesthetized rats. The microscope will be easily portable by a rat or mouse and thus should enable functional imaging in freely behaving animals.

  10. Imaging of surgical margin in pancreatic metastasis using two-photon excited fluorescence microscopy

    NASA Astrophysics Data System (ADS)

    Chen, Jing; Hong, Zhipeng; Chen, Hong; Chen, Youting; Xu, Yahao; Zhu, Xiaoqin; Zhuo, Shuangmu; Shi, Zheng; Chen, Jianxin

    2014-09-01

    Two-photon excited fluorescence (TPEF) microscopy, has become a powerful tool for imaging unstained tissue samples at subcellular level in biomedical research. The purpose of this study was to determine whether TPEF imaging of histological sections without H-E staining can be used to identify the boundary between normal pancreas and pancreatic metastasis from renal cell carcinoma (RCC). The typical features such as the significant increase of cancerous nests, the absence of pancreatic ductal, the appearance of cancer cells were observed to present the boundary between normal pancreas and pancreatic metastasis from RCC. These results correlated well with the corresponding histological outcomes. With the advent of clinically miniaturized TPEF microscopy and integrative endoscopy, TPEF microscopy has the potential application on surgical location of pancreatic metastasis from RCC in the near future.

  11. Resonance Fluorescence of an InGaAs Quantum Dot in a Planar Cavity Using Orthogonal Excitation and Detection.

    PubMed

    Chen, Disheng; Lander, Gary R; Flagg, Edward B

    2017-10-13

    The ability to perform simultaneous resonant excitation and fluorescence detection is important for quantum optical measurements of quantum dots (QDs). Resonant excitation without fluorescence detection - for example, a differential transmission measurement - can determine some properties of the emitting system, but does not allow applications or measurements based on the emitted photons. For example, the measurement of photon correlations, observation of the Mollow triplet, and realization of single photon sources all require collection of the fluorescence. Incoherent excitation with fluorescence detection - for example, above band-gap excitation - can be used to create single photon sources, but the disturbance of the environment due to the excitation reduces the indistinguishability of the photons. Single photon sources based on QDs will have to be resonantly excited to have high photon indistinguishability, and simultaneous collection of the photons will be necessary to make use of them. We demonstrate a method to resonantly excite a single QD embedded in a planar cavity by coupling the excitation beam into this cavity from the cleaved face of the sample while collecting the fluorescence along the sample's surface normal direction. By carefully matching the excitation beam to the waveguide mode of the cavity, the excitation light can couple into the cavity and interact with the QD. The scattered photons can couple to the Fabry-Perot mode of the cavity and escape in the surface normal direction. This method allows complete freedom in the detection polarization, but the excitation polarization is restricted by the propagation direction of the excitation beam. The fluorescence from the wetting layer provides a guide to align the collection path with respect to the excitation beam. The orthogonality of the excitation and detection modes enables resonant excitation of a single QD with negligible laser scattering background.

  12. Two-photon or higher-order absorbing optical materials and methods of use

    NASA Technical Reports Server (NTRS)

    Perry, Joseph (Inventor); Marder, Seth (Inventor)

    2001-01-01

    Compositions capable of simultaneous two-photon absorption and higher order absorptivities are disclosed. Many of these compositions are compounds satisfying the formulae D-.PI.-D, A-.PI.-A, D-A-D and A-D-A, wherein D is an electron donor group, A is an electron acceptor group and .PI. comprises a bridge of .pi.-conjugated bonds connecting the electron donor groups and electron acceptor groups. In A-D-A and D-A-D compounds, the .pi. bridge is substituted with electron donor groups and electron acceptor groups, respectively. Also disclosed are methods that generate an electronically excited state of a compound, including those satisfying one of these formulae. The electronically excited state is achieved in a method that includes irradiating the compound with light. Then, the compound is converted to a multi-photon electronically excited state upon simultaneous absorption of at least two photons of light. The sum of the energies of all of the absorbed photons is greater than or equal to the transition energy from a ground state of the compound to the multi-photon excited state. The energy of each absorbed photon is less than the transition energy between the ground state and the lowest single-photon excited state of the compound is less than the transition energy between the multi-photon excited state and the ground state.

  13. [Phosphorescent effect of Ir (ppy)3 on the luminescent characteristic of Rubrene].

    PubMed

    Xu, Hong-Hua; Xu, Zheng; Zhang, Fu-Jun; Zhao, Su-Ling; Yuan, Guang-Cai; Chen, Yue-Ning

    2008-07-01

    Many organic matters including heavy metal ions can validly utilize the singlet and triplet for luminescence owiog to the spin-orbit coupling. As a result, the internal quantum efficiency can easily achieve a value higher than traditional organic light emitting diodes in theory. There is a strong luminescence of PVK in PVK : PBD : Rubrene system. PL spectra excited by 345 nm of PVK : PBD : Rubrene thin film has a 410 nm PVK luminescent peak and a 560 nm Rubrene peak. EL still has a PVK luminescent peak, which should be kept from happening. Excitons can not adequately transferred from the matrix solution to Rubrene. The doping with Ir(ppy)3 improves the PVK : PBD : Rubrene system performance. PL spectra excited by 345 nm of PVK : PBD : Ir(ppy)3 : Rubrene with low concentration of Rubrene has a 510 nm Ir(ppy)3 peak and a new 548 nm one. However, the Ir(ppy)3 peak is smaller and the Rubrene one is bigger in EL spectra. Notably a strong and single luminescence of Rubrene is obtained in EL and PL spectra excited by 345 nm of PVK : PBD : Ir(ppy)3 : Rubrene with high concentration of Rubrene. Meanwhile, the Ir(ppy)3 luminescent peak disappears. The mechanism originates from the phosphorescent effect of Ir (ppy)3. The singlet excitons can basically be transferred from PVK : PBD or Ir(ppy)3 to Rubrene. But most excitons from Ir (ppy)3 can directly tunnel to the fluorescent material and come into being singlet states that can return to ground states and cause luminescence. Rubrene can accept proportional excitons with low concentration. While the concentration of Rubrene is higher, excitons can be entirely accepted by Rubrene. The effect also restricts the luminescent intensity of Ir(ppy)3 and boosts up that of Rubrene. Furthermore, the energy transfer in PVK : PBD : Ir(ppy)3 : Rubrene system is primary the Forester energy transfer. Excitation spectra of Rubrene and emission spectra of Ir(ppy)3 have a large overlap revealing that there is a strong energy transfer and further

  14. Mapping of hemoglobin in erythrocytes and erythrocyte ghosts using two photon excitation fluorescence microscopy

    NASA Astrophysics Data System (ADS)

    Bukara, Katarina; Jovanić, Svetlana; Drvenica, Ivana T.; Stančić, Ana; Ilić, Vesna; Rabasović, Mihailo D.; Pantelić, Dejan; Jelenković, Branislav; Bugarski, Branko; Krmpot, Aleksandar J.

    2017-02-01

    The present study describes utilization of two photon excitation fluorescence (2PE) microscopy for visualization of the hemoglobin in human and porcine erythrocytes and their empty membranes (i.e., ghosts). High-quality, label- and fixation-free visualization of hemoglobin was achieved at excitation wavelength 730 nm by detecting visible autofluorescence. Localization in the suspension and spatial distribution (i.e., mapping) of residual hemoglobin in erythrocyte ghosts has been resolved by 2PE. Prior to the 2PE mapping, the presence of residual hemoglobin in the bulk suspension of erythrocyte ghosts was confirmed by cyanmethemoglobin assay. 2PE analysis revealed that the distribution of hemoglobin in intact erythrocytes follows the cells' shape. Two types of erythrocytes, human and porcine, characterized with discocyte and echinocyte morphology, respectively, showed significant differences in hemoglobin distribution. The 2PE images have revealed that despite an extensive washing out procedure after gradual hypotonic hemolysis, a certain amount of hemoglobin localized on the intracellular side always remains bound to the membrane and cannot be eliminated. The obtained results open the possibility to use 2PE microscopy to examine hemoglobin distribution in erythrocytes and estimate the purity level of erythrocyte ghosts in biotechnological processes.

  15. IR-IR Conformation Specific Spectroscopy of Na +(Glucose) Adducts

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

    Voss, Jonathan M.; Kregel, Steven J.; Fischer, Kaitlyn C.

    Here in this paper we report an IR-IR double resonance study of the structural landscape present in the Na +(glucose) complex. Our experimental approach involves minimal modifications to a typical IR predissociation setup, and can be carried out via ion-dip or isomer-burning methods, providing additional flexibility to suit different experimental needs. In the current study, the single-laser IR predissociation spectrum of Na +(glucose), which clearly indicates contributions from multiple structures, was experimentally disentangled to reveal the presence of three α-conformers and five β-conformers. Comparisons with calculations show that these eight conformations correspond to the lowest energy gas-phase structures with distinctivemore » Na+ coordination.« less

  16. IR-IR Conformation Specific Spectroscopy of Na +(Glucose) Adducts

    DOE PAGES

    Voss, Jonathan M.; Kregel, Steven J.; Fischer, Kaitlyn C.; ...

    2017-09-27

    Here in this paper we report an IR-IR double resonance study of the structural landscape present in the Na +(glucose) complex. Our experimental approach involves minimal modifications to a typical IR predissociation setup, and can be carried out via ion-dip or isomer-burning methods, providing additional flexibility to suit different experimental needs. In the current study, the single-laser IR predissociation spectrum of Na +(glucose), which clearly indicates contributions from multiple structures, was experimentally disentangled to reveal the presence of three α-conformers and five β-conformers. Comparisons with calculations show that these eight conformations correspond to the lowest energy gas-phase structures with distinctivemore » Na+ coordination.« less

  17. Three-dimensional imaging of threading dislocations in GaN crystals using two-photon excitation photoluminescence

    NASA Astrophysics Data System (ADS)

    Tanikawa, Tomoyuki; Ohnishi, Kazuki; Kanoh, Masaya; Mukai, Takashi; Matsuoka, Takashi

    2018-03-01

    The three-dimensional imaging of threading dislocations in GaN films was demonstrated using two-photon excitation photoluminescence. The threading dislocations were shown as dark lines. The spatial resolutions near the surface were about 0.32 and 3.2 µm for the in-plane and depth directions, respectively. The threading dislocations with a density less than 108 cm-2 were resolved, although the aberration induced by the refractive index mismatch was observed. The decrease in threading dislocation density was clearly observed by increasing the GaN film thickness. This can be considered a novel method for characterizing threading dislocations in GaN films without any destructive preparations.

  18. Electrophoretically mediated microanalysis of leucine aminopeptidase using two-photon excited fluorescence detection on a microchip.

    PubMed

    Zugel, S A; Burke, B J; Regnier, F E; Lytle, F E

    2000-11-15

    Two-photon excited fluorescence detection was performed on a microfabricated electrophoresis chip. A calibration curve of the fluorescent tag beta-naphthylamine was performed, resulting in a sensitivity of 2.5 x 10(9) counts M(-1) corresponding to a detection limit of 60 nM. Additionally, leucine aminopeptidase was assayed on the chip using electrophoretically mediated microanalysis. The differential electroosmotic mobilities of the enzyme and substrate, L-leucine beta-naphthylamide, allowed for efficient mixing in an open channel, resulting in the detection of a 30 nM enzyme solution under constant potential. A zero potential incubation for 1 min yielded a calculated detection limit of 4 nM enzyme.

  19. Carcinogenic damage to deoxyribonucleic acid is induced by near-infrared laser pulses in multiphoton microscopy via combination of two- and three-photon absorption

    NASA Astrophysics Data System (ADS)

    Nadiarnykh, Oleg; Thomas, Giju; Van Voskuilen, Johan; Sterenborg, Henricus J. C. M.; Gerritsen, Hans C.

    2012-11-01

    Nonlinear optical imaging modalities (multiphoton excited fluorescence, second and third harmonic generation) applied in vivo are increasingly promising for clinical diagnostics and the monitoring of cancer and other disorders, as they can probe tissue with high diffraction-limited resolution at near-infrared (IR) wavelengths. However, high peak intensity of femtosecond laser pulses required for two-photon processes causes formation of cyclobutane-pyrimidine-dimers (CPDs) in cellular deoxyribonucleic acid (DNA) similar to damage from exposure to solar ultraviolet (UV) light. Inaccurate repair of subsequent mutations increases the risk of carcinogenesis. In this study, we investigate CPD damage that results in Chinese hamster ovary cells in vitro from imaging them with two-photon excited autofluorescence. The CPD levels are quantified by immunofluorescent staining. We further evaluate the extent of CPD damage with respect to varied wavelength, pulse width at focal plane, and pixel dwell time as compared with more pronounced damage from UV sources. While CPD damage has been expected to result from three-photon absorption, our results reveal that CPDs are induced by competing two- and three-photon absorption processes, where the former accesses UVA absorption band. This finding is independently confirmed by nonlinear dependencies of damage on laser power, wavelength, and pulse width.

  20. Multiple emitters in a waveguide: Nonreciprocity and correlated photons at perfect elastic transmission

    NASA Astrophysics Data System (ADS)

    Fang, Yao-Lung L.; Baranger, Harold U.

    2017-07-01

    We investigate interference and correlation effects when several detuned emitters are placed along a one-dimensional photonic waveguide. Such a setup allows multiple interactions between the photons and the strongly coupled emitters, and underlies proposed devices for quantum information processing. We show, first, that a pair of detuned two-level systems (2LS) separated by a half wavelength mimic a driven Λ -type three-level system (3LS) in both the single- and two-photon sectors. There is an interference-induced transparency peak at which the fluorescence is quenched, leaving the transmitted photons completely uncorrelated. Slightly away from this separation, we find that the inelastic scattering (fluorescence) is large, leading to nonlinear effects such as nonreciprocity (rectification). We connect this nonreciprocity to inelastic scattering caused by driving a dark pole and so derive a condition for maximum rectification. Finally, by placing a true 3LS midway between the two 2LS, we show that elastic scattering produces only transmission, but inelastic scattering nevertheless occurs (the fluorescence is not quenched) causing substantial photon correlations.

  1. Nearly Blinking-Free, High-Purity Single-Photon Emission by Colloidal InP/ZnSe Quantum Dots.

    PubMed

    Chandrasekaran, Vigneshwaran; Tessier, Mickaël D; Dupont, Dorian; Geiregat, Pieter; Hens, Zeger; Brainis, Edouard

    2017-10-11

    Colloidal core/shell InP/ZnSe quantum dots (QDs), recently produced using an improved synthesis method, have a great potential in life-science applications as well as in integrated quantum photonics and quantum information processing as single-photon emitters. Single-particle spectroscopy of 10 nm QDs with 3.2 nm cores reveals strong photon antibunching attributed to fast (70 ps) Auger recombination of multiple excitons. The QDs exhibit very good photostability under strong optical excitation. We demonstrate that the antibunching is preserved when the QDs are excited above the saturation intensity of the fundamental-exciton transition. This result paves the way toward their usage as high-purity on-demand single-photon emitters at room temperature. Unconventionally, despite the strong Auger blockade mechanism, InP/ZnSe QDs also display very little luminescence intermittency ("blinking"), with a simple on/off blinking pattern. The analysis of single-particle luminescence statistics places these InP/ZnSe QDs in the class of nearly blinking-free QDs, with emission stability comparable to state-of-the-art thick-shell and alloyed-interface CdSe/CdS, but with improved single-photon purity.

  2. Broad band nonlinear optical absorption measurements of the laser dye IR26 using white light continuum Z-scan

    NASA Astrophysics Data System (ADS)

    Dey, Soumyodeep; Bongu, Sudhakara Reddy; Bisht, Prem Ballabh

    2017-03-01

    We study the nonlinear optical response of a standard dye IR26 using the Z-scan technique, but with the white light continuum. The continuum source of wavelength from 450 nm to 1650 nm has been generated from the photonic crystal fiber on pumping with 772 nm of Ti:Sapphire oscillator. The use of broadband incident pulse enables us to probe saturable absorption (SA) and reverse saturable absorption (RSA) over the large spectral range with a single Z-scan measurement. The system shows SA in the resonant region while it turns to RSA in the non-resonant regions. The low saturation intensity of the dye can be explained based on the simultaneous excitation from ground states to various higher energy levels with the help of composite energy level diagram. The cumulative effects of excited state absorption and thermal induced nonlinear optical effects are responsible for the observed RSA.

  3. A new architecture as transparent electrodes for solar and IR applications based on photonic structures via soft lithography

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

    Kuang, Ping

    2011-01-01

    Transparent conducting electrodes with the combination of high optical transmission and good electrical conductivity are essential for solar energy harvesting and electric lighting devices. Currently, indium tin oxide (ITO) is used because ITO offers relatively high transparency (>80%) to visible light and low sheet resistance (R s = 10 ohms/square (Ω /2)) for electrical conduction. However, ITO is costly due to limited indium reserves, and it is brittle. These disadvantages have motivated the search for other conducting electrodes with similar or better properties. There has been research on a variety of electrode structures involving carbon nanotube networks, graphene films, nanowiremore » and nanopatterned meshes and grids. Due to their novel characteristics in light manipulation and collection, photonic crystal structures show promise for further improvement. Here, we report on a new architecture consisting of nanoscale high aspect ratio metallic photonic structures as transparent electrodes fabricated via a combination of processes. For (Au) and silver (Ag) structures, the visible light transmission can reach as high as 80%, and the sheet resistance of the structure can be as low as 3.2Ω /2. The optical transparency of the high aspect ratio metal structures at visible wavelength range is comparable to that of ITO glass, while their sheet resistance is more than 3 times lower, which indicates a much higher electrical conductivity of the metal structures. Furthermore, the high aspect ratio metal structures have very high infrared (IR) reflection (90%) for the transverse magnetic (TM) mode, which can lead to the development of fabrication of metallic structures as IR filters for heat control applications. Investigations of interdigitated structures based on the high aspect ratio metal electrodes are ongoing to study the feasibility in smart window applications in light transmission modulation.« less

  4. Up-conversion multiwave (White) luminescence in the visible spectral range under excitation by IR laser diodes in the active BaY2F8:Yb3+,Pr3+ medium

    NASA Astrophysics Data System (ADS)

    Pushkar', A. A.; Uvarova, T. V.; Kiiko, V. V.

    2011-08-01

    The possibilities of occupying high-lying 4 f states of Pr3+ ions in the active BaY2F8:Yb3+,Pr3+ medium according to the photon avalanche and step-by-step sensitization mechanisms are compared. It is shown that the photon avalanche is unlikely to occur in the BaY2F8:Yb3+,Pr3+ crystal. The multiband luminescence spectra in the visible spectral range (white emission) under single- and multiwave pumping of BaY2F8:Yb3+,Pr3+ crystal by IR laser diodes are reported.

  5. Development of novel two-photon absorbing chromophores

    NASA Astrophysics Data System (ADS)

    Rogers, Joy E.; Slagle, Jonathan E.; McLean, Daniel G.; Sutherland, Richard L.; Krein, Douglas M.; Cooper, Thomas M.; Brant, Mark; Heinrichs, James; Kannan, Ramamurthi; Tan, Loon-Seng; Urbas, Augustine M.; Fleitz, Paul A.

    2006-08-01

    There has been much interest in the development of two-photon absorbing materials and many efforts to understand the nonlinear absorption properties of these dyes but this area is still not well understood. A computational model has been developed in our lab to understand the nanosecond nonlinear absorption properties that incorporate all of the measured one-photon photophysical parameters of a class of materials called AFX. We have investigated the nonlinear and photophysical properties of the AFX chromophores including the two-photon absorption cross-section, the excited state cross-section, the intersystem crossing quantum yield, and the singlet and triplet excited state lifetimes using a variety of experimental techniques that include UV-visible, fluorescence and phosphorescence spectroscopy, time correlated single photon counting, ultrafast transient absorption, and nanosecond laser flash photolysis. The model accurately predicts the nanosecond nonlinear transmittance data using experimentally measured parameters. Much of the strong nonlinear absorption has been shown to be due to excited state absorption from both the singlet and triplet excited states. Based on this understanding of the nonlinear absorption and the importance of singlet and triplet excited states we have begun to develop new two-photon absorbing molecules within the AFX class as well as linked to other classes of nonlinear absorbing molecules. This opens up the possibilities of new materials with unique and interesting properties. Specifically we have been working on a new class of two-photon absorbing molecules linked to platinum poly-ynes. In the platinum poly-yne chromophores the photophysics are more complicated and we have just started to understand what drives both the linear and non-linear photophysical properties.

  6. Fast and long-range triplet exciton diffusion in metal-organic frameworks for photon upconversion at ultralow excitation power.

    PubMed

    Mahato, Prasenjit; Monguzzi, Angelo; Yanai, Nobuhiro; Yamada, Teppei; Kimizuka, Nobuo

    2015-09-01

    The conversion of low-energy light into photons of higher energy based on sensitized triplet-triplet annihilation upconversion (TTA-UC) has emerged as a promising wavelength-shifting methodology because it permits UC at excitation powers as low as the solar irradiance. However, its application has been significantly hampered by the slow diffusion of excited molecules in solid matrices. Here, we introduce metal-organic frameworks (MOFs) that promote TTA-UC by taking advantage of triplet exciton migration among fluorophores that are regularly aligned with spatially controlled chromophore orientations. We synthesized anthracene-containing MOFs with different molecular orientations, and the analysis of TTA-UC emission kinetics unveiled a high triplet diffusion rate with a micrometre-scale diffusion length. Surface modification of MOF nanocrystals with donor molecules and their encapsulation in glassy poly(methyl methacrylate) (PMMA) allowed the construction of molecular-diffusion-free solid-state upconverters, which lead to an unprecedented maximization of overall UC quantum yield at excitation powers comparable to or well below the solar irradiance.

  7. Dissociative recombination and electron-impact de-excitation in CH photon emission under ITER divertor-relevant plasma conditions

    NASA Astrophysics Data System (ADS)

    van Swaaij, G. A.; Bystrov, K.; Borodin, D.; Kirschner, A.; van der Vegt, L. B.; van Rooij, G. J.; De Temmerman, G.; Goedheer, W. J.

    2012-09-01

    For understanding carbon erosion and redeposition in nuclear fusion devices, it is important to understand the transport and chemical break-up of hydrocarbon molecules in edge plasmas, often diagnosed by emission of the CH A 2Δ-X 2Π Gerö band around 430 nm. The CH A-level can be excited either by electron-impact (EI) or by dissociative recombination (DR) of hydrocarbon ions. These processes were included in the 3D Monte Carlo impurity transport code ERO. A series of methane injection experiments was performed in the high-density, low-temperature linear plasma generator Pilot-PSI, and simulated emission intensity profiles were benchmarked against these experiments. It was confirmed that excitation by DR dominates at Te < 1.5 eV. The results indicate that the fraction of DR events that lead to a CH radical in the A-level and consequent photon emission is at least 10%. Additionally, quenching of the excited CH radicals by EI de-excitation was included in the modeling. This quenching is shown to be significant: depending on the electron density, it reduces the effective CH emission by a factor of 1.4 at ne = 1.3 × 1020 m-3, to 2.8 at ne = 9.3 × 1020 m-3. Its inclusion significantly improved agreement between experiment and modeling.

  8. Near-IR photon number resolving detector design

    NASA Astrophysics Data System (ADS)

    Bogdanski, Jan; Huntington, Elanor H.

    2013-05-01

    Photon-Number-Resolving-Detection (PNRD) capability is crucial for many Quantum-Information (QI) applications, e.g. for Coherent-State-Quantum-Computing, Linear-Optics-Quantum-Computing. In Quantum-Key-Distribution and Quantum-Secret-Sharing over 1310/1550 nm fiber, two other important, defense and information security related, QI applications, it's crucial for the information transmission security to guarantee that the information carriers (photons) are single. Thus a PNRD can provide an additional security level against eavesdropping. Currently, there are at least a couple of promising PNRD technologies in the Near-Infrared, but all of them require cryogenic cooling. Thus a compact, portable PNRD, based on commercial Avalanche-Photo-Diodes (APDs), could be a very useful instrument for many QI experiments. For an APD-based PNRD, it is crucial to measure the APD-current in the beginning of the avalanche. Thus an efficient cancellation of the APD capacitive spikes is a necessary condition for the very weak APD current measurement. The detector's principle is based on two commercial, pair-matched InGaAs/InP APDs, connected in series. It leads to a great cancelation of the capacitive spikes caused by the narrow (300 ps), differential gate-pulses of maximum 4V amplitude assuming that both pulses are perfectly matched in regards to their phases, amplitudes, and shapes. The cancellation scheme could be used for other APD-technologies, e.g. Silicon, extending the detection spectrum from visible to NIR. The design distinguishes itself from other, APD-based, schemes by its scalability feature and its computer controlled cancellation of the capacitive spikes. Furthermore, both APDs could be equally used for the detection purpose, which opens a possibility for the odd-even photon number parity detection.

  9. Controllably releasing long-lived quantum memory for photonic polarization qubit into multiple spatially-separate photonic channels

    PubMed Central

    Chen, Lirong; Xu, Zhongxiao; Zeng, Weiqing; Wen, Yafei; Li, Shujing; Wang, Hai

    2016-01-01

    We report an experiment in which long-lived quantum memories for photonic polarization qubits (PPQs) are controllably released into any one of multiple spatially-separate channels. The PPQs are implemented with an arbitrarily-polarized coherent signal light pulses at the single-photon level and are stored in cold atoms by means of electromagnetic-induced-transparency scheme. Reading laser pulses propagating along the direction at a small angle relative to quantum axis are applied to release the stored PPQs into an output channel. By changing the propagating directions of the read laser beam, we controllably release the retrieved PPQs into 7 different photonic output channels, respectively. At a storage time of δt = 5 μs, the least quantum-process fidelity in 7 different output channels is ~89%. At one of the output channels, the measured maximum quantum-process fidelity for the PPQs is 94.2% at storage time of δt = 0.85 ms. At storage time of 6 ms, the quantum-process fidelity is still beyond the bound of 78% to violate the Bell’s inequality. The demonstrated controllable release of the stored PPQs may extend the capabilities of the quantum information storage technique. PMID:27667262

  10. Enhanced eumelanin emission by stepwise three-photon excitation

    NASA Astrophysics Data System (ADS)

    Kerimo, Josef; Rajadhyaksha, Milind; DiMarzio, Charles A.

    2011-03-01

    Eumelanin fluorescence from Sepia officinalis and black human hair was activated with near-infrared radiation and multiphoton excitation. A third order multiphoton absorption by a step-wise process appears to be the underlying mechanism. The activation was caused by a photochemical process since it could not be reproduced by simple heating. Both fluorescence and brightfield imaging indicate the near-infrared irradiation caused photodamage to the eumelanin and the activated emission originated from the photodamaged region. At least two different components with about thousand-fold enhanced fluorescence were activated and could be distinguished by their excitation properties. One component was excited with wavelengths in the visible region and exhibited linear absorption dependence. The second component could be excited with near-infrared wavelengths and had a third order dependence on the laser power. The third order dependence is explained by a step-wise excited state absorption (ESA) process since it could be observed equally with the CW and femtosecond lasers. The new method for photoactivating the eumelanin fluorescence was used to map the melanin content in human hair.

  11. Indistinguishable and efficient single photons from a quantum dot in a planar nanobeam waveguide

    NASA Astrophysics Data System (ADS)

    KiršanskÄ--, Gabija; Thyrrestrup, Henri; Daveau, Raphaël S.; Dreeßen, Chris L.; Pregnolato, Tommaso; Midolo, Leonardo; Tighineanu, Petru; Javadi, Alisa; Stobbe, Søren; Schott, Rüdiger; Ludwig, Arne; Wieck, Andreas D.; Park, Suk In; Song, Jin D.; Kuhlmann, Andreas V.; Söllner, Immo; Löbl, Matthias C.; Warburton, Richard J.; Lodahl, Peter

    2017-10-01

    We demonstrate a high-purity source of indistinguishable single photons using a quantum dot embedded in a nanophotonic waveguide. The source features a near-unity internal coupling efficiency and the collected photons are efficiently coupled off chip by implementing a taper that adiabatically couples the photons to an optical fiber. By quasiresonant excitation of the quantum dot, we measure a single-photon purity larger than 99.4 % and a photon indistinguishability of up to 94 ±1 % by using p -shell excitation combined with spectral filtering to reduce photon jitter. A temperature-dependent study allows pinpointing the residual decoherence processes, notably the effect of phonon broadening. Strict resonant excitation is implemented as well as another means of suppressing photon jitter, and the additional complexity of suppressing the excitation laser source is addressed. The paper opens a clear pathway towards the long-standing goal of a fully deterministic source of indistinguishable photons, which is integrated on a planar photonic chip.

  12. Two-photon fluorescent sensor for K+ imaging in live cells (Conference Presentation)

    NASA Astrophysics Data System (ADS)

    Sui, Binglin; Yue, Xiling; Kim, Bosung; Belfield, Kevin D.

    2016-03-01

    It is difficult to overstate the physiological importance of potassium for life as its indispensable roles in a variety of biological processes are widely known. As a result, efficient methods for determining physiological levels of potassium are of paramount importance. Despite this, relatively few K+ fluorescence sensors have been reported, with only one being commercially available. A new two-photon excited fluorescent K+ sensor is reported. The sensor is comprised of three moieties, a highly selective K+ chelator as the K+ recognition unit, a boron-dipyrromethene (BODIPY) derivative modified with phenylethynyl groups as the fluorophore, and two polyethylene glycol chains to afford water solubility. The sensor displays very high selectivity (<52-fold) in detecting K+ over other physiological metal cations. Upon binding K+, the sensor switches from non-fluorescent to highly fluorescent, emitting red to near-IR (NIR) fluorescence. The sensor exhibited a good two-photon absorption cross section, 500 GM at 940 nm. Moreover, it is not sensitive to pH in the physiological pH range. Time-dependent cell imaging studies via both one- and two-photon fluorescence microscopy demonstrate that the sensor is suitable for dynamic K+ sensing in living cells.

  13. Excitation and characterization of image potential state electrons on quasi-free-standing graphene

    NASA Astrophysics Data System (ADS)

    Lin, Yi; Li, Yunzhe; Sadowski, Jerzy T.; Jin, Wencan; Dadap, Jerry I.; Hybertsen, Mark S.; Osgood, Richard M.

    2018-04-01

    We investigate the band structure of image potential states in quasi-free-standing graphene (QFG) monolayer islands using angle-resolved two-photon-photoemission spectroscopy. Direct probing by low-energy electron diffraction shows that QFG is formed following oxygen intercalation into the graphene-Ir(111) interface. Despite the apparent decoupling of the monolayer graphene from the Ir substrate, we find that the binding energy of the n =1 image potential state on these QFG islands increases by 0.17 eV, as compared to the original Gr/Ir(111) interface. We use calculations based on density-functional theory to construct an empirical, one-dimensional potential that quantitatively reproduces the image potential state binding energy and links the changes in the interface structure to the shift in energy. Specifically, two factors contribute comparably to this energy shift: a deeper potential well arising from the presence of intercalated oxygen adatoms and a wider potential well associated with the increase in the graphene-Ir distance. While image potential states have not been observed previously on QFG by photoemission, our paper now demonstrates that they may be strongly excited in a well-defined QFG system produced by oxygen intercalation. This opens an opportunity for studying the surface electron dynamics in QFG systems, beyond those found in typical nonintercalated graphene-on-substrate systems.

  14. Excitation and characterization of image potential state electrons on quasi-free-standing graphene

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

    Lin, Yi; Li, Yunzhe; Sadowski, Jerzy T.

    We investigate the band structure of image potential states in quasi-free-standing graphene (QFG) monolayer islands using angle-resolved two-photon-photoemission spectroscopy. Direct probing by low-energy electron diffraction shows that QFG is formed following oxygen intercalation into the graphene-Ir(111) interface. Despite the apparent decoupling of the monolayer graphene from the Ir substrate, we find that the binding energy of the n = 1 image potential state on these QFG islands increases by 0.17 eV, as compared to the original Gr/Ir(111) interface. We use calculations based on density-functional theory to construct an empirical, one-dimensional potential that quantitatively reproduces the image potential state binding energymore » and links the changes in the interface structure to the shift in energy. Specifically, two factors contribute comparably to this energy shift: a deeper potential well arising from the presence of intercalated oxygen adatoms and a wider potential well associated with the increase in the graphene-Ir distance. While image potential states have not been observed previously on QFG by photoemission, our paper now demonstrates that they may be strongly excited in a well-defined QFG system produced by oxygen intercalation. Finally, this opens an opportunity for studying the surface electron dynamics in QFG systems, beyond those found in typical nonintercalated graphene-on-substrate systems.« less

  15. Excitation and characterization of image potential state electrons on quasi-free-standing graphene

    DOE PAGES

    Lin, Yi; Li, Yunzhe; Sadowski, Jerzy T.; ...

    2018-04-09

    We investigate the band structure of image potential states in quasi-free-standing graphene (QFG) monolayer islands using angle-resolved two-photon-photoemission spectroscopy. Direct probing by low-energy electron diffraction shows that QFG is formed following oxygen intercalation into the graphene-Ir(111) interface. Despite the apparent decoupling of the monolayer graphene from the Ir substrate, we find that the binding energy of the n = 1 image potential state on these QFG islands increases by 0.17 eV, as compared to the original Gr/Ir(111) interface. We use calculations based on density-functional theory to construct an empirical, one-dimensional potential that quantitatively reproduces the image potential state binding energymore » and links the changes in the interface structure to the shift in energy. Specifically, two factors contribute comparably to this energy shift: a deeper potential well arising from the presence of intercalated oxygen adatoms and a wider potential well associated with the increase in the graphene-Ir distance. While image potential states have not been observed previously on QFG by photoemission, our paper now demonstrates that they may be strongly excited in a well-defined QFG system produced by oxygen intercalation. Finally, this opens an opportunity for studying the surface electron dynamics in QFG systems, beyond those found in typical nonintercalated graphene-on-substrate systems.« less

  16. Single-photon absorption by single photosynthetic light-harvesting complexes

    NASA Astrophysics Data System (ADS)

    Chan, Herman C. H.; Gamel, Omar E.; Fleming, Graham R.; Whaley, K. Birgitta

    2018-03-01

    We provide a unified theoretical approach to the quantum dynamics of absorption of single photons and subsequent excitonic energy transfer in photosynthetic light-harvesting complexes. Our analysis combines a continuous mode < n > -photon quantum optical master equation for the chromophoric system with the hierarchy of equations of motion describing excitonic dynamics in presence of non-Markovian coupling to vibrations of the chromophores and surrounding protein. We apply the approach to simulation of absorption of single-photon coherent states by pigment-protein complexes containing between one and seven chromophores, and compare with results obtained by excitation using a thermal radiation field. We show that the values of excitation probability obtained under single-photon absorption conditions can be consistently related to bulk absorption cross-sections. Analysis of the timescale and efficiency of single-photon absorption by light-harvesting systems within this full quantum description of pigment-protein dynamics coupled to a quantum radiation field reveals a non-trivial dependence of the excitation probability and the excited state dynamics induced by exciton-phonon coupling during and subsequent to the pulse, on the bandwidth of the incident photon pulse. For bandwidths equal to the spectral bandwidth of Chlorophyll a, our results yield an estimation of an average time of ˜0.09 s for a single chlorophyll chromophore to absorb the energy equivalent of one (single-polarization) photon under irradiation by single-photon states at the intensity of sunlight.

  17. Experimental demonstration of photon upconversion via cooperative energy pooling

    PubMed Central

    Weingarten, Daniel H.; LaCount, Michael D.; van de Lagemaat, Jao; Rumbles, Garry; Lusk, Mark T.; Shaheen, Sean E.

    2017-01-01

    Photon upconversion is a fundamental interaction of light and matter that has applications in fields ranging from bioimaging to microfabrication. However, all photon upconversion methods demonstrated thus far involve challenging aspects, including requirements of high excitation intensities, degradation in ambient air, requirements of exotic materials or phases, or involvement of inherent energy loss processes. Here we experimentally demonstrate a mechanism of photon upconversion in a thin film, binary mixture of organic chromophores that provides a pathway to overcoming the aforementioned disadvantages. This singlet-based process, called Cooperative Energy Pooling (CEP), utilizes a sensitizer-acceptor design in which multiple photoexcited sensitizers resonantly and simultaneously transfer their energies to a higher-energy state on a single acceptor. Data from this proof-of-concept implementation is fit by a proposed model of the CEP process. Design guidelines are presented to facilitate further research and development of more optimized CEP systems. PMID:28294129

  18. Experimental demonstration of photon upconversion via cooperative energy pooling

    NASA Astrophysics Data System (ADS)

    Weingarten, Daniel H.; Lacount, Michael D.; van de Lagemaat, Jao; Rumbles, Garry; Lusk, Mark T.; Shaheen, Sean E.

    2017-03-01

    Photon upconversion is a fundamental interaction of light and matter that has applications in fields ranging from bioimaging to microfabrication. However, all photon upconversion methods demonstrated thus far involve challenging aspects, including requirements of high excitation intensities, degradation in ambient air, requirements of exotic materials or phases, or involvement of inherent energy loss processes. Here we experimentally demonstrate a mechanism of photon upconversion in a thin film, binary mixture of organic chromophores that provides a pathway to overcoming the aforementioned disadvantages. This singlet-based process, called Cooperative Energy Pooling (CEP), utilizes a sensitizer-acceptor design in which multiple photoexcited sensitizers resonantly and simultaneously transfer their energies to a higher-energy state on a single acceptor. Data from this proof-of-concept implementation is fit by a proposed model of the CEP process. Design guidelines are presented to facilitate further research and development of more optimized CEP systems.

  19. Dual photon excitation microscopy and image threshold segmentation in live cell imaging during compression testing.

    PubMed

    Moo, Eng Kuan; Abusara, Ziad; Abu Osman, Noor Azuan; Pingguan-Murphy, Belinda; Herzog, Walter

    2013-08-09

    Morphological studies of live connective tissue cells are imperative to helping understand cellular responses to mechanical stimuli. However, photobleaching is a constant problem to accurate and reliable live cell fluorescent imaging, and various image thresholding methods have been adopted to account for photobleaching effects. Previous studies showed that dual photon excitation (DPE) techniques are superior over conventional one photon excitation (OPE) confocal techniques in minimizing photobleaching. In this study, we investigated the effects of photobleaching resulting from OPE and DPE on morphology of in situ articular cartilage chondrocytes across repeat laser exposures. Additionally, we compared the effectiveness of three commonly-used image thresholding methods in accounting for photobleaching effects, with and without tissue loading through compression. In general, photobleaching leads to an apparent volume reduction for subsequent image scans. Performing seven consecutive scans of chondrocytes in unloaded cartilage, we found that the apparent cell volume loss caused by DPE microscopy is much smaller than that observed using OPE microscopy. Applying scan-specific image thresholds did not prevent the photobleaching-induced volume loss, and volume reductions were non-uniform over the seven repeat scans. During cartilage loading through compression, cell fluorescence increased and, depending on the thresholding method used, led to different volume changes. Therefore, different conclusions on cell volume changes may be drawn during tissue compression, depending on the image thresholding methods used. In conclusion, our findings confirm that photobleaching directly affects cell morphology measurements, and that DPE causes less photobleaching artifacts than OPE for uncompressed cells. When cells are compressed during tissue loading, a complicated interplay between photobleaching effects and compression-induced fluorescence increase may lead to interpretations in

  20. Photoinduced coherent acoustic phonon dynamics inside Mott insulator Sr2IrO4 films observed by femtosecond X-ray pulses

    NASA Astrophysics Data System (ADS)

    Zhang, Bing-Bing; Liu, Jian; Wei, Xu; Sun, Da-Rui; Jia, Quan-Jie; Li, Yuelin; Tao, Ye

    2017-04-01

    We investigate the transient photoexcited lattice dynamics in a layered perovskite Mott insulator Sr2IrO4 film by femtosecond X-ray diffraction using a laser plasma-based X-ray source. The ultrafast structural dynamics of Sr2IrO4 thin films are determined by observing the shift and broadening of (0012) Bragg diffraction after excitation by 1.5 eV and 3.0 eV pump photons for films with different thicknesses. The observed transient lattice response can be well interpreted as a distinct three-step dynamics due to the propagation of coherent acoustic phonons generated by photoinduced quasiparticles (QPs). Employing a normalized phonon propagation model, we found that the photoinduced angular shifts of the Bragg peak collapse into a universal curve after introducing normalized coordinates to account for different thicknesses and pump photon energies, pinpointing the origin of the lattice distortion and its early evolution. In addition, a transient photocurrent measurement indicates that the photoinduced QPs are charge neutral excitons. Mapping the phonon propagation and correlating its dynamics with the QP by ultrafast X-ray diffraction (UXRD) establish a powerful way to study electron-phonon coupling and uncover the exotic physics in strongly correlated systems under nonequilibrium conditions.

  1. The Path to a UV/optical/IR Flagship: ATLAST and Its Predecessors

    NASA Technical Reports Server (NTRS)

    Thronson, Harley; Bolcar, Matthew R.; Clampin, Mark; Crooke, Julie; Feinberg, Lee; Oegerle, William; Postman, Marc; Rioux, Norman; Stahl, H. Philip; Stapelfeldt, Karl

    2016-01-01

    The recently completed study for the Advanced Technology Large-Aperture Telescope (ATLAST) was the culmination of three years of work that built upon earlier engineering designs, science objectives, and sustained recommendations for technology investments. Since the mid-1980s, multiple teams of astronomers, technologists, and engineers have developed concepts for a large-aperture UV/optical/IR space observatory to follow the Hubble Space Telescope (HST). Especially over the past decade, technology advances and exciting scientific results has led to growing support for development in the 2020s of a large UVOIR space observatory. Here we summarize the history of major mission designs, scientific goals, key technology recommendations, community workshops and conferences, and recommendations to NASA for a major UV/optical/IR observatory to follow HST. We conclude with a capsule summary of the ATLAST reference design developed over the past three years.

  2. Photonic-assisted microwave signal multiplication and modulation using a silicon Mach–Zehnder modulator

    PubMed Central

    Long, Yun; Zhou, Linjie; Wang, Jian

    2016-01-01

    Photonic generation of microwave signal is obviously attractive for many prominent advantages, such as large bandwidth, low loss, and immunity to electromagnetic interference. Based on a single integrated silicon Mach–Zehnder modulator (MZM), we propose and experimentally demonstrate a simple and compact photonic scheme to enable frequency-multiplicated microwave signal. Using the fabricated integrated MZM, we also demonstrate the feasibility of microwave amplitude-shift keying (ASK) modulation based on integrated photonic approach. In proof-of-concept experiments, 2-GHz frequency-doubled microwave signal is generated using a 1-GHz driving signal. 750-MHz/1-GHz frequency-tripled/quadrupled microwave signals are obtained with a driving signal of 250 MHz. In addition, a 50-Mb/s binary amplitude coded 1-GHz microwave signal is also successfully generated. PMID:26832305

  3. Defect States in Copper Indium Gallium Selenide Solar Cells from Two-Wavelength Excitation Photoluminescence Spectroscopy

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

    Jensen, Soren A.; Dippo, Patricia; Mansfield, Lorelle M.

    2016-11-21

    We use two-wavelength excitation photoluminescence spectroscopy to probe defect states in CIGS thin films. Above-Eg excitation is combined with a tunable IR bias light that modulates the population of the defect states. We find that IR illumination in the range of 1400-2000 nm (0.62-0.89 eV) causes a reduction of the PL intensity, the magnitude of which scales linearly with IR power. Further, KF post deposition treatment has only a modest influence on the effect of the IR excitation. Initial data suggest that we have developed an optical characterization tool for band-gap defect states.

  4. Wide field-of-view, multi-region two-photon imaging of neuronal activity in the mammalian brain

    PubMed Central

    Stirman, Jeffrey N.; Smith, Ikuko T.; Kudenov, Michael W.; Smith, Spencer L.

    2016-01-01

    Two-photon calcium imaging provides an optical readout of neuronal activity in populations of neurons with subcellular resolution. However, conventional two-photon imaging systems are limited in their field of view to ~1 mm2, precluding the visualization of multiple cortical areas simultaneously. Here, we demonstrate a two-photon microscope with an expanded field of view (>9.5 mm2) for rapidly reconfigurable simultaneous scanning of widely separated populations of neurons. We custom designed and assembled an optimized scan engine, objective, and two independently positionable, temporally multiplexed excitation pathways. We used this new microscope to measure activity correlations between two cortical visual areas in mice during visual processing. PMID:27347754

  5. Performance analysis of GeSn-alloy-based multiple quantum well transistor laser

    NASA Astrophysics Data System (ADS)

    Ranjan, Ravi; Pareek, Prakash; Anwer Askari, Syed Sadique; Das, Mukul K.

    2018-02-01

    The Group IV Photonics (GFP) which include an alloy of Si, Ge & Sn that gives a direct bandgap material (GeSn, SiGeSn) in near and mid-IR region used as an active material in photonics devices. The multiple quantum well SiGeSn/GeSn transistor laser structure is considered in this paper and performance parameters are evaluated for the same. The result shows that the threshold base current density (2.6 kA/cm2) for the proposed device initially decreases with increasing number of quantum well (QW) and later on it saturates. The current gain and output photon density of the device decreases and increases respectively, with increasing number of QW.

  6. Circuit QED with qutrits: Coupling three or more atoms via virtual-photon exchange

    NASA Astrophysics Data System (ADS)

    Zhao, Peng; Tan, Xinsheng; Yu, Haifeng; Zhu, Shi-Liang; Yu, Yang

    2017-10-01

    We present a model to describe a generic circuit QED system which consists of multiple artificial three-level atoms, namely, qutrits, strongly coupled to a cavity mode. When the state transition of the atoms disobeys the selection rules the process that does not conserve the number of excitations can happen determinatively. Therefore, we can realize coherent exchange interaction among three or more atoms mediated by the exchange of virtual photons. In addition, we generalize the one-cavity-mode mediated interactions to the multicavity situation, providing a method to entangle atoms located in different cavities. Using experimentally feasible parameters, we investigate the dynamics of the model including three cyclic-transition three-level atoms, for which the two lowest energy levels can be treated as qubits. Hence, we have found that two qubits can jointly exchange excitation with one qubit in a coherent and reversible way. In the whole process, the population in the third level of atoms is negligible and the cavity photon number is far smaller than 1. Our model provides a feasible scheme to couple multiple distant atoms together, which may find applications in quantum information processing.

  7. Enhancement of the dynamic Casimir effect within a metal photonic crystal

    NASA Astrophysics Data System (ADS)

    Ueta, Tsuyoshi

    2013-05-01

    If the counterposed metal plates are vibrated, when the gap between the plates becomes narrow, the energy of stationary states between the plates increases, and when it spreads, the energy decreases. Light with the energy for this energy difference arises. This is called dynamical Casimir effect. The author has so far investigated the interaction between lattice vibration and light in a one-dimensional metal photonic crystal whose stacked components are artificially vibrated by using actuators. A simple model was numerically analyzed, and the following novel phenomena were found out. The lattice vibration generates the light of frequency which added the integral multiple of the vibration frequency to that of the incident wave and also amplifies the incident wave resonantly. On a resonance, the amplification factor increases very rapidly with the number of layers. Resonance frequencies change with the phases of lattice vibration. The amplification phenomenon was analytically discussed for low frequency of the lattice vibration and is confirmed by numerical works. The lattice-vibrating metal photonic crystal is a system of dynamical Casimir effect connected in series, and so we can expect that a dynamical Casimir effect is enhanced by the photonic band effect. In the present study, when an electromagnetic field between metal plates is in the ground state in a one-dimensional metal photonic crystal, the radiation of electromagnetic wave in excited states has been investigated by artificially introducing lattice vibration to the photonic crystal. In this case as well as a dynamical Casimir effect, it has been shown that the harmonics of a ground state are generated just by vibrating a photonic crystal even without an incident wave. The dependencies of the radiating power on the number of layers and on the wavenumber of the lattice vibration are remarkable. It has found that the radiation amplitude on lower excited states is not necessarily large and radiation on

  8. Broadband multiple responses of surface modes in quasicrystalline plasmonic structure

    PubMed Central

    Yuan, Haiming; Jiang, Xiangqian; Huang, Feng; Sun, Xiudong

    2016-01-01

    We numerically study the multiple excitation of surface modes in 2D photonic quasicrystal/metal/substrate structure. An improved rigorous coupled wave analysis method that can handle the quasicrystalline structure is presented. The quasicrystalline lattice, which refers to Penrose tiling in this paper, is generated by the cut-and-project method. The normal incidence spectrum presents a broadband multiple responses property. We find that the phase matching condition determines the excitation frequency for a given incident angle, while the depth of the reflection valley depends on the incident polarization. The modes will split into several sub-modes at oblique incidence, which give rise to the appearance of more responses on the spectrum. PMID:27492782

  9. Integrated and dispersed photon echo studies of nitrile stretching vibration of 4-cyanophenol in methanol.

    PubMed

    Ha, Jeong-Hyon; Lee, Kyung-Koo; Park, Kwang-Hee; Choi, Jun-Ho; Jeon, Seung-Joon; Cho, Minhaeng

    2009-05-28

    By means of integrated and dispersed IR photon echo measurement methods, the vibrational dynamics of C-N stretch modes in 4-cyanophenol and 4-cyanophenoxide in methanol is investigated. The vibrational frequency-frequency correlation function (FFCF) is retrieved from the integrated photon echo signals by assuming that the FFCF is described by two exponential functions with about 400 fs and a few picosecond components. The excited state lifetimes of the C-N stretch modes of neutral and anionic 4-cyanophenols are 1.45 and 0.91 ps, respectively, and the overtone anharmonic frequency shifts are 25 and 28 cm(-1). At short waiting times, a notable underdamped oscillation, which is attributed to a low-frequency intramolecular vibration coupled to the CN stretch, in the integrated and dispersed vibrational echo as well as transient grating signals was observed. The spectral bandwidths of IR absorption and dispersed vibrational echo spectra of the 4-cyanophenoxide are significantly larger than those of its neutral form, indicating that the strong interaction between phenoxide and methanol causes large frequency fluctuation and rapid population relaxation. The resonance effects in a paradisubstituted aromatic compound would be of interest in understanding the conjugation effects and their influences on chemical reactivity of various aromatic compounds in organic solvents.

  10. Excited-state dynamics of acetylene excited to individual rotational level of the V04K01 subband

    NASA Astrophysics Data System (ADS)

    Makarov, Vladimir I.; Kochubei, Sergei A.; Khmelinskii, Igor V.

    2006-01-01

    Dynamics of the IR emission induced by excitation of the acetylene molecule using the (32Ka0,1,2,ÃAu1←41la1,X˜Σg+1) transition was investigated. The observed IR emission was assigned to transitions between the ground-state vibrational levels. Acetylene fluorescence quenching induced by external electric and magnetic fields acting upon the system prepared using the (34Ka1,ÃAu1←00la0,X˜Σg+1) excitation was also studied. External electric field creates an additional radiationless pathway to the ground-state levels, coupling levels of the ÃAu1 excited state to the quasiresonant levels of the X˜Σg+1 ground state. The level density of the ground state in the vicinity of the excited state is very high, thus the electric-field-induced transition is irreversible, with the rate constant described by the Fermi rule. Magnetic field alters the decay profile without changing the fluorescence quantum yield in collisionless conditions. IR emission from the CCH transient was detected, and was also affected by the external electric and magnetic fields. Acetylene predissociation was demonstrated to proceed by the direct S1→S0 mechanism. The results were explained using the previously developed theoretical approach, yielding values of the relevant model parameters.

  11. Excitation of multiple surface-plasmon-polariton waves using a compound surface-relief grating

    NASA Astrophysics Data System (ADS)

    Faryad, Muhammad; Lakhtakia, Akhlesh

    2012-01-01

    The excitation of multiple surface-plasmon-polariton waves, all of the same frequency but different polarization states, phase speeds, spatial profiles and degrees of localization, by a compound surface-relief grating formed by a metal and a rugate filter, both of finite thickness, was studied using the rigorous coupled-wave approach. Each period of the compound surface-relief grating was chosen to have an integral number of periods of two different simple surface-relief gratings. The excitation of different SPP waves was inferred from the absorptance peaks that were independent of the thickness of the rugate filter. The excitation of each SPP wave could be attributed to either a simple surface-relief grating present in the compound surface-relief grating or to the compound surface-relief grating itself. However, the excitation of SPP waves was found to be less efficient with the compound surface-relief grating than with a simple surface-relief grating.

  12. Thermal Photon Radiation in High Multiplicity p + Pb Collisions at the Large Hadron Collider

    DOE PAGES

    Shen, Chun; Paquet, Jean-François; Denicol, Gabriel S.; ...

    2016-02-18

    We observed the collective behavior of hadronic particles in high multiplicity proton-lead collisions at the Large Hadron Collider, as well as in deuteron-gold collisions at the Relativistic Heavy-Ion Collider. In our work we present the first calculation, in the hydrodynamic framework, of thermal photon radiation from such small collision systems. Owing to their compact size, these systems can reach temperatures comparable to those in central nucleus-nucleus collisions. Moreover, the thermal photons can thus shine over the prompt background, and increase the low p T direct photon spectrum by a factor of 2–3 in 0%–1% p+Pb collisions at 5.02 TeV. Thismore » thermal photon enhancement can therefore serve as a signature of the existence of a hot quark-gluon plasma during the evolution of these small collision systems, as well as validate hydrodynamic behavior in small systems.« less

  13. Optical properties of an inhomogeneously broadened ΛV-system with multiple excited states

    NASA Astrophysics Data System (ADS)

    Kaur, Paramjit; Bharti, Vineet; Wasan, Ajay

    2014-09-01

    We present a theoretical model using a density matrix approach to show the influence of multiple excited states on the optical properties of an inhomogeneously broadened ?V-system of the ?Rb D2 line. These closely spaced multiple excited states cause asymmetry in absorption and dispersion profiles. We observe the reduced absorption profiles, due to dressed state interactions of the applied electromagnetic fields, which results the Mollow sideband-like transparency windows. In a room temperature vapor, we obtain a narrow enhanced absorption and steep positive dispersion at the line center when the strengths of control and pump fields are equal. Here, we show how the probe transmittance varies when it passes through the atomic medium. We also discuss the transient behavior of our system which agrees well with the corresponding absorption and dispersion profiles. This study has potential applications in controllability of group velocity, and for optical and quantum information processing.

  14. Extracting diagnostic stromal organization features based on intrinsic two-photon excited fluorescence and second-harmonic generation signals

    NASA Astrophysics Data System (ADS)

    Zhuo, Shuangmu; Chen, Jianxin; Xie, Shusen; Hong, Zhibin; Jiang, Xingshan

    2009-03-01

    Intrinsic two-photon excited fluorescence (TPEF) and second-harmonic generation (SHG) signals are shown to differentiate between normal and neoplastic human esophageal stroma. It was found that TPEF and SHG signals from normal and neoplastic stroma exhibit different organization features, providing quantitative information about the biomorphology and biochemistry of tissue. By comparing normal with neoplastic stroma, there were significant differences in collagen-related changes, elastin-related changes, and alteration in proportions of matrix molecules, giving insight into the stromal changes associated with cancer progression and providing substantial potential to be applied in vivo to the clinical diagnosis of epithelial precancers and cancers.

  15. Label-free distinguishing between neurons and glial cells based on two-photon excited fluorescence signal of neuron perinuclear granules

    NASA Astrophysics Data System (ADS)

    Du, Huiping; Jiang, Liwei; Wang, Xingfu; Liu, Gaoqiang; Wang, Shu; Zheng, Liqin; Li, Lianhuang; Zhuo, Shuangmu; Zhu, Xiaoqin; Chen, Jianxin

    2016-08-01

    Neurons and glial cells are two critical cell types of brain tissue. Their accurate identification is important for the diagnosis of psychiatric disorders such as depression and schizophrenia. In this paper, distinguishing between neurons and glial cells by using the two-photon excited fluorescence (TPEF) signals of intracellular intrinsic sources was performed. TPEF microscopy combined with TUJ-1 and GFAP immunostaining and quantitative image analysis demonstrated that the perinuclear granules of neurons in the TPEF images of brain tissue and the primary cultured cortical cells were a unique characteristic of neurons compared to glial cells which can become a quantitative feature to distinguish neurons from glial cells. With the development of miniaturized TPEF microscope (‘two-photon fiberscopes’) imaging devices, TPEF microscopy can be developed into an effective diagnostic and monitoring tool for psychiatric disorders such as depression and schizophrenia.

  16. Experimental demonstration of photon upconversion via cooperative energy pooling

    DOE PAGES

    Weingarten, Daniel H.; LaCount, Michael D.; van de Lagemaat, Jao; ...

    2017-03-15

    Photon upconversion is a fundamental interaction of light and matter that has applications in fields ranging from bioimaging to microfabrication. However, all photon upconversion methods demonstrated thus far involve challenging aspects, including requirements of high excitation intensities, degradation in ambient air, requirements of exotic materials or phases, or involvement of inherent energy loss processes. Here we experimentally demonstrate a mechanism of photon upconversion in a thin film, binary mixture of organic chromophores that provides a pathway to overcoming the aforementioned disadvantages. This singlet-based process, called Cooperative Energy Pooling (CEP), utilizes a sensitizer-acceptor design in which multiple photoexcited sensitizers resonantly andmore » simultaneously transfer their energies to a higher-energy state on a single acceptor. Data from this proof-of-concept implementation is fit by a proposed model of the CEP process. As a result, design guidelines are presented to facilitate further research and development of more optimized CEP systems.« less

  17. Novel microfabrication stage allowing for one-photon and multi-photon light assisted molecular immobilization and for multi-photon microscope

    NASA Astrophysics Data System (ADS)

    Gonçalves, Odete; Snider, Scott; Zadoyan, Ruben; Nguyen, Quoc-Thang; Vorum, Henrik; Petersen, Steffen B.; Neves-Petersen, Maria Teresa

    2017-02-01

    Light Assisted Molecular Immobilization (LAMI) results in spatially oriented and localized covalent coupling of biomolecules onto thiol reactive surfaces. LAMI is possible due to the conserved spatial proximity between aromatic residues and disulfide bridges in proteins. When aromatic residues are excited with UV light (275-295nm), disulphide bridges are disrupted and the formed thiol groups covalently bind to surfaces. Immobilization hereby reported is achieved in a microfabrication stage coupled to a fs-laser, through one- or multi-photon excitation. The fundamental 840nm output is tripled to 280nm and focused onto the sample, leading to one-photon excitation and molecular immobilization. The sample rests on a xyz-stage with micrometer step resolution and is illuminated according to a pattern uploaded to the software controlling the stage and the shutter. Molecules are immobilized according to such pattern, with micrometer spatial resolution. Spatial masks inserted in the light path lead to light diffraction patterns used to immobilize biomolecules with submicrometer spatial resolution. Light diffraction patterns are imaged by an inbuilt microscope. Two-photon microscopy and imaging of the fluorescent microbeads is shown. Immobilization of proteins, e.g. C-reactive protein, and of an engineered molecular beacon has been successfully achieved. The beacon was coupled to a peptide containing a disulfide bridge neighboring a tryptophan residue, being this way possible to immobilize the beacon on a surface using one-photon LAMI. This technology is being implemented in the creation of point-of-care biosensors aiming at the detection of cancer and cardiovascular disease markers.

  18. WFC3 TV3 Testing: IR Channel Blue Leaks

    NASA Astrophysics Data System (ADS)

    Brown, Thomas R.

    2008-03-01

    A new IR detector (IR4; FPA165) is housed in WFC3 during the current campaign of thermal vacuum (TV) ground testing at GSFC. As part of these tests, we measured the IR channel throughput. Compared to the previous IR detectors, IR4 has much higher quantum efficiency at all wavelengths, particularly in the optical. The total throughput for the IR channel is still low in the optical, due to the opacity of the IR filters at these wavelengths, but there is a small wavelength region (~710-830 nm) where these filters do not offer as much blocking as needed to meet Contract End Item specifications. For this reason, the throughput measurements were extended into the blue to quantify the amount of blue leak in the narrow and medium IR bandpasses where a few percent of the measured flux could come from optical photons when observing hot sources. The results are tabulated here.

  19. Early-Time Excited-State Relaxation Dynamics of Iridium Compounds: Distinct Roles of Electron and Hole Transfer.

    PubMed

    Liu, Xiang-Yang; Zhang, Ya-Hui; Fang, Wei-Hai; Cui, Ganglong

    2018-06-28

    Excited-state and photophysical properties of Ir-containing complexes have been extensively studied because of their potential applications as organic light-emitting diode emitting materials. However, their early time excited-state relaxation dynamics are less explored computationally. Herein we have employed our recently implemented TDDFT-based generalized surface-hopping dynamics method to simulate excited-state relaxation dynamics of three Ir(III) compounds having distinct ligands. According to our multistate dynamics simulations including five excited singlet states i.e., S n ( n = 1-5) and ten excited triplet states, i.e., T n ( n = 1-10), we have found that the intersystem crossing (ISC) processes from the S n to T n are very efficient and ultrafast in these three Ir(III) compounds. The corresponding ISC rates are estimated to be 65, 81, and 140 fs, which are reasonably close to the experimentally measured ca. 80, 80, and 110 fs. In addition, the internal conversion (IC) processes within respective singlet and triplet manifolds are also ultrafast. These ultrafast IC and ISC processes are caused by large nonadiabatic and spin-orbit couplings, respectively, as well as small energy gaps. Importantly, although these Ir(III) complexes share similar macroscopic phenomena, i.e., ultrafast IC and ISC, their microscopic excited-state relaxation mechanism and dynamics are qualitatively distinct. Specifically, the dynamical behaviors of electron and hole and their roles are variational in modulating the excited-state relaxation dynamics of these Ir(III) compounds. In other words, the electronic properties of the ligands that are coordinated with the central Ir(III) atom play important roles in regulating the microscopic excited-state relaxation dynamics. These gained insights could be useful for rationally designing Ir(III) compounds with excellent photoluminescence.

  20. Linear and Nonlinear Optical Properties of Photoresponsive [60]Fullerene Hybrid Triads and Tetrads with Dual NIR Two-Photon Absorption Characteristics

    PubMed Central

    Jeon, Seaho; Haley, Joy; Flikkema, Jonathan; Nalla, Venkatram; Wang, Min; Sfeir, Matthew; Tan, Loon-Seng; Cooper, Thomas; Ji, Wei; Hamblin, Michael R.; Chiang, Long Y.

    2013-01-01

    Two C60-(antenna)x analogous compounds having branched hybrid triad C60(>DPAF-C18)(>CPAF-C2M) and tetrad C60(>DPAF-C18)(>CPAF-C2M)2 nanostructures were synthesized and characterized. The structural design was intended to facilitate the ultrafast fs intramolecular energy-transfer from photoexcited C60[>1(DPAF)*-C18](>CPAF-C2M)1or2 or C60(>DPAF-C18)[>1(CPAF)*-C2M]1or2 to the C60> cage moiety upon two-photon pumping at either 780 or 980 nm, respectively. The latter nanostructure showed approximately equal extinction coefficients of optical absorption over 400–550 nm that corresponds to near-IR two-photon based excitation wavelengths at 780–1100 nm for broadband nonlinear optical (NLO) applications. Aside from their enhanced two-photon absorption (2PA) activity at 780 nm, we also demonstrated ultrafast photo-responses at 980 nm showing 2PA cross-section (σ2) values of 995–1100 GM for the hybrid tetrad. These σ2 values were correlated to the observed good efficiency in reducing fs light-transmittance down to 35% at the light intensity of 110 GW/cm2. Accordingly, 2PA characteristics of these nanostructures at multiple NIR wavelengths provided support for their suitability in uses as broadband NLO nanomaterials at 600–1100 nm that includes the 2PA ability of two antenna, DPAF (700–850 nm) and CPAF (850–1100 nm), and the fullerene cage at shorter wavelengths (600–700 nm). PMID:24163713

  1. Two-photon interband absorption coefficients in tungstate and molybdate crystals

    NASA Astrophysics Data System (ADS)

    Lukanin, V. I.; Karasik, A. Ya.

    2015-02-01

    Two-photon absorption (TPA) coefficients were measured in tungstate and molybdate crystals - BaWO4, KGW, CaMoO4, BaMoO4, CaWO4, PbWO4 and ZnWO4 upon different orientations of excitation polarization with respect to the crystallographic axes. Trains of 25 ps pulses with variable radiation intensities of third (349 nm) harmonics of passively mode-locked 1047 nm Nd:YLF laser were used for interband two-photon excitation of the crystals. It was suggested that in the case, when 349 nm radiation pumping energy exceeds the bandgap width (hν>Eg), the nonlinear excitation process can be considered as two-step absorption. The interband two-photon absorption in all the studied crystals induces the following one-photon absorption from the exited states, which affects the nonlinear process dynamics and leads to a hysteresis in the dependence of the transmission on the excitation intensity. This fact was taken into account under analysis of the experimental dependences of the reciprocal transmission on the excitation intensity. Laser excitation in the transparency region of the crystals caused stimulated Raman scattering (SRS) not for all the crystals studied. The measured nonlinear coefficients allowed us to explain the suppression of SRS in crystals as a result of competition between the SRS and TPA.

  2. Three-photon Gaussian-Gaussian-Laguerre-Gaussian excitation of a localized atom to a highly excited Rydberg state

    NASA Astrophysics Data System (ADS)

    Mashhadi, L.

    2017-12-01

    Optical vortices are currently one of the most intensively studied topics in light-matter interaction. In this work, a three-step axial Doppler- and recoil-free Gaussian-Gaussian-Laguerre-Gaussian (GGLG) excitation of a localized atom to the highly excited Rydberg state is presented. By assuming a large detuning for intermediate states, an effective quadrupole excitation related to the Laguerre-Gaussian (LG) excitation to the highly excited Rydberg state is obtained. This special excitation system radially confines the single highly excited Rydberg atom independently of the trapping system into a sharp potential landscape into the so-called ‘far-off-resonance optical dipole-quadrupole trap’ (FORDQT). The key parameters of the Rydberg excitation to the highly excited state, namely the effective Rabi frequency and the effective detuning including a position-dependent AC Stark shift, are calculated in terms of the basic parameters of the LG beam and of the polarization of the excitation lasers. It is shown that the obtained parameters can be tuned to have a precise excitation of a single atom to the desired Rydberg state as well. The features of transferring the optical orbital and spin angular momentum of the polarized LG beam to the atom via quadrupole Rydberg excitation offer a long-lived and controllable qudit quantum memory. In addition, in contrast to the Gaussian laser beam, the doughnut-shaped LG beam makes it possible to use a high intensity laser beam to increase the signal-to-noise ratio in quadrupole excitation with minimized perturbations coming from stray light broadening in the last Rydberg excitation process.

  3. Engaging college physics students with photonics research

    NASA Astrophysics Data System (ADS)

    Adams, Rhys; Chen, Lawrence R.

    2017-08-01

    As educators and researchers in the field of photonics, we find what we do to be very exciting, and sharing this passion and excitement to our university students is natural to us. Via outreach programs and college research funding, a new college and university collaboration has broadened our student audience: photonics is brought into the college classroom and research opportunities are provided to college students. Photonics-themed active learning activities are conducted in the college Waves and Modern Physics class, helping students forge relationships between course content and modern communications technologies. Presentations on photonics research are prepared and presented by the professor and past college student-researchers. The students are then given a full tour of the photonics university laboratories. Furthermore, funds are set aside to give college students a unique opportunity to assist the college professor with experiments during a paid summer research internship.

  4. Molecular hydrogen in the vicinity of NGC 7538 IRS 1 and IRS 2 - Temperature and ortho-to-para ratio

    NASA Technical Reports Server (NTRS)

    Hoban, Susan; Reuter, Dennis C.; Mumma, Michael J.; Storrs, Alex D.

    1991-01-01

    Near-infrared spectroscopic observations of the active star-forming region near NGC 7538 IRS 1 and IRS 2 were made. The relative intensities of the v = 1-0 Q(1), Q(3), and Q(5) lines of molecular hydrogen are used to calculate a rotational excitation temperature. Comparison of the measured intensity of the Q(2) transition relative to the intensity of Q(1) and Q(3) permitted the retrieval of the ratio of ortho-to-para hydrogen. It is found that an ortho-to-para ratio of between 1.6 and 2.35 is needed to explain the Q-branch line intensity ratios, depending on the excitation model used. This range in ortho-to-para ratios implies a range of molecular hydrogen formation temperature of approximately 105 K to 140 K.

  5. Molecular structures and excited states of CpM(CO)(2) (Cp = eta(5)-C(5)H(5); M = Rh, Ir) and [Cl(2)Rh(CO)(2)](-). Theoretical evidence for a competitive charge transfer mechanism.

    PubMed

    Hu, Zhenming; Boyd, Russell J; Nakatsuji, Hiroshi

    2002-03-20

    Molecular structures and excited states of CpM(CO)(2) (Cp = eta(5)-C(5)H(5); M = Rh, Ir) and [Cl(2)Rh(CO)(2)](-) complexes have been investigated using the B3LYP and the symmetry-adapted cluster (SAC)/SAC-configuration interaction (SAC-CI) theoretical methods. All the dicarbonyl complexes have singlet ground electronic states with large singlet-triplet separations. Thermal dissociations of CO from the parent dicarbonyls are energetically unfavorable. CO thermal dissociation is an activation process for [Cl(2)Rh(CO)(2)](-) while it is a repulsive potential for CpM(CO)(2). The natures of the main excited states of CpM(CO)(2) and [Cl(2)Rh(CO)(2)](-) are found to be quite different. For [Cl(2)Rh(CO)(2)](-), all the strong transitions are identified to be metal to ligand CO charge transfer (MLCT) excitations. A significant feature of the excited states of CpM(CO)(2) is that both MLCT excitation and a ligand Cp to metal and CO charge transfer excitation are strongly mixed in the higher energy states with the latter having the largest oscillator strength. A competitive charge transfer excited state has therefore been identified theoretically for CpRh(CO)(2) and CpIr(CO)(2). The wavelength dependence of the quantum efficiencies for the photoreactions of CpM(CO)(2) reported by Lees et al. can be explained by the existence of two different types of excited states. The origin of the low quantum efficiencies for the C-H/S-H bond activations of CpM(CO)(2) can be attributed to the smaller proportion of the MLCT excitation in the higher energy states.

  6. Acceleration of a ground-state reaction by selective femtosecond-infrared-laser-pulse excitation

    NASA Astrophysics Data System (ADS)

    Stensitzki, Till; Yang, Yang; Kozich, Valeri; Ahmed, Ashour A.; Kössl, Florian; Kühn, Oliver; Heyne, Karsten

    2018-02-01

    Infrared (IR) excitation of vibrations that participate in the reaction coordinate of an otherwise thermally driven chemical reaction are believed to lead to its acceleration. Attempts at the practical realization of this concept have been hampered so far by competing processes leading to sample heating. Here we demonstrate, using femtosecond IR-pump IR-probe experiments, the acceleration of urethane and polyurethane formation due to vibrational excitation of the reactants for 1:1 mixtures of phenylisocyanate and cyclohexanol, and toluene-2,4-diisocyanate and 2,2,2-trichloroethane-1,1-diol, respectively. We measured reaction rate changes upon selective vibrational excitation with negligible heating of the sample and observed an increase of the reaction rate up to 24%. The observation is rationalized using reactant and transition-state structures obtained from quantum chemical calculations. We subsequently used IR-driven reaction acceleration to write a polyurethane square on sample windows using a femtosecond IR pulse.

  7. High-resolution Near-IR Spectral Mapping with H2 and [Fe II] Lines of Multiple Outflows around LkHα 234

    NASA Astrophysics Data System (ADS)

    Oh, Heeyoung; Pyo, Tae-Soo; Koo, Bon-Chul; Yuk, In-Soo; Kaplan, Kyle F.; Lee, Yong-Hyun; Sokal, Kimberly R.; Mace, Gregory N.; Park, Chan; Lee, Jae-Joon; Park, Byeong-Gon; Hwang, Narae; Kim, Hwihyun; Jaffe, Daniel T.

    2018-05-01

    We present a high-resolution, near-IR spectroscopic study of multiple outflows in the LkHα 234 star formation region using the Immersion GRating INfrared Spectrometer (IGRINS). Spectral mapping over the blueshifted emission of HH 167 allowed us to distinguish at least three separate, spatially overlapped outflows in H2 and [Fe II] emission. We show that the H2 emission represents not a single jet but rather complex multiple outflows driven by three known embedded sources: MM1, VLA 2, and VLA 3. There is a redshifted H2 outflow at a low velocity, V LSR <+50 km s‑1, with respect to the systemic velocity of V LSR = ‑11.5 km s‑1, that coincides with the H2O masers seen in earlier radio observations 2″ southwest of VLA 2. We found that the previously detected [Fe II] jet with | {V}LSR}| > 100 km s‑1 driven by VLA 3B is also detected in H2 emission and confirm that this jet has a position angle of about 240°. Spectra of the redshifted knots at 14″–65″ northeast of LkHα 234 are presented for the first time. These spectra also provide clues to the existence of multiple outflows. We detected high-velocity (50–120 km s‑1) H2 gas in the multiple outflows around LkHα 234. Since these gases move at speeds well over the dissociation velocity (>40 km s‑1), the emission must originate from the jet itself rather than H2 gas in the ambient medium. Also, position–velocity and excitation diagrams indicate that emission from knot C in HH 167 comes from two different phenomena, shocks and photodissociation.

  8. Amplified Photon Upconversion by Photonic Shell of Cholesteric Liquid Crystals.

    PubMed

    Kang, Ji-Hwan; Kim, Shin-Hyun; Fernandez-Nieves, Alberto; Reichmanis, Elsa

    2017-04-26

    As an effective platform to exploit triplet-triplet-annihilation-based photon upconversion (TTA-UC), microcapsules composed of a fluidic UC core and photonic shell are microfluidically prepared using a triple emulsion as the template. The photonic shell consists of cholesteric liquid crystals (CLCs) with a periodic helical structure, exhibiting a photonic band gap. Combined with planar anchoring at the boundaries, the shell serves as a resonance cavity for TTA-UC emission and enables spectral tuning of the UC under low-power-density excitation. The CLC shell can be stabilized by introducing a polymerizable mesogen in the LC host. Because of the microcapsule spherical symmetry, spontaneous emission of the delayed fluorescence is omnidirectionally amplified at the edge of the stop band. These results demonstrate the range of opportunities provided by TTA-UC systems for the future design of low-threshold photonic devices.

  9. Simple fibre based dispersion management for two-photon excited fluorescence imaging through an endoscope

    NASA Astrophysics Data System (ADS)

    Dimopoulos, Konstantinos; Marti, Dominik; Andersen, Peter E.

    2018-02-01

    We want to implement two-photon excitation fluorescence microscopy (TPEFM) into endoscopes, since TPEFM can provide relevant biomarkers for cancer staging and grading in hollow organs, endoscopically accessible through natural orifices. However, many obstacles must be overcome, among others the delivery of short laser pulses to the distal end of the endoscope. To this avail, we present imaging results using an all-fibre dispersion management scheme in a TPEFM setup. The scheme has been conceived by Jespersen et al. in 20101 and relies on the combination of a single mode fibre with normal and a higher order mode fibre with anomalous dispersion properties, fused in series using a long period grating. We show that using this fibre assembly, a simple and robust pulsed laser delivery system without any free-space optics, which is thus suitable for clinical use, can be realised.

  10. Dual photon effects in nitrogen dioxide photolysis

    NASA Technical Reports Server (NTRS)

    Hakala, D.; Harteck, P.; Reeves, R. R.

    1974-01-01

    A previous study demonstrated two-photon consecutive absorption as being the most probable mechanism for the photodissociation of NO2 using a pulsed ruby laser at 6943 A. Additional data discussed here confirmed this and also examined an associated phenomenon, that of multiphoton induced fluorescence. The dissociation of NO2 by ON-O bond cleavage requires 3.4 eV, while the laser energy corresponds to 1.785 eV. The pooling of the energy of two photons would give more than enough energy to dissociate the NO2 into NO + O. Several mechanisms including (1) simultaneous absorption of two photons; (2) reaction of two singly excited NO2; (3) reaction of a singly excited NO2 with a ground state NO2; and (4) consecutive absorption of two photons were examined.

  11. The dynamic Casimir effect within a vibrating metal photonic crystal

    NASA Astrophysics Data System (ADS)

    Ueta, Tsuyoshi

    2014-09-01

    The lattice-vibrating metal photonic crystal is exactly a system of dynamical Casimir effect connected in series, and so we can expect that a dynamical Casimir effect is enhanced by the photonic band effect. In the present study, when an electromagnetic field between metal plates is in the ground state in a one-dimensional metal photonic crystal, the radiation of electromagnetic wave in excited states has been investigated by artificially introducing lattice vibration to the photonic crystal. In this case as well as a dynamical Casimir effect, it has been shown that the harmonics of a ground state are generated just by vibrating a photonic crystal even without an incident wave. The dependencies of the radiating power on the number of layers and on the wavenumber of the lattice vibration are remarkable. It has been found that the radiation amplitude on lower excited states is not necessarily large and radiation on specific excited levels is large.

  12. All-near-infrared multiphoton microscopy interrogates intact tissues at deeper imaging depths than conventional single- and two-photon near-infrared excitation microscopes

    PubMed Central

    Sarder, Pinaki; Yazdanfar, Siavash; Akers, Walter J.; Tang, Rui; Sudlow, Gail P.; Egbulefu, Christopher

    2013-01-01

    Abstract. The era of molecular medicine has ushered in the development of microscopic methods that can report molecular processes in thick tissues with high spatial resolution. A commonality in deep-tissue microscopy is the use of near-infrared (NIR) lasers with single- or multiphoton excitations. However, the relationship between different NIR excitation microscopic techniques and the imaging depths in tissue has not been established. We compared such depth limits for three NIR excitation techniques: NIR single-photon confocal microscopy (NIR SPCM), NIR multiphoton excitation with visible detection (NIR/VIS MPM), and all-NIR multiphoton excitation with NIR detection (NIR/NIR MPM). Homologous cyanine dyes provided the fluorescence. Intact kidneys were harvested after administration of kidney-clearing cyanine dyes in mice. NIR SPCM and NIR/VIS MPM achieved similar maximum imaging depth of ∼100  μm. The NIR/NIR MPM enabled greater than fivefold imaging depth (>500  μm) using the harvested kidneys. Although the NIR/NIR MPM used 1550-nm excitation where water absorption is relatively high, cell viability and histology studies demonstrate that the laser did not induce photothermal damage at the low laser powers used for the kidney imaging. This study provides guidance on the imaging depth capabilities of NIR excitation-based microscopic techniques and reveals the potential to multiplex information using these platforms. PMID:24150231

  13. Spectral and energy characteristics of four-photon parametric scattering in sodium vapor

    NASA Astrophysics Data System (ADS)

    Vaicaitis, V.; Ignatavicius, M.; Kudriashov, V. A.; Pimenov, Iu. N.; Jakyte, R.

    1987-04-01

    Consideration is given to processes of four-photon interaction upon two-photon resonance excitation of the 3d level of sodium by two-frequency radiation from a monopulse picosecond YAG:Nd laser with frequency doubling and an optical parametric oscillator utilizing KDP crystrals. The spatial and frequency spectra of the four-photon parametric scattering (FPS) are recorded and studied at different sodium vapor concentrations (10 to the 15th to 10 to the 17th/cu cm) and upon both collinear and noncollinear excitation. It is shown that the observed conical structure of the FPS radiation can be interpreted from an analysis of the realization of the frequency and spatial phase-matching conditions. The dependences of the FPS radiation intensity on the exciting radiation intensity, the sodium vapor concentration, and the mismatching of the exciting radiation from the two-photon resonance are obtained.

  14. On-chip photonic system using suspended p-n junction InGaN/GaN multiple quantum wells device and multiple waveguides

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

    Wang, Yongjin, E-mail: wangyj@njupt.edu.cn; Zhu, Guixia; Gao, Xumin

    We propose, fabricate, and characterize the on-chip integration of suspended p-n junction InGaN/GaN multiple quantum wells (MQWs) device and multiple waveguides on the same GaN-on-silicon platform. The integrated devices are fabricated via a wafer-level process and exhibit selectable functionalities for diverse applications. As the suspended p-n junction InGaN/GaN MQWs device operates under a light emitting diode (LED) mode, part of the light emission is confined and guided by the suspended waveguides. The in-plane propagation along the suspended waveguides is measured by a micro-transmittance setup. The on-chip data transmission is demonstrated for the proof-of-concept photonic integration. As the suspended p-n junctionmore » InGaN/GaN MQWs device operates under photodiode mode, the light is illuminated on the suspended waveguides with the aid of the micro-transmittance setup and, thus, coupled into the suspended waveguides. The guided light is finally sensed by the photodiode, and the induced photocurrent trace shows a distinct on/off switching performance. These experimental results indicate that the on-chip photonic integration is promising for the development of sophisticated integrated photonic circuits in the visible wavelength region.« less

  15. Software-defined networking control plane for seamless integration of multiple silicon photonic switches in Datacom networks.

    PubMed

    Shen, Yiwen; Hattink, Maarten H N; Samadi, Payman; Cheng, Qixiang; Hu, Ziyiz; Gazman, Alexander; Bergman, Keren

    2018-04-16

    Silicon photonics based switches offer an effective option for the delivery of dynamic bandwidth for future large-scale Datacom systems while maintaining scalable energy efficiency. The integration of a silicon photonics-based optical switching fabric within electronic Datacom architectures requires novel network topologies and arbitration strategies to effectively manage the active elements in the network. We present a scalable software-defined networking control plane to integrate silicon photonic based switches with conventional Ethernet or InfiniBand networks. Our software-defined control plane manages both electronic packet switches and multiple silicon photonic switches for simultaneous packet and circuit switching. We built an experimental Dragonfly network testbed with 16 electronic packet switches and 2 silicon photonic switches to evaluate our control plane. Observed latencies occupied by each step of the switching procedure demonstrate a total of 344 µs control plane latency for data-center and high performance computing platforms.

  16. Stepwise photochromism of bisnaphthopyrans exhibiting an excitation intensity-dependent color change.

    PubMed

    Inagaki, Yuki; Mutoh, Katsuya; Abe, Jiro

    2018-06-07

    Non-linear photoresponses against excitation light intensity are important for the development of attractive photofunctional materials exhibiting high spatial selective photoswitching that is not affected by weak background light. Biphotochromic systems composed of two fast photochromic units have the potential to show a stepwise two-photon absorption process in which the optical properties can be non-linearly controlled by changing the excitation light conditions. Herein, we designed and synthesized novel bisnaphthopyran derivatives containing fast photoswitchable naphthopyran units. The bisnaphthopyran derivatives show a stepwise two-photon-induced photochromic reaction upon UV light irradiation accompanied by a drastic color change due to a large change in the molecular structure between the one-photon product and the two-photon product. Consequently, the color of the bisnaphthopyran derivatives can be non-linearly controlled by changing the excitation intensity. This characteristic photochromic property of the biphotochromic system provides important insight into advanced photoresponsive materials.

  17. Nanostructured Surfaces and Detection Instrumentation for Photonic Crystal Enhanced Fluorescence

    PubMed Central

    Chaudhery, Vikram; George, Sherine; Lu, Meng; Pokhriyal, Anusha; Cunningham, Brian T.

    2013-01-01

    Photonic crystal (PC) surfaces have been demonstrated as a compelling platform for improving the sensitivity of surface-based fluorescent assays used in disease diagnostics and life science research. PCs can be engineered to support optical resonances at specific wavelengths at which strong electromagnetic fields are utilized to enhance the intensity of surface-bound fluorophore excitation. Meanwhile, the leaky resonant modes of PCs can be used to direct emitted photons within a narrow range of angles for more efficient collection by a fluorescence detection system. The multiplicative effects of enhanced excitation combined with enhanced photon extraction combine to provide improved signal-to-noise ratios for detection of fluorescent emitters, which in turn can be used to reduce the limits of detection of low concentration analytes, such as disease biomarker proteins. Fabrication of PCs using inexpensive manufacturing methods and materials that include replica molding on plastic, nano-imprint lithography on quartz substrates result in devices that are practical for single-use disposable applications. In this review, we will describe the motivation for implementing high-sensitivity fluorescence detection in the context of molecular diagnosis and gene expression analysis though the use of PC surfaces. Recent efforts to improve the design and fabrication of PCs and their associated detection instrumentation are summarized, including the use of PCs coupled with Fabry-Perot cavities and external cavity lasers. PMID:23624689

  18. Harmonic Quantum Coherence of Multiple Excitons in PbS/CdS Core-Shell Nanocrystals

    NASA Astrophysics Data System (ADS)

    Tahara, Hirokazu; Sakamoto, Masanori; Teranishi, Toshiharu; Kanemitsu, Yoshihiko

    2017-12-01

    The generation and recombination dynamics of multiple excitons in nanocrystals (NCs) have attracted much attention from the viewpoints of fundamental physics and device applications. However, the quantum coherence of multiple exciton states in NCs still remains unclear due to a lack of experimental support. Here, we report the first observation of harmonic dipole oscillations in PbS/CdS core-shell NCs using a phase-locked interference detection method for transient absorption. From the ultrafast coherent dynamics and excitation-photon-fluence dependence of the oscillations, we found that multiple excitons cause the harmonic dipole oscillations with ω , 2 ω , and 3 ω oscillations, even though the excitation pulse energy is set to the exciton resonance frequency, ω . This observation is closely related to the quantum coherence of multiple exciton states in NCs, providing important insights into multiple exciton generation mechanisms.

  19. Kerr-gated picosecond Raman spectroscopy and Raman photon migration of equine bone tissue with 400-nm excitation

    NASA Astrophysics Data System (ADS)

    Morris, Michael D.; Goodship, Allen E.; Draper, Edward R. C.; Matousek, Pavel; Towrie, Michael; Parker, Anthony W.

    2004-07-01

    We show that Raman spectroscopy with visible lasers, even in the deep blue is possible with time-gated Raman spectroscopy. A 4 picosec time gate allows efficient fluorescence rejection, up to 1000X, and provides almost background-free Raman spectra with low incident laser power. The technology enables spectroscopy with better than 10X higher scattering efficiency than is possible with the NIR (785 nm and 830 nm) lasers that are conventionally used. Raman photon migration is shown to allow depth penetration. We show for the first time that Kerr-gated Raman spectra of bone tissue with blue laser excitation enables both fluorescence rejection and depth penetration.

  20. Atmospheric Trace Gas Abundances and Stable Isotope Ratios via IR-LIF

    NASA Technical Reports Server (NTRS)

    Blake, Geoffrey A.

    2004-01-01

    We propose to develop new technologies with support provided by PIDDP that will enable the in situ measurements of abundances and stable isotope ratios in important radiatively and biogenically active gases such as carbon dioxide, carbon monoxide, water, methane, nitrous oxide, and hydrogen sulfide to very high precision (0.1 per mil or better for the isotopic ratios, for example). Such measurements, impossible at present, could provide pivotal new constraints on the global (bio)geochemical budgets of these critical species, and could also be used to examine the dynamics of atmospheric transport on Mars, Titan, and other solar system bodies. We believe the combination of solid state light sources with imaging of the IR laser induced fluorescence (IR-LIF) via newly available detector arrays will make such in situ measurements possible for the first time. Even under ambient terrestrial conditions, the LIF yield from vibrational excitation of species such as water and carbon dioxide should produce emission measures well in excess of ten billion photons/sec from samples volumes of order 1 c.c. These count rates can, in principle, yield detection limits into the sub-ppt range that are required for the in situ isotopic study of atmospheric trace gases. While promising, such technologies are relatively immature, but developing rapidly, and there are a great many uncertainties regarding their applicability to in situ IR-LIF planetary studies. We therefore feel PIDDP support will be critical to developing these new tools, and propose a three-year program to combine microchip near-IR lasers with low background detection axes and state-of-the-art HgCdTe detectors developed for astronomical spectroscopy to investigate the sensitivity of IR-LIF under realistic planetary conditions, to optimize the optical pumping and filtering schemes for important species, and to apply the spectrometer to the non-destructive measurement of stable isotopes in a variety of test samples. These

  1. Closing a Venus Flytrap with electrical and mid-IR photon stimulations

    NASA Astrophysics Data System (ADS)

    Eisen, David; Janssen, Douglas; Chen, Xing; Choa, Fow-Sen; Kostov, Dan; Fan, Jenyu

    2013-03-01

    Plants have mechanisms to perceive and transmit information between its organs and tissues. These signals had long been considered as hormonal or hydraulic in nature, but recent studies have shown that electrical signals are also produced causing physiological responses. In this work we show that Venus Flytrap, Dionaea muscipula, can respond to both electrical and optical signals beside mechanical stimulations. While the Venus Flytrap does not have any neurons, it does contain transport cells with very similar characteristics to neurotransmitters and uses ionic mechanisms, as human neurons do, to generate action potentials. In our electrical stimulation study, electrodes made out of soft cloth were soaked in salt water before being placed to the midrib (+) and lobe (-). The flytrap's surface resistance was determined by subtracting out the average electrode resistance from the measured electrode to plant surface resistance, yielding an average contact resistance of around 0.98MΩ. A logarithmic amplifier was used to monitor mechanically generated electrical signals. Two electrical pulses were generated by mechanically touching the trigger hairs in the lobe twice within 20 seconds. By discharging around 600μC charge stored in a capacitor we demonstrated electrically closing of the flytrap. For optical excitation we found in our FTIR study it's tissue contains very similar protein absorption peaks to that of insects. A 7.35μm laser with 50mw power was then used for the stimulation study. Electrical action potential was generated twice by mid-infrared photons before closure of the flytrap.

  2. Entangled, guided photon generation in (1+1)-dimensional photonic crystals

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

    Sciscione, L.; Centini, M.; Sibilia, C.

    A scheme based on photonic crystal technology is proposed as an ultrabright source of entangled photons on a miniaturized scale. The geometry consists of a multilayer microcavity, excited by a resonant pump frequency, such that the emitted photons are guided transversally to the direction of the incident pump. The entanglement occurs in direction, frequency, and polarization, and the bandwidth of the emitted photons is of the order of 1 nm. We propose a feasible design based on Al{sub 0.3}Ga{sub 0.7}As/Al{sub 2}O{sub 3} structures and predict an emission rate 10{sup 5} pairs per second with 100 mW pump power. These resultsmore » are promising for realization of chip and future quantum computer applications.« less

  3. Software-defined networking control plane for seamless integration of multiple silicon photonic switches in Datacom networks

    DOE PAGES

    Shen, Yiwen; Hattink, Maarten; Samadi, Payman; ...

    2018-04-13

    Silicon photonics based switches offer an effective option for the delivery of dynamic bandwidth for future large-scale Datacom systems while maintaining scalable energy efficiency. The integration of a silicon photonics-based optical switching fabric within electronic Datacom architectures requires novel network topologies and arbitration strategies to effectively manage the active elements in the network. Here, we present a scalable software-defined networking control plane to integrate silicon photonic based switches with conventional Ethernet or InfiniBand networks. Our software-defined control plane manages both electronic packet switches and multiple silicon photonic switches for simultaneous packet and circuit switching. We built an experimental Dragonfly networkmore » testbed with 16 electronic packet switches and 2 silicon photonic switches to evaluate our control plane. Observed latencies occupied by each step of the switching procedure demonstrate a total of 344 microsecond control plane latency for data-center and high performance computing platforms.« less

  4. Software-defined networking control plane for seamless integration of multiple silicon photonic switches in Datacom networks

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

    Shen, Yiwen; Hattink, Maarten; Samadi, Payman

    Silicon photonics based switches offer an effective option for the delivery of dynamic bandwidth for future large-scale Datacom systems while maintaining scalable energy efficiency. The integration of a silicon photonics-based optical switching fabric within electronic Datacom architectures requires novel network topologies and arbitration strategies to effectively manage the active elements in the network. Here, we present a scalable software-defined networking control plane to integrate silicon photonic based switches with conventional Ethernet or InfiniBand networks. Our software-defined control plane manages both electronic packet switches and multiple silicon photonic switches for simultaneous packet and circuit switching. We built an experimental Dragonfly networkmore » testbed with 16 electronic packet switches and 2 silicon photonic switches to evaluate our control plane. Observed latencies occupied by each step of the switching procedure demonstrate a total of 344 microsecond control plane latency for data-center and high performance computing platforms.« less

  5. Results from the Air Force Geophysics Laboratory survey catalog. [IR astronomy

    NASA Technical Reports Server (NTRS)

    Price, S. D.; Walker, R. G.

    1977-01-01

    Results of an IR survey program designed to obtain the spatial and brightness distributions of a representative sample of IR-emitting objects in the 3-30 micron range are analyzed. Small cryogenically cooled telescopes carried above the atmosphere on sounding rockets were employed in the research. Minimization of sky noise and photon background, experimental equipment, and data reduction techniques are discussed.

  6. Antimicrobial Amino-Functionalized Nitrogen-Doped Graphene Quantum Dots for Eliminating Multidrug-Resistant Species in Dual-Modality Photodynamic Therapy and Bioimaging under Two-Photon Excitation.

    PubMed

    Kuo, Wen-Shuo; Shao, Yu-Ting; Huang, Keng-Shiang; Chou, Ting-Mao; Yang, Chih-Hui

    2018-05-02

    Developing a nanomaterial, for use in highly efficient dual-modality two-photon photodynamic therapy (PDT) involving reactive oxygen species (ROS) generation and for use as a two-photon imaging contrast probe, is currently desirable. Here, graphene quantum dots (GQDs) doped with nitrogen and functionalized with an amino group (amino-N-GQDs) serving as a photosensitizer in PDT had the superior ability to generate ROS as compared to unmodified GQDs. Multidrug-resistant (MDR) species were completely eliminated at an ultralow energy (239.36 nJ pixel -1 ) through only 12 s two-photon excitation (TPE) in the near-infrared region (800 nm). Furthermore, the amino-N-GQDs had an absorption wavelength of approximately 800 nm, quantum yield of 0.33, strong luminescence, an absolute cross section of approximately 54 356 Göeppert-Mayer units, a lifetime of 1.09 ns, a ratio of the radiative to nonradiative decay rates of approximately 0.49, and high two-photon stability under TPE. These favorable properties enabled the amino-N-GQDs to act as a two-photon contrast probe for tracking and localizing analytes through in-depth two-photon imaging in a three-dimensional biological environment and concurrently easily eliminating MDR species through PDT.

  7. White light for the fast lane: supercontinuum generation in all-normal dispersion fibers for ultrafast photonics

    NASA Astrophysics Data System (ADS)

    Heidt, Alexander M.

    2014-03-01

    This talk will give an overview of the unique properties of supercontinuum generation (SCG) in all-normal dispersion (ANDi) fibers pumped by ultrashort pulses and the possibilities they offer for ultrafast photonics applications. In contrast to their anomalously pumped counterparts, the SCG process in ANDi fibers conserves a single ultrashort pulse in the time domain, completely suppresses soliton formation and decay, and avoids noise-amplifying nonlinear dynamics. The resulting spectra combine the best of both worlds - the broad, more than octave-spanning bandwidths usually associated with anomalous dispersion pumping with the high temporal coherence, pulse-to-pulse stability and well-defined temporal pulse characteristics known from the normal dispersion regime. These characteristics are ideally suited for ultrafast photonics, and I will present application examples including the generation of high quality single-cycle pulses and their amplification, as well as ultrafast spectroscopy. This talk will also explore the exciting new possibilities enabled by extending this approach into the mid-IR spectral region using novel soft glass fiber designs.

  8. Localized excitations in hydrogen-bonded molecular crystals

    NASA Astrophysics Data System (ADS)

    Alexander, D. M.; Krumhansl, J. A.

    1986-05-01

    Localized excitations analogous to the small Holstein polaron, to localized modes in alkali halides, and to localized excitonic states, are postulated for a set of internal vibrational modes in crystalline acetanilide. The theoretical framework in which one can describe the characteristics of the ir and Raman spectroscopy peaks associated with these localized states is adequately provided by the Davydov model (formally equivalent to the Holstein polaron model). The possible low-lying excitations arising from this model are determined using a variational approach. Hence, the contribution to the spectral function due to each type of excitation can be calculated. The internal modes of chief concern here are the amide-I (CO stretch) and the N-H stretch modes for which we demonstrate consistency of the theoretical model with the available ir data. Past theoretical approaches will be discussed and reasons why one should prefer one description over another will be examined.

  9. On-chip single photon filtering and multiplexing in hybrid quantum photonic circuits.

    PubMed

    Elshaari, Ali W; Zadeh, Iman Esmaeil; Fognini, Andreas; Reimer, Michael E; Dalacu, Dan; Poole, Philip J; Zwiller, Val; Jöns, Klaus D

    2017-08-30

    Quantum light plays a pivotal role in modern science and future photonic applications. Since the advent of integrated quantum nanophotonics different material platforms based on III-V nanostructures-, colour centers-, and nonlinear waveguides as on-chip light sources have been investigated. Each platform has unique advantages and limitations; however, all implementations face major challenges with filtering of individual quantum states, scalable integration, deterministic multiplexing of selected quantum emitters, and on-chip excitation suppression. Here we overcome all of these challenges with a hybrid and scalable approach, where single III-V quantum emitters are positioned and deterministically integrated in a complementary metal-oxide-semiconductor-compatible photonic circuit. We demonstrate reconfigurable on-chip single-photon filtering and wavelength division multiplexing with a foot print one million times smaller than similar table-top approaches, while offering excitation suppression of more than 95 dB and efficient routing of single photons over a bandwidth of 40 nm. Our work marks an important step to harvest quantum optical technologies' full potential.Combining different integration platforms on the same chip is currently one of the main challenges for quantum technologies. Here, Elshaari et al. show III-V Quantum Dots embedded in nanowires operating in a CMOS compatible circuit, with controlled on-chip filtering and tunable routing.

  10. Detecting infrared luminescence and non-chemical signaling of living cells: single cell mid-IR spectroscopy in cryogenic environments

    NASA Astrophysics Data System (ADS)

    Pereverzev, Sergey

    2017-02-01

    Many life-relevant interaction energies are in IR range, and it is reasonable to believe that some biochemical reactions inside cells can results in emission of IR photons. Cells can use this emission for non-chemical and non-electrical signaling. Detecting weak infrared radiation from live cells is complicated because of strong thermal radiation background and absorption of radiation by tissues. A microfluidic device with live cells inside a vacuum cryogenic environment should suppress this background, and thereby permit observation of live cell auto-luminescence or signaling in the IR regime. One can make IR-transparent windows not emitting in this range, so only the cell and a small amount of liquid around it will emit infrared radiation. Currently mid-IR spectroscopy of single cells requires the use of a synchrotron source to measure absorption or reflection spectra. Decreasing of thermal radiation background will allow absorption and reflection spectroscopy of cells without using synchrotron light. Moreover, cell auto-luminescence can be directly measured. The complete absence of thermal background radiation for cryogenically cooled samples allows the use IR photon-sensitive detectors and obtaining single molecule sensitivity in IR photo-luminescence measurements. Due to low photon energies, photo-luminescence measurements will be non-distractive for pressures samples. The technique described here is based upon US patent 9366574.

  11. Hong-Ou-Mandel Interference between Two Deterministic Collective Excitations in an Atomic Ensemble

    NASA Astrophysics Data System (ADS)

    Li, Jun; Zhou, Ming-Ti; Jing, Bo; Wang, Xu-Jie; Yang, Sheng-Jun; Jiang, Xiao; Mølmer, Klaus; Bao, Xiao-Hui; Pan, Jian-Wei

    2016-10-01

    We demonstrate deterministic generation of two distinct collective excitations in one atomic ensemble, and we realize the Hong-Ou-Mandel interference between them. Using Rydberg blockade we create single collective excitations in two different Zeeman levels, and we use stimulated Raman transitions to perform a beam-splitter operation between the excited atomic modes. By converting the atomic excitations into photons, the two-excitation interference is measured by photon coincidence detection with a visibility of 0.89(6). The Hong-Ou-Mandel interference witnesses an entangled NOON state of the collective atomic excitations, and we demonstrate its two times enhanced sensitivity to a magnetic field compared with a single excitation. Our work implements a minimal instance of boson sampling and paves the way for further multimode and multiexcitation studies with collective excitations of atomic ensembles.

  12. Multiple hydrogen bonding in excited states of aminopyrazine in methanol solution: time-dependent density functional theory study.

    PubMed

    Chai, Shuo; Yu, Jie; Han, Yong-Chang; Cong, Shu-Lin

    2013-11-01

    Aminopyrazine (AP) and AP-methanol complexes have been theoretically studied by using density functional theory (DFT) and time-dependent density functional theory (TDDFT). The excited-state hydrogen bonds are discussed in detail. In the ground state the intermolecular multiple hydrogen bonds can be formed between AP molecule and protic solvents. The AP monomer and hydrogen-bonded complex of AP with one methanol are photoexcited initially to the S2 state, and then transferred to the S1 state via internal conversion. However the complex of AP with two methanol molecules is directly excited to the S1 state. From the calculated electronic excited energies and simulated absorption spectra, we find that the intermolecular hydrogen bonds are strengthened in the electronic excited states. The strengthening is confirmed by the optimized excited-state geometries. The photochemical processes in the electronic excited states are significantly influenced by the excited-state hydrogen bond strengthening. Copyright © 2013 Elsevier B.V. All rights reserved.

  13. Nonadiabatic excited-state molecular dynamics: modeling photophysics in organic conjugated materials.

    PubMed

    Nelson, Tammie; Fernandez-Alberti, Sebastian; Roitberg, Adrian E; Tretiak, Sergei

    2014-04-15

    To design functional photoactive materials for a variety of technological applications, researchers need to understand their electronic properties in detail and have ways to control their photoinduced pathways. When excited by photons of light, organic conjugated materials (OCMs) show dynamics that are often characterized by large nonadiabatic (NA) couplings between multiple excited states through a breakdown of the Born-Oppenheimer (BO) approximation. Following photoexcitation, various nonradiative intraband relaxation pathways can lead to a number of complex processes. Therefore, computational simulation of nonadiabatic molecular dynamics is an indispensable tool for understanding complex photoinduced processes such as internal conversion, energy transfer, charge separation, and spatial localization of excitons. Over the years, we have developed a nonadiabatic excited-state molecular dynamics (NA-ESMD) framework that efficiently and accurately describes photoinduced phenomena in extended conjugated molecular systems. We use the fewest-switches surface hopping (FSSH) algorithm to treat quantum transitions among multiple adiabatic excited state potential energy surfaces (PESs). Extended molecular systems often contain hundreds of atoms and involve large densities of excited states that participate in the photoinduced dynamics. We can achieve an accurate description of the multiple excited states using the configuration interaction single (CIS) formalism with a semiempirical model Hamiltonian. Analytical techniques allow the trajectory to be propagated "on the fly" using the complete set of NA coupling terms and remove computational bottlenecks in the evaluation of excited-state gradients and NA couplings. Furthermore, the use of state-specific gradients for propagation of nuclei on the native excited-state PES eliminates the need for simplifications such as the classical path approximation (CPA), which only uses ground-state gradients. Thus, the NA-ESMD methodology

  14. Smart Phase Tuning in Microwave Photonic Integrated Circuits Toward Automated Frequency Multiplication by Design

    NASA Astrophysics Data System (ADS)

    Nabavi, N.

    2018-07-01

    The author investigates the monitoring methods for fine adjustment of the previously proposed on-chip architecture for frequency multiplication and translation of harmonics by design. Digital signal processing (DSP) algorithms are utilized to create an optimized microwave photonic integrated circuit functionality toward automated frequency multiplication. The implemented DSP algorithms are formed on discrete Fourier transform and optimization-based algorithms (Greedy and gradient-based algorithms), which are analytically derived and numerically compared based on the accuracy and speed of convergence criteria.

  15. Distribution of geometric quantum discord in photon-added coherent states

    NASA Astrophysics Data System (ADS)

    Daoud, M.; Kaydi, W.; El Hadfi, H.

    2015-12-01

    In this paper, we examine the influence of photon excitation on the monogamy property of quantum discord in tripartite coherent states of Greenberger-Horne-Zeilinger (GHZ) type. The Hilbert-Schmidt norm is used as quantifier of pairwise quantum correlations. The geometric quantum discord in all bipartite subsystems are explicitly given. We show that the geometric discord is monogamous for any photon excitation order.

  16. Integrated ultrasonic particle positioning and low excitation light fluorescence imaging

    NASA Astrophysics Data System (ADS)

    Bernassau, A. L.; Al-Rawhani, M.; Beeley, J.; Cumming, D. R. S.

    2013-12-01

    A compact hybrid system has been developed to position and detect fluorescent micro-particles by combining a Single Photon Avalanche Diode (SPAD) imager with an acoustic manipulator. The detector comprises a SPAD array, light-emitting diode (LED), lenses, and optical filters. The acoustic device is formed of multiple transducers surrounding an octagonal cavity. By stimulating pairs of transducers simultaneously, an acoustic landscape is created causing fluorescent micro-particles to agglomerate into lines. The fluorescent pattern is excited by a low power LED and detected by the SPAD imager. Our technique combines particle manipulation and visualization in a compact, low power, portable setup.

  17. Differentiation of closely related isomers: application of data mining techniques in conjunction with variable wavelength infrared multiple photon dissociation mass spectrometry for identification of glucose-containing disaccharide ions.

    PubMed

    Stefan, Sarah E; Ehsan, Mohammad; Pearson, Wright L; Aksenov, Alexander; Boginski, Vladimir; Bendiak, Brad; Eyler, John R

    2011-11-15

    Data mining algorithms have been used to analyze the infrared multiple photon dissociation (IRMPD) patterns of gas-phase lithiated disaccharide isomers irradiated with either a line-tunable CO(2) laser or a free electron laser (FEL). The IR fragmentation patterns over the wavelength range of 9.2-10.6 μm have been shown in earlier work to correlate uniquely with the asymmetry at the anomeric carbon in each disaccharide. Application of data mining approaches for data analysis allowed unambiguous determination of the anomeric carbon configurations for each disaccharide isomer pair using fragmentation data at a single wavelength. In addition, the linkage positions were easily assigned. This combination of wavelength-selective IRMPD and data mining offers a powerful and convenient tool for differentiation of structurally closely related isomers, including those of gas-phase carbohydrate complexes.

  18. On-demand generation of background-free single photons from a solid-state source

    NASA Astrophysics Data System (ADS)

    Schweickert, Lucas; Jöns, Klaus D.; Zeuner, Katharina D.; Covre da Silva, Saimon Filipe; Huang, Huiying; Lettner, Thomas; Reindl, Marcus; Zichi, Julien; Trotta, Rinaldo; Rastelli, Armando; Zwiller, Val

    2018-02-01

    True on-demand high-repetition-rate single-photon sources are highly sought after for quantum information processing applications. However, any coherently driven two-level quantum system suffers from a finite re-excitation probability under pulsed excitation, causing undesirable multi-photon emission. Here, we present a solid-state source of on-demand single photons yielding a raw second-order coherence of g(2 )(0 )=(7.5 ±1.6 )×10-5 without any background subtraction or data processing. To this date, this is the lowest value of g(2 )(0 ) reported for any single-photon source even compared to the previously reported best background subtracted values. We achieve this result on GaAs/AlGaAs quantum dots embedded in a low-Q planar cavity by employing (i) a two-photon excitation process and (ii) a filtering and detection setup featuring two superconducting single-photon detectors with ultralow dark-count rates of (0.0056 ±0.0007 ) s-1 and (0.017 ±0.001 ) s-1, respectively. Re-excitation processes are dramatically suppressed by (i), while (ii) removes false coincidences resulting in a negligibly low noise floor.

  19. Bright long-lived luminescence of silicon nanocrystals sensitized by two-photon absorbing antenna

    PubMed Central

    Ravotto, Luca; Chen, Qi; Ma, Yuguo; Vinogradov, Sergei A.; Locritani, Mirko; Bergamini, Giacomo; Negri, Fabrizia; Yu, Yixuan; Korgel, Brian A.; Ceroni, Paola

    2017-01-01

    Summary Silicon nanocrystals of the average diameter of 5 nm, functionalized with 4,7-di(2-thienyl)-2,1,3-benzothiadiazole chromophores (TBT) and dodecyl chains, exhibit near-infrared emission upon one-photon (1P) excitation at 515 nm and two-photon (2P) excitation at 960 nm. By using TBT chromophores as an antenna we were able to enhance both 1P and 2P absorption cross-sections of the silicon nanocrystals to more efficiently excite their long-lived luminescence. These results chart a path to two-photon-excitable imaging probes with long-lived oxygen-independent luminescence - a rare combination of properties that should allow for a substantial increase in imaging contrast. PMID:28966989

  20. Optical Emission Studies of Copper Plasma Induced Using Infrared Transversely Excited Atmospheric (IR TEA) Carbon Dioxide Laser Pulses.

    PubMed

    Momcilovic, Milos; Kuzmanovic, Miroslav; Rankovic, Dragan; Ciganovic, Jovan; Stoiljkovic, Milovan; Savovic, Jelena; Trtica, Milan

    2015-04-01

    Spatially resolved, time-integrated optical emission spectroscopy was applied for investigation of copper plasma produced by a nanosecond infrared (IR) transversely excited atmospheric (TEA) CO2 laser, operating at 10.6 μm. The effect of surrounding air pressure, in the pressure range 0.1 to 1013 mbar, on plasma formation and its characteristics was investigated. A linear dependence of intensity threshold for plasma formation on logarithm of air pressure was found. Lowering of the air pressure reduces the extent of gas breakdown, enabling better laser-target coupling and thus increases ablation. Optimum air pressure for target plasma formation was 0.1 mbar. Under that pressure, the induced plasma consisted of two clearly distinguished and spatially separated regions. The maximum intensity of emission, with sharp and well-resolved spectral lines and negligibly low background emission, was obtained from a plasma zone 8 mm from the target surface. The estimated excitation temperature in this zone was around 7000 K. The favorable signal to background ratio obtained in this plasma region indicates possible analytical application of TEA CO2 laser produced copper plasma. Detection limits of trace elements present in the Cu sample were on the order of 10 ppm (parts per million). Time-resolved measurements of spatially selected plasma zones were used to find a correlation between the observed spatial position and time delay.

  1. Electron Dynamics in the Core-Excited CS2 Molecule Revealed through Resonant Inelastic X-Ray Scattering Spectroscopy

    NASA Astrophysics Data System (ADS)

    Marchenko, T.; Carniato, S.; Journel, L.; Guillemin, R.; Kawerk, E.; Žitnik, M.; Kavčič, M.; Bučar, K.; Bohinc, R.; Petric, M.; Vaz da Cruz, V.; Gel'mukhanov, F.; Simon, M.

    2015-07-01

    We present an experimental and theoretical study of resonant inelastic x-ray scattering (RIXS) in the carbon disulphide CS2 molecule near the sulfur K-absorption edge. We observe a strong evolution of the RIXS spectral profile with the excitation energy tuned below the lowest unoccupied molecular orbital (LUMO) absorption resonance. The reason for this is twofold. Reducing the photon energy in the vicinity of the LUMO absorption resonance leads to a relative suppression of the LUMO contribution with respect to the emission signal from the higher unoccupied molecular orbitals, which results in the modulation of the total RIXS profile. At even larger negative photon-energy detuning from the resonance, the excitation-energy dependence of the RIXS profile is dominated by the onset of electron dynamics triggered by a coherent excitation of multiple electronic states. Furthermore, our study demonstrates that in the hard x-ray regime, localization of the S 1s core hole occurs in CS2 during the RIXS process because of the orientational dephasing of interference between the waves scattering on the two sulfur atoms. Core-hole localization leads to violation of the symmetry selection rules for the electron transitions observed in the spectra.

  2. Optical behaviors of flexible photonic films via the developed multiple UV-exposed fabrications.

    PubMed

    Chien, Chih-Chieh; Liu, Jui-Hsiang

    2014-07-01

    Recently, extensive investigations are carried out on design of highly controlled architecture and morphology by polymerizing the monomers doped in well-defined liquid crystalline materials, followed by removal of the template liquid crystal molecules. In this communication, a photonic structure used as a new photonic bandgap (PBG) material is developed by imprinting helical structures on polymer matrices through multiple photocrosslinking processes in an induced chiral nematic mesophase using flexible polyethylene terephthalate (PET) films as substrates. The tuning properties of the reflection band of the imprinted cell are achieved using an uniaxial thermo-stretching equipment. Furthermore, refilling of isotropic materials into the imprinted cells tune the reflection light wavelength leads to the change of color. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  3. Polarized two-photon photoselection in EGFP: Theory and experiment

    NASA Astrophysics Data System (ADS)

    Masters, T. A.; Marsh, R. J.; Blacker, T. S.; Armoogum, D. A.; Larijani, B.; Bain, A. J.

    2018-04-01

    In this work, we present a complete theoretical description of the excited state order created by two-photon photoselection from an isotropic ground state; this encompasses both the conventionally measured quadrupolar (K = 2) and the "hidden" degree of hexadecapolar (K = 4) transition dipole alignment, their dependence on the two-photon transition tensor and emission transition dipole moment orientation. Linearly and circularly polarized two-photon absorption (TPA) and time-resolved single- and two-photon fluorescence anisotropy measurements are used to determine the structure of the transition tensor in the deprotonated form of enhanced green fluorescent protein. For excitation wavelengths between 800 nm and 900 nm, TPA is best described by a single element, almost completely diagonal, two-dimensional (planar) transition tensor whose principal axis is collinear to that of the single-photon S0 → S1 transition moment. These observations are in accordance with assignments of the near-infrared two-photon absorption band in fluorescent proteins to a vibronically enhanced S0 → S1 transition.

  4. Polarized two-photon photoselection in EGFP: Theory and experiment.

    PubMed

    Masters, T A; Marsh, R J; Blacker, T S; Armoogum, D A; Larijani, B; Bain, A J

    2018-04-07

    In this work, we present a complete theoretical description of the excited state order created by two-photon photoselection from an isotropic ground state; this encompasses both the conventionally measured quadrupolar (K = 2) and the "hidden" degree of hexadecapolar (K = 4) transition dipole alignment, their dependence on the two-photon transition tensor and emission transition dipole moment orientation. Linearly and circularly polarized two-photon absorption (TPA) and time-resolved single- and two-photon fluorescence anisotropy measurements are used to determine the structure of the transition tensor in the deprotonated form of enhanced green fluorescent protein. For excitation wavelengths between 800 nm and 900 nm, TPA is best described by a single element, almost completely diagonal, two-dimensional (planar) transition tensor whose principal axis is collinear to that of the single-photon S 0 → S 1 transition moment. These observations are in accordance with assignments of the near-infrared two-photon absorption band in fluorescent proteins to a vibronically enhanced S 0 → S 1 transition.

  5. Applications of two-photon fluorescence microscopy in deep-tissue imaging

    NASA Astrophysics Data System (ADS)

    Dong, Chen-Yuan; Yu, Betty; Hsu, Lily L.; Kaplan, Peter D.; Blankschstein, D.; Langer, Robert; So, Peter T. C.

    2000-07-01

    Based on the non-linear excitation of fluorescence molecules, two-photon fluorescence microscopy has become a significant new tool for biological imaging. The point-like excitation characteristic of this technique enhances image quality by the virtual elimination of off-focal fluorescence. Furthermore, sample photodamage is greatly reduced because fluorescence excitation is limited to the focal region. For deep tissue imaging, two-photon microscopy has the additional benefit in the greatly improved imaging depth penetration. Since the near- infrared laser sources used in two-photon microscopy scatter less than their UV/glue-green counterparts, in-depth imaging of highly scattering specimen can be greatly improved. In this work, we will present data characterizing both the imaging characteristics (point-spread-functions) and tissue samples (skin) images using this novel technology. In particular, we will demonstrate how blind deconvolution can be used further improve two-photon image quality and how this technique can be used to study mechanisms of chemically-enhanced, transdermal drug delivery.

  6. Enhanced Emission from Single Isolated Gold Quantum Dots Investigated Using Two-Photon-Excited Fluorescence Near-Field Scanning Optical Microscopy.

    PubMed

    Abeyasinghe, Neranga; Kumar, Santosh; Sun, Kai; Mansfield, John F; Jin, Rongchao; Goodson, Theodore

    2016-12-21

    New approaches in molecular nanoscopy are greatly desired for interrogation of biological, organic, and inorganic objects with sizes below the diffraction limit. Our current work investigates emergent monolayer-protected gold quantum dots (nanoclusters, NCs) composed of 25 Au atoms by utilizing two-photon-excited fluorescence (TPEF) near-field scanning optical microscopy (NSOM) at single NC concentrations. Here, we demonstrate an approach to synthesize and isolate single NCs on solid glass substrates. Subsequent investigation of the NCs using TPEF NSOM reveals that, even when they are separated by distances of several tens of nanometers, we can excite and interrogate single NCs individually. Interestingly, we observe an enhanced two-photon absorption (TPA) cross section for single Au 25 NCs that can be attributed to few-atom local field effects and to local field-induced microscopic cascading, indicating their potential for use in ultrasensitive sensing, disease diagnostics, cancer cell therapy, and molecular computers. Finally, we report room-temperature aperture-based TPEF NSOM imaging of these NCs for the first time at 30 nm point resolution, which is a ∼5-fold improvement compared to the previous best result for the same technique. This report unveils the unique combination of an unusually large TPA cross section and the high photostability of Au NCs to (non-destructively) investigate stable isolated single NCs using TPEF NSOM. This is the first reported optical study of monolayer-protected single quantum clusters, opening some very promising opportunities in spectroscopy of nanosized objects, bioimaging, ultrasensitive sensing, molecular computers, and high-density data storage.

  7. A photonic link for donor spin qubits in silicon

    NASA Astrophysics Data System (ADS)

    Simmons, Stephanie

    Atomically identical donor spin qubits in silicon offer excellent native quantum properties, which match or outperform many qubit rivals. To scale up such systems it would be advantageous to connect silicon donor spin qubits in a cavity-QED architecture. Many proposals in this direction introduce strong electric dipole interactions to the otherwise largely isolated spin qubit ground state in order to couple to superconducting cavities. Here I present an alternative approach, which uses the built-in strong electric dipole (optical) transitions of singly-ionized double donors in silicon. These donors, such as chalcogen donors S +, Se + and Te +, have the same ground-state spin Hamiltonians as shallow donors yet offer mid-gap binding energies and mid-IR optical access to excited orbital states. This photonic link is spin-selective which could be harnessed to measure and couple donor qubits using photonic cavity-QED. This approach should be robust to device environments with variable strains and electric fields, and will allow for CMOS- compatible, bulk-like, spatially separated donor qubit placement, optical parity measurements, and 4.2K operation. I will present preliminary data in support of this approach, including 4.2K optical initialization/readout in Earth's magnetic field, where long T1 and T2 times have been measured.

  8. On-demand semiconductor single-photon source with near-unity indistinguishability.

    PubMed

    He, Yu-Ming; He, Yu; Wei, Yu-Jia; Wu, Dian; Atatüre, Mete; Schneider, Christian; Höfling, Sven; Kamp, Martin; Lu, Chao-Yang; Pan, Jian-Wei

    2013-03-01

    Single-photon sources based on semiconductor quantum dots offer distinct advantages for quantum information, including a scalable solid-state platform, ultrabrightness and interconnectivity with matter qubits. A key prerequisite for their use in optical quantum computing and solid-state networks is a high level of efficiency and indistinguishability. Pulsed resonance fluorescence has been anticipated as the optimum condition for the deterministic generation of high-quality photons with vanishing effects of dephasing. Here, we generate pulsed single photons on demand from a single, microcavity-embedded quantum dot under s-shell excitation with 3 ps laser pulses. The π pulse-excited resonance-fluorescence photons have less than 0.3% background contribution and a vanishing two-photon emission probability. Non-postselective Hong-Ou-Mandel interference between two successively emitted photons is observed with a visibility of 0.97(2), comparable to trapped atoms and ions. Two single photons are further used to implement a high-fidelity quantum controlled-NOT gate.

  9. Nuclear Photonics

    NASA Astrophysics Data System (ADS)

    Nedorezov, V. G.; Savel'ev-Trofimov, A. B.

    2017-12-01

    A review of works performed at the Institute for Nuclear Research of the Russian Academy of Sciences and at the International Laser Center of the Moscow State University in the context of the new research area called "nuclear photonics" is presented. Nuclear photonics is based on creation of the new-generation gamma-ray sources which make it possible to solve a number of fundamental and applied problems, including research of low-energy photonuclear reactions, namely, investigation of collective excitations of nuclei near the threshold (pygmy resonances); nuclear safety assurance; production of low-energy positron beams; and phase-contrast X-ray imaging.

  10. Cr:ZnSe planar waveguide mid-IR laser

    NASA Astrophysics Data System (ADS)

    Willimas, J. E.; Martyshkin, D. V.; Fedorov, V. V.; Moskalev, I. S.; Camata, R. P.; Mirov, S. B.

    2011-02-01

    Middle infrared (mid-IR) chromium-doped zinc selenide (Cr:ZnSe) bulk lasers have attracted a lot of attention due to their unique combination of optical and laser properties facilitating a wide range of potential scientific, industrial, and medical applications. Utilization of thin film waveguide geometry enabling good thermal management and control of beam quality is a viable pathway for compact chip-integrated optical laser design. Cr:ZnSe thin films are also promising as saturable absorbers and mode-lockers of the cavities of solid state lasers operating over 1.3-2.1 μm. We recently reported the first successful demonstration of mid-IR Cr:ZnSe planar waveguide lasing at 2.6 μm under gain-switched short-pulse (5 ns) 1.56 μm excitation as well as the passive Q-switching of the cavity of a fiber-pumped Er:YAG laser operating at 1645 nm using a highly doped Cr:ZnSe thin film. PLD grown Cr:ZnSe waveguide were fabricated on sapphire substrates (Cr:ZnSe/sapphire) with chromium concentration of 1018-1019 cm-3. Further development of mid-IR lasing in the Cr:ZnSe planar waveguide under continuous wave excitation were investigated. In addition, deposition of Cr:ZnSe-based thin film structures on n-type GaAs substrates were also investigated for possible mid-IR electroluminescence.

  11. Single-photon sensitive fast ebCMOS camera system for multiple-target tracking of single fluorophores: application to nano-biophotonics

    NASA Astrophysics Data System (ADS)

    Cajgfinger, Thomas; Chabanat, Eric; Dominjon, Agnes; Doan, Quang T.; Guerin, Cyrille; Houles, Julien; Barbier, Remi

    2011-03-01

    Nano-biophotonics applications will benefit from new fluorescent microscopy methods based essentially on super-resolution techniques (beyond the diffraction limit) on large biological structures (membranes) with fast frame rate (1000 Hz). This trend tends to push the photon detectors to the single-photon counting regime and the camera acquisition system to real time dynamic multiple-target tracing. The LUSIPHER prototype presented in this paper aims to give a different approach than those of Electron Multiplied CCD (EMCCD) technology and try to answer to the stringent demands of the new nano-biophotonics imaging techniques. The electron bombarded CMOS (ebCMOS) device has the potential to respond to this challenge, thanks to the linear gain of the accelerating high voltage of the photo-cathode, to the possible ultra fast frame rate of CMOS sensors and to the single-photon sensitivity. We produced a camera system based on a 640 kPixels ebCMOS with its acquisition system. The proof of concept for single-photon based tracking for multiple single-emitters is the main result of this paper.

  12. Two-photon excitation in chip electrophoresis enabling label-free fluorescence detection in non-UV transparent full-body polymer chips.

    PubMed

    Geissler, David; Belder, Detlev

    2015-12-01

    One of the most commonly employed detection methods in microfluidic research is fluorescence detection, due to its ease of integration and excellent sensitivity. Many analytes though do not show luminescence when excited in the visible light spectrum, require suitable dyes. Deep-ultraviolet (UV) excitation (<300 nm) allows label-free detection of a broader range of analytes but also mandates the use of expensive fused silica glass, which is transparent to UV light. Herein, we report the first application of label-free deep UV fluorescence detection in non-UV transparent full-body polymer microfluidic devices. This was achieved by means of two-photon excitation in the visible range (λex = 532 nm). Issues associated with the low optical transmittance of plastics in the UV range were successfully circumvented in this way. The technique was investigated by application to microchip electrophoresis of small aromatic compounds. Various polymers, such as poly(methyl methacrylate), cyclic olefin polymer, and copolymer as well as poly(dimethylsiloxane) were investigated and compared with respect to achievable LOD and ruggedness against photodamage. To demonstrate the applicability of the technique, the method was also applied to the determination of serotonin and tryptamine in fruit samples. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  13. Low Noise Mid-Wavelength IR Photodetectors

    DTIC Science & Technology

    2014-02-19

    Theoretical Framework and Calculated Results We will first review the theoretical limit for single-stage photovoltaic (PV) detectors and then proceed...efficient the device utilizes the incident photons. We see that Eq. 12 reduces to the standard expression for a single-absorber photovoltaic detector...mid-IR spectrum, one can expect growing demands and applications for high-speed detectors that operate at thermoelectric cooler temperatures with

  14. Nonlinear coupled mode approach for modeling counterpropagating solitons in the presence of disorder-induced multiple scattering in photonic crystal waveguides

    NASA Astrophysics Data System (ADS)

    Mann, Nishan; Hughes, Stephen

    2018-02-01

    We present the analytical and numerical details behind our recently published article [Phys. Rev. Lett. 118, 253901 (2017), 10.1103/PhysRevLett.118.253901], describing the impact of disorder-induced multiple scattering on counterpropagating solitons in photonic crystal waveguides. Unlike current nonlinear approaches using the coupled mode formalism, we account for the effects of intraunit cell multiple scattering. To solve the resulting system of coupled semilinear partial differential equations, we introduce a modified Crank-Nicolson-type norm-preserving implicit finite difference scheme inspired by the transfer matrix method. We provide estimates of the numerical dispersion characteristics of our scheme so that optimal step sizes can be chosen to either minimize numerical dispersion or to mimic the exact dispersion. We then show numerical results of a fundamental soliton propagating in the presence of multiple scattering to demonstrate that choosing a subunit cell spatial step size is critical in accurately capturing the effects of multiple scattering, and illustrate the stochastic nature of disorder by simulating soliton propagation in various instances of disordered photonic crystal waveguides. Our approach is easily extended to include a wide range of optical nonlinearities and is applicable to various photonic nanostructures where power propagation is bidirectional, either by choice, or as a result of multiple scattering.

  15. Photonic crystals possessing multiple Weyl points and the experimental observation of robust surface states

    PubMed Central

    Chen, Wen-Jie; Xiao, Meng; Chan, C. T.

    2016-01-01

    Weyl points, as monopoles of Berry curvature in momentum space, have captured much attention recently in various branches of physics. Realizing topological materials that exhibit such nodal points is challenging and indeed, Weyl points have been found experimentally in transition metal arsenide and phosphide and gyroid photonic crystal whose structure is complex. If realizing even the simplest type of single Weyl nodes with a topological charge of 1 is difficult, then making a real crystal carrying higher topological charges may seem more challenging. Here we design, and fabricate using planar fabrication technology, a photonic crystal possessing single Weyl points (including type-II nodes) and multiple Weyl points with topological charges of 2 and 3. We characterize this photonic crystal and find nontrivial 2D bulk band gaps for a fixed kz and the associated surface modes. The robustness of these surface states against kz-preserving scattering is experimentally observed for the first time. PMID:27703140

  16. Time-resolved scattering of a single photon by a single atom

    PubMed Central

    Leong, Victor; Seidler, Mathias Alexander; Steiner, Matthias; Cerè, Alessandro; Kurtsiefer, Christian

    2016-01-01

    Scattering of light by matter has been studied extensively in the past. Yet, the most fundamental process, the scattering of a single photon by a single atom, is largely unexplored. One prominent prediction of quantum optics is the deterministic absorption of a travelling photon by a single atom, provided the photon waveform matches spatially and temporally the time-reversed version of a spontaneously emitted photon. Here we experimentally address this prediction and investigate the influence of the photon's temporal profile on the scattering dynamics using a single trapped atom and heralded single photons. In a time-resolved measurement of atomic excitation we find a 56(11)% increase of the peak excitation by photons with an exponentially rising profile compared with a decaying one. However, the overall scattering probability remains unchanged within the experimental uncertainties. Our results demonstrate that envelope tailoring of single photons enables precise control of the photon–atom interaction. PMID:27897173

  17. Interstellar polycyclic aromatic hydrocarbons - The infrared emission bands, the excitation/emission mechanism, and the astrophysical implications

    NASA Technical Reports Server (NTRS)

    Allamandola, L. J.; Tielens, G. G. M.; Barker, J. R.

    1989-01-01

    A comprehensive study of the PAH hypothesis is presented, including the interstellar, IR spectral features which have been attributed to emission from highly vibrationally excited PAHs. Spectroscopic and IR emission features are discussed in detail. A method for calculating the IR fluorescence spectrum from a vibrationally excited molecule is described. Analysis of interstellar spectrum suggests that the PAHs which dominate the IR spectra contain between 20 and 40 C atoms. The results are compared with results from a thermal approximation. It is found that, for high levels of vibrational excitation and emission from low-frequency modes, the two methods produce similar results. Also, consideration is given to the relationship between PAH molecules and amorphous C particles, the most likely interstellar PAH molecular structures, the spectroscopic structure produced by PAHs and PAH-related materials in the UV portion of the interstellar extinction curve, and the influence of PAH charge on the UV, visible, and IR regions.

  18. IR Variability of Eta Carinae

    NASA Astrophysics Data System (ADS)

    Smith, Nathan

    2007-02-01

    Every 5.5 years, η Carinae experiences a dramatic ``spectroscopic event'' when high-excitation lines in its UV, optical, and IR spectrum disappear, and its hard X-ray and radio continuum flux crash. This periodicity has been attributed to an eccentric binary system with a shell ejection occurring at periastron. In addition, η Car shows long term changes as it is still recovering from its giant 19th century outburst. Both types of variability are directly linked to the current mass-loss rate and dust formation in its wind. Mid-IR images and spectra with T-ReCS provide a direct measure of changes in the current bolometric luminosity and trace dust formation episodes. This will provide a direct measurement of the mass ejected. Near-IR emission lines trace related changes in the post-event wind and ionization changes in the circumstellar environment needed to test specific models for the cause of η Car's variability as it recovers from its recent ``event''. High resolution near-IR spectra with GNIRS will continue the important work of HST/STIS, investigating changes in the direct and reflected spectrum of the stellar wind, and ionization changes in the nebula.

  19. Low-energy measurements of electron-photon angular correlation in electron-impact excitation of the 2/sup 1/P state of helium

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

    Steph, N.C.; Golden, D.E.

    1983-03-01

    Electron-photon angular correlations between electrons which have excited the 2/sup 1/P state of He and photons from the 2/sup 1/P..-->..1/sup 1/S transition have been studied for 27-, 30-, 35-, and 40-eV incident electrons. Values of lambda and Vertical BarchiVertical Bar obtained from these measurements are compared to values obtained in distorted-wave and R-matrix calculations. The values of lambda and Vertical BarchiVertical Bar have been combined to examine the behavior of Vertical BarO/sub 1//sub -//sup colvertical-bar/ (lambda(1-lambda)sinVertical BarchiVertical Bar), the nonvanishing component of orientation. At 27 eV, a substantial decrease was observed in the values of lambda and Vertical BarO/sub 1//submore » -//sup colvertical-bar/, compared with their values for E> or =30 eV.« less

  20. Comparison of TLD calibration methods for  192Ir dosimetry

    PubMed Central

    Butler, Duncan J.; Wilfert, Lisa; Ebert, Martin A.; Todd, Stephen P.; Hayton, Anna J.M.; Kron, Tomas

    2013-01-01

    For the purpose of dose measurement using a high‐dose rate  192Ir source, four methods of thermoluminescent dosimeter (TLD) calibration were investigated. Three of the four calibration methods used the  192Ir source. Dwell times were calculated to deliver 1 Gy to the TLDs irradiated either in air or water. Dwell time calculations were confirmed by direct measurement using an ionization chamber. The fourth method of calibration used 6 MV photons from a medical linear accelerator, and an energy correction factor was applied to account for the difference in sensitivity of the TLDs in  192Ir and 6 M V. The results of the four TLD calibration methods are presented in terms of the results of a brachytherapy audit where seven Australian centers irradiated three sets of TLDs in a water phantom. The results were in agreement within estimated uncertainties when the TLDs were calibrated with the  192Ir source. Calibrating TLDs in a phantom similar to that used for the audit proved to be the most practical method and provided the greatest confidence in measured dose. When calibrated using 6 MV photons, the TLD results were consistently higher than the  192Ir−calibrated TLDs, suggesting this method does not fully correct for the response of the TLDs when irradiated in the audit phantom. PACS number: 87 PMID:23318392

  1. Collaborative Research. Atmospheric Pressure Microplasma Chemistry-Photon Synergies

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

    Park, Sung-Jin; Eden, James Gary

    Combining the effects of low temperature, atmospheric pressure microplasmas and microplasma photon sources offers the promise of greatly expanding the range of applications for each of them. The plasma sources create active chemical species and these can be activated further by the addition of photons and the associated photochemistry. There are many ways to combine the effects of plasma chemistry and photochemistry, especially if there are multiple phases present. This project combined the construction of appropriate test experimental systems, various spectroscopic diagnostics and mathematical modeling. Through a continuous discussion and co-design process with the UC-Berkeley Team, we have successfully completedmore » the fabrication and testing of all components for a microplasma array-assisted system designed for photon-activated plasma chemistry research. Microcavity plasma lamps capable of generating more than 20 mW/cm 2 at 172 nm (Xe dimer) were fabricated with a custom form factor to mate to the plasma chemistry setup, and a lamp was current being installed by the Berkeley team so as to investigate plasma chemistry-photon synergies at a higher photon energy (~7.2 eV) as compared to the UVA treatment that is afforded by UV LEDs operating at 365 nm. In particular, motivated by the promising results from the Berkeley team with UVA treatment, we also produced the first generation of lamps that can generate photons in the 300-370 nm wavelength range. Another set of experiments, conducted under the auspices of this grant, involved the use of plasma microjet arrays. The combination of the photons and excited radicals produced by the plasma column resulted in broad area deactivation of bacteria.« less

  2. Hybrid colloidal plasmonic-photonic crystals.

    PubMed

    Romanov, Sergei G; Korovin, Alexander V; Regensburger, Alois; Peschel, Ulf

    2011-06-17

    We review the recently emerged class of hybrid metal-dielectric colloidal photonic crystals. The hybrid approach is understood as the combination of a dielectric photonic crystal with a continuous metal film. It allows to achieve a strong modification of the optical properties of photonic crystals by involving the light scattering at electronic excitations in the metal component into moulding of the light flow in series to the diffraction resonances occurring in the body of the photonic crystal. We consider different realizations of hybrid plasmonic-photonic crystals based on two- and three-dimensional colloidal photonic crystals in association with flat and corrugated metal films. In agreement with model calculations, different resonance phenomena determine the optical response of hybrid crystals leading to a broadly tuneable functionality of these crystals. Copyright © 2011 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  3. Integrated femtosecond stimulated Raman scattering and two-photon fluorescence imaging of subcellular lipid and vesicular structures

    NASA Astrophysics Data System (ADS)

    Li, Xuesong; Lam, Wen Jiun; Cao, Zhe; Hao, Yan; Sun, Qiqi; He, Sicong; Mak, Ho Yi; Qu, Jianan Y.

    2015-11-01

    The primary goal of this study is to demonstrate that stimulated Raman scattering (SRS) as a new imaging modality can be integrated into a femtosecond (fs) nonlinear optical (NLO) microscope system. The fs sources of high pulse peak power are routinely used in multimodal nonlinear microscopy to enable efficient excitation of multiple NLO signals. However, with fs excitations, the SRS imaging of subcellular lipid and vesicular structures encounters significant interference from proteins due to poor spectral resolution and a lack of chemical specificity, respectively. We developed a unique NLO microscope of fs excitation that enables rapid acquisition of SRS and multiple two-photon excited fluorescence (TPEF) signals. In the in vivo imaging of transgenic C. elegans animals, we discovered that by cross-filtering false positive lipid signals based on the TPEF signals from tryptophan-bearing endogenous proteins and lysosome-related organelles, the imaging system produced highly accurate assignment of SRS signals to lipid. Furthermore, we demonstrated that the multimodal NLO microscope system could sequentially image lipid structure/content and organelles, such as mitochondria, lysosomes, and the endoplasmic reticulum, which are intricately linked to lipid metabolism.

  4. Giant spin gap and magnon localization in the disordered Heisenberg antiferromagnet Sr2Ir1 -xRuxO4

    NASA Astrophysics Data System (ADS)

    Cao, Yue; Liu, X.; Xu, Wenhu; Yin, Wei-Guo; Meyers, D.; Kim, Jungho; Casa, Diego; Upton, M. H.; Gog, Thomas; Berlijn, Tom; Alvarez, Gonzalo; Yuan, Shujuan; Terzic, Jasminka; Tranquada, J. M.; Hill, John P.; Cao, Gang; Konik, Robert M.; Dean, M. P. M.

    2017-03-01

    We study the evolution of magnetic excitations in the disordered two-dimensional antiferromagnet Sr2Ir1 -xRuxO4 . The maximum energy of the magnetic excitation remains robust up to x =0.77 , with a gap opening at low dopings and increasing to over 150 meV at x =0.77 . At these higher Ru concentrations, the dispersive magnetic excitations in Sr2IrO4 are rendered essentially momentum independent. Up to a Ru concentration of x =0.77 , both experiments and first-principles calculations show the Ir Jeff=1 /2 state remains intact. The magnetic gap arises from the local interaction anisotropy in the proximity of the Ru disorder. Under the coherent potential approximation, we reproduce the experimental magnetic excitations using the disordered Heisenberg antiferromagnetic model with suppressed next-nearest-neighbor ferromagnetic coupling.

  5. Single photon source with individualized single photon certifications

    NASA Astrophysics Data System (ADS)

    Migdall, Alan L.; Branning, David A.; Castelletto, Stefania; Ware, M.

    2002-12-01

    As currently implemented, single-photon sources cannot be made to produce single photons with high probability, while simultaneously suppressing the probability of yielding two or more photons. Because of this, single photon sources cannot really produce single photons on demand. We describe a multiplexed system that allows the probabilities of producing one and more photons to be adjusted independently, enabling a much better approximation of a source of single photons on demand. The scheme uses a heralded photon source based on parametric downconversion, but by effectively breaking the trigger detector area into multiple regions, we are able to extract more information about a heralded photon than is possible with a conventional arrangement. This scheme allows photons to be produced along with a quantitative 'certification' that they are single photons. Some of the single-photon certifications can be significantly better than what is possible with conventional downconversion sources, as well as being better than faint laser sources. With such a source of more tightly certified single photons, it should be possible to improve the maximum secure bit rate possible over a quantum cryptographic link. We present an analysis of the relative merits of this method over the conventional arrangement.

  6. Signatures of two-photon pulses from a quantum two-level system

    NASA Astrophysics Data System (ADS)

    Fischer, Kevin A.; Hanschke, Lukas; Wierzbowski, Jakob; Simmet, Tobias; Dory, Constantin; Finley, Jonathan J.; Vučković, Jelena; Müller, Kai

    2017-07-01

    A two-level atom can generate a strong many-body interaction with light under pulsed excitation. The best known effect is single-photon generation, where a short Gaussian laser pulse is converted into a Lorentzian single-photon wavepacket. However, recent studies suggested that scattering of intense laser fields off a two-level atom may generate oscillations in two-photon emission that come out of phase with the Rabi oscillations, as the power of the pulse increases. Here, we provide an intuitive explanation for these oscillations using a quantum trajectory approach and show how they may preferentially result in emission of two-photon pulses. Experimentally, we observe the signatures of these oscillations by measuring the bunching of photon pulses scattered off a two-level quantum system. Our theory and measurements provide insight into the re-excitation process that plagues on-demand single-photon sources while suggesting the possibility of producing new multi-photon states.

  7. Theoretical analysis of photon statistics on excited number of modes and dopant concentration in Er3+:Ti:LiNbO, waveguide amplifiers

    NASA Astrophysics Data System (ADS)

    Ducariu, A.; Constantin, G. C.; Puscas, N. N.

    2005-08-01

    In the small gain approximation and the unsaturated regime in this paper we report some original results concerning the evaluation of the Fano factor, statistical fluctuation and spontaneous emission factor which characterize the photon statistics on the number of excited modes, dopant concentration and power pumping in the single and double pass Er3+ - doped LiNbO, straight waveguide amplifiers pumped near 1484 nm using erfc, Gaussian and constant profile of the Er3+ ions in LiNbO, crystal. We demonstrated that for 50 mW input pump power the Poisson photon statistics are maintained in the above mentioned amplifiers for concentrations of the Er ions smaller than l026 m-3 and also high gains and low noise figures are achievable. The obtained results can be used for the design of optoelectronic integrated circuits.

  8. Infrared photonic bandgap materials and structures

    NASA Astrophysics Data System (ADS)

    Sundaram, S. K.; Keller, P. E.; Riley, B. J.; Martinez, J. E.; Johnson, B. R.; Allen, P. J.; Saraf, L. V.; Anheier, N. C., Jr.; Liau, F.

    2006-02-01

    Three-dimensional periodic dielectric structure can be described by band theory, analogous to electron waves in a crystal. Photonic band gap (PBG) structures were introduced in 1987. The PBG is an energy band in which optical modes, spontaneous emission, and zero-point fluctuations are all absent. It was first theoretically predicted that a three-dimensional photonic crystal could have a complete band gap. E. Yablonovitch built the first three-dimensional photonic crystal (Yablonovite) on microwave length scale, with a complete PBG. In nature, photonic crystals occur as semiprecious opal and the microscopic structures on the wings of some tropical butterflies, which are repeating structures (PBG structure/materials) that inhibit the propagation of some frequencies of light. Pacific Northwest National Laboratory (PNNL) has been developing tunable (between 3.5 and 16 μm) quantum cascade lasers (QCL), chalcogenides, and all other components for an integrated approach to chemical sensing. We have made significant progress in modeling and fabrication of infrared photonic band gap (PBG) materials and structures. We modeled several 2-D designs and defect configurations. Transmission spectra were computed by the Finite Difference Time Domain Method (with FullWAVE TM). The band gaps were computed by the Plane Wave Expansion Method (with BandSOLVE TM). The modeled designs and defects were compared and the best design was identified. On the experimental front, chalcogenide glasses were used as the starting materials. As IIS 3, a common chalcogenide, is an important infrared (IR) transparent material with a variety of potential applications such as IR sensors, waveguides, and photonic crystals. Wet-chemical lithography has been extended to PBG fabrication and challenges identified. An overview of results and challenges will be presented.

  9. Dead-time optimized time-correlated photon counting instrument with synchronized, independent timing channels

    NASA Astrophysics Data System (ADS)

    Wahl, Michael; Rahn, Hans-Jürgen; Gregor, Ingo; Erdmann, Rainer; Enderlein, Jörg

    2007-03-01

    Time-correlated single photon counting is a powerful method for sensitive time-resolved fluorescence measurements down to the single molecule level. The method is based on the precisely timed registration of single photons of a fluorescence signal. Historically, its primary goal was the determination of fluorescence lifetimes upon optical excitation by a short light pulse. This goal is still important today and therefore has a strong influence on instrument design. However, modifications and extensions of the early designs allow for the recovery of much more information from the detected photons and enable entirely new applications. Here, we present a new instrument that captures single photon events on multiple synchronized channels with picosecond resolution and over virtually unlimited time spans. This is achieved by means of crystal-locked time digitizers with high resolution and very short dead time. Subsequent event processing in programmable logic permits classical histogramming as well as time tagging of individual photons and their streaming to the host computer. Through the latter, any algorithms and methods for the analysis of fluorescence dynamics can be implemented either in real time or offline. Instrument test results from single molecule applications will be presented.

  10. Near-infrared continuous-wave light driving a two-photon photochromic reaction with the assistance of localized surface plasmon.

    PubMed

    Tsuboi, Yasuyuki; Shimizu, Ryosuke; Shoji, Tatsuya; Kitamura, Noboru

    2009-09-09

    We demonstrate that a photochromic reaction can be driven by irradiation from a weak, near-infrared continuous-wave (NIR-CW) laser light. A two-photon ring-opening photochromic reaction of a diarylethene (DE) derivative can be induced by irradiation with a NIR-CW laser light (lambda = 808 nm). An ultrathin polymer film doped with DE in its closed form was coated onto a gold-nanoparticle-integrated glass substrate. Upon irradiation of the sample with a CW laser at low fluence (0.1-4.0 W/cm(2)), we could clearly observe bleaching of the DE (ring-opening reaction). Following the IR irradiation, the bleached absorption could be reversibly recovered by applying UV irradiation (ring-closing reaction). We verified that the yield of the photochromic ring-opening reaction of the DE was proportional to the square of the irradiation fluence. The origin of this NIR-CW-induced two-photon photochromic reaction is an "enhancing effect" that acts on the electromagnetic field (localized surface plasmon) of the gold nanoparticles. The DE interacts with the surface plasmon and receives energy from two photons, which excites it to a state from which the ring-opening reaction can be initiated.

  11. Enhancing the sensitivity of fluorescence correlation spectroscopy by using time-correlated single photon counting.

    PubMed

    Lamb, D C; Müller, B K; Bräuchle, C

    2005-10-01

    Fluorescence correlation spectroscopy (FCS) and fluorescence cross-correlation spectroscopy (FCCS) are methods that extract information about a sample from the influence of thermodynamic equilibrium fluctuations on the fluorescence intensity. This method allows dynamic information to be obtained from steady state equilibrium measurements and its popularity has dramatically increased in the last 10 years due to the development of high sensitivity detectors and its combination with confocal microscopy. Using time-correlated single-photon counting (TCSPC) detection and pulsed excitation, information over the duration of the excited state can be extracted and incorporated in the analysis. In this short review, we discuss new methodologies that have recently emerged which incorporated fluorescence lifetime information or TCSPC data in the FCS and FCCS analysis. Time-gated FCS discriminates between which photons are to be incorporated in the analysis dependent upon their arrival time after excitation. This allows for accurate FCS measurements in the presence of fluorescent background, determination of sample homogeneity, and the ability to distinguish between static and dynamic heterogeneities. A similar method, time-resolved FCS can be used to resolve the individual correlation functions from multiple fluorophores through the different fluorescence lifetimes. Pulsed interleaved excitation (PIE) encodes the excitation source into the TCSPC data. PIE can be used to perform dual-channel FCCS with a single detector and allows elimination of spectral cross-talk with dual-channel detection. For samples that undergo fluorescence resonance energy transfer (FRET), quantitative FCCS measurements can be performed in spite of the FRET and the static FRET efficiency can be determined.

  12. Quantum Discord in Photon-Added Glauber Coherent States of GHZ-Type

    NASA Astrophysics Data System (ADS)

    Daoud, M.; Kaydi, W.; El Hadfi, H.

    2015-11-01

    We investigate the influence of photon excitations on quantum correlations in tripartite Glauber coherent states of Greenberger-Horne-Zeilinger type (GHZ-type). The pairwise correlations are measured by means of the entropy-based quantum discord. We also analyze the monogamy property of quantum discord in this class of tripartite states in terms of the strength of Glauber coherent states and the photon excitation order.

  13. A long Stokes shift red fluorescent Ca2+ indicator protein for two-photon and ratiometric imaging

    PubMed Central

    Wu, Jiahui; Abdelfattah, Ahmed S.; Miraucourt, Loïs S.; Kutsarova, Elena; Ruangkittisakul, Araya; Zhou, Hang; Ballanyi, Klaus; Wicks, Geoffrey; Drobizhev, Mikhail; Rebane, Aleksander; Ruthazer, Edward S.; Campbell, Robert E.

    2016-01-01

    The introduction of calcium ion (Ca2+) indicators based on red fluorescent proteins (RFPs) has created new opportunities for multicolour visualization of intracellular Ca2+ dynamics. However, one drawback of these indicators is that they have optimal two-photon excitation outside the near-infrared window (650–1,000 nm) where tissue is most transparent to light. To address this shortcoming, we developed a long Stokes shift RFP-based Ca2+ indicator, REX-GECO1, with optimal two-photon excitation at <1,000 nm. REX-GECO1 fluoresces at 585 nm when excited at 480 nm or 910 nm by a one- or two-photon process, respectively. We demonstrate that REX-GECO1 can be used as either a ratiometric or intensiometric Ca2+ indicator in organotypic hippocampal slice cultures (one- and two-photon) and the visual system of albino tadpoles (two-photon). Furthermore, we demonstrate single excitation wavelength two-colour Ca2+ and glutamate imaging in organotypic cultures. PMID:25358432

  14. Three-dimensional weight-accumulation algorithm for generating multiple excitation spots in fast optical stimulation

    NASA Astrophysics Data System (ADS)

    Takiguchi, Yu; Toyoda, Haruyoshi

    2017-11-01

    We report here an algorithm for calculating a hologram to be employed in a high-access speed microscope for observing sensory-driven synaptic activity across all inputs to single living neurons in an intact cerebral cortex. The system is based on holographic multi-beam generation using a two-dimensional phase-only spatial light modulator to excite multiple locations in three dimensions with a single hologram. The hologram was calculated with a three-dimensional weighted iterative Fourier transform method using the Ewald sphere restriction to increase the calculation speed. Our algorithm achieved good uniformity of three dimensionally generated excitation spots; the standard deviation of the spot intensities was reduced by a factor of two compared with a conventional algorithm.

  15. Three-dimensional weight-accumulation algorithm for generating multiple excitation spots in fast optical stimulation

    NASA Astrophysics Data System (ADS)

    Takiguchi, Yu; Toyoda, Haruyoshi

    2018-06-01

    We report here an algorithm for calculating a hologram to be employed in a high-access speed microscope for observing sensory-driven synaptic activity across all inputs to single living neurons in an intact cerebral cortex. The system is based on holographic multi-beam generation using a two-dimensional phase-only spatial light modulator to excite multiple locations in three dimensions with a single hologram. The hologram was calculated with a three-dimensional weighted iterative Fourier transform method using the Ewald sphere restriction to increase the calculation speed. Our algorithm achieved good uniformity of three dimensionally generated excitation spots; the standard deviation of the spot intensities was reduced by a factor of two compared with a conventional algorithm.

  16. Quantification of fluorescent samples by photon-antibunching

    NASA Astrophysics Data System (ADS)

    Kurz, Anton; Schwering, Michael; Herten, Dirk-Peter

    2012-02-01

    Typical problems in molecular biology, like oligomerization of proteins, appear on non-resolvable length scales. Therefore a method which allows counting numbers of fluorescent emitters beyond this barrier can help to unveil these questions. One approach engaging this task makes use of the photon antibunching (PAB) effect. Most fluorophores are single photon emitters. Therefore upon a narrow excitation pulse they might only run through one excitation cycle and emit one photon at a time. This behavior is known as PAB. By analyzing coincident events of photon detections (Coincidence Analysis, CCA ) over many excitation cycles the number of fluorophores residing in the confocal volume can be estimated. Simulations have shown that up to 40 fluorophores can be distinguished with a reasonable error. In follow-up experiments five fluorophores could be distinguished by CCA. In this work the method is applied to a whole sample set and statistical variance and robustness are determined. CCA is critical to several parameters like photo stability, background noise, label efficiency and photopysical properties of the dye, like brightness and blinking. Therefore a reasonable scheme for analysis is introduced and setup parameters are optimized. To proof the superiority of CCA, it has been applied to estimate the number of dyes for a well-defined probe and the results have been compared with bleach step analysis (BS analysis), a method based on the ability to observe single bleach-steps.

  17. AFM-IR: Technology and Applications in Nanoscale Infrared Spectroscopy and Chemical Imaging.

    PubMed

    Dazzi, Alexandre; Prater, Craig B

    2016-12-13

    Atomic force microscopy-based infrared spectroscopy (AFM-IR) is a rapidly emerging technique that provides chemical analysis and compositional mapping with spatial resolution far below conventional optical diffraction limits. AFM-IR works by using the tip of an AFM probe to locally detect thermal expansion in a sample resulting from absorption of infrared radiation. AFM-IR thus can provide the spatial resolution of AFM in combination with the chemical analysis and compositional imaging capabilities of infrared spectroscopy. This article briefly reviews the development and underlying technology of AFM-IR, including recent advances, and then surveys a wide range of applications and investigations using AFM-IR. AFM-IR applications that will be discussed include those in polymers, life sciences, photonics, solar cells, semiconductors, pharmaceuticals, and cultural heritage. In the Supporting Information , the authors provide a theoretical section that reviews the physics underlying the AFM-IR measurement and detection mechanisms.

  18. Two-photon absorption in arsenic sulfide glasses

    NASA Astrophysics Data System (ADS)

    Chunaev, D. S.; Snopatin, G. E.; Plotnichenko, V. G.; Karasik, A. Ya.

    2016-10-01

    The two-photon absorption coefficient of 1047-{\\text{nm}} light in {\\text{As}}35{\\text{S}}65 chalcogenide glass has been measured. CW probe radiation has been used to observe the linear absorption in glass induced by two-photon excitation. The induced absorption lifetime was found to be ∼ 2 {\\text{ms}}.

  19. Two-Photon Activation of p-Hydroxyphenacyl Phototriggers: Toward Spatially Controlled Release of Diethyl Phosphate and ATP.

    PubMed

    Houk, Amanda L; Givens, Richard S; Elles, Christopher G

    2016-03-31

    Two-photon activation of the p-hydroxyphenacyl (pHP) photoactivated protecting group is demonstrated for the first time using visible light at 550 nm from a pulsed laser. Broadband two-photon absorption measurements reveal a strong two-photon transition (>10 GM) near 4.5 eV that closely resembles the lowest-energy band at the same total excitation energy in the one-photon absorption spectrum of the pHP chromophore. The polarization dependence of the two-photon absorption band is consistent with excitation to the same S3 ((1)ππ*) excited state for both one- and two-photon activation. Monitoring the progress of the uncaging reaction under nonresonant excitation at 550 nm confirms a quadratic intensity dependence and that two-photon activation of the uncaging reaction is possible using visible light in the range 500-620 nm. Deprotonation of the pHP chromophore under mildly basic conditions shifts the absorption band to lower energy (3.8 eV) in both the one- and two-photon absorption spectra, suggesting that two-photon activation of the pHP chromophore may be possible using light in the range 550-720 nm. The results of these measurements open the possibility of spatially and temporally selective release of biologically active compounds from the pHP protecting group using visible light from a pulsed laser.

  20. Two-photon oxygen nanosensors based on a conjugated fluorescent polymer doped with platinum porphyrins.

    PubMed

    Wang, Xiao-Hui; Peng, Hong-Shang; Cheng, Kun; Liu, Xiao-Ming; Liu, Yuan-An; Yang, Wei

    2018-04-27

    Ratiometric fluorescent nanoparticles (NPs) under two-photon excitation are successfully developed for sensing dissolved oxygen. The NPs comprise the oxygen probe Pt(II)-porphyrins (PtTFPP) and fluorescent organic semiconducting polymer (PFO). PFO polymer acts as both a two-photon antenna and a reference dye, while PtTFPP absorbs the photonic energy transferred by the PFO under two-photon excitation at 740 nm to sense oxygen. The red fluorescence of PtTFPP is sensitive to oxygen with a quenching response of 88% from nitrogen saturation to oxygen saturation, and PFO gives oxygen-insensitive referenced blue fluorescence. The fluorescence quenching of the NPs against oxygen at two-photon excitation follows a linear Stern-Volmer behavior. The nanosensors exhibit low cytotoxic effects as well as effortless cellular uptake. When incorporated into cells, the ratio of the signals increases up to about 500% from oxygen-saturated to oxygen-free environment.

  1. Impact excitation and electron-hole multiplication in graphene and carbon nanotubes.

    PubMed

    Gabor, Nathaniel M

    2013-06-18

    In semiconductor photovoltaics, photoconversion efficiency is governed by a simple competition: the incident photon energy is either transferred to the crystal lattice (heat) or transferred to electrons. In conventional materials, energy loss to the lattice is more efficient than energy transferred to electrons, thus limiting the power conversion efficiency. Quantum electronic systems, such as quantum dots, nanowires, and two-dimensional electronic membranes, promise to tip the balance in this competition by simultaneously limiting energy transfer to the lattice and enhancing energy transfer to electrons. By exploring the optical, thermal, and electronic properties of quantum materials, we may perhaps find an ideal optoelectronic material that provides low cost fabrication, facile systems integration, and a means to surpass the standard limit for photoconversion efficiency. Nanoscale carbon materials, such as graphene and carbon nanotubes, provide ideal experimental quantum systems in which to explore optoelectronic behavior for applications in solar energy harvesting. Within essentially the same material, researchers can achieve a broad spectrum of energetic configurations, from a gapless semimetal to a large band-gap semiconducting nanowire. Owing to their nanoscale dimensions, graphene and carbon nanotubes exhibit electronic and optical properties that reflect strong electron-electron interactions. Such strong interactions may lead to exotic low-energy electron transport behavior and high-energy electron scattering processes such as impact excitation and the inverse process of Auger recombination. High-energy processes, which become very important under photoexcitation, may be particularly efficient in nanoscale carbon materials due to the relativistic-like, charged particle band structure and sensitivity to the dielectric environment. In addition, due to the covalently bonded carbon framework that makes up these materials, electron-phonon coupling is very weak

  2. Two-Photon Fluorescence Microscope for Microgravity Research

    NASA Technical Reports Server (NTRS)

    Fischer, David G.; Zimmerli, Gregory A.; Asipauskas, Marius

    2005-01-01

    A two-photon fluorescence microscope has been developed for the study of biophysical phenomena. Two-photon microscopy is a novel form of laser-based scanning microscopy that enables three-dimensional imaging without many of the problems inherent in confocal microscopy. Unlike one-photon optical microscopy, two-photon microscopy utilizes the simultaneous nonlinear absorption of two near-infrared photons. However, the efficiency of two-photon absorption is much lower than that of one-photon absorption, so an ultra-fast pulsed laser source is typically employed. On the other hand, the critical energy threshold for two-photon absorption leads to fluorophore excitation that is intrinsically localized to the focal volume. Consequently, two-photon microscopy enables optical sectioning and confocal performance without the need for a signal-limiting pinhole. In addition, there is a reduction (relative to one-photon optical microscopy) in photon-induced damage because of the longer excitation wavelength. This reduction is especially advantageous for in vivo studies. Relative to confocal microscopy, there is also a reduction in background fluorescence, and, because of a reduction in Rayleigh scattering, there is a 4 increase of penetration depth. The prohibitive cost of a commercial two-photon fluorescence-microscope system, as well as a need for modularity, has led to the construction of a custom-built system (see Figure 1). This system includes a coherent mode-locked titanium: sapphire laser emitting 120-fs-duration pulses at a repetition rate of 80 MHz. The pulsed laser has an average output power of 800 mW and a wavelength tuning range of 700 to 980 nm, enabling the excitation of a variety of targeted fluorophores. The output from the laser is attenuated, spatially filtered, and then directed into a confocal scanning head that has been modified to provide for side entry of the laser beam. The laser output coupler has been replaced with a dichroic filter that reflects the

  3. Attosecond Pulse Carrier-Envelope Phase Effects: Roles of Frequency, Intensity and an Additional IR Pulse

    NASA Astrophysics Data System (ADS)

    Pronin, Evgeny A.; Peng, Liang-You; Starace, Anthony F.

    2008-05-01

    The effects of the carrier-envelope phase (CEP) of a few-cycle attosecond pulse on ionized electron momentum and energy spectra are analyzed, both with and without an additional few-cycle IR pulse [1, 2]. In the absence of an IR pulse, the CEP-induced asymmetries in the ionized electron momentum distributions are shown to vary as the 3/2 power of the attosecond pulse intensity. These asymmetries are also found to satisfy an approximate scaling law involving the frequency and intensity of the attosecond pulse. In the presence of even a very weak IR pulse, the attosecond pulse CEP-induced asymmetries are found to be significantly augmented. In addition, for higher IR laser intensities, we observe for low electron energies peaks separated by the IR photon energy in one electron momentum direction along the laser polarization axis; in the opposite direction, we find structured peaks that are spaced by twice the IR photon energy. Possible physical mechanisms for such asymmetric, low-energy structures in the ionized electron momentum distribution are proposed. Our results are based on single-active-electron solutions of the 3D TDSE for H and He. [1] Peng LY, Pronin EA, and Starace AF, New J. Phys. 10, xxx (2008); [2] Peng LY, Starace AF, Phys. Rev. A 76, 043401 (2007)

  4. Development of pixellated Ir-TESs

    NASA Astrophysics Data System (ADS)

    Zen, Nobuyuki; Takahashi, Hiroyuki; Kunieda, Yuichi; Damayanthi, Rathnayaka M. T.; Mori, Fumiakira; Fujita, Kaoru; Nakazawa, Masaharu; Fukuda, Daiji; Ohkubo, Masataka

    2006-04-01

    We have been developing Ir-based pixellated superconducting transition edge sensors (TESs). In the area of material or astronomical applications, the sensor with few eV energy resolution and over 1000 pixels imaging property is desired. In order to achieve this goal, we have been analyzing signals from pixellated TESs. In the case of a 20 pixel array of Ir-TESs, with 45 μm×45 μm pixel sizes, the incident X-ray signals have been classified into 16 groups. We have applied numerical signal analysis. On the one hand, the energy resolution of our pixellated TES is strongly degraded. However, using pulse shape analysis, we can dramatically improve the resolution. Thus, we consider that the pulse signal analysis will lead this device to be used as a practical photon incident position identifying TES.

  5. Deterministic photon-emitter coupling in chiral photonic circuits.

    PubMed

    Söllner, Immo; Mahmoodian, Sahand; Hansen, Sofie Lindskov; Midolo, Leonardo; Javadi, Alisa; Kiršanskė, Gabija; Pregnolato, Tommaso; El-Ella, Haitham; Lee, Eun Hye; Song, Jin Dong; Stobbe, Søren; Lodahl, Peter

    2015-09-01

    Engineering photon emission and scattering is central to modern photonics applications ranging from light harvesting to quantum-information processing. To this end, nanophotonic waveguides are well suited as they confine photons to a one-dimensional geometry and thereby increase the light-matter interaction. In a regular waveguide, a quantum emitter interacts equally with photons in either of the two propagation directions. This symmetry is violated in nanophotonic structures in which non-transversal local electric-field components imply that photon emission and scattering may become directional. Here we show that the helicity of the optical transition of a quantum emitter determines the direction of single-photon emission in a specially engineered photonic-crystal waveguide. We observe single-photon emission into the waveguide with a directionality that exceeds 90% under conditions in which practically all the emitted photons are coupled to the waveguide. The chiral light-matter interaction enables deterministic and highly directional photon emission for experimentally achievable on-chip non-reciprocal photonic elements. These may serve as key building blocks for single-photon optical diodes, transistors and deterministic quantum gates. Furthermore, chiral photonic circuits allow the dissipative preparation of entangled states of multiple emitters for experimentally achievable parameters, may lead to novel topological photon states and could be applied for directional steering of light.

  6. Deterministic photon-emitter coupling in chiral photonic circuits

    NASA Astrophysics Data System (ADS)

    Söllner, Immo; Mahmoodian, Sahand; Hansen, Sofie Lindskov; Midolo, Leonardo; Javadi, Alisa; Kiršanskė, Gabija; Pregnolato, Tommaso; El-Ella, Haitham; Lee, Eun Hye; Song, Jin Dong; Stobbe, Søren; Lodahl, Peter

    2015-09-01

    Engineering photon emission and scattering is central to modern photonics applications ranging from light harvesting to quantum-information processing. To this end, nanophotonic waveguides are well suited as they confine photons to a one-dimensional geometry and thereby increase the light-matter interaction. In a regular waveguide, a quantum emitter interacts equally with photons in either of the two propagation directions. This symmetry is violated in nanophotonic structures in which non-transversal local electric-field components imply that photon emission and scattering may become directional. Here we show that the helicity of the optical transition of a quantum emitter determines the direction of single-photon emission in a specially engineered photonic-crystal waveguide. We observe single-photon emission into the waveguide with a directionality that exceeds 90% under conditions in which practically all the emitted photons are coupled to the waveguide. The chiral light-matter interaction enables deterministic and highly directional photon emission for experimentally achievable on-chip non-reciprocal photonic elements. These may serve as key building blocks for single-photon optical diodes, transistors and deterministic quantum gates. Furthermore, chiral photonic circuits allow the dissipative preparation of entangled states of multiple emitters for experimentally achievable parameters, may lead to novel topological photon states and could be applied for directional steering of light.

  7. Enhanced-locality fiber-optic two-photon-fluorescence live-brain interrogation

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

    Fedotov, I. V.; Doronina-Amitonova, L. V.; Russian Quantum Center, ul. Novaya 100, Skolkovo, Moscow Region 1430125

    2014-02-24

    Two-photon excitation is shown to substantially enhance the locality of fiber-based optical interrogation of strongly scattering biotissues. In our experiments, a high-numerical-aperture, large-core-are fiber probe is used to deliver the 200-fs output of a 100-MHz mode-locked ytterbium fiber laser to samples of live mouse brain, induce two-photon fluorescence of nitrogen–vacancy centers in diamond markers in brain sample. Fiber probes with a high numerical aperture and a large core area are shown to enable locality enhancement in fiber-laser–fiber-probe two-photon brain excitation and interrogation without sacrificing the efficiency of fluorescence response collection.

  8. Simultaneous multi-beam planar array IR (pair) spectroscopy

    DOEpatents

    Elmore, Douglas L.; Rabolt, John F.; Tsao, Mei-Wei

    2005-09-13

    An apparatus and method capable of providing spatially multiplexed IR spectral information simultaneously in real-time for multiple samples or multiple spatial areas of one sample using IR absorption phenomena requires no moving parts or Fourier Transform during operation, and self-compensates for background spectra and degradation of component performance over time. IR spectral information and chemical analysis of the samples is determined by using one or more IR sources, sampling accessories for positioning the samples, optically dispersive elements, a focal plane array (FPA) arranged to detect the dispersed light beams, and a processor and display to control the FPA, and display an IR spectrograph. Fiber-optic coupling can be used to allow remote sensing. Portability, reliability, and ruggedness is enhanced due to the no-moving part construction. Applications include determining time-resolved orientation and characteristics of materials, including polymer monolayers. Orthogonal polarizers may be used to determine certain material characteristics.

  9. Enhanced Single-Photon Emission from Carbon-Nanotube Dopant States Coupled to Silicon Microcavities.

    PubMed

    Ishii, Akihiro; He, Xiaowei; Hartmann, Nicolai F; Machiya, Hidenori; Htoon, Han; Doorn, Stephen K; Kato, Yuichiro K

    2018-06-13

    Single-walled carbon nanotubes are a promising material as quantum light sources at room temperature and as nanoscale light sources for integrated photonic circuits on silicon. Here, we show that the integration of dopant states in carbon nanotubes and silicon microcavities can provide bright and high-purity single-photon emitters on a silicon photonics platform at room temperature. We perform photoluminescence spectroscopy and observe the enhancement of emission from the dopant states by a factor of ∼50, and cavity-enhanced radiative decay is confirmed using time-resolved measurements, in which a ∼30% decrease of emission lifetime is observed. The statistics of photons emitted from the cavity-coupled dopant states are investigated by photon-correlation measurements, and high-purity single photon generation is observed. The excitation power dependence of photon emission statistics shows that the degree of photon antibunching can be kept high even when the excitation power increases, while the single-photon emission rate can be increased to ∼1.7 × 10 7 Hz.

  10. Two-photon fluorescence imaging super-enhanced by multishell nanophotonic particles, with application to subcellular pH.

    PubMed

    Ray, Aniruddha; Lee, Yong-Eun Koo; Kim, Gwangseong; Kopelman, Raoul

    2012-07-23

    A novel nanophotonic method for enhancing the two-photon fluorescence signal of a fluorophore is presented. It utilizes the second harmonic (SH) of the exciting light generated by noble metal nanospheres in whose near-field the dye molecules are placed, to further enhance the dye's fluorescence signal in addition to the usual metal-enhanced fluorescence phenomenon. This method enables demonstration, for the first time, of two-photon fluorescence enhancement inside a biological system, namely live cells. A multishell hydrogel nanoparticle containing a silver core, a protective citrate capping, which serves also as an excitation quenching inhibitor spacer, a pH indicator dye shell, and a polyacrylamide cladding are employed. Utilizing this technique, an enhancement of up to 20 times in the two-photon fluorescence of the indicator dye is observed. Although a significant portion of the enhanced fluorescence signal is due to one-photon processes accompanying the SH generation of the exciting light, this method preserves all the advantages of infrared-excited, two-photon microscopy: enhanced penetration depth, localized excitation, low photobleaching, low autofluorescence, and low cellular damage. Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  11. Experimenting liver fibrosis diagnostic by two photon excitation microscopy and Bag-of-Features image classification.

    PubMed

    Stanciu, Stefan G; Xu, Shuoyu; Peng, Qiwen; Yan, Jie; Stanciu, George A; Welsch, Roy E; So, Peter T C; Csucs, Gabor; Yu, Hanry

    2014-04-10

    The accurate staging of liver fibrosis is of paramount importance to determine the state of disease progression, therapy responses, and to optimize disease treatment strategies. Non-linear optical microscopy techniques such as two-photon excitation fluorescence (TPEF) and second harmonic generation (SHG) can image the endogenous signals of tissue structures and can be used for fibrosis assessment on non-stained tissue samples. While image analysis of collagen in SHG images was consistently addressed until now, cellular and tissue information included in TPEF images, such as inflammatory and hepatic cell damage, equally important as collagen deposition imaged by SHG, remain poorly exploited to date. We address this situation by experimenting liver fibrosis quantification and scoring using a combined approach based on TPEF liver surface imaging on a Thioacetamide-induced rat model and a gradient based Bag-of-Features (BoF) image classification strategy. We report the assessed performance results and discuss the influence of specific BoF parameters to the performance of the fibrosis scoring framework.

  12. Experimenting Liver Fibrosis Diagnostic by Two Photon Excitation Microscopy and Bag-of-Features Image Classification

    PubMed Central

    Stanciu, Stefan G.; Xu, Shuoyu; Peng, Qiwen; Yan, Jie; Stanciu, George A.; Welsch, Roy E.; So, Peter T. C.; Csucs, Gabor; Yu, Hanry

    2014-01-01

    The accurate staging of liver fibrosis is of paramount importance to determine the state of disease progression, therapy responses, and to optimize disease treatment strategies. Non-linear optical microscopy techniques such as two-photon excitation fluorescence (TPEF) and second harmonic generation (SHG) can image the endogenous signals of tissue structures and can be used for fibrosis assessment on non-stained tissue samples. While image analysis of collagen in SHG images was consistently addressed until now, cellular and tissue information included in TPEF images, such as inflammatory and hepatic cell damage, equally important as collagen deposition imaged by SHG, remain poorly exploited to date. We address this situation by experimenting liver fibrosis quantification and scoring using a combined approach based on TPEF liver surface imaging on a Thioacetamide-induced rat model and a gradient based Bag-of-Features (BoF) image classification strategy. We report the assessed performance results and discuss the influence of specific BoF parameters to the performance of the fibrosis scoring framework. PMID:24717650

  13. Experimenting Liver Fibrosis Diagnostic by Two Photon Excitation Microscopy and Bag-of-Features Image Classification

    NASA Astrophysics Data System (ADS)

    Stanciu, Stefan G.; Xu, Shuoyu; Peng, Qiwen; Yan, Jie; Stanciu, George A.; Welsch, Roy E.; So, Peter T. C.; Csucs, Gabor; Yu, Hanry

    2014-04-01

    The accurate staging of liver fibrosis is of paramount importance to determine the state of disease progression, therapy responses, and to optimize disease treatment strategies. Non-linear optical microscopy techniques such as two-photon excitation fluorescence (TPEF) and second harmonic generation (SHG) can image the endogenous signals of tissue structures and can be used for fibrosis assessment on non-stained tissue samples. While image analysis of collagen in SHG images was consistently addressed until now, cellular and tissue information included in TPEF images, such as inflammatory and hepatic cell damage, equally important as collagen deposition imaged by SHG, remain poorly exploited to date. We address this situation by experimenting liver fibrosis quantification and scoring using a combined approach based on TPEF liver surface imaging on a Thioacetamide-induced rat model and a gradient based Bag-of-Features (BoF) image classification strategy. We report the assessed performance results and discuss the influence of specific BoF parameters to the performance of the fibrosis scoring framework.

  14. Excitations in opal photonic crystals infiltrated with polarizable media

    NASA Astrophysics Data System (ADS)

    Eradat, Nayer; Sivachenko, A. Y.; Raikh, Mikhail E.; Vardeny, Z. Valy; Zakhidov, Anvar A.; Li, S.; Baughman, Ray H.

    2002-12-01

    Photonic crystals (PC) are a class of artificial structures with a periodic dielectric function. PCs can be a laboratory for testing fundamental processes involving interactions of radiation with matter in novel conditions. We have studied the optical properties of opal PCs that are infiltrated with highly polarizable media such as j-aggregates of cyanine dyes. Opals are self-assembled structures of silica spheres. We report our studies on clarifying the relationship between a polaritonic gap and a photonic stop band (Bragg gap) when they resonantly coexist in the same structure. Infiltration of opal with polarizable molecules combines the polaritonic and Bragg diffractive effects. Both effects exist independently when the Bragg (at ω = ωB) and polaritonic (ω = ωT) resonances are well separated in frequency. A completely different situation occurs when ωT ~ωB. Such a condition was achieved in opals that were infiltrated with J-aggregates of cyanine dyes that have large Rabi frequency. Our measurements show some dramatic changes in the shape of the reflectivity plateaus, which are due to the interplay between the photonic band gap and the polaritonic gap. The experimental results on reflectivity and its dependence on the light propagation angle and concentration of the cyanie dyes are in agreement with the theoretical calculations.

  15. Transition-matrix theory for two-photon ionization of rare-gas atoms and isoelectronic ions with application to argon

    NASA Astrophysics Data System (ADS)

    Starace, Anthony F.; Jiang, Tsin-Fu

    1987-08-01

    A transition-matrix theory for two-photon ionization processes in rare-gas atoms or isoelectronic ions is presented. Uncoupled ordinary differential equations are obtained for the radial functions needed to calculate the two-photon transition amplitude. The implications of these equations are discussed in detail. In particular, the role of correlations involving virtually excited electron pairs, which are known to be essential to the description of single-photon processes, is examined for multiphoton ionization processes. Additionally, electron scattering interactions between two electron-hole pairs are introduced into our transition amplitude in the boson approximation since these have been found important in two-photon ionization of xenon by L'Huillier and Wendin [J. Phys. B 20, L37 (1987)]. Application of our theory is made to two-photon ionization of the 3p subshell of argon below the one-photon ionization threshold. Our results are compared to previous calculations of McGuire [Phys. Rev. A 24, 835 (1981)], of Moccia, Rahman, and Rizzo [J. Phys. B 16, 2737 (1983)], and of Pindzola and Kelly [Phys. Rev. A 11, 1543 (1975)]. Results are presented for both circularly and linearly polarized photons. Among our findings are, firstly, that the electron scattering interactions, which have not been included in previous calculations for argon, produce a substantial reduction in the two-photon single-ionization cross section below the one-photon ionization threshold, which is in agreement with findings of L'Huillier and Wendin for xenon. Secondly, we find that de-excitation of virtually excited electron pairs by absorption of a photon is important for describing the interaction of the atom with the photon field, as in the case of single-photon ionization processes, but that further excitation of virtually excited electron pairs by the photon field has completely negligible effects, indicating a major simplification of the theory for higher-order absorption processes.

  16. Broadband sensitized photon up-conversion at subsolar irradiance (Conference Presentation)

    NASA Astrophysics Data System (ADS)

    Pedrini, Jacopo; Monguzzi, Angelo; Meinardi, Francesco

    2016-09-01

    A crucial limit of solar devices is their inability to harvest the full solar spectrum. Currently, sensitized up-conversion based on triplet-tripled annihilation (STTA-UC) in bi-component organic systems is the most promising technique to recover sub-bandgap photons, showing good efficiencies also at excitation intensities comparable to the solar irradiance. In STTA-UC, high-energy light is generated through annihilation of metastable triplet states of molecules acting as emitters, which are populated via resonant energy transfer from a light-harvesting sensitizer. However, suitable sensitizers show narrow absorption bands, limiting the fraction of recoverable photons, therefore preventing the application of STTA-UC to real-world devices. Here we demonstrate how to overcome the described limit by using multiple sensitizers that work cooperatively to broaden the overall system absorption band. This is obtained using an additional sensitizer that transfers the extra harvested energy to the main one (sensitization of the sensitizer), or a set of properly designed complementary absorbing sensitizers all able to excite simultaneously the same emitter (multi-sensitizers). In both cases STTA-UC performances result strongly enhanced compared to the corresponding mono-sensitizer system, increasing the up-converted light intensity generated at AM 1.5 up to two times. Remarkably, by coupling our light converters to a DSSC we prove its operation by exploiting exclusively sub-bandgap photons. A detailed modeling of the photophysical processes involved in these complex systems allows us to draw the guidelines for the design of the next generation STTA-UC materials, encouraging their application to photovoltaic technologies.

  17. Coupling mid-infrared light from a photonic crystal waveguide to metallic transmission lines

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

    Blanco-Redondo, Andrea, E-mail: andrea.blanco@tecnalia.com, E-mail: r.hillenbrand@nanogune.eu; Dpto. Electronica y Telecom., E.T.S. Ingeniería Bilbao, UPV/EHU, Alda. Urquijo, 48103 Bilbao, Bizkaia; Sarriugarte, Paulo

    2014-01-06

    We propose and theoretically study a hybrid structure consisting of a photonic crystal waveguide (PhC-wg) and a two-wire metallic transmission line (TL), engineered for efficient transfer of mid-infrared (mid-IR) light between them. An efficiency of 32% is obtained for the coupling from the transverse magnetic (TM) photonic mode to the symmetric mode of the TL, with a predicted intensity enhancement factor of 53 at the transmission line surface. The strong coupling is explained by the small phase velocity mismatch and sufficient spatial overlapping between the modes. This hybrid structure could find applications in highly integrated mid-IR photonic-plasmonic devices for biologicalmore » and gas sensing, among others.« less

  18. Di-lepton yield from the decay of excited 28Si states

    NASA Astrophysics Data System (ADS)

    Bacelar, J. C.; Buda, A.; Bałanda, A.; Krasznahorkay, A.; van der Ploeg, H.; Sujkowski, Z.; van der Woude, A.

    1994-03-01

    The first dilepton yield measurements from excited nuclear states obtained with a new Positron-Electron Pair Spectroscopic Instrument (PEPSI) are reported. Nuclear states in 28Si, with an initial excitation energy E∗ = 50 MeV, were populated via the isospin T = 0 reaction 4He + 24Mg and the mixed-isospin 3He + 25Mg reaction. In both reactions the dilepton (e +e -) and photon decay yields were measured concurrently. An excess of counts in the e +e - spectrum, over the converted photon yield, is observed in the energy region above 15 MeV. An analyses is discussed whereby the observed excess counts are assumed to represent the isoscalar E0 strength in excited nuclear states.

  19. Time-resolved two-photon spectroscopy of photosystem I determines hidden carotenoid dark-state dynamics.

    PubMed

    Wehling, Axel; Walla, Peter J

    2005-12-29

    We present time-resolved fs two-photon pump-probe data measured with photosystem I (PS I) of Thermosynechococcus elongatus. Two-photon excitation (lambda(exc)/2 = 575 nm) in the spectral region of the optically forbidden first excited singlet state of the carotenoids, Car S1, gives rise to a 800 fs and a 9 ps decay component of the Car S1 --> S(n) excited-state absorption with an amplitude of about 47 +/- 16% and 53 +/- 10%, respectively. By measuring a solution of pure beta-carotene under exactly the same conditions, only a 9 ps decay component can be observed. Exciting PS I at exactly the same spectral region via one-photon excitation (lambda(exc) = 575 nm) also does not show any sub-ps component. We ascribe the observed constant of 800 fs to a portion of about 47 +/- 16% beta-carotene states that can potentially transfer their energy efficiently to chlorophyll pigments via the optically dark Car S1 state. We compared these data with conventional one-photon pump-probe data, exciting the optically allowed second excited state, Car S2. This comparison demonstrates that the fast dynamics of the optically forbidden state can hardly be unravelled via conventional one-photon excitation only because the corresponding Car S1 populations are too small after Car S2 --> Car S1 internal conversion. A direct comparison of the amplitudes of the Car S1 --> S(n) excited-state absorption of PS I and beta-carotene observed after Car S2 excitation allows determination of a quantum yield for the Car S1 formation in PS I of 44 +/- 5%. In conclusion, an overall Car S2 --> Chl energy-transfer efficiency of approximately 69 +/- 5% is observed at room temperature with 56 +/- 5% being transferred via Car S2 and probably very hot Car S1 states and 13 +/- 5% being transferred via hot and "cold" Car S1 states.

  20. IR Variability of Eta Carinae

    NASA Astrophysics Data System (ADS)

    Smith, Nathan

    2008-02-01

    Every 5.5 years, η Carinae experiences a dramatic ``spectroscopic event'' when high-excitation lines in its UV, optical, and IR spectrum disappear, and its hard X-ray and radio continuum flux crash. This periodicity has been attributed to an eccentric binary system with a shell ejection occurring at periastron, and the next periastron event will occur at the very end of 2008. In addition, η Car shows long term changes as it is still recovering from its giant 19th century outburst. Both types of variability are directly linked to the current mass-loss rate and dust formation in its wind. Mid-IR images and spectra with T-ReCS provide a direct measure of changes in the current bolometric luminosity and a direct measure of the massw in dust formation episodes that may occur at periastron in the colliding wind shock. Near-IR emission lines trace related changes in the post-event wind and ionization changes in the circumstellar environment needed to test specific models for the cause of η Car's variability as it recovers from its recent ``event''. High resolution near-IR spectra with Phoenix will continue the important work of HST/STIS, investigating changes in the direct and reflected spectrum of the stellar wind, and ionization changes in the nebula.

  1. Multiphoton dynamics of qutrits in the ultrastrong coupling regime with a quantized photonic field

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

    Avetissian, H. K., E-mail: avetissian@ysu.am; Avetissian, A. K.; Mkrtchian, G. F.

    2015-12-15

    Multiphoton resonant excitation of a three-state quantum system (a qutrit) with a single-mode photonic field is considered in the ultrastrong coupling regime, when the qutrit–photonic field coupling rate is comparable to appreciable fractions of the photon frequency. For ultrastrong couplings, the obtained solutions of the Schrödinger equation that reveal multiphoton Rabi oscillations in qutrits with the interference effects leading to the collapse and revival of atomic excitation probabilities at the direct multiphoton resonant transitions.

  2. Numerical modeling of two-photon focal modulation microscopy with a sinusoidal phase filter.

    PubMed

    Chen, Rui; Shen, Shuhao; Chen, Nanguang

    2018-05-01

    A spatiotemporal phase modulator (STPM) is theoretically investigated using the vectorial diffraction theory. The STPM is equivalent to a time-dependent phase-only pupil filter that alternates between a homogeneous filter and a stripe-shaped filter with a sinusoidal phase distribution. It is found that two-photon focal modulation microscopy (TPFMM) using this STPM can significantly suppress the background contribution from out-of-focus ballistic excitation and achieve almost the same resolution as two-photon microscopy. The modulation depth is also evaluated and a compromise exists between the signal-to-background ratio and signal-to-noise ratio. The theoretical investigations provide important insights into future implementations of TPFMM and its potential to further extend the penetration depth of nonlinear microscopy in imaging multiple-scattering biological tissues. (2018) COPYRIGHT Society of Photo-Optical Instrumentation Engineers (SPIE).

  3. Quantum Nonlinear Optics without Photons

    NASA Astrophysics Data System (ADS)

    Macrı, Vincenzo

    Here we propose a physical process analogous to spontaneous parametric down-conversion, where one excited atom directly transfers its excitation to a couple of spatially separated atoms with probability approaching one. The interaction is mediated by the exchange of virtual rather than real photons. This nonlinear optical process is coherent and reversible, so that the couple of excited atoms can transfer back the excitation to the first one: the analogous for atoms of sum-frequency generation. The parameters used here correspond to experimentally-demonstrated values in circuit QED. This approach can be expanded to consider other nonlinear inter-atomic processes as the four-qubit mixing and is an attractive architecture for the realization of quantum devices on a chip.

  4. Cross Modulation of Two Laser Beams at the Individual-Photon Level

    DTIC Science & Technology

    2014-09-12

    medium, such that the photons travel as slow-light polaritons [15,25,26], whose atomic excitation component can block the transmission of another light...through the ensemble, traveling in the medium as slow-light polaritons , a superposition of a photon and a collective atomic excitation to the state...unclassified Standard Form 298 (Rev. 8-98) Prescribed by ANSI Std Z39-18 slow-light polariton , the polariton’s atomic component in state jci reduces

  5. High heralding-efficiency of near-IR fiber coupled photon pairs for quantum technologies

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

    Dixon, P. Ben; Murphy, Ryan; Rosenberg, Danna

    We report on the development and use of a high heralding-efficiency, single-mode-fiber coupled telecom-band source of entangled photons for quantum technology applications. The source development efforts consisted of theoretical and experimental efforts and we demonstrated a correlated-mode coupling efficiency of 97% 2%, the highest efficiency yet achieved for this type of system. We then incorporated these beneficial source development techniques in a Sagnac configured telecom-band entangled photon source that generates photon pairs entangled in both time/energy and polarization degrees of freedom. We made use of these highly desirable entangled states to investigate several promising quantum technologies.

  6. Ultrafast optical excitation of magnetic skyrmions

    NASA Astrophysics Data System (ADS)

    Ogawa, N.; Seki, S.; Tokura, Y.

    2015-04-01

    Magnetic skyrmions in an insulating chiral magnet Cu2OSeO3 were studied by all-optical spin wave spectroscopy. The spins in the conical and skyrmion phases were excited by the impulsive magnetic field from the inverse-Faraday effect, and resultant spin dynamics were detected by using time-resolved magneto-optics. Clear dispersions of the helimagnon were observed, which is accompanied by a distinct transition into the skyrmion phase, by sweeping temperature and magnetic field. In addition to the collective excitations of skyrmions, i.e., rotation and breathing modes, several spin precession modes were identified, which would be specific to optical excitation. The ultrafast, nonthermal, and local excitation of the spin systems by photons would lead to the efficient manipulation of nano-magnetic structures.

  7. Efficiency of surface plasmon excitation at the photonic crystal – metal interface

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

    Kuznetsova, T I; Raspopov, N A

    2015-11-30

    We report the results of a theoretical investigation of light wave transformation in a one-dimensional photonic crystal. The scheme considered comprises an incident wave directed in parallel with layers of the photonic crystal under an assumption that the wave vector is far from a forbidden zone. Expressions for propagating and evanescent electromagnetic waves in a periodic medium of the photonic crystal are obtained. It is found that the transverse structure of the propagating wave comprises a strong constant component and a weak oscillating component with a period determined by that of the photonic crystal. On the contrary, the dependence ofmore » evanescent waves on transverse coordinates is presented by a strong oscillating component and a weak constant component. The process of transformation of propagating waves to evanescent waves at a crystal – metal interface is investigated. Parameters of the photonic crystal typical for synthetic opals are used in all numerical simulations. The theoretical approach elaborated yields in an explicit form the dependence of the amplitude of a generated surface wave on the period of the dielectric function modulation in the photonic crystal. The results obtained show that in the conditions close to plasmon resonance the amplitude of the surface wave may be on the order of or even exceed that of the initial incident wave. (light wave transformation)« less

  8. Giant spin gap and magnon localization in the disordered Heisenberg antiferromagnet Sr 2 Ir 1 - x Ru x O 4

    DOE PAGES

    Cao, Yue; Liu, X.; Xu, Wenhu; ...

    2017-03-06

    Here, we study the evolution of magnetic excitations in the disordered two-dimensional antiferromagnet Sr 2Ir 1–xRuxO 4. The maximum energy of the magnetic excitation remains robust up to x = 0.77, with a gap opening at low dopings and increasing to over 150 meV at x = 0.77. At these higher Ru concentrations, the dispersive magnetic excitations in Sr 2IrO 4 are rendered essentially momentum independent. Up to a Ru concentration of x = 0.77, both experiments and first-principles calculations show the Ir J eff = 1/2 state remains intact. The magnetic gap arises from the local interaction anisotropy inmore » the proximity of the Ru disorder. Under the coherent potential approximation, we reproduce the experimental magnetic excitations using the disordered Heisenberg antiferromagnetic model with suppressed next-nearest-neighbor ferromagnetic coupling.« less

  9. Three-photon tissue imaging using moxifloxacin.

    PubMed

    Lee, Seunghun; Lee, Jun Ho; Wang, Taejun; Jang, Won Hyuk; Yoon, Yeoreum; Kim, Bumju; Jun, Yong Woong; Kim, Myoung Joon; Kim, Ki Hean

    2018-06-20

    Moxifloxacin is an antibiotic used in clinics and has recently been used as a clinically compatible cell-labeling agent for two-photon (2P) imaging. Although 2P imaging with moxifloxacin labeling visualized cells inside tissues using enhanced fluorescence, the imaging depth was quite limited because of the relatively short excitation wavelength (<800 nm) used. In this study, the feasibility of three-photon (3P) excitation of moxifloxacin using a longer excitation wavelength and moxifloxacin-based 3P imaging were tested to increase the imaging depth. Moxifloxacin fluorescence via 3P excitation was detected at a >1000 nm excitation wavelength. After obtaining the excitation and emission spectra of moxifloxacin, moxifloxacin-based 3P imaging was applied to ex vivo mouse bladder and ex vivo mouse small intestine tissues and compared with moxifloxacin-based 2P imaging by switching the excitation wavelength of a Ti:sapphire oscillator between near 1030 and 780 nm. Both moxifloxacin-based 2P and 3P imaging visualized cellular structures in the tissues via moxifloxacin labeling, but the image contrast was better with 3P imaging than with 2P imaging at the same imaging depths. The imaging speed and imaging depth of moxifloxacin-based 3P imaging using a Ti:sapphire oscillator were limited by insufficient excitation power. Therefore, we constructed a new system for moxifloxacin-based 3P imaging using a high-energy Yb fiber laser at 1030 nm and used it for in vivo deep tissue imaging of a mouse small intestine. Moxifloxacin-based 3P imaging could be useful for clinical applications with enhanced imaging depth.

  10. Giant Spin Gap and Magnon Localization in the Disordered Heisenberg Antiferromagnet Sr2Ir1-xRuxO4

    NASA Astrophysics Data System (ADS)

    Cao, Yue; Liu, Xuerong; Xu, Wenhu; Yin, Weiguo; Meyers, Derek; Kim, Jungho; Casa, Diego; Upton, Mary; Gog, Thomas; Berlijn, Tom; Alvarez, Gonzalo; Yuan, Shujuan; Terzic, Jasminka; Tranquada, J. M.; Hill, John; Cao, Gang; Konik, Robert; Dean, M. P. M.

    We study the evolution of magnetic excitations in the disordered two-dimensional antiferromagnet Sr_2Ir_1-xRu_xO_4. A gigantic magnetic gap greater than 40 meV opens at x = 0.27 and increases with Ru concentration, from 40 meV to >150 meV, rendering the dispersive magnetic excitations in Sr2IrO4 almost momentum independent. Up to a Ru concentration of x = 0.77, both experiments and first-principles calculations show the Ir J_eff = 1/2 state remains intact. The magnetic gap arises from the local interaction anisotropy in the proximity of the Ru disorder. Under the coherent potential approximation, we reproduce the experimental magnetic excitations using the disordered Heisenberg antiferromagnetic model with suppressed next-nearest neighbor ferromagnetic coupling.

  11. Multiphoton near-infrared femtosecond laser pulse-induced DNA damage with and without the photosensitizer proflavine.

    PubMed

    Shafirovich, V; Dourandin, A; Luneva, N P; Singh, C; Kirigin, F; Geacintov, N E

    1999-03-01

    The excitation of pBr322 supercoiled plasmid DNA with intense near-IR 810 nm fs laser pulses by a simultaneous multiphoton absorption mechanism results in single-strand breaks after treatment of the irradiated samples with Micrococcus luteus UV endonuclease. This enzyme cleaves DNA strands at sites of cyclobutane dimers that are formed by the simultaneous absorption of three (or more) 810 nm IR photons (pulse width approximately 140 fs, 76 MHz pulse repetition, average power output focused through 10x microscope objective is approximately 1.2 MW/cm2). Direct single-strand breaks (without treatment with M. luteus) were not observed under these conditions. However, in the presence of 6 microM of the intercalator proflavine (PF), both direct single- and double-strand breaks are observed under conditions where substantial fractions of undamaged supercoiled DNA molecules are still present. The fraction of direct double-strand breaks is 30 +/- 5% of all measurable strand cleavage events, is independent of dosage (up to 6.4 GJ/cm2) and is proportional to In, where I is the average power/area of the 810 nm fs laser pulses, and n = 3 +/- 1. The nicking of two DNA strands in the immediate vicinity of the excited PF molecules gives rise to this double-strand cleavage. In contrast, excitation of the same samples under low-power, single-photon absorption conditions (approximately 400-500 nm) gives rise predominantly to single-strand breaks, but some double-strand breaks are observed at the higher dosages. Thus, single-photon excitation with 400-500 nm light and multiphoton activation of PF by near-IR fs laser pulses produces different distributions of single- and double-strand breaks. These results suggest that DNA strand cleavage originates from unrelaxed, higher excited states when PF is excited by simultaneous IR multiphoton absorption processes.

  12. Collective Autoionization in Multiply-Excited Systems: A novel ionization process observed in Helium Nanodroplets

    PubMed Central

    LaForge, A. C.; Drabbels, M.; Brauer, N. B.; Coreno, M.; Devetta, M.; Di Fraia, M.; Finetti, P.; Grazioli, C.; Katzy, R.; Lyamayev, V.; Mazza, T.; Mudrich, M.; O'Keeffe, P.; Ovcharenko, Y.; Piseri, P.; Plekan, O.; Prince, K. C.; Richter, R.; Stranges, S.; Callegari, C.; Möller, T.; Stienkemeier, F.

    2014-01-01

    Free electron lasers (FELs) offer the unprecedented capability to study reaction dynamics and image the structure of complex systems. When multiple photons are absorbed in complex systems, a plasma-like state is formed where many atoms are ionized on a femtosecond timescale. If multiphoton absorption is resonantly-enhanced, the system becomes electronically-excited prior to plasma formation, with subsequent decay paths which have been scarcely investigated to date. Here, we show using helium nanodroplets as an example that these systems can decay by a new type of process, named collective autoionization. In addition, we show that this process is surprisingly efficient, leading to ion abundances much greater than that of direct single-photon ionization. This novel collective ionization process is expected to be important in many other complex systems, e.g. macromolecules and nanoparticles, exposed to high intensity radiation fields. PMID:24406316

  13. Particle and Photon Detection: Counting and Energy Measurement

    PubMed Central

    Janesick, James; Tower, John

    2016-01-01

    Fundamental limits for photon counting and photon energy measurement are reviewed for CCD and CMOS imagers. The challenges to extend photon counting into the visible/nIR wavelengths and achieve energy measurement in the UV with specific read noise requirements are discussed. Pixel flicker and random telegraph noise sources are highlighted along with various methods used in reducing their contribution on the sensor’s read noise floor. Practical requirements for quantum efficiency, charge collection efficiency, and charge transfer efficiency that interfere with photon counting performance are discussed. Lastly we will review current efforts in reducing flicker noise head-on, in hopes to drive read noise substantially below 1 carrier rms. PMID:27187398

  14. Excitation mechanism in the photoisomerization of a surface-bound azobenzene derivative: Role of the metallic substrate.

    PubMed

    Hagen, Sebastian; Kate, Peter; Leyssner, Felix; Nandi, Dhananjay; Wolf, Martin; Tegeder, Petra

    2008-10-28

    Two-photon photoemission spectroscopy is employed to elucidate the electronic structure and the excitation mechanism in the photoinduced isomerization of the molecular switch tetra-tert-butyl-azobenzene (TBA) adsorbed on Au(111). Our results demonstrate that the optical excitation and the mechanism of molecular switching at a metal surface is completely different compared to the corresponding process for the free molecule. In contrast to direct (intramolecular) excitation operative in the isomerization in the liquid phase, the conformational change in the surface-bound TBA is driven by a substrate-mediated charge transfer process. We find that photoexcitation above a threshold hnu approximately 2.2 eV leads to hole formation in the Au d-band followed by a hole transfer to the highest occupied molecular orbital of TBA. This transiently formed positive ion resonance subsequently results in a conformational change. The photon energy dependent photoisomerization cross section exhibit an unusual shape for a photochemical reaction of an adsorbate on a metal surface. It shows a thresholdlike behavior below hnu approximately 2.2 eV and above hnu approximately 4.4 eV. These thresholds correspond to the minimum energy required to create single or multiple hot holes in the Au d-bands, respectively. This study provides important new insights into the use of light to control the structure and function of molecular switches in direct contact with metal electrodes.

  15. Excitation mechanism in the photoisomerization of a surface-bound azobenzene derivative: Role of the metallic substrate

    NASA Astrophysics Data System (ADS)

    Hagen, Sebastian; Kate, Peter; Leyssner, Felix; Nandi, Dhananjay; Wolf, Martin; Tegeder, Petra

    2008-10-01

    Two-photon photoemission spectroscopy is employed to elucidate the electronic structure and the excitation mechanism in the photoinduced isomerization of the molecular switch tetra-tert-butyl-azobenzene (TBA) adsorbed on Au(111). Our results demonstrate that the optical excitation and the mechanism of molecular switching at a metal surface is completely different compared to the corresponding process for the free molecule. In contrast to direct (intramolecular) excitation operative in the isomerization in the liquid phase, the conformational change in the surface-bound TBA is driven by a substrate-mediated charge transfer process. We find that photoexcitation above a threshold hν ≈2.2 eV leads to hole formation in the Au d-band followed by a hole transfer to the highest occupied molecular orbital of TBA. This transiently formed positive ion resonance subsequently results in a conformational change. The photon energy dependent photoisomerization cross section exhibit an unusual shape for a photochemical reaction of an adsorbate on a metal surface. It shows a thresholdlike behavior below hν ≈2.2 eV and above hν ≈4.4 eV. These thresholds correspond to the minimum energy required to create single or multiple hot holes in the Au d-bands, respectively. This study provides important new insights into the use of light to control the structure and function of molecular switches in direct contact with metal electrodes.

  16. High efficiency carrier multiplication in PbSe nanocrystals: implications for solar energy conversion.

    PubMed

    Schaller, R D; Klimov, V I

    2004-05-07

    We demonstrate for the first time that impact ionization (II) (the inverse of Auger recombination) occurs with very high efficiency in semiconductor nanocrystals (NCs). Interband optical excitation of PbSe NCs at low pump intensities, for which less than one exciton is initially generated per NC on average, results in the formation of two or more excitons (carrier multiplication) when pump photon energies are more than 3 times the NC band gap energy. The generation of multiexcitons from a single photon absorption event is observed to take place on an ultrafast (picosecond) time scale and occurs with up to 100% efficiency depending upon the excess energy of the absorbed photon. Efficient II in NCs can be used to considerably increase the power conversion efficiency of NC-based solar cells.

  17. Enhanced Single-Photon Emission from Carbon-Nanotube Dopant States Coupled to Silicon Microcavities

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

    Ishii, Akihiro; He, Xiaowei; Hartmann, Nicolai F.

    Single-walled carbon nanotubes are a promising material as quantum light sources at room temperature and as nanoscale light sources for integrated photonic circuits on silicon. Here, we show that the integration of dopant states in carbon nanotubes and silicon microcavities can provide bright and high-purity single-photon emitters on a silicon photonics platform at room temperature. We perform photoluminescence spectroscopy and observe the enhancement of emission from the dopant states by a factor of ~50, and cavity-enhanced radiative decay is confirmed using time-resolved measurements, in which a ~30% decrease of emission lifetime is observed. The statistics of photons emitted from themore » cavity-coupled dopant states are investigated by photon-correlation measurements, and high-purity single photon generation is observed. The excitation power dependence of photon emission statistics shows that the degree of photon antibunching can be kept high even when the excitation power increases, while the single-photon emission rate can be increased to ~1.7 × 10 7 Hz.« less

  18. Enhanced Single-Photon Emission from Carbon-Nanotube Dopant States Coupled to Silicon Microcavities

    DOE PAGES

    Ishii, Akihiro; He, Xiaowei; Hartmann, Nicolai F.; ...

    2018-05-21

    Single-walled carbon nanotubes are a promising material as quantum light sources at room temperature and as nanoscale light sources for integrated photonic circuits on silicon. Here, we show that the integration of dopant states in carbon nanotubes and silicon microcavities can provide bright and high-purity single-photon emitters on a silicon photonics platform at room temperature. We perform photoluminescence spectroscopy and observe the enhancement of emission from the dopant states by a factor of ~50, and cavity-enhanced radiative decay is confirmed using time-resolved measurements, in which a ~30% decrease of emission lifetime is observed. The statistics of photons emitted from themore » cavity-coupled dopant states are investigated by photon-correlation measurements, and high-purity single photon generation is observed. The excitation power dependence of photon emission statistics shows that the degree of photon antibunching can be kept high even when the excitation power increases, while the single-photon emission rate can be increased to ~1.7 × 10 7 Hz.« less

  19. Optical sensors based on photonic crystal: a new route

    NASA Astrophysics Data System (ADS)

    Romano, S.; Torino, S.; Coppola, G.; Cabrini, S.; Mocella, V.

    2017-05-01

    The realization of miniaturized devices able to accumulate a higher number of information in a smallest volume is a challenge of the technological development. This trend increases the request of high sensitivity and selectivity sensors which can be integrated in microsystems. In this landscape, optical sensors based on photonic crystal technology can be an appealing solution. Here, a new refractive index sensor device, based on the bound states in the continuum (BIC) resonance shift excited in a photonic crystal membrane, is presented. A microfluidic cell was used to control the injection of fluids with different refractive indices over the photonic crystal surface. The shift of very high Q-factor resonances excited into the photonic crystal open cavity was monitored as a function of the refractive index n of the test liquid. The excellent stability we found and the minimal, loss-free optical equipment requirement, provide a new route for achieving high performance in sensing applications.

  20. Phonon-Assisted Two-Photon Interference from Remote Quantum Emitters.

    PubMed

    Reindl, Marcus; Jöns, Klaus D; Huber, Daniel; Schimpf, Christian; Huo, Yongheng; Zwiller, Val; Rastelli, Armando; Trotta, Rinaldo

    2017-07-12

    Photonic quantum technologies are on the verge of finding applications in everyday life with quantum cryptography and quantum simulators on the horizon. Extensive research has been carried out to identify suitable quantum emitters and single epitaxial quantum dots have emerged as near-optimal sources of bright, on-demand, highly indistinguishable single photons and entangled photon-pairs. In order to build up quantum networks, it is essential to interface remote quantum emitters. However, this is still an outstanding challenge, as the quantum states of dissimilar "artificial atoms" have to be prepared on-demand with high fidelity and the generated photons have to be made indistinguishable in all possible degrees of freedom. Here, we overcome this major obstacle and show an unprecedented two-photon interference (visibility of 51 ± 5%) from remote strain-tunable GaAs quantum dots emitting on-demand photon-pairs. We achieve this result by exploiting for the first time the full potential of a novel phonon-assisted two-photon excitation scheme, which allows for the generation of highly indistinguishable (visibility of 71 ± 9%) entangled photon-pairs (fidelity of 90 ± 2%), enables push-button biexciton state preparation (fidelity of 80 ± 2%) and outperforms conventional resonant two-photon excitation schemes in terms of robustness against environmental decoherence. Our results mark an important milestone for the practical realization of quantum repeaters and complex multiphoton entanglement experiments involving dissimilar artificial atoms.

  1. Conditions for entangled photon emission from (111)B site-controlled pyramidal quantum dots

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

    Juska, G., E-mail: gediminas.juska@tyndall.ie; Murray, E.; Dimastrodonato, V.

    A study of highly symmetric site-controlled pyramidal In{sub 0.25}Ga{sub 0.75}As quantum dots (QDs) is presented. It is discussed that polarization-entangled photons can be also obtained from pyramidal QDs of different designs from the one already reported in Juska et al. [Nat. Photonics 7, 527 (2013)]. Moreover, some of the limitations for a higher density of entangled photon emitters are addressed. Among these issues are (1) a remaining small fine-structure splitting and (2) an effective QD charging under non-resonant excitation conditions, which strongly reduce the number of useful biexciton-exciton recombination events. A possible solution of the charging problem is investigated exploitingmore » a dual-wavelength excitation technique, which allows a gradual QD charge tuning from strongly negative to positive and, eventually, efficient detection of entangled photons from QDs, which would be otherwise ineffective under a single-wavelength (non-resonant) excitation.« less

  2. In vivo three-photon microscopy of subcortical structures within an intact mouse brain

    NASA Astrophysics Data System (ADS)

    Horton, Nicholas G.; Wang, Ke; Kobat, Demirhan; Clark, Catharine G.; Wise, Frank W.; Schaffer, Chris B.; Xu, Chris

    2013-03-01

    Two-photon fluorescence microscopy enables scientists in various fields including neuroscience, embryology and oncology to visualize in vivo and ex vivo tissue morphology and physiology at a cellular level deep within scattering tissue. However, tissue scattering limits the maximum imaging depth of two-photon fluorescence microscopy to the cortical layer within mouse brain, and imaging subcortical structures currently requires the removal of overlying brain tissue or the insertion of optical probes. Here, we demonstrate non-invasive, high-resolution, in vivo imaging of subcortical structures within an intact mouse brain using three-photon fluorescence microscopy at a spectral excitation window of 1,700 nm. Vascular structures as well as red fluorescent protein-labelled neurons within the mouse hippocampus are imaged. The combination of the long excitation wavelength and the higher-order nonlinear excitation overcomes the limitations of two-photon fluorescence microscopy, enabling biological investigations to take place at a greater depth within tissue.

  3. Effect of multiple plasmon excitation on single, double and multiple ionizations of C60 in collisions with fast highly charged Si ions

    NASA Astrophysics Data System (ADS)

    Kelkar, A. H.; Kadhane, U.; Misra, D.; Kumar, A.; Tribedi, L. C.

    2007-06-01

    We have investigated the single and multiple ionizations of the C60 molecule in collisions with fast Siq+ projectiles for various projectile charge states (q) between q = 6 and 14. The q-dependence of the ionization cross sections and their ratios is compared with the giant dipole plasmon resonance (GDPR) model. The excellent qualitative agreement with the model in case of single and double ionizations and also a reasonable agreement with the triple (and to some extent with quadruple) ionization (without evaporation) yields signify dominant contributions of the single-, double- and triple-plasmon excitations on the single- and multiple-ionization process.

  4. Influence of the asymmetry parameter and dissipation coefficient of the K coordinate on different aspects of fission of excited compound nuclei

    NASA Astrophysics Data System (ADS)

    Eslamizadeh, H.; Abdollahi, N.

    2018-02-01

    The dynamics of fission of the excited compound nuclei 256Fm, 215Fr, 187Ir, 172Yb, 162Yb, and 142Ce produced in fusion reactions with 158.8 MeV 18O has been studied by solving three- and four-dimensional Langevin equations with dissipation generated through the chaos weighted wall and window friction formula. The constant dissipation coefficients of K , γK=0.077 (MeVzs ) -1 /2 , γK=0.2 (MeVzs ) -1 /2 and a nonconstant dissipation coefficient of K have been used to reproduce the experimental data for both symmetric and asymmetric splitting of the fissioning systems. The average kinetic energies of fission fragments, the pre-scission neutron multiplicities, the fission time, and the variances of the mass and kinetic energy of fission fragments are calculated for the excited compound nuclei 256Fm, 215Fr, 187Ir, 172Yb, 162Yb, 142Ce, and results of the calculations are compared with each other and with the experimental data. Comparison of the theoretical results with the experimental data calculated by using different values of γK shows that the difference is small between the results of calculations for symmetric and asymmetric simulations of the fission process of excited intermediate nuclei, whereas for heavy compound nuclei the difference is slightly high. In other words, the effect of the asymmetry parameter on the fission process of intermediate nuclei is smaller than the effect on heavy nuclei. Furthermore, we show that the pre-scission neutron multiplicity decreases rapidly with increasing fragment asymmetry.

  5. Steric hindrance inhibits excited-state relaxation and lowers the extent of intramolecular charge transfer in two-photon absorbing dyes.

    PubMed

    Stewart, David J; Dalton, Matthew J; Long, Stephanie L; Kannan, Ramamurthi; Yu, Zhenning; Cooper, Thomas M; Haley, Joy E; Tan, Loon-Seng

    2016-02-21

    The two-photon absorbing dye AF240 [1, (7-benzothiazol-2-yl-9,9-diethylfluoren-2-yl)diphenylamine] is modified by adding bulky alkyl groups to the diphenylamino moiety. Three new compounds are synthesized which have ethyl groups in both ortho positions of each phenyl ring (2), t-butyl groups in one ortho position of each phenyl ring (3), and t-butyl groups in the para position of each phenyl ring (4). The dyes are examined in several aprotic solvents with varying polarity to observe the effects of the sterically hindering bulky groups on the ground and excited-state photophysical properties. While the ground state shows minimal solvent dependence, there is significant dependence on the fluorescence quantum yield and lifetime, as well as the excited-state energy levels. This effect is caused by the formation of an intramolecular charge-transfer (ICT) state, which is observed in the solvents more polar than n-hexane and supported by TD-DFT calculations. Electronic effects of ortho or para alkyl substitution should be similar, yet drastic differences are observed. A red shift in the fluorescence maximum is observed in 4 relative to 1, yet a blue shift occurs in 2 and 3 because the substituents at the sterically sensitive ortho-positions inhibit excited-state geometric relaxation and result in less ICT character than 1. Coupled with theoretical calculations, the data support a planar ICT (PICT) excited state where the diphenylamino nitrogen in an sp(2)-like geometry is integral with the plane containing the fluorene and benzothiazole moieties. Ultrafast transient absorption experiments show that ICT occurs rapidly (<150 fs) followed by geometric and solvent relaxation in ∼ 1-4 ps to form the PICT or solvent-stabilized ICT (SSICT) state. This relaxation is not observed in non-polar n-hexane because the solvent dependent ICT state energy lies higher than the locally-excited (LE) state. Finally, formation of a triplet state (T1) is only efficiently observed in n

  6. Measurement of IR optics with linear coupling's action-angle parametrization

    NASA Astrophysics Data System (ADS)

    Luo, Y.; Bai, M.; Pilat, F.; Satogata, T.; Trbojevic, D.

    2005-08-01

    Linear coupling’s action-angle parametrization is convenient for interpretation of turn-by-turn beam position monitor (BPM) data. We demonstrate how to apply this parametrization to extract Twiss and coupling parameters in interaction regions (IRs), using BPMs on each side of a long IR drift region. Example data were acquired at the Relativistic Heavy Ion Collider, using an ac dipole to excite a single transverse eigenmode. We have measured the waist of the β function and its Twiss and coupling parameters.

  7. Broadband IR polarizing beam splitter using a subwavelength-structured one-dimensional photonic-crystal layer embedded in a high-index prism.

    PubMed

    Khanfar, H K; Azzam, R M A

    2009-09-20

    An iterative procedure for the design of a polarizing beam splitter (PBS) that uses a form-birefringent, subwavelength-structured, one-dimensional photonic-crystal layer (SWS 1-D PCL) embedded in a high-index cubical prism is presented. The PBS is based on index matching and total transmission for the p polarization and total internal reflection for the s polarization at the prism-PCL interface at 45 degrees angle of incidence. A high extinction ratio in reflection (>50 dB) over the 4-12 microm IR spectral range is achieved using a SWS 1-D PCL of ZnTe embedded in a ZnS cube within an external field of view of +/-6.6 degrees and in the presence of grating filling factor errors of up to +/-10%. Comparable results, but with wider field of view, are also obtained with a Ge PCL embedded in a Si prism.

  8. Special purpose modes in photonic band gap fibers

    DOEpatents

    Spencer, James; Noble, Robert; Campbell, Sara

    2013-04-02

    Photonic band gap fibers are described having one or more defects suitable for the acceleration of electrons or other charged particles. Methods and devices are described for exciting special purpose modes in the defects including laser coupling schemes as well as various fiber designs and components for facilitating excitation of desired modes. Results are also presented showing effects on modes due to modes in other defects within the fiber and due to the proximity of defects to the fiber edge. Techniques and devices are described for controlling electrons within the defect(s). Various applications for electrons or other energetic charged particles produced by such photonic band gap fibers are also described.

  9. Quantum teleportation of multiple degrees of freedom of a single photon

    NASA Astrophysics Data System (ADS)

    Wang, Xi-Lin; Cai, Xin-Dong; Su, Zu-En; Chen, Ming-Cheng; Wu, Dian; Li, Li; Liu, Nai-Le; Lu, Chao-Yang; Pan, Jian-Wei

    2015-02-01

    Quantum teleportation provides a `disembodied' way to transfer quantum states from one object to another at a distant location, assisted by previously shared entangled states and a classical communication channel. As well as being of fundamental interest, teleportation has been recognized as an important element in long-distance quantum communication, distributed quantum networks and measurement-based quantum computation. There have been numerous demonstrations of teleportation in different physical systems such as photons, atoms, ions, electrons and superconducting circuits. All the previous experiments were limited to the teleportation of one degree of freedom only. However, a single quantum particle can naturally possess various degrees of freedom--internal and external--and with coherent coupling among them. A fundamental open challenge is to teleport multiple degrees of freedom simultaneously, which is necessary to describe a quantum particle fully and, therefore, to teleport it intact. Here we demonstrate quantum teleportation of the composite quantum states of a single photon encoded in both spin and orbital angular momentum. We use photon pairs entangled in both degrees of freedom (that is, hyper-entangled) as the quantum channel for teleportation, and develop a method to project and discriminate hyper-entangled Bell states by exploiting probabilistic quantum non-demolition measurement, which can be extended to more degrees of freedom. We verify the teleportation for both spin-orbit product states and hybrid entangled states, and achieve a teleportation fidelity ranging from 0.57 to 0.68, above the classical limit. Our work is a step towards the teleportation of more complex quantum systems, and demonstrates an increase in our technical control of scalable quantum technologies.

  10. Quantum teleportation of multiple degrees of freedom of a single photon.

    PubMed

    Wang, Xi-Lin; Cai, Xin-Dong; Su, Zu-En; Chen, Ming-Cheng; Wu, Dian; Li, Li; Liu, Nai-Le; Lu, Chao-Yang; Pan, Jian-Wei

    2015-02-26

    Quantum teleportation provides a 'disembodied' way to transfer quantum states from one object to another at a distant location, assisted by previously shared entangled states and a classical communication channel. As well as being of fundamental interest, teleportation has been recognized as an important element in long-distance quantum communication, distributed quantum networks and measurement-based quantum computation. There have been numerous demonstrations of teleportation in different physical systems such as photons, atoms, ions, electrons and superconducting circuits. All the previous experiments were limited to the teleportation of one degree of freedom only. However, a single quantum particle can naturally possess various degrees of freedom--internal and external--and with coherent coupling among them. A fundamental open challenge is to teleport multiple degrees of freedom simultaneously, which is necessary to describe a quantum particle fully and, therefore, to teleport it intact. Here we demonstrate quantum teleportation of the composite quantum states of a single photon encoded in both spin and orbital angular momentum. We use photon pairs entangled in both degrees of freedom (that is, hyper-entangled) as the quantum channel for teleportation, and develop a method to project and discriminate hyper-entangled Bell states by exploiting probabilistic quantum non-demolition measurement, which can be extended to more degrees of freedom. We verify the teleportation for both spin-orbit product states and hybrid entangled states, and achieve a teleportation fidelity ranging from 0.57 to 0.68, above the classical limit. Our work is a step towards the teleportation of more complex quantum systems, and demonstrates an increase in our technical control of scalable quantum technologies.

  11. Generation of Single Photons and Entangled Photon Pairs from a Quantum Dot

    NASA Astrophysics Data System (ADS)

    Yamamoto, Y.; Pelton, M.; Santori, C.; Solomon, G. S.

    2002-10-01

    Current quantum cryptography systems are limited by the Poissonian photon statistics of a standard light source: a security loophole is opened up by the possibility of multiple-photon pulses. By replacing the source with a single-photon emitter, transmission rates of secure information can be improved. A single photon source is also essential to implement a linear optics quantum computer. We have investigated the use of single self-assembled InAs/GaAs quantum dots as such single-photon sources, and have seen a hundred-fold reduction in the multi-photon probability as compared to Poissonian pulses. An extension of our experiment should also allow for the generation of triggered, polarizationentangled photon pairs.

  12. Photonic Integrated Circuits

    NASA Technical Reports Server (NTRS)

    Krainak, Michael; Merritt, Scott

    2016-01-01

    Integrated photonics generally is the integration of multiple lithographically defined photonic and electronic components and devices (e.g. lasers, detectors, waveguides passive structures, modulators, electronic control and optical interconnects) on a single platform with nanometer-scale feature sizes. The development of photonic integrated circuits permits size, weight, power and cost reductions for spacecraft microprocessors, optical communication, processor buses, advanced data processing, and integrated optic science instrument optical systems, subsystems and components. This is particularly critical for small spacecraft platforms. We will give an overview of some NASA applications for integrated photonics.

  13. Electron-driven excitation of O 2 under night-time auroral conditions: Excited state densities and band emissions

    NASA Astrophysics Data System (ADS)

    Jones, D. B.; Campbell, L.; Bottema, M. J.; Teubner, P. J. O.; Cartwright, D. C.; Newell, W. R.; Brunger, M. J.

    2006-01-01

    Electron impact excitation of vibrational levels in the ground electronic state and seven excited electronic states in O 2 have been simulated for an International Brightness Coefficient-Category 2+ (IBC II+) night-time aurora, in order to predict O 2 excited state number densities and volume emission rates (VERs). These number densities and VERs are determined as a function of altitude (in the range 80-350 km) in the present study. Recent electron impact excitation cross-sections for O 2 were combined with appropriate altitude dependent IBC II+ auroral secondary electron distributions and the vibrational populations of the eight O 2 electronic states were determined under conditions of statistical equilibrium. Pre-dissociation, atmospheric chemistry involving atomic and molecular oxygen, radiative decay and quenching of excited states were included in this study. This model predicts relatively high number densities for the X3Σg-(v'⩽4),a1Δandb1Σg+ metastable electronic states and could represent a significant source of stored energy in O 2* for subsequent thermospheric chemical reactions. Particular attention is directed towards the emission intensities of the infrared (IR) atmospheric (1.27 μm), Atmospheric (0.76 μm) and the atomic oxygen 1S→ 1D transition (5577 Å) lines and the role of electron-driven processes in their origin. Aircraft, rocket and satellite observations have shown both the IR atmospheric and Atmospheric lines are dramatically enhanced under auroral conditions and, where possible, we compare our results to these measurements. Our calculated 5577 Å intensity is found to be in good agreement with values independently measured for a medium strength IBC II+ aurora.

  14. Multiple photon emission in heavy particle decays

    NASA Technical Reports Server (NTRS)

    Asakimori, K.; Burnett, T. H.; Cherry, M. L.; Christl, M. J.; Dake, S.; Derrickson, J. H.; Fountain, W. F.; Fuki, M.; Gregory, J. C.; Hayashi, T.

    1994-01-01

    Cosmic ray interactions, at energies above 1 TeV/nucleon, in emulsion chambers flown on high altitude balloons have yielded two events showing apparent decays of a heavy particle into one charged particle and four photons. The photons converted into electron pairs very close to the decay vertex. Attempts to explain this decay topology with known particle decays are presented. Unless both events represent a b yields u transition, which is statistically unlikely, then other known decay modes for charmed or bottom particles do not account satisfactorily for these observations. This could indicate, possibly, a new decay channel.

  15. Progress in neuromorphic photonics

    NASA Astrophysics Data System (ADS)

    Ferreira de Lima, Thomas; Shastri, Bhavin J.; Tait, Alexander N.; Nahmias, Mitchell A.; Prucnal, Paul R.

    2017-03-01

    As society's appetite for information continues to grow, so does our need to process this information with increasing speed and versatility. Many believe that the one-size-fits-all solution of digital electronics is becoming a limiting factor in certain areas such as data links, cognitive radio, and ultrafast control. Analog photonic devices have found relatively simple signal processing niches where electronics can no longer provide sufficient speed and reconfigurability. Recently, the landscape for commercially manufacturable photonic chips has been changing rapidly and now promises to achieve economies of scale previously enjoyed solely by microelectronics. By bridging the mathematical prowess of artificial neural networks to the underlying physics of optoelectronic devices, neuromorphic photonics could breach new domains of information processing demanding significant complexity, low cost, and unmatched speed. In this article, we review the progress in neuromorphic photonics, focusing on photonic integrated devices. The challenges and design rules for optoelectronic instantiation of artificial neurons are presented. The proposed photonic architecture revolves around the processing network node composed of two parts: a nonlinear element and a network interface. We then survey excitable lasers in the recent literature as candidates for the nonlinear node and microring-resonator weight banks as the network interface. Finally, we compare metrics between neuromorphic electronics and neuromorphic photonics and discuss potential applications.

  16. Selective two-photon absorption in carbon dots: a piece of the photoluminescence emission puzzle.

    PubMed

    Santos, Carla I M; Mariz, Inês F A; Pinto, Sandra N; Gonçalves, Gil; Bdikin, Igor; Marques, Paula A A P; Neves, Maria Graça P M S; Martinho, José M G; Maçôas, Ermelinda M S

    2018-06-22

    Carbon nanodots (Cdots) are now emerging as promising nonlinear fluorophores for applications in biological environments. A thorough and systematic approach to the two-photon induced emission of Cdots that could provide design guidelines to control their nonlinear emission properties is still missing. In this work, we address the nonlinear optical spectroscopy of Cdots prepared by controlled chemical cutting of graphene oxide (GO). The two-photon absorption in the 700-1000 nm region and the corresponding emission spectrum are carefully investigated. The highest two-photon absorption cross-section estimated was 130 GM at 720 nm. This value is comparable with the one reported for graphene nanoribbons with push-pull architecture. The emission spectrum depends on the excitation mode. At the same excitation energy, nonlinear excitation results in excitation-wavelength independent emission, while upon linear excitation the emission is excitation-wavelength dependent. The biphotonic interaction seems to be selective towards sp2 clusters bearing electron donor and acceptor groups found in push-pull architectures. Both linear and nonlinear emission can be understood based on the existence of isolated sp2 clusters involved in π-π stacking interactions with clusters in adjacent layers.

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

    PubMed

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

    2017-12-13

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

  18. Rydberg interaction induced enhanced excitation in thermal atomic vapor.

    PubMed

    Kara, Dushmanta; Bhowmick, Arup; Mohapatra, Ashok K

    2018-03-27

    We present the experimental demonstration of interaction induced enhancement in Rydberg excitation or Rydberg anti-blockade in thermal atomic vapor. We have used optical heterodyne detection technique to measure Rydberg population due to two-photon excitation to the Rydberg state. The anti-blockade peak which doesn't satisfy the two-photon resonant condition is observed along with the usual two-photon resonant peak which can't be explained using the model with non-interacting three-level atomic system. A model involving two interacting atoms is formulated for thermal atomic vapor using the dressed states of three-level atomic system to explain the experimental observations. A non-linear dependence of vapor density is observed for the anti-blockade peak which also increases with increase in principal quantum number of the Rydberg state. A good agreement is found between the experimental observations and the proposed interacting model. Our result implies possible applications towards quantum logic gates using Rydberg anti-blockade in thermal atomic vapor.

  19. UV-visible-NIR light generation through frequency upconversion in Tm3+-doped low silica calcium aluminosilicate glasses using multiple excitation around 1.2 μm

    NASA Astrophysics Data System (ADS)

    Trindade, C. M.; Rego-Filho, F. G.; Astrath, N. G. C.; Jacinto, C.; Gouveia-Neto, A. S.

    2018-04-01

    Intense ultraviolet upconversion emission was produced in single Tm3+-doped OH--free low silica calcium aluminosilicate glasses. A new excitation route based upon multi-Stokes Raman emissions generated in an optical fiber pumped at 1.064 μm, and exploiting the absorption band around 1.2 μm by means of the 3H5 thulium excited state, was used. Furthermore, the other bands of the stimulated Raman scattering spectrum resonantly enhances all the upconversion processes, resulting in efficient ultraviolet (295 nm, 360 nm), blue (456 nm, 480 nm), red (650 nm, 667 nm), and near-infrared (800 nm) emissions. The population of the 1P0, 1D2, 1G4, 3F2 and 3H4 excited-state emitting levels was accomplished through stepwise multi-photon absorption. Results indicate competing cross-relaxation processes involving Tm3+ ion-pairs producing UV emission population quenching Simplified energy-level diagram of Tm3+- doped sample excited using multi-stokes emissions. The λp indication describes all excitation wavelengths, represented by a single arrow for the sake of simplicity.

  20. Excitation of propagating surface plasmons with a scanning tunnelling microscope.

    PubMed

    Wang, T; Boer-Duchemin, E; Zhang, Y; Comtet, G; Dujardin, G

    2011-04-29

    Inelastic electron tunnelling excitation of propagating surface plasmon polaritons (SPPs) on a thin gold film is demonstrated. This is done by combining a scanning tunnelling microscope (STM) with an inverted optical microscope. Analysis of the leakage radiation in both the image and Fourier planes unambiguously shows that the majority (up to 99.5%) of the detected photons originate from propagating SPPs with propagation lengths of the order of 10  µm. The remaining photon emission is localized under the STM tip and is attributed to a tip-gold film coupled plasmon resonance as evidenced by the bimodal spectral distribution and enhanced emission intensity observed using a silver STM tip for excitation.

  1. Ultrafast Dynamics of 1,3-Cyclohexadiene in Highly Excited States

    DOE PAGES

    Bühler, Christine C.; Minitti, Michael P.; Deb, Sanghamitra; ...

    2011-01-01

    The ultrafast dynamics of 1,3-cyclohexadiene has been investigated via structurally sensitive Rydberg electron binding energies and shown to differ upon excitation to the 1B state and the 3p Rydberg state. Excitation of the molecule with 4.63 eV photons into the ultrashort-lived 1B state yields the well-known ring opening to 1,3,5-hexatriene, while a 5.99 eV photon lifts the molecule directly into the 3p-Rydberg state. Excitation to 3p does not induce ring opening. In both experiments, time-dependent shifts of the Rydberg electron binding energy reflect the structural dynamics of the molecular core. Structural distortions associated with 3p-excitation cause a dynamical shift in the -more » and -binding energies by 10 and 26 meV/ps, respectively, whereas after excitation into 1B, more severe structural transformations along the ring-opening coordinate produce shifts at a rate of 40 to 60 meV/ps. The experiment validates photoionization-photoelectron spectroscopy via Rydberg states as a powerful technique to observe structural dynamics of polyatomic molecules.« less

  2. Radiating dipoles in photonic crystals

    PubMed

    Busch; Vats; John; Sanders

    2000-09-01

    The radiation dynamics of a dipole antenna embedded in a photonic crystal are modeled by an initially excited harmonic oscillator coupled to a non-Markovian bath of harmonic oscillators representing the colored electromagnetic vacuum within the crystal. Realistic coupling constants based on the natural modes of the photonic crystal, i.e., Bloch waves and their associated dispersion relation, are derived. For simple model systems, well-known results such as decay times and emission spectra are reproduced. This approach enables direct incorporation of realistic band structure computations into studies of radiative emission from atoms and molecules within photonic crystals. We therefore provide a predictive and interpretative tool for experiments in both the microwave and optical regimes.

  3. Efficient room-temperature source of polarized single photons

    DOEpatents

    Lukishova, Svetlana G.; Boyd, Robert W.; Stroud, Carlos R.

    2007-08-07

    An efficient technique for producing deterministically polarized single photons uses liquid-crystal hosts of either monomeric or oligomeric/polymeric form to preferentially align the single emitters for maximum excitation efficiency. Deterministic molecular alignment also provides deterministically polarized output photons; using planar-aligned cholesteric liquid crystal hosts as 1-D photonic-band-gap microcavities tunable to the emitter fluorescence band to increase source efficiency, using liquid crystal technology to prevent emitter bleaching. Emitters comprise soluble dyes, inorganic nanocrystals or trivalent rare-earth chelates.

  4. Fabrication of self-assembled photonic-crystal structures by centrifugation and spin coating

    NASA Astrophysics Data System (ADS)

    Xu, Yan; Schneider, Garrett J.; Wetzel, Eric D.; Prather, Dennis W.

    2003-11-01

    We have developed a simple, low-cost process for the fabrication of high-quality three-dimensional artificial-opal and inverse-opal photonic crystals. The process is based on the self-assembly of a template from a uniform suspension of polystyrene microspheres, which is sintered for added strength and subsequently back-filled with high-index material. The template formation is assisted by a combination of centrifugation and spin-annealing, which requires relatively short process times and inexpensive laboratory equipment. The process has been used to fabricate polycrystalline photonic crystals with photonic stop gaps in the mid-IR portion of the spectrum. Details of the fabrication process and fabricated samples will be presented. In addition, Fourier-transform IR reflection spectroscopy has been used to characterize the samples; the results are shown to be in excellent agreement with band structure diffraction calculations.

  5. Quantum Nonlinear Optics without real Photons

    NASA Astrophysics Data System (ADS)

    Macrí, Vincenzo; Frisk Kockum, Anton; Stassi, Roberto; di Stefano, Omar; Savasta, Salvatore; Nori, Franco

    We propose a physical process analogous to spontaneous parametric down-conversion, where one excited atom directly transfers its excitation to a couple of spatially-separated atoms with probability approaching one. The interaction is mediated by the exchange of virtual, rather than real, photons. This nonlinear optical process is coherent and reversible, so that the two excited atoms can transfer back the excitation to the first one: the atomic analogue of sum-frequency generation. The parameters used here correspond to experimentally-demonstrated values in circuit QED. This approach can be extended to consider other nonlinear interatomic processes, e.g. four-qubit mixing, and is an attractive architecture for the realization of quantum devices on a chip. Univ. of Michigan, USA.

  6. Access to long-term optical memories using photon echoes retrieved from electron spins in semiconductor quantum wells

    NASA Astrophysics Data System (ADS)

    Poltavtsev, S. V.; Langer, L.; Yugova, I. A.; Salewski, M.; Kapitonov, Y. V.; Yakovlev, D. R.; Karczewski, G.; Wojtowicz, T.; Akimov, I. A.; Bayer, M.

    2016-10-01

    We use spontaneous (two-pulse) and stimulated (three-pulse) photon echoes for studying the coherent evolution of optically excited ensemble of trions which are localized in semiconductor CdTe/CdMgTe quantum well. Application of transverse magnetic field leads to the Larmor precession of the resident electron spins, which shuffles optically induced polarization between optically accessible and inaccessible states. This results in several spectacular phenomena. First, magnetic field induces oscillations of spontaneous photon echo amplitude. Second, in three-pulse excitation scheme, the photon echo decay is extended by several orders of magnitude. In this study, short-lived optical excitation which is created by the first pulse is coherently transferred into a long-lived electron spin state using the second optical pulse. This coherent spin state of electron ensemble persists much longer than any optical excitation in the system, preserving information on initial optical field, which can be retrieved as a photon echo by means of third optical pulse.

  7. High-Efficiency Solar Cells Using Photonic-Bandgap Materials

    NASA Technical Reports Server (NTRS)

    Dowling, Jonathan; Lee, Hwang

    2005-01-01

    Solar photovoltaic cells would be designed to exploit photonic-bandgap (PBG) materials to enhance their energy-conversion efficiencies, according to a proposal. Whereas the energy-conversion efficiencies of currently available solar cells are typically less than 30 percent, it has been estimated that the energy-conversion efficiencies of the proposed cells could be about 50 percent or possibly even greater. The primary source of inefficiency of a currently available solar cell is the mismatch between the narrow wavelength band associated with the semiconductor energy gap (the bandgap) and the broad wavelength band of solar radiation. This mismatch results in loss of power from both (1) long-wavelength photons, defined here as photons that do not have enough energy to excite electron-hole pairs across the bandgap, and (2) short-wavelength photons, defined here as photons that excite electron- hole pairs with energies much above the bandgap. It follows that a large increase in efficiency could be obtained if a large portion of the incident solar energy could be funneled into a narrow wavelength band corresponding to the bandgap. In the proposed approach, such funneling would be effected by use of PBG materials as intermediaries between the Sun and photovoltaic cells.

  8. Light-Harvesting Organic Nanocrystals Capable of Photon Upconversion.

    PubMed

    Li, Li; Zeng, Yi; Yu, Tianjun; Chen, Jinping; Yang, Guoqiang; Li, Yi

    2017-11-23

    Harvesting and converting low energy photons into higher ones through upconversion have great potential in solar energy conversion. A light-harvesting nanocrystal assembled from 9,10-distyrylanthracene and palladium(II) meso-tetraphenyltetrabenzoporphyrin as the acceptor and the sensitizer, respectively effects red-to-green upconversion under incoherent excitation of low power density. An upconversion quantum yield of 0.29±0.02 % is obtained upon excitation with 640 nm laser of 120 mW cm -2 . The well-organized packing of acceptor molecules with aggregation-induced emission in the nanocrystals dramatically reduces the nonradiative decay of the excited acceptor, benefits the triplet-triplet annihilation (TTA) upconversion and guides the consequent upconverted emission. This work provides a straightforward strategy to develop light-harvesting nanocrystals based on TTA upconversion, which is attractive for energy conversion and photonic applications. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  9. Design and Calibration of a Dispersive Imaging Spectrometer Adaptor for a Fast IR Camera on NSTX-U

    NASA Astrophysics Data System (ADS)

    Reksoatmodjo, Richard; Gray, Travis; Princeton Plasma Physics Laboratory Team

    2017-10-01

    A dispersive spectrometer adaptor was designed, constructed and calibrated for use on a fast infrared camera employed to measure temperatures on the lower divertor tiles of the NSTX-U tokamak. This adaptor efficiently and evenly filters and distributes long-wavelength infrared photons between 8.0 and 12.0 microns across the 128x128 pixel detector of the fast IR camera. By determining the width of these separated wavelength bands across the camera detector, and then determining the corresponding average photon count for each photon wavelength, a very accurate measurement of the temperature, and thus heat flux, of the divertor tiles can be calculated using Plank's law. This approach of designing an exterior dispersive adaptor for the fast IR camera allows accurate temperature measurements to be made of materials with unknown emissivity. Further, the relative simplicity and affordability of this adaptor design provides an attractive option over more expensive, slower, dispersive IR camera systems. This work was made possible by funding from the Department of Energy for the Summer Undergraduate Laboratory Internship (SULI) program. This work is supported by the US DOE Contract No. DE-AC02-09CH11466.

  10. IR and visible luminescence studies in the infrared multiphoton dissociation of 1,2-dibromo-1,1-difluoroethane

    NASA Astrophysics Data System (ADS)

    Pushpa, K. K.; Kumar, Awadhesh; Vatsa, R. K.; Naik, P. D.; Annaji Rao, K.; Mittal, J. P.; Parthasarathy, V.; Sarkar, S. K.

    1995-07-01

    The infrared multiphoton dissociation of 1,2-dibromo-1,1-difluoroethane gives rise to IR and visible luminescence. Vibrationally excited parent molecules dissociate via two primary channels yielding bromine and vibrationally excited HBr. The strong visible emission observed between 350 to 750 nm has been assigned to electronically excited carbene CF 2Br CH.

  11. Optically Pumped Atomic Rubidium Lasers: Two-Photon and Exciplex Excitation Mechanisms

    DTIC Science & Technology

    2013-06-01

    gain is very high with photon build-up times of 1−3.7 ns. Laser induced heating and subsequent condensation of alkali vapor in the heat pipe...encouragement during our time in classes, and recommendations while in the lab were invaluable. Finally, I want to thank the High Energy Laser Joint...intensity. The more non-traditional method is to use a single laser pulse to sketch out all needed energies. A photon build-up time was determined from

  12. Influence of primary fragment excitation energy and spin distributions on fission observables

    NASA Astrophysics Data System (ADS)

    Litaize, Olivier; Thulliez, Loïc; Serot, Olivier; Chebboubi, Abdelaziz; Tamagno, Pierre

    2018-03-01

    Fission observables in the case of 252Cf(sf) are investigated by exploring several models involved in the excitation energy sharing and spin-parity assignment between primary fission fragments. In a first step the parameters used in the FIFRELIN Monte Carlo code "reference route" are presented: two parameters for the mass dependent temperature ratio law and two constant spin cut-off parameters for light and heavy fragment groups respectively. These parameters determine the initial fragment entry zone in excitation energy and spin-parity (E*, Jπ). They are chosen to reproduce the light and heavy average prompt neutron multiplicities. When these target observables are achieved all other fission observables can be predicted. We show here the influence of input parameters on the saw-tooth curve and we discuss the influence of a mass and energy-dependent spin cut-off model on gamma-rays related fission observables. The part of the model involving level densities, neutron transmission coefficients or photon strength functions remains unchanged.

  13. High-resolution two-photon spectroscopy of a 5 p56 p ←5 p6 transition of xenon

    NASA Astrophysics Data System (ADS)

    Altiere, Emily; Miller, Eric R.; Hayamizu, Tomohiro; Jones, David J.; Madison, Kirk W.; Momose, Takamasa

    2018-01-01

    We report high-resolution Doppler-free two-photon excitation spectroscopy of Xe from the ground state to the 5 p5(P 3 /2 2 ) 6 p [3 /2 ] 2 2 electronic excited state. This is a first step to developing a comagnetometer using polarized 129Xe atoms for planned neutron electric dipole moment measurements at TRIUMF. Narrow linewidth radiation at 252.5 nm produced by a continuous wave laser was built up in an optical cavity to excite the two-photon transition, and the near-infrared emission from the 5 p56 p excited state to the 5 p56 s intermediate electronic state was used to detect the two-photon transition. Hyperfine constants and isotope shift parameters were evaluated and compared with previously reported values. In addition, the detected photon count rate was estimated from the observed intensities.

  14. Correlating two-photon excited fluorescence imaging of breast cancer cellular redox state with seahorse flux analysis of normalized cellular oxygen consumption

    NASA Astrophysics Data System (ADS)

    Hou, Jue; Wright, Heather J.; Chan, Nicole; Tran, Richard; Razorenova, Olga V.; Potma, Eric O.; Tromberg, Bruce J.

    2016-06-01

    Two-photon excited fluorescence (TPEF) imaging of the cellular cofactors nicotinamide adenine dinucleotide and oxidized flavin adenine dinucleotide is widely used to measure cellular metabolism, both in normal and pathological cells and tissues. When dual-wavelength excitation is used, ratiometric TPEF imaging of the intrinsic cofactor fluorescence provides a metabolic index of cells-the "optical redox ratio" (ORR). With increased interest in understanding and controlling cellular metabolism in cancer, there is a need to evaluate the performance of ORR in malignant cells. We compare TPEF metabolic imaging with seahorse flux analysis of cellular oxygen consumption in two different breast cancer cell lines (MCF-7 and MDA-MB-231). We monitor metabolic index in living cells under both normal culture conditions and, for MCF-7, in response to cell respiration inhibitors and uncouplers. We observe a significant correlation between the TPEF-derived ORR and the flux analyzer measurements (R=0.7901, p<0.001). Our results confirm that the ORR is a valid dynamic index of cell metabolism under a range of oxygen consumption conditions relevant for cancer imaging.

  15. Development of the Nano-HEB Array for Low-Background Far-IR Applications

    NASA Technical Reports Server (NTRS)

    Karasik, Boris S.; Pereverzev, Sergey V.; Olaya, David; Gershenson, Michael E.; Cantor, Robin; Kawamura, Jonathan H.; Day, Peter K.; Bumble, Bruce; LeDuc, Henry G.; Monacos, Steve P.; hide

    2010-01-01

    We present an overview of the recent progress made in the development of a far-IR array of ultrasensitive hot-electronnanobolometers (nano-HEB) made from thin titanium (Ti) films. We studied electrical noise, signal and noisebandwidth, single-photon detection, optical noise equivalent power (NEP), and a microwave SQUID (MSQUID) basedfrequency domain multiplexing (FDM) scheme. The obtained results demonstrate the very low electrical NEP down to1.5x10-(sup 2)? W/Hz(sup 1)/(sup 2) at 50 mK determined by the dominating phonon noise. The NEP increases with temperature as T(sup 3)reaching 10-(sup 1)? W/Hz(sup 1)/(sup 2) at the device critical temperature TC = 330-360 mK. Optical NEP = 8.6x10-(sup 1)? W/Hz(sup 1)/(sup 2) at 357mK and 1.4x10-(sup 1)? W/Hz(sup 1)/(sup 2) at 100 mK respectively, agree with thermal and electrical data. The optical couplingefficiency provided by a planar antenna was greater than 50%. Single 8-?m photons have been detected for the first timeusing a nano-HEB operating at 50-200 mK thus demonstrating a potential of these detectors for future photon-countingapplications in mid-IR and far-IR. In order to accommodate the relatively high detector speed ( ?s at 300 mK, 100 ?sat 100 mK), an MSQUID based FDM multiplexed readout with GHz carrier frequencies has been built. Both the readoutnoise 2 pA/Hz(sup 1)/(sup 2) and the bandwidth > 150 kHz are suitable for nano-HEB detectors.

  16. Deterministic and storable single-photon source based on a quantum memory.

    PubMed

    Chen, Shuai; Chen, Yu-Ao; Strassel, Thorsten; Yuan, Zhen-Sheng; Zhao, Bo; Schmiedmayer, Jörg; Pan, Jian-Wei

    2006-10-27

    A single-photon source is realized with a cold atomic ensemble (87Rb atoms). A single excitation, written in an atomic quantum memory by Raman scattering of a laser pulse, is retrieved deterministically as a single photon at a predetermined time. It is shown that the production rate of single photons can be enhanced considerably by a feedback circuit while the single-photon quality is conserved. Such a single-photon source is well suited for future large-scale realization of quantum communication and linear optical quantum computation.

  17. Changing optical band structure with single photons

    NASA Astrophysics Data System (ADS)

    Albrecht, Andreas; Caneva, Tommaso; Chang, Darrick E.

    2017-11-01

    Achieving strong interactions between individual photons enables a wide variety of exciting possibilities in quantum information science and many-body physics. Cold atoms interfaced with nanophotonic structures have emerged as a platform to realize novel forms of nonlinear interactions. In particular, when atoms are coupled to a photonic crystal waveguide, long-range atomic interactions can arise that are mediated by localized atom-photon bound states. We theoretically show that in such a system, the absorption of a single photon can change the band structure for a subsequent photon. This occurs because the first photon affects the atoms in the chain in an alternating fashion, thus leading to an effective period doubling of the system and a new optical band structure for the composite atom-nanophotonic system. We demonstrate how this mechanism can be engineered to realize a single-photon switch, where the first incoming photon switches the system from being highly transmissive to highly reflective, and analyze how signatures can be observed via non-classical correlations of the outgoing photon field.

  18. Comprehensive investigation of the excited-state dynamics of push-pull triphenylamine dyes as models for photonic applications.

    PubMed

    Ishow, Eléna; Clavier, Gilles; Miomandre, Fabien; Rebarz, Mateusz; Buntinx, Guy; Poizat, Olivier

    2013-09-07

    A series of emitting push-pull triarylamine derivatives, models of their widely used homologues in photonics and organic electronics, was investigated by steady-state and time-resolved spectroscopy. Their structural originality stems from the sole change of the electron-withdrawing substituent X (-H: 1, -CN: 2, -NO2: 3, -CHC(CN)2: 4), giving rise to efficient emission tuning from blue to red upon increasing the X electron-withdrawing character. All compounds are highly fluorescent in alkanes. The more polar compounds 2-4 undergo considerable Stokes shift and emission quenching in polar solvents. Femtosecond transient absorption data allowed us to identify the nature of the emissive state which varies as a function of the compound and surrounding polarity. A long-lived ππ* excited state with weak charge transfer character was found for 1. This excited state evolves into a long-lived ICT state with red-shifted emission for 2 in polar solvents. For 3 and 4, the ICT state is directly populated in all solvents. Long-lived and emissive in n-hexane, it relaxes in toluene to a new ICT' conformation with stronger charge transfer character and enhanced Stokes shift. In more polar THF, ethanol, and nitrile solvents, ICT relaxes to a dark excited state ICT'' with viscosity-dependent kinetics (<10 ps). The ICT'' state lifetime drops with increasing solvent polarity (150 ps for 3 in THF, 8.5 ps in butyronitrile, 1.9 ps in acetonitrile), denoting an efficient radiationless deactivation to the ground state (back charge transfer). This result reveals a very small S0-S1 energy gap at the relaxed ICT'' geometry, with a possible close-lying S0-S1 conical intersection, which suggests that the ICT → ICT'' process results from a structural change involving a large-amplitude molecular distortion. This fast structural change can account for the strong fluorescence quenching observed for 3 and 4 in polar solvents. Finally, the magnitude of intersystem crossing between the singlet and

  19. Transient quantum coherent effects in the acetylene-filled hollow-core photonic crystal fiber

    NASA Astrophysics Data System (ADS)

    Stepanov, S.; Rodríguez Casillas, N.; Ocegueda Miramontes, M.; Hernández Hernández, E.

    2017-02-01

    Low-pressure acetylene in the hollow-core photonic crystal structure fibers is an excellent medium for the room-temperature investigation of the coherent quantum effects in communication wavelength region. Pulsed excitation enables observation of new coherent phenomena like optical nutation or photon echo and evaluation of important temporal characteristics of the light-molecule interactions. We also report original experimental results on the pulsed excitation of the electromagnetically induced transparency in co- and counter-propagation configurations.

  20. The triplet excited state of Bodipy: formation, modulation and application.

    PubMed

    Zhao, Jianzhang; Xu, Kejing; Yang, Wenbo; Wang, Zhijia; Zhong, Fangfang

    2015-12-21

    Boron dipyrromethene (Bodipy) is one of the most extensively investigated organic chromophores. Most of the investigations are focused on the singlet excited state of Bodipy, such as fluorescence. In stark contrast, the study of the triplet excited state of Bodipy is limited, but it is an emerging area, since the triplet state of Bodipy is tremendously important for several areas, such as the fundamental photochemistry study, photodynamic therapy (PDT), photocatalysis and triplet-triplet annihilation (TTA) upconversion. The recent developments in the study of the production, modulation and application of the triplet excited state of Bodipy are discussed in this review article. The formation of the triplet state of Bodipy upon photoexcitation, via the well known approach such as the heavy atom effect (including I, Br, Ru, Ir, etc.), and the new methods, such as using a spin converter (e.g. C60), charge recombination, exciton coupling and the doubly substituted excited state, are summarized. All the Bodipy-based triplet photosensitizers show strong absorption of visible or near IR light and the long-lived triplet excited state, which are important for the application of the triplet excited state in PDT or photocatalysis. Moreover, the methods for switching (or modulation) of the triplet excited state of Bodipy were discussed, such as those based on the photo-induced electron transfer (PET), by controlling the competing Förster-resonance-energy-transfer (FRET), or the intermolecular charge transfer (ICT). Controlling the triplet excited state will give functional molecules such as activatable PDT reagents or molecular devices. It is worth noting that switching of the singlet excited state and the triplet state of Bodipy may follow different principles. Application of the triplet excited state of Bodipy in PDT, hydrogen (H2) production, photoredox catalytic organic reactions and TTA upconversion were discussed. The challenges and the opportunities in these areas were