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Sample records for resonance-enhanced two-photon ionization

  1. Resonance-enhanced two-photon ionization of ions by Lyman alpha radiation in gaseous nebulae.

    PubMed

    Johansson, S; Letokhov, V

    2001-01-26

    One of the mysteries of nebulae in the vicinity of bright stars is the appearance of bright emission spectral lines of ions, which imply fairly high excitation temperatures. We suggest that an ion formation mechanism, based on resonance-enhanced two-photon ionization (RETPI) by intense H Lyman alpha radiation (wavelength of 1215 angstroms) trapped inside optically thick nebulae, can produce these spectral lines. The rate of such an ionization process is high enough for rarefied gaseous media where the recombination rate of the ions formed can be 10(-6) to 10(-8) per second for an electron density of 10(3) to 10(5) per cubic centimeter in the nebula. Under such conditions, the photo-ions formed may subsequently undergo further RETPI, catalyzed by intense He i and He ii radiation, which also gets enhanced in optically thick nebulae that contain enough helium. PMID:11158669

  2. Electron angular distribution in resonance-enhanced two-photon ionization of H{sub 2}{sup +} by ultrashort laser pulses

    SciTech Connect

    Selstoe, S.; Palacios, A.; Fernandez, J.; Martin, F.

    2007-03-15

    We present a theoretical study of the electron angular distribution produced in resonance enhanced two-photon ionization of the H{sub 2}{sup +} molecular ion using ultrashort laser pulses. The method consists in solving the time dependent Schroedinger equation and includes all electronic and vibrational degrees of freedom. Differential (in proton energy and electron emission solid angle) ionization probabilities have been evaluated for various photon energies, laser intensities, and pulse durations. We show that (1+1) resonance-enhanced multiphoton ionization (REMPI) leads to angular distributions significantly different from those produced in direct two-photon ionization. The REMPI process is observed even at photon energies not matching the energy difference between two electronic states in a perfect vertical transition. Interestingly, there is no trace of REMPI effects in the electron angular distribution when the fully differential probabilities are integrated over proton energy.

  3. Resonance-enhanced two-photon ionization mass spectroscopy of ephedrine: Indication for a state-selective fragmentation in a flexible molecule

    NASA Astrophysics Data System (ADS)

    Karaminkov, R.; Chervenkov, S.; Härter, P.; Neusser, H. J.

    2007-07-01

    The vibronic structure of the S 1 ← S 0 spectrum of ephedrine was measured by resonance-enhanced two-photon ionization spectroscopy with mass resolution under cold molecular beam conditions. The spectra recorded at four different mass channels, m/ z = 165 (parent), 58, and the hitherto unknown 71, 85 fragment ions show dissimilar vibronic fine structure and the observed mass pattern strongly depends on the selected intermediate vibrational state. This points to an intermediate state-selected process resulting in a different fragmentation mass pattern. Ab initio calculations at the MP2/6-311++G ∗∗ level demonstrate that the AG (a) conformer is more stable by 238 cm -1 than the next stable GG (a) conformer.

  4. High resolution UV resonance enhanced two-photon ionization spectroscopy with mass selection of biologically relevant molecules in the gas phase

    NASA Astrophysics Data System (ADS)

    Chervenkov, S.; Wang, P. Q.; Karaminkov, R.; Chakraborty, T.; Braun, Juergen E.; Neusser, Hans J.

    2005-04-01

    The high resolution Doppler-free resonance-enhanced two-photon ionization (R2PI) spectroscopy with mass selection of jet-cooled (2-12 K) molecular species is a powerful experimental method providing comprehensive information on both isolated molecules and molecular clusters. We have demonstrated for the first time that this technique can be applied to large molecules and provides detailed information on their conformational structure. It allows rotationally resolved (FWHM = 70 MHz) spectra of the vibronic bands of the S1<--S0 electronic transition of the studied molecular systems to be measured. A specially designed computer-assisted fitting routine based on genetic algorithms is used to determine their rotational constants in the ground and excited electronic states, respectively, and the transition moment ratio. To interpret the experimental information and to discriminate and unambiguously assign the observed approach to the study of the neurotransmitter molecule, ephedrine. The results elucidate the role of the intramolecular hydrogen bonds stabilizing the respective conformations and affecting their intrinsic properties.

  5. Single protein sensing with asymmetric plasmonic hexamer via Fano resonance enhanced two-photon luminescence

    NASA Astrophysics Data System (ADS)

    Deng, Hai-Dong; Chen, Xing-Yu; Xu, Yi; Miroshnichenko, Andrey E.

    2015-12-01

    Fano resonances in plasmonic systems have been proved to facilitate various sensing applications in the nanoscale. In this work, we propose an experimental scheme to realize a single protein sensing by utilizing its two-photon luminescence enhanced by a plasmonic Fano resonance system. The asymmetric gold hexamer supporting polarization-dependent Fano resonances and plasmonic modes without in-plane rotational symmetry is used as a referenced spatial coordinate for bio-sensing. We demonstrate via the full-vectorial three-dimensional simulation that the moving direction and the spatial location of a protein can be detected via its two-photon luminescence, which benefits from the resonant near-field interaction with the electromagnetic hot-spots. The sensitivity to changes in position of our method is substantially better compared with the conventional linear sensing approach. Our strategy would facilitate the sensing, tracking and imaging of a single biomolecule in deep sub-wavelength scale and with a small optical extinction cross-section.Fano resonances in plasmonic systems have been proved to facilitate various sensing applications in the nanoscale. In this work, we propose an experimental scheme to realize a single protein sensing by utilizing its two-photon luminescence enhanced by a plasmonic Fano resonance system. The asymmetric gold hexamer supporting polarization-dependent Fano resonances and plasmonic modes without in-plane rotational symmetry is used as a referenced spatial coordinate for bio-sensing. We demonstrate via the full-vectorial three-dimensional simulation that the moving direction and the spatial location of a protein can be detected via its two-photon luminescence, which benefits from the resonant near-field interaction with the electromagnetic hot-spots. The sensitivity to changes in position of our method is substantially better compared with the conventional linear sensing approach. Our strategy would facilitate the sensing, tracking and

  6. Single protein sensing with asymmetric plasmonic hexamer via Fano resonance enhanced two-photon luminescence.

    PubMed

    Deng, Hai-Dong; Chen, Xing-Yu; Xu, Yi; Miroshnichenko, Andrey E

    2015-12-28

    Fano resonances in plasmonic systems have been proved to facilitate various sensing applications in the nanoscale. In this work, we propose an experimental scheme to realize a single protein sensing by utilizing its two-photon luminescence enhanced by a plasmonic Fano resonance system. The asymmetric gold hexamer supporting polarization-dependent Fano resonances and plasmonic modes without in-plane rotational symmetry is used as a referenced spatial coordinate for bio-sensing. We demonstrate via the full-vectorial three-dimensional simulation that the moving direction and the spatial location of a protein can be detected via its two-photon luminescence, which benefits from the resonant near-field interaction with the electromagnetic hot-spots. The sensitivity to changes in position of our method is substantially better compared with the conventional linear sensing approach. Our strategy would facilitate the sensing, tracking and imaging of a single biomolecule in deep sub-wavelength scale and with a small optical extinction cross-section.

  7. Angular distributions for two-photon double ionization of lithium

    NASA Astrophysics Data System (ADS)

    Armstrong, G. S. J.; Colgan, J.

    2012-08-01

    We present angular distributions for two-photon double ionization of lithium at photon energies of 50 eV (λ = 25 nm) and 59 eV (λ = 21 nm). The results are obtained from full-dimensional solution of the two-active-electron time-dependent Schrödinger equation using the time-dependent close-coupling method. We investigate two different double ionization mechanisms. First, we consider direct double ionization of the Li ground state following the absorption of two photons. Secondly, we consider an initial photoexcitation of the 1s2s2p doubly excited state, followed by photoionization of the 2s and 2p electrons. We find significant differences between the angular distributions obtained for these two distinct processes. We also compare the characteristics of the angular distributions for Li with those of other two-electron atoms.

  8. Time-resolved view on charge-resonance-enhanced ionization

    SciTech Connect

    Takemoto, Norio; Becker, Andreas

    2011-08-15

    We theoretically investigate the electronic dynamics in the hydrogen molecular ion at fixed intermediate internuclear distances in two-dimensional space for the electron in a linearly polarized laser field. Our results of numerical simulations confirm the predictions of multiple bursts of ionization within a half cycle of the laser field oscillation as recently reported for one-dimensional models. Based on the analysis of the Floquet states for a two-state model of the molecular ion, we discuss the relation of the multiple ionization bursts to the so-called charge-resonance-enhanced ionization phenomenon and the momentum gates.

  9. Direct two-photon double ionization of H2

    NASA Astrophysics Data System (ADS)

    Simonsen, A. S.; Sørngård, S. A.; Nepstad, R.; Førre, M.

    2012-06-01

    We have studied the process of direct (nonsequential) two-photon double ionization of molecular hydrogen (H2). Solving the time-dependent Schrödinger equation by an ab initio method, total (generalized) and single-differential cross sections are obtained at photon energies from 26 to 33 eV. Both parallel and perpendicular orientation of the molecule with respect to the laser polarization direction are considered, and the results are compared with previously calculated cross sections at 30 eV, as well as the predictions of a simple model.

  10. Experimental Resonance Enhanced Multiphoton Ionization (REMPI) studies of small molecules

    NASA Technical Reports Server (NTRS)

    Dehmer, J. L.; Dehmer, P. M.; Pratt, S. T.; Ohalloran, M. A.; Tomkins, F. S.

    1987-01-01

    Resonance enhanced multiphoton ionization (REMPI) utilizes tunable dye lasers to ionize an atom or molecule by first preparing an excited state by multiphoton absorption and then ionizing that state before it can decay. This process is highly selective with respect to both the initial and resonant intermediate states of the target, and it can be extremely sensitive. In addition, the products of the REMPI process can be detected as needed by analyzing the resulting electrons, ions, fluorescence, or by additional REMPI. This points to a number of exciting opportunities for both basic and applied science. On the applied side, REMPI has great potential as an ultrasensitive, highly selective detector for trace, reactive, or transient species. On the basic side, REMPI affords an unprecedented means of exploring excited state physics and chemistry at the quantum-state-specific level. An overview of current studies of excited molecular states is given to illustrate the principles and prospects of REMPI.

  11. Plasma induced by resonance enhanced multiphoton ionization in inert gas

    SciTech Connect

    Shneider, Mikhail N.; Zhang Zhili; Miles, Richard B.

    2007-12-15

    We present a detailed model for the evolution of resonance enhanced multiphoton ionization (REMPI) produced plasma during and after the ionizing laser pulse in inert gas (argon, as an example) at arbitrary pressures. Our theory includes the complete process of the REMPI plasma generation and losses, together with the changing gas thermodynamic parameters. The model shows that the plasma expansion follows a classical ambipolar diffusion and that gas heating results in a weak shock or acoustic wave. The gas becomes involved in the motion not only from the pressure gradient due to the heating, but also from the momentum transfer from the charged particles to gas atoms. The time dependence of the total number of electrons computed in theory matches closely with the results of coherent microwave scattering experiments.

  12. Rotationally resolved nonresonant two-photon ionization of SH

    SciTech Connect

    Hsu, C.; Baldwin, D.P.; Liao, C.; Ng, C.Y. Department of Chemistry, Iowa State University, Ames, Iowa 50011 )

    1994-06-01

    The threshold photoelectron (PE) spectrum for nascent SH formed in the ultraviolet photodissociation of H[sub 2]S has been measured using the nonresonant two-photon pulsed field ionization (N2P-PFI) technique. The rotationally resolved N2P-PFI-PE spectrum of SH indicates that photoionization dynamics favor the rotational angular momentum change [Delta][ital N][le]0 with the [Delta][ital N] values up to [minus]3, an observation similar to that found in the PFI-PE spectra of OH (OD) and NO. The ionization energy for SH([ital X] [sup 2][Pi][sub 3/2]) is determined to be 84 057.5 [plus minus] 3 cm[sup [minus]1] (10.4219 [plus minus] 0.0004 eV). The spin--orbit splitting for SH([ital X] [sup 2][Pi][sub 3/2,1/2]) is 377 [plus minus] 2 cm[sup [minus]1], in agreement with the literature value. This study illustrates that the PFI-PE detection method can be a sensitive probe for the nascent internal energy distribution of photoproducts.

  13. Simultaneous resonant enhanced multiphoton ionization and electron avalanche ionization in gas mixtures

    SciTech Connect

    Shneider, Mikhail N.; Zhang Zhili; Miles, Richard B.

    2008-07-15

    Resonant enhanced multiphoton ionization (REMPI) and electron avalanche ionization (EAI) are measured simultaneously in Ar:Xe mixtures at different partial pressures of mixture components. A simple theory for combined REMPI+EAI in gas mixture is developed. It is shown that the REMPI electrons seed the avalanche process, and thus the avalanche process amplifies the REMPI signal. Possible applications are discussed.

  14. Resonance-enhanced multiphoton ionization of CH₂Br₂: Rydberg states, photofragmentation, and CH spectra.

    PubMed

    Long, Jingming; Wang, Huasheng; Kvaran, Ágúst

    2014-03-13

    Mass-resolved (2 + n) resonance-enhanced multiphoton ionization (REMPI) spectra of CH2Br2 in the two-photon resonance excitation region from 71 200 to 82 300 cm(-1) were recorded and analyzed. Spectral structures allowed characterization of new molecular Rydberg states. C*((1)D2) was found to be an important intermediate in the photodissociation processes. A broad spectral feature peaking at about 80 663 cm(-1) in the C(+) spectrum and frequently seen in related studies is reinterpreted and associated with switching between three- and two-photon ionization of C*((1)D2). Analysis of band structures due to transitions from the A(2)Δ state of CH* that were seen in the CH(+) and C(+) REMPI spectra allowed characterization of three electronic states of CH, assigned as E(2)Π, D(2)Π, and F(2)Σ(+), which clarifies a long-term puzzle concerning the energetics of the CH radical. Predissociation of the E, D, and F states to form C*((1)D2) occurs. Bromine atomic lines were observed and are believed to be associated with bromine atom formation via predissociation of CH2Br2 Rydberg states.

  15. Competition between two-photon-resonant three-photon ionization and four-wave mixing in Xe

    SciTech Connect

    Nagai, Hidekazu; Nakanaga, Taisuke

    2011-12-15

    Competitive inhibition of a resonance enhanced multiphoton ionization process by a resonant four-wave mixing has been observed in Xe atoms. When an intense IR (1064 nm) laser was applied to a sample of Xe which was also being irradiated by a UV laser tuned to the two-photon absorption line of Xe, the two-photon-resonant three-photon ionization signals decreased with increasing IR laser power. This phenomenon is dependent on the resonant states of Xe and the polarization of the two laser beams. Three 6s excited states [5/2]{sub 2}, [3/2]{sub 2}, and [1/2]{sub 0} were examined. At the [1/2]{sub 0} resonant state, the ion signals were not decreased but slightly increased with the increase of the IR laser power. No suppression of the ion signal was observed at the [5/2]{sub 2} resonant state, when the polarization directions of the lasers were perpendicular to each other. The result of the polarization dependence reflects the selection rules of four-wave mixing. A simple rate equation analysis including the contribution of two-photon ionization from the [1/2]{sub 0} state by the IR laser well represents the IR laser-power dependence of the ion signal.

  16. Photofragmentation, state interaction, and energetics of Rydberg and ion-pair states: Resonance enhanced multiphoton ionization of HI

    SciTech Connect

    Hróðmarsson, Helgi Rafn; Wang, Huasheng; Kvaran, Ágúst

    2014-06-28

    Mass resolved resonance enhanced multiphoton ionization data for hydrogen iodide (HI), for two-photon resonance excitation to Rydberg and ion-pair states in the 69 600–72 400 cm{sup −1} region were recorded and analyzed. Spectral perturbations due to homogeneous and heterogeneous interactions between Rydberg and ion-pair states, showing as deformations in line-positions, line-intensities, and line-widths, were focused on. Parameters relevant to photodissociation processes, state interaction strengths and spectroscopic parameters for deperturbed states were derived. Overall interaction and dynamical schemes to describe the observations are proposed.

  17. (2+1) resonance-enhanced multiphoton ionization-photoelectron spectroscopy of the OH radical

    NASA Astrophysics Data System (ADS)

    de Beer, Esther; Koopmans, M. P.; de Lange, C. A.; Wang, Yumin; Chupka, W. A.

    1991-06-01

    A (2+1) resonance-enhanced multiphoton ionization-photoelectron spectroscopy (REMPIPES) study of the OH radical is carried out in the two-photon energy region between 81,300 and 88,900/cm, using a frequency-doubled excimer-pumped dye laser with a pulse width of about 10 ns at a repetition rate of 30 Hz. The laser output was focused into the ionization region of a 'magnetic bottle' spectrometer. The known D 2Sigma(-) (v-prime = 0-2) and the hitherto unobserved 3 2Sigma(-) (v-prime = 0) intermediate states in this region are shown to possess a predominant Rydberg character. Spectrum physical parameters are derived for these states from the rotational structure in the REMPI spectrum. The observed new state is demonstrated to be in excellent agreement with a previous calculation. Theory also predicts that the repulsive 2 2Pi state diabatically crosses the potential curves of the ns-sigma and np-sigma Rydberg states, with the effect that significant heterogeneous predissociation might be expected.

  18. Effects of autoionizing states on two-photon double ionization of the H2 molecule

    NASA Astrophysics Data System (ADS)

    Guan, Xiaoxu; Bartschat, Klaus; Koesterke, Lars; Schneider, Barry I.

    2014-04-01

    We report angle-resolved and angle-integrated cross sections for two-photon double-ionization of H by a strong laser pulse. The effect of doubly excited states on the predicted cross sections is addressed.

  19. Two photon double ionization of H2 using exterior complex scaling

    NASA Astrophysics Data System (ADS)

    Morales, F.; Martín, F.; Horner, D. A.; Rescigno, T. N.; McCurdy, C. W.

    2009-11-01

    We report converged calculations of fully, singly differential and total cross sections for two-photon double ionization of the hydrogen molecule in the range of 26-30 eV. These results have been obtained by using the method of exterior complex scaling combined with the use of DVR basis set.

  20. Two-photon double ionization of H2 using exterior complex scaling

    SciTech Connect

    Horner, Daniel A; Morales, F; Martin, F; Rescigno, T N; Mccurdy, C W

    2009-03-09

    We report converged calculations of fully, singly differential and total cross sections for two-photon double ionization of the hydrogen molecule in the range of 26-30 eV. These results have been obtained by using the method of exterior complex scaling combined with the use of DVR basis set.

  1. Spectroscopic Study of ThCl+ by Two-Photon Ionization

    NASA Astrophysics Data System (ADS)

    Bartlett, Joshua; VanGundy, Robert A.; Heaven, Michael; Peterson, Kirk

    2016-06-01

    Despite the irreplaceable role experimental data plays for evaluating the performance of computational predictions, diatomic actinide species have not received much spectroscopic attention. As an early actinide element, thorium-containing species are ideal candidates for these types of studies. The electronic structure is expected to be relatively simple compared to later actinides, and therefore allows straightforward assessment of calculations. Here, we have studied ThCl+ for the first time via resonant two-photon ionization of jet-cooled ThCl produced by laser ablation of the metal reacted with dilute Cl2. Laser-induced Fluorescence (LIF) spectra have been recorded for the neutral molecule from 16000 - 23500 cm-1 in search of a suitable intermediate state for subsequent two-photon ionization experiments. Monochromator dispersion of the fluorescence has recovered the ground state vibration and anharmonic constants of ThCl. Resonant Two-Photon Ionization (R2PI) within a time-of-flight mass spectrometer was used to confirm ThCl production, and Pulsed Field Ionization Zero Kinetic Energy photoelectron spectroscopy (PFI-ZEKE) has been performed to identify the ionization energy as well as several of the low-lying states of the ThCl+ molecule. These constants have been predicted at the CASPT2 and CCSD(T) levels of theory, and a discussion of the calculations' performance will be presented alongside the recorded spectra.

  2. Two-photon double ionization of the helium atom by ultrashort pulses

    SciTech Connect

    Palacios, Alicia; Horner, Daniel A; Rescigno, Thomas N; McCurdy, C William

    2010-05-14

    Two-photon double ionization of the helium atom was the subject of early experiments at FLASH and will be the subject of future benchmark measurements of the associated electron angular and energy distributions. As the photon energy of a single femtosecond pulse is raised from the threshold for two-photon double ionization at 39.5 eV to beyond the sequential ionization threshold at 54.4 eV, the electron ejection dynamics change from the highly correlated motion associated with nonsequential absorption to the much less correlated sequential ionization process. The signatures of both processes have been predicted in accurate \\textit{ab initio} calculations of the joint angular and energy distributions of the electrons, and those predictions contain some surprises. The dominant terms that contribute to sequential ionization make their presence apparent several eV below that threshold. In two-color pump probe experiments with short pulses whose central frequencies require that the sequential ionization process necessarily dominates, a two-electron interference pattern emerges that depends on the pulse delay and the spin state of the atom.

  3. Perturbative calculation of two-photon double electron ionization of helium

    NASA Astrophysics Data System (ADS)

    Ivanov, I. A.; Kheifets, A. S.

    2008-05-01

    We report the total integrated cross-section (TICS) of two-photon double ionization of helium in the photon energy range from 40 to 54 eV. We compute the TICS in the lowest order perturbation theory (LOPT) using the length and Kramers-Henneberger gauges of the electromagnetic interaction. Our findings indicate that the LOPT gives results for the TICS in agreement with our earlier non-perturbative calculations.

  4. Two-photon double ionization of the H2 molecule: Cross sections and amplitude analysis

    NASA Astrophysics Data System (ADS)

    Ivanov, I. A.; Kheifets, A. S.

    2013-02-01

    We perform time-dependent calculations of triply differential cross sections (TDCS) of two-photon double-electron ionization of the aligned H2 molecule. Our TDCS results for equal energy sharing between photoelectrons agree quite well with a recent time-dependent calculation by Guan [X. Guan, K. Bartschat, and B. I. Schneider, Phys. Rev. APLRAAN1050-294710.1103/PhysRevA.77.043421 77, 043421 (2008)] who employed a slightly different numerical technique. We supplement these studies by calculating TDCS at an unequal energy sharing and by generating symmetrized ionization amplitudes.

  5. Effects of autoionizing states on two-photon double ionization of the H2 molecule

    NASA Astrophysics Data System (ADS)

    Guan, Xiaoxu; Bartschat, Klaus; Schneider, Barry I.; Koesterke, Lars

    2014-04-01

    Treating the effects of autoionizing intermediate states on two-photon double ionization (DI) of the H2 molecule using time-dependent laser pulses is a significant computational challenge. Relatively long exposure times are critical to understanding the dynamics. Using the fixed-nuclei approximation, we demonstrate how the doubly excited states enhance the angle-integrated generalized cross sections in H2, and how they affect the angular distribution pattern of the ejected electrons. As the energy approaches the threshold for sequential DI, there is a sharp rise in the cross section due to virtual sequential ionization.

  6. Resonance effects in two-photon double ionization of H2 by femtosecond XUV laser pulses

    NASA Astrophysics Data System (ADS)

    Guan, Xiaoxu; Bartschat, Klaus; Schneider, Barry I.; Koesterke, Lars

    2013-10-01

    We investigate the effect of the pulse length on the two-photon double ionization (DI) of H2 in the direct domain, for a femtosecond (fs) laser with a polarization vector oriented along the molecular axis. In the fixed-nuclei approximation, we find that the doubly excited Q11Σu+ states manifest themselves as resonances in the angle-integrated cross sections if the laser interaction lasts longer than about 3 fs. Decay into single-ionization channels does not significantly affect the shape of the angular distribution. A sharp rise in the probability for DI, due to virtual sequential ionization, occurs when the photon energy approaches the threshold for sequential DI.

  7. Multiphoton Ionization and Two-Photon Excitation of Aromatic Molecules in Liquids

    NASA Astrophysics Data System (ADS)

    Faidas, Homer

    1985-12-01

    The two-photon excitation of benzene and toluene in a number of different nonpolar liquids (n-pentane, tetramethylsilane, perfluoro-n-hexane, perfluoromethylcyclohexane, and perfluorodimethylcyclobutane) was studied over the 360-560 nm laser excitation wavelength range. The effect of the solvent on the upper excited states was investigated and a peak, observed in the two -photon excitation spectra of benzene, was assigned to the (3s)('1)E(,1g) Rydberg state based on the unusual solvent dependence of its relative intensity and spectral shift. Polarization studies and signal vs. laser intensity measurements were also carried out. Virbrational analyses of the entire range of the ('1)B(,2u) state of benzene and of the ('1)B(,2) state of toluene, including the hot bands, were performed based on the spectra measured in perfluoro-n-hexane. The O-O transitions of these states in perfluoro-n-hexane and n -pentane were observed at 38050 cm('-1) and 37853 cm('-1) for benzene and at 37411 cm('-1) and 37220 cm('-1) for toluene, respectively. The two-photon excitation spectrum of fluoranthene in a solution of n-pentane over the 420-860 nm laser excitation range was also measured. The O-O transition of the first singlet state was observed at 24800 cm('-1), resolving thus the ambiguity about the exact position of that state. The multiphoton ionization of benzene in dilute solutions of n-pentane and tetramethylsilane was also studied, over the 360-570 nm laser excitation range. Polarization studies and signal vs. laser intensity measurements were performed and the dependence of the spectral features and of the polarization ratio on the laser intensity was studied. The multiphoton ionization mechanism, the location of the ionization threshold of benzene in n-pentane and in tetramethylsilane and the effect of the medium on the ionization threshold are discussed. A particular ionization behavior was observed in a wavelength region corresponding to the channel 3 relaxation which

  8. Different escape modes in two-photon double ionization of helium

    SciTech Connect

    Kheifets, A. S.; Ivanov, A. I.; Bray, I.

    2007-02-15

    The quadrupole channel of two-photon double ionization of He exhibits two distinctly different modes of correlated motion of the photoelectron pair. The kinematics of the mode associated with the center-of-mass motion favors large total momenta maximized at parallel emission where the interelectron repulsion is strong. In contrast, the mode associated with the relative motion favors large relative momenta maximized at antiparallel emission where the interelectron repulsion is relatively weak. This difference in the interelectron repulsion allows for much wider angular correlation width in the relative motion mode as compared to the center-of-mass mode.

  9. Temperature sensitivity of molecular oxygen resonant-enhanced multiphoton ionization spectra involving the C 3Π g intermediate state

    NASA Astrophysics Data System (ADS)

    Wu, Yue; Zhang, Zhili; Adams, Steven F.

    2016-05-01

    The technique of measuring O2 rotational temperature by coherent microwave Rayleigh scattering from resonance-enhanced multiphoton ionization (Radar REMPI) has been studied to determine temperature sensitivity and range. The molecular oxygen Rydberg state of ( {3sσ } )C{{}3}Πg ( {v^' } = 2} ) has been selected as the intermediate state in the 2 + 1 REMPI process, which is known to provide a relatively strong REMPI signal. Rotational-resolved spectra representing the two-photon C{{}3}Πg ( {v^' } = 2} ) leftarrow leftarrow X{{}3}Σ g^{ - } ( {v^' ' } = 0} ) transition have been obtained under several gas conditions including pure oxygen, air-like syngas, ambient air, and flame environments from room temperature ( 300 K) to flame temperature ( 1700 K). An O2 REMPI spectral model has been developed to simulate the experimental spectral line intensity distribution which is dependent on the O2 ground-state temperature. The model has been verified at a low-temperature condition ( 5 K) and then applied to various oxygen environments over an extended temperature range with an overall error of less than ±10 %. The current O2 REMPI spectral model is an improvement over a previously reported version in both accuracy and the quantity of lines fit to provide rotational temperature measurements. This work details an optimized model that fits simulated spectra to full experimental spectral bands over various conditions with a wide temperature range, including both low temperature (<300 K) and high temperature ranges (>1300 K).

  10. Interference effects in one- and two-photon ionization by femtosecond VUV pulses

    NASA Astrophysics Data System (ADS)

    Gryzlova, Elena V.; Staroselskaya, Ekaterina I.; Grum-Grzhimailo, Alexei N.; Venzke, Joel; Bartschat, Klaus

    2015-05-01

    Investigations of coherent control of atomic and molecular processes have rapidly developed since the advent of coherent light sources such as X-ray free electron lasers (XFELs) and achievements in high harmonic generation. In practice, radiation from XFELs contains a small fraction of the second harmonic, which is difficult to filter out but can strongly influence experimental data on the two-photon ionization process, such as the angular distribution. Specifically, the direct first-order second-harmonic ionization process may interfere with, and possibly even dominate a second-order two-photon process caused by the fundamental. While this interference has been investigated in the optical regime with many-cycle pulses, possible effects due to short pulses, as well as a physical intermediate resonance state that may serve as a stepping stone for the second-order process, need a careful study for particular experimental conditions. Here we consider the photoionization of atomic hydrogen for photon energies near the excitation energy of the 2p state (0.375 a.u. or 121.6 nm). We compare results obtained from a direct numerical solution of the time-dependent Schrödinger equation and second-order perturbation theory. This work is supported by the United States National Science Foundation under grant No. PHY-1430245 and the XSEDE allocation PHY-090031, and by the Russian Foundation for Basic Research under Grant No. 12-02-01123.

  11. Electron correlation in two-photon double ionization of helium from attosecond to FEL pulses

    SciTech Connect

    Collins, Lee

    2009-01-01

    We investigate the role of electron correlation in the two-photon double ionization of helium for ultrashort pulses in the extreme ultraviolet (XUV) regime with durations ranging from a hundred attoseconds to a few femtoseconds. We perform time-dependent ab initio calculations for pulses with mean frequencies in the so-called 'sequential' regime ({Dirac_h}{omega} > 54.4 eV). Electron correlation induced by the time correlation between emission events manifests itself in the angular distribution of the ejected electrons, which strongly depends on the energy sharing between them. We show that for ultrashort pulses two-photon double ionization probabilities scale non-uniformly with pulse duration depending on the energy sharing between the electrons. Most interestingly we find evidence for an interference between direct ('nonsequential') and indirect ('sequential') double photoionization with intermediate shake-up states, the strength of which is controlled by the pulse duration. This observation may provide a route towards measuring the pulse duration of x-ray free-electron laser (XFEL) pulses.

  12. Resonance-Enhanced Multiphoton Ionization Mass Spectrometry (REMPI-MS): Applications for Process Analysis

    NASA Astrophysics Data System (ADS)

    Streibel, Thorsten; Zimmermann, Ralf

    2014-06-01

    Process analysis is an emerging discipline in analytical sciences that poses special requirements on analytical techniques, especially when conducted in an online manner. Mass spectrometric methods seem exceedingly suitable for this task, particularly if a soft ionization method is applied. Resonance-enhanced multiphoton ionization (REMPI) in combination with time-of-flight mass spectrometry (TOFMS) provides a selective and sensitive means for monitoring (poly)aromatic compounds in process flows. The properties of REMPI and various variations of the ionization process are presented. The potential of REMPI for process analysis is highlighted with several examples, and drawbacks of the method are also noted. Applications of REMPI-TOFMS for the detection and monitoring of aromatic species in a large variety of combustion processes comprising flames, vehicle exhaust, and incinerators are discussed. New trends in technical development and combination with other analytical methods are brought forward.

  13. Effects of non-adiabatic coupling in photofragmentation of CO(2) using resonance enhanced multiphoton ionization techniques

    NASA Astrophysics Data System (ADS)

    Dharmasena, Kushlani Chandima

    1997-07-01

    We observed Resonance Enhanced Multiphoton Ionization (REMPI) spectra of nf2ΠΩ Rydberg states of CO2 for n=4 to 8. In addition, we also did a laser power dependence study of these states for n=5 to 7. We compared our results to two other studies by Johnson and coworkers and Dobber and coworkers. In the present study we observed that dissociation rate increased with increasing frequency. Also, we observed a clear difference in rates of dissociation for the two spin-orbit components of each nf state. This difference was not consistent, in some states the /Omega=1/2 component dissociated more while in the others /Omega=3/2 dissociated more. When comparing with Dobber and coworkers' REMPI-Photoelectron Spectra (REMPI-PES), a good correlation between the observed symmetric vibrational progressions and our dissociation rates was noticed. We also found that these rates stayed remarkably constant for different powers of the laser even though the production of CO+ ions required more photons than CO2+ ions. From this observation we came to the conclusion that the two-photon transition was saturated. What was surprising was, the amount of CO2+ ions observed despite the fact that the two-photon transition X 2Πg/to/to[ C]2Σg+ was saturated. The observed ratio of CO+/CO2+ ratio never was lower than 6. These observations led us to believe that CO+ ions were predominantly made by predissociation rather than direct dissociation. We propose that the two- photon transition is X 2Πg/to/to[ C]2Σg+ followed by predissociation of the C2ΣG+ state. In our model, predissociation must occur through a potential barrier in the C2Σg+ state which is on the order of an electron volt above the dissociation limit. We estimated the mean lifetime of this state to be about 600 psec by using the ratio of CO+/CO2+ from our spectra. This model explains two other phenomena observed in REMPI spectra. First is the observation of increased dissociation with increasing principal quantum number in the

  14. Two-photon double-ionization of the H2 molecule: effects of pulse duration

    NASA Astrophysics Data System (ADS)

    Guan, Xiaoxu; Bartschat, Klaus; Koesterke, Lars; Schneider, Barry

    2013-05-01

    In previous work, we solved the time-dependent Schrödinger equation to calculate the two-photon double ionization of the hydrogen molecule induced by non-sequential absorption of photons with a central energy of 30 eV in a short laser pulse lasting for about 1.6 femtoseconds. At the equilibrium internuclear separation, however, several doubly excited 1Σg , u states lie about 30 eV above the ground X1Σg state. There is significant disagreement among various results published to date on this problem already for the angle-integrated cross section, and hence for the angular distribution as well. In the present work we address and clarify the fundamental role of those doubly excited states, which are accessible through photon absorption, on the two-photon breakup process. This can only be achieved by allowing for much longer laser pulses. Work supported by the NSF under PHY-1068140 and the XSEDE allocation PHY-090031.

  15. Resonant two-photon ionization electronic spectroscopy of the silver trimer

    NASA Astrophysics Data System (ADS)

    Cheng, P. Y.; Duncan, M. A.

    1989-10-01

    Silver metal clusters are produced by excimer lasers vaporization (308 nm) in a pulsed supersonic nozzle cluster source. The triatomic species is selectively ionized in a resonant two-photon absorption process via an excited electronic state with an origin at 26971±10 cm-1 (3.35 eV). Vibronic structure extending over 1500 cm-1 involves cleanly resolved bands at low energy merging to a quasi-continuum at higher energy. Vibronic analysis are considered for a triangular structure with or without Jahn-Teller interaction in the excited state. No simple analytic expression successfully fits the level structure. However, the spectrum is qualitatively consistent with a 2E` excited state with intermediate Jahn-Teller interaction.

  16. Two-photon double ionization of H2 in intense femtosecond laser pulses

    NASA Astrophysics Data System (ADS)

    Guan, Xiaoxu; Bartschat, Klaus; Schneider, Barry I.

    2010-10-01

    Triple-differential cross sections for two-photon double ionization of molecular hydrogen are presented for a central photon energy of 30 eV. The calculations are based on a fully ab initio, nonperturbative approach to the time-dependent Schrödinger equation in prolate spheroidal coordinates, discretized by a finite-element discrete-variable representation. The wave function is propagated in time for a few femtoseconds using the short, iterative Lanczos method to study the correlated response of the two photoelectrons to short, intense laser radiation. The current results often lie in between those of Colgan [J. Phys. BJPAPEH0953-407510.1088/0953-4075/41/12/121002 41, 121002 (2008)] and Morales [J. Phys. BJPAPEH0953-407510.1088/0953-4075/42/13/134013 42, 134013 (2009)]. However, we argue that these individual predictions should not be compared directly with each other, but preferably with experimental data generated under well-defined conditions.

  17. Molecular beam resonant two-photon ionization study of caffeine and its hydrated clusters

    NASA Astrophysics Data System (ADS)

    Kim, Doory; Kim, Hyung Min; Yang, Key Young; Kim, Seong Keun; Kim, Nam Joon

    2008-04-01

    We investigated electronically excited states of caffeine and its 1:1 complex with water by using resonant two-photon ionization (R2PI) and UV-UV hole-burning techniques. Strong vibronic coupling between a pair of close-lying π-π * and n-π * transitions is proposed to be responsible for the broad spectral feature observed. By comparing the experimental results with those of theoretical calculations, both the O-bonded and N-bonded forms were suggested to be initially produced for the 1:1 complex. The electronic transitions of the O-bonded complex were blueshifted in the R2PI spectrum. For the N-bonded complex, the excited state undergoes an ultrafast decay process, followed by dissociation on a repulsive potential energy surface, which gives rise to a characteristically anomalous cluster distribution in nanosecond experiments.

  18. Resonant two-photon ionization spectroscopy of Al atoms and dimers solvated in helium nanodroplets

    SciTech Connect

    Krasnokutski, Serge A.; Huisken, Friedrich

    2015-02-28

    Resonant two-photon ionization (R2PI) spectroscopy has been applied to investigate the solvation of Al atoms in helium droplets. The R2PI spectra reveal vibrational progressions that can be attributed to Al–He{sub n} vibrations. It is found that small helium droplets have very little chance to pick up an aluminum atom after collision. However, the pick-up probability increases with the size of the helium droplets. The absorption band that is measured by monitoring the ions on the mass of the Al dimer is found to be very little shifted with respect to the Al monomer band (∼400 cm{sup −1}). However, using the same laser wavelength, we were unable to detect any Al{sub n} photoion with n larger than two.

  19. Resonantly enhanced multiphoton ionization under XUV FEL radiation: a case study of the role of harmonics

    NASA Astrophysics Data System (ADS)

    Nikolopoulos, G. M.; Lambropoulos, P.

    2015-12-01

    We provide a detailed quantitative study of the possible role of a small admixture of harmonics on resonant two-photon ionization. The motivation comes from the occasional presence of 2nd and 3rd harmonics in FEL radiation. We obtain the dependence of ionic yields on the intensity of the fundamental, the percentage of 2nd harmonic and the detuning of the fundamental from resonance. Having examined the cases of one and two intermediate resonances, we arrive at results of general validity and global behaviour, showing that even a small amount of harmonic may seem deceptively innocuous.

  20. Alignment effects in two-photon double ionization of H2 in femtosecond xuv laser pulses

    NASA Astrophysics Data System (ADS)

    Guan, Xiaoxu; Bartschat, Klaus; Schneider, Barry I.

    2011-09-01

    Triple-differential cross sections for two-photon double ionization of the aligned hydrogen molecule at the equilibrium distance are presented for a central photon energy of 30 eV. The temporal response of the laser-driven molecule is investigated by solving the time-dependent Schrödinger equation in full dimensionality using two-center elliptical coordinates and a finite-element discrete-variable-representation approach. The molecular orientation is found to have a strong effect on the emission modes of the two correlated photoelectrons. This molecular effect is most noticeable when the molecular axis and the laser polarization vector are oriented parallel to each other. For intermediate cases between the parallel and perpendicular geometries, the dominant emission modes for two-electron ejection oscillate between those for the two extreme cases. The contributions from different ionization channels are also analyzed in detail. Depending on the emission direction of the reference electron, the interference contributions from the various channels can be constructive or destructive at small alignment angles, while they always contribute constructively to the triple-differential cross sections near the perpendicular geometry.

  1. Resonant two-photon ionization spectroscopy of jet-cooled NiPt

    NASA Astrophysics Data System (ADS)

    Taylor, Scott; Spain, Eileen M.; Morse, Michael D.

    1990-03-01

    Resonant two-photon ionization spectroscopy of jet-cooled NiPt has been used to investigate the possibility of d-electron contributions to the bonding in this species. Based on an abrupt onset of predissociation, the bond strength of NiPt is assigned as D0(NiPt)=2.798±0.003 eV. Comparisons of scans using ArF (6.42 eV) or F2 (7.87 eV) radiation as the ionization laser yield IP(NiPt)=8.02±0.15 eV, from which we derive D0(Ni+-Pt)=2.41±0.15 eV and D0(Ni-Pt+) =3.58±0.35 eV. High resolution studies of the 6-0 and 8-0 bands of one of the three identifiable progressions demonstrate an Ω'=0←Ω`=0 transition with r'e =2.3396±0.0039Å and r″0 =2.2078±0.0023Å. The short bond length and large bond strength of NiPt, as compared to the corresponding values (re=2.330±0.003Å and D0=2.34±0.10 eV) for the coinage metal analog, CuAu, demonstrate significant d-orbital contributions to the bonding in NiPt.

  2. Quantitative determination of H2, HD, and D2 internal-state distributions by (2+1) resonance-enhanced multiphoton ionization

    NASA Astrophysics Data System (ADS)

    Rinnen, Klaus-Dieter; Buntine, Mark A.; Kliner, Dahv A. V.; Zare, Richard N.; Huo, Winifred M.

    1991-07-01

    Results are presented of an experimental study of (2+1) resonance-enhanced multiphoton ionization (REMPI) detection of H2, HD, and D2 via the E,F two-photon transition, in which the relationship between ion signals and quantum-state populations was determined by calibration against a thermal effusive source. Vibrational and rotational correction factors were obtained for 102 rovibrational levels for v-double-prime = 0, 1, and 2 and for J-double-prime ranging from 0 to 17. These correction factors make it possible to convert ion signals into relative quantum-state populations without relying on a theoretical description of the (2+1) REMPI process.

  3. Quantitative determination of H2, HD, and D2 internal-state distributions by (2+1) resonance-enhanced multiphoton ionization

    NASA Technical Reports Server (NTRS)

    Rinnen, Klaus-Dieter; Buntine, Mark A.; Kliner, Dahv A. V.; Zare, Richard N.; Huo, Winifred M.

    1991-01-01

    Results are presented of an experimental study of (2+1) resonance-enhanced multiphoton ionization (REMPI) detection of H2, HD, and D2 via the E,F two-photon transition, in which the relationship between ion signals and quantum-state populations was determined by calibration against a thermal effusive source. Vibrational and rotational correction factors were obtained for 102 rovibrational levels for v-double-prime = 0, 1, and 2 and for J-double-prime ranging from 0 to 17. These correction factors make it possible to convert ion signals into relative quantum-state populations without relying on a theoretical description of the (2+1) REMPI process.

  4. Identification of four rotamers of m-methoxystyrene by resonant two-photon ionization and mass analyzed threshold ionization spectroscopy

    SciTech Connect

    Xu, Yanqi; Tzeng, Sheng Yuan; Takahashi, Kaito; Shivatare, Vidya; Zhang, Bing; Tzeng, Wen Bih

    2015-03-28

    We report the vibronic and cation spectra of four rotamers of m-methoxystyrene, recorded by using the two-color resonant two-photon ionization and mass-analyzed threshold ionization techniques. The excitation energies of the S{sub 1}← S{sub 0} electronic transition are found to be 32 767, 32 907, 33 222, and 33 281 cm{sup −1}, and the corresponding adiabatic ionization energies are 65 391, 64 977, 65 114, and 64 525 cm{sup −1} for these isomeric species. Most of the observed active vibrations in the electronically excited S{sub 1} and cationic ground D{sub 0} states involve in-plane ring deformation and substituent-sensitive bending motions. It is found that the relative orientation of the methoxyl with respect to the vinyl group does not influence the vibrational frequencies of the ring-substituent bending modes. The two dimensional potential energy surface calculations support our experimental finding that the isomerization is restricted in the S{sub 1} and D{sub 0} states.

  5. Identification of four rotamers of m-methoxystyrene by resonant two-photon ionization and mass analyzed threshold ionization spectroscopy.

    PubMed

    Xu, Yanqi; Tzeng, Sheng Yuan; Shivatare, Vidya; Takahashi, Kaito; Zhang, Bing; Tzeng, Wen Bih

    2015-03-28

    We report the vibronic and cation spectra of four rotamers of m-methoxystyrene, recorded by using the two-color resonant two-photon ionization and mass-analyzed threshold ionization techniques. The excitation energies of the S1← S0 electronic transition are found to be 32 767, 32 907, 33 222, and 33 281 cm(-1), and the corresponding adiabatic ionization energies are 65 391, 64 977, 65 114, and 64 525 cm(-1) for these isomeric species. Most of the observed active vibrations in the electronically excited S1 and cationic ground D0 states involve in-plane ring deformation and substituent-sensitive bending motions. It is found that the relative orientation of the methoxyl with respect to the vinyl group does not influence the vibrational frequencies of the ring-substituent bending modes. The two dimensional potential energy surface calculations support our experimental finding that the isomerization is restricted in the S1 and D0 states.

  6. Laser induced fluorescence and resonant two-photon ionization spectroscopy of jet-cooled 1-hydroxy-9,10-anthraquinone

    NASA Astrophysics Data System (ADS)

    Cho, Sung Haeng; Huh, Hyun; Kim, Hyung Min; Kim, Choong Ik; Kim, Nam Joon; Kim, Seong Keun

    2005-01-01

    We carried out laser induced fluorescence and resonance enhanced two-color two-photon ionization spectroscopy of jet-cooled 1-hydroxy-9,10-anthraquinone (1-HAQ). The 0-0 band transition to the lowest electronically excited state was found to be at 461.98 nm (21 646 cm-1). A well-resolved vibronic structure was observed up to 1100 cm-1 above the 0-0 band, followed by a rather broad absorption band in the higher frequency region. Dispersed fluorescence spectra were also obtained. Single vibronic level emissions from the 0-0 band showed Stokes-shifted emission spectra. The peak at 2940 cm-1 to the red of the origin in the emission spectra was assigned as the OH stretching vibration in the ground state, whose combination bands with the C=O bending and stretching vibrations were also seen in the emission spectra. In contrast to the excitation spectrum, no significant vibronic activity was found for low frequency fundamental vibrations of the ground state in the emission spectrum. The spectral features of the fluorescence excitation and emission spectra indicate that a significant change takes place in the intramolecular hydrogen bonding structure upon transition to the excited state, such as often seen in the excited state proton (or hydrogen) transfer. We suggest that the electronically excited state of interest has a double minimum potential of the 9,10-quinone and the 1,10-quinone forms, the latter of which, the proton-transferred form of 1-HAQ, is lower in energy. On the other hand, ab initio calculations at the B3LYP/6-31G(d,p) level predicted that the electronic ground state has a single minimum potential distorted along the reaction coordinate of tautomerization. The 9,10-quinone form of 1-HAQ is the lowest energy structure in the ground state, with the 1,10-quinone form lying ˜5000 cm-1 above it. The intramolecular hydrogen bond of the 9,10-quinone was found to be unusually strong, with an estimated bond energy of ˜13 kcal/mol (˜4500 cm-1), probably due to

  7. Resonant two-photon ionization spectroscopy of jet-cooled UN: Determination of the ground state

    NASA Astrophysics Data System (ADS)

    Matthew, Daniel J.; Morse, Michael D.

    2013-05-01

    The optical transitions of supersonically cooled uranium nitride (UN) have been investigated in the range from 19 200 to 23 900 cm-1 using resonant two-photon ionization spectroscopy. A large number of bands have been observed, of which seven have been rotationally resolved and analyzed. All are found to arise from the same state, which is presumably the ground state of the molecule. From the analysis of the bands, the ground state has Ω = 3.5, with a bond length of 1.7650(12) Å. Comparisons to the known isovalent molecules are made, and the variations in ground state configuration are explained in terms of the configurational reordering that occurs with changes in the nuclear and ligand charges. It is concluded that the UN molecule is best considered as a U3+N3- species in which the closed shell nitride ligand interacts with a U3+ ion. The ground state of the molecule derives from a U3+ ion in its 7s15f 2 atomic configuration.

  8. Verification Results of Jet Resonance-enhanced Multiphoton Ionization as a Real-time PCDD/F Emission Monitor

    EPA Science Inventory

    The Jet REMPI (Resonance Enhanced Multiphoton Ionization) monitor was tested on a hazardous waste firing boiler for its ability to determine concentrations of polychlorinated dibenzodioxins and dibenzofurans (PCDDs/Fs). Jet REMPI is a real time instrument capable of highly selec...

  9. Studies of 4-CHLORO-2-FLUOROANISOLE by Two-Color Resonant Two-Photon Mass-Analyzed Threshold Ionization Spectroscopy

    NASA Astrophysics Data System (ADS)

    Wu, Pei-Ying; Tzeng, Wen-Bih

    2016-06-01

    We applied the two-color resonant two-photon mass analyzed threshold ionization technique to record the cation spectra of 4-chloro-2-fluoroanisole by ionizing via five intermediate vibronic levels. The excitation and adiabatic ionization energies were determined to be 35 227, and 67 218 wn, respectively. Spectral analysis and theoretical calculation suggest that the geometry of the aromatic ring of the neutral species in the S1 state is non-planar, but that of the cation in the D0 state is planar.

  10. Resonantly enhanced multiphoton ionization and zero kinetic energy photoelectron spectroscopy of chrysene: a comparison with tetracene.

    PubMed

    Zhang, Jie; Harthcock, Colin; Kong, Wei

    2012-07-01

    We report the electronic and vibrational spectroscopy of chrysene using resonantly enhanced multiphoton ionization (REMPI) and zero kinetic energy (ZEKE) photoelectron spectroscopy. As an isomer of tetracene, chrysene contains a kink in the middle of the four fused hexagonal rings, which complicates not just the symmetry but, more importantly, the molecular orbitals and hence vibronic transitions. Incidentally, the two nearby electronically excited states of chrysene have the same symmetry, and vibronic coupling introduces no out-of-plane vibrational modes. As a result, the REMPI spectrum of chrysene contains essentially only in-plane ring deformation modes, similar to that of tetracene. However, density functional calculations using gaussian even after the inclusion of vibronic coupling can only duplicate the observed REMPI spectrum in a qualitative sense, and the agreement is considerably worse than our recent work on a few pericondensed polycyclic aromatic hydrocarbons and on tetracene. The ZEKE spectrum of chrysene via the origin band of the intermediate electronic state S(1), however, can be qualitatively reproduced by a straightforward Franck-Condon calculation. The ZEKE spectra from vibrationally excited states of the S(1), on the other hand, demonstrate some degree of mode selectivity: the overall intensity of the ZEKE spectrum can vary by an order of magnitude depending on the vibrational mode of the intermediate state. A scaling factor in the theoretical vibrational frequency for the cation is also needed to compare with the experimental result, unlike tetracene and pentacene.

  11. Spatially resolved measurement of singlet delta oxygen by radar resonance-enhanced multiphoton ionization.

    PubMed

    Wu, Yue; Zhang, Zhili; Ombrello, Timothy M

    2013-07-01

    Coherent microwave Rayleigh scattering (Radar) from resonance-enhanced multiphoton ionization (REMPI) was demonstrated to directly and nonintrusively measure singlet delta oxygen, O(2)(a(1)Δ(g)), with high spatial resolution. Two different approaches, photodissociation of ozone and microwave discharge plasma in an argon and oxygen flow, were utilized for O(2)(a(1)Δ(g)) generation. The d(1)Π(g)←a(1)Δ(g) (3-0) and d(1)Π(g)←a(1)Δ(g) (1-0) bands of O(2)(a(1)Δ(g)) were detected by Radar REMPI for two different flow conditions. Quantitative absorption measurements using sensitive off-axis integrated cavity output spectroscopy (ICOS) was used simultaneously to evaluate the accuracy and sensitivity of the Radar REMPI technique. The detection limit of Radar REMPI was found to be comparable to the ICOS technique with a detection threshold of approximately 10(14) molecules/cm(3) but with a spatial resolution that was 8 orders of magnitude smaller than the ICOS technique.

  12. Two-photon double ionization of H2 at 30 eV using Exterior Complex Scaling

    SciTech Connect

    Morales, Felipe; Martin, Fernando; Horner, Daniel; Rescigno, Thomas N.; McCurdy, C. William

    2009-01-20

    Calculations of fully differential cross sections for two-photon double ionization of the hydrogen molecule with photons of 30 eV are reported. The results have been obtained by using the method of exterior complex scaling, which allows one to construct essentially exact wave functions that describe thedouble continuum on a large, but finite, volume. The calculated cross sections are compared with those previously obtained by Colgan et al., and discrepancies are found for specific molecular orientations and electron ejection directions.

  13. Electron capture of dopants in two-photonic ionization in a poly(methyl methacrylate) solid

    SciTech Connect

    Tsuchida, Akira; Sakai, Wataru; Nakano, Mitsuru; Yamamoto, Masahide

    1992-10-29

    Behavior of the electron produced by two-photonic excitation of an aromatic donor in a poly(methyl methacrylate) solid was studied by the addition of the electron scavengers to the system. According to the Perrin type analysis for the two-photonically ejected electron, the capture radii (R{sub c}) of the scavengers examined were estimated to be from 8 to 40 {Angstrom}. For the two-photonically ejected electrons, R{sub c} is a capture radius for thermalized electrons. In this case the parent electron donor is not necessarily within this radius. On the other hand, for the fluorescence quenching, the distance between the donor and acceptor is within the static quenching radius (R{sub q}) of the donor. 13 refs., 4 figs., 2 tabs.

  14. Angular anisotropy parameters and recoil-ion momentum distribution in two-photon double ionization of helium

    SciTech Connect

    Kheifets, A. S.; Ivanov, I. A.; Bray, Igor

    2007-08-15

    We present convergent-close-coupling (CCC) calculations of the angular anisotropy parameters {beta}{sub 2},{beta}{sub 4} and the recoil ion momentum distribution d{sigma}/dp in two-photon double ionization (TPDI) of helium. In a stark contrast to single-photon double ionization (SPDI), where the {beta}{sub 2} parameter varies widely changing the angular distribution from isotropic to nearly dipole for slow and fast photoelectrons, respectively, the {beta} parameters for TPDI show very little change. The angular distribution of the recoil ion is fairly isotropic in TPDI as opposed to a strong alignment with the polarization of light in SPDI.

  15. Investigating two-photon double ionization of D{sub 2} by XUV-pump-XUV-probe experiments

    SciTech Connect

    Jiang, Y. H.; Kurka, M.; Kuehnel, K. U.; Toppin, M.; Schroeter, C. D.; Moshammer, R.; Rudenko, A.; Foucar, L.; Perez-Torres, J. F.; Plesiat, E.; Morales, F.; Martin, F.; Herrwerth, O.; Lezius, M.; Kling, M. F.; Jahnke, T.; Doerner, R.; Sanz-Vicario, J. L.; Tilborg, J. van; Belkacem, A.

    2010-05-15

    We used a split-mirror setup attached to a reaction microscope at the free-electron laser in Hamburg (FLASH) to perform an XUV-pump-XUV-probe experiment by tracing the ultrafast nuclear wave-packet motion in the D{sub 2}{sup +}(1s{sigma}{sub g}) with <10 fs time resolution. Comparison with time-dependent calculations shows excellent agreement with the measured vibrational period of 22{+-}4 fs in D{sub 2}{sup +}, points to the importance of accurately knowing the internuclear distance-dependent ionization probability, and paves the way to control sequential and nonsequential two-photon double-ionization contributions.

  16. The role of autoionizing states in two-photon dissociative ionization of H2 by xuv ultrashort laser pulses

    NASA Astrophysics Data System (ADS)

    Pérez-Torres, J. F.; Sanz-Vicario, J. L.; Bachau, H.; Martín, F.

    2010-01-01

    A theoretical study of two-photon ionization of H2 by low-intensity ultrashort xuv laser pulses is reported. The method is based on the solution of the time-dependent Schrödinger equation in a basis of stationary molecular vibronic states which include all electronic and vibrational degrees of freedom. In contrast with previous work, the \\mathcal {Q}_1 doubly excited states, which also contribute to the ionization probabilities through autoionization, are explicitly included. We have found that, just below the one-photon ionization threshold, molecular autoionization leads to an enhancement of dissociative ionization, whose corresponding probability can be an order of magnitude larger than that of the nondissociative ionization process, and even larger than the corresponding dissociative probability in the one-photon absorption region. This result suggests that multicoincidence experiments, in which the orientation of the molecule with respect to the polarization axis is determined, might be easier to perform in the two-photon absorption regime than in the one-photon absorption regime. Electron angular distributions in the same range of photon energies are also reported.

  17. Grid-based methods for diatomic quantum scattering problems II: Time-dependent treatment of single- and two-photon ionization of H2+

    SciTech Connect

    Rescigno, Thomas N.; Tao, L.; McCurdy, C.W.

    2009-04-20

    The time-dependent Schr\\"odinger equation for H2+ in a time-varying electromagnetic field is solved in the fixed-nuclei approximation using a previously developed finite-element/ discrete variable representation in prolate spheroidal coordinates. Amplitudes for single- and two-photon ionization are obtained using the method of exterior complex scaling to effectively propagate the field-free solutions from the end of the radiation pulse to infinite times. Cross sections are presented for one-and two-photon ionization for both parallel and perpendicular polarization of the photon field, as well as photoelectron angular distributions for two-photon ionization.

  18. Electronic dynamics of charge resonance enhanced ionization probed by laser-induced alignment in C2H2

    NASA Astrophysics Data System (ADS)

    Cornaggia, C.

    2016-10-01

    Although charge resonance enhanced ionization (CREI) be an ubiquitous effect in molecules in strong laser fields, the associated electron emission remains difficult to deal with. The main reason relies on the fact that CREI is part of an overall multielectron ionization, where the initial steps of single and dissociative ionization of neutral species dominate the electron spectrum. Using the rescattered electrons, we show that it is possible to address the electron signal from CREI without any contribution from other electron signals. The electrons from CREI are preferentially emitted when the molecular axis is parallel to the laser electric field as expected from its electronic dynamics. Acetylene is chosen for demonstration purpose because single ionization, which is not related to CREI, is more pronounced when the C2H2 molecular axis is perpendicular to the laser electric field.

  19. Two-photon double ionization of H2 at 30 eV using exterior complex scaling

    NASA Astrophysics Data System (ADS)

    Morales, F.; Martín, F.; Horner, D. A.; Rescigno, T. N.; McCurdy, C. W.

    2009-07-01

    Calculations of fully differential cross sections for two-photon double ionization of the hydrogen molecule with photons of 30 eV are reported. The results have been obtained by using the method of exterior complex scaling, which allows one to construct essentially exact wavefunctions that describe the double continuum on a large, but finite, volume. The calculated cross sections are compared with those previously obtained by Colgan et al (J. Phys. B: At. Mol. Opt. Phys. 41 121002), and discrepancies are found for specific molecular orientations and electron ejection directions.

  20. Two-photon double ionization of H2 at 30 eV using exterior complex scaling

    SciTech Connect

    Horner, Daniel A; Morales, F; Martin, F; Rescigno, T N; Mccurdy, C W

    2009-01-01

    Calculations of fully differential cross sections for two-photon double ionization of the hydrogen molecule with photons of 30 eV are reported. The results have been obtained by using the method of exterior complex scaling, which allows one to construct essentially exact wave functions that describe the double continuum on a large, but finite, volume. The calculated cross sections are compared with those previously obtained by Colgan et al [1], and discrepancies are found for specific molecular orientations and electron ejection directions.

  1. Investigating two-photon double ionization of D2 by XUV-Pump -- XUV-Probe experiments at FLASH

    SciTech Connect

    FLASH Collaboration; Jiang, Y.; Rudenko, A.; Perez-Torres, J.; Foucar, L.; Kurka, M.; Kuhnel, K.; Toppin, M.; Plesiat, E.; Morales, F.; Martin, F.; Herrwerth, O.; Lezius, M.; Kling, M.; Jahnke, T.; Dorner, R.; Sanz-Vicario, J.; van Tilborg, J.; Belkacem, A.; Schulz, M.; Ueda, K.; Zouros, T.; Dusterer, S.; Treusch, R.; Schroter, C.; Moshammer, R.; Ullrich, J.

    2010-08-02

    Using a novel split-mirror set-up attached to a Reaction Microscope at the Free electron LASer in Hamburg (FLASH) we demonstrate an XUV-pump -- XUV-probe ((hbar omega = 38 eV) experiment by tracing the ultra-fast nuclear wave-packet motion in the D2+ (1s sigma g-state) with<10 fs time resolution. Comparison with time-dependent calculations yields excellent agreement with the measured vibrational period of 22+-4 fs in D2+, points to the importance of the inter-nuclear distance dependent ionization probability and paves the way to control sequential and non-sequential two-photon double ionization contributions.

  2. Two-color resonantly enhanced multiphoton ionization and zero-kinetic-energy photoelectron spectroscopy of jet-cooled indan

    NASA Astrophysics Data System (ADS)

    He, Yonggang; Kong, Wei

    2005-06-01

    We report studies of supersonically cooled indan using two-color resonantly enhanced multiphoton ionization and two-color zero-kinetic-energy photoelectron spectroscopy. With the aid of ab initio and density-functional calculations, vibrational modes of the first electronically excited state of the neutral species and those of the cation have been assigned, and the adiabatic ionization energy has been determined to be 68458±5cm-1. Similar to the ground state and the first electronically excited state of the neutral molecule, the ground state of the cation is also proven to be nonplanar, with an estimated barrier of 213cm-1 and a puckering angle of 15.0°. These conclusions will be discussed in comparison with a previous study of an indan derivative 1,3-benzodioxole.

  3. Two-photon ionization of H{sub 2}{sup +} by short laser pulses

    SciTech Connect

    Palacios, A.; Martin, F.; Barmaki, S.; Bachau, H.

    2005-06-15

    We present a theoretical study of dissociative multiphoton ionization of the H{sub 2}{sup +} molecular ion in perturbative and nonperturbative regimes including both electronic and nuclear degrees of freedom. Differential (in proton and electron energy) ionization cross sections have been evaluated for various photon energies, laser intensities, and pulse lengths. We have found that the proton energy distribution is modulated by vertical Franck-Condon transitions but also by vibrational resonances associated with intermediate electronic states. We have also found that, as expected, nonperturbative results tend to the time-independent perturbative ones when both the pulse length increases and the laser intensity decreases. No divergence near intermediate-state resonances is found in the perturbative results when the nuclear motion is properly taken into account in the calculations.

  4. Two-photon double ionization of helium in the region of photon energies 42-50eV

    NASA Astrophysics Data System (ADS)

    Ivanov, I. A.; Kheifets, A. S.

    2007-03-01

    We report the total integrated cross section (TICS) of two-photon double ionization of helium in the photon energy range from 42to50eV . Our computational procedure relies on a numerical solution of the time-dependent Schrödinger equation on a square-integrable basis and subsequent projection of this solution on a set of final field-free states describing correlation in the two-electron continuum. Our results suggest that the TICS grows monotonically as a function of photon energy in the region of 42-50eV , possibly reaching a maximum in the vicinity of 50eV . We also present fully resolved triple-differential cross sections for selected photon energies.

  5. Absolute Rb one-color two-photon ionization cross-section measurement near a quantum interference

    SciTech Connect

    Takekoshi, T.; Brooke, G.M.; Patterson, B.M.; Knize, R.J.

    2004-05-01

    We observe destructive interference in the ground-state Rb two-photon ionization cross section when the single photon energy is tuned between the 5S{yields}5P and 5S{yields}6P transition energies. The minimum cross section is 5.9(1.5)x10{sup -52} cm{sup 4} s and it occurs at a wavelength of 441.0(3) nm (in vacuo). Relative measurements of these cross sections are made at various wavelengths by counting ions produced when magneto-optically trapped Rb atoms are exposed to light from a tunable pulsed laser. This relative curve is calibrated to an absolute cross-section measurement at 532 nm using the trap loss method. A simple calculation agrees reasonably with our results.

  6. Two-photon double ionization of helium in the region of photon energies 42-50 eV

    SciTech Connect

    Ivanov, I. A.; Kheifets, A. S.

    2007-03-15

    We report the total integrated cross section (TICS) of two-photon double ionization of helium in the photon energy range from 42 to 50 eV. Our computational procedure relies on a numerical solution of the time-dependent Schroedinger equation on a square-integrable basis and subsequent projection of this solution on a set of final field-free states describing correlation in the two-electron continuum. Our results suggest that the TICS grows monotonically as a function of photon energy in the region of 42-50 eV, possibly reaching a maximum in the vicinity of 50 eV. We also present fully resolved triple-differential cross sections for selected photon energies.

  7. Studies of photoionization in liquids using a laser two-photon ionization conductivity technique. [Potoionization of pyrene, fluoranthene and TMPD in liquid n-pentane

    SciTech Connect

    Siomos, K.; Christophorou, L.G.

    1981-01-01

    One-photon ionization studies of solute molecules in a liquid medium are limited by the absorption of the host medium. A laser two-photon ionization (TPI) technique using a frequency tunable dye laser has been developed, whereby the photoionization threshold of a solute molecule was determined from the induced conductivity in the liquid medium under study due to electron-ion pair formation via two-photon ionization of the solute. The two-photon induced electron-ion current is measured as a function of the laser wavelength, lambda/sub laser/. In this paper, results are reported and discussed on the photoionization of N,N,N',N'-tetramethyl-p-phenylenediamine (TMPD), pyrene and fluoranthene in liquid n-pentane (n-Pt).

  8. Alignment effects in two-photon double ionization of H{sub 2} in femtosecond xuv laser pulses

    SciTech Connect

    Guan Xiaoxu; Bartschat, Klaus; Schneider, Barry I.

    2011-09-15

    Triple-differential cross sections for two-photon double ionization of the aligned hydrogen molecule at the equilibrium distance are presented for a central photon energy of 30 eV. The temporal response of the laser-driven molecule is investigated by solving the time-dependent Schroedinger equation in full dimensionality using two-center elliptical coordinates and a finite-element discrete-variable-representation approach. The molecular orientation is found to have a strong effect on the emission modes of the two correlated photoelectrons. This molecular effect is most noticeable when the molecular axis and the laser polarization vector are oriented parallel to each other. For intermediate cases between the parallel and perpendicular geometries, the dominant emission modes for two-electron ejection oscillate between those for the two extreme cases. The contributions from different ionization channels are also analyzed in detail. Depending on the emission direction of the reference electron, the interference contributions from the various channels can be constructive or destructive at small alignment angles, while they always contribute constructively to the triple-differential cross sections near the perpendicular geometry.

  9. Double-arm three-dimensional ion imaging apparatus for the study of ion pair channels in resonance enhanced multiphoton ionization.

    PubMed

    Poretskiy, M S; Chichinin, A I; Maul, C; Gericke, K-H

    2016-02-01

    We present a novel experimental configuration for the full quantitative characterization of the multichannel resonance enhanced multiphoton ionization (REMPI) of small molecules in cases when the ion-pair dissociation channel is important. For this purpose, a double-arm time-of-flight mass spectrometer with three-dimensional (3D) ion imaging detectors at both arms is constructed. The REMPI of HCl molecules is used to examine the constructed setup. The apparatus allows us to perform simultaneous measurements of the 3D velocity vector distributions of positive (H(+), HCl(+), and Cl(+)) and negative (Cl(-)) photoions. The characterization consists of the determination of "two-photon absorption cross sections" for the process HCl(X)+2hν → HCl*, one-photon absorption cross sections for subsequent processes HCl* + hν → HCl*, and the probability of the subsequent non-adiabatic transition HCl* → HCl(B) → H(+) + Cl(-), which leads to ionic pairs. All these data should be obtained from the analysis of the dependencies of the number of ions on the laser energy. The full characterization of the laser beam and the knowledge of the ion detection probability are necessary parts of the analysis. Detailed knowledge of losses of produced ions in the mass spectrometer before detection requires understanding and characterization of such processes like electron emission from metallic grids under ion bombardment or charge transfer between positive ions and the metal surface of the grids, like Cl(+) + (grid) → Cl(-). These important phenomena from surface science are rarely discussed in the imaging literature, and here, we try to compensate for this shortcoming. PMID:26931834

  10. The design of double electrostatic-lens optics for resonance enhanced multiphoton ionization and photoelectron imaging experiments

    SciTech Connect

    Qu, Zehua; Li, Chunsheng; Qin, Zhengbo E-mail: xfzheng@mail.ahnu.edu.cn; Zheng, Xianfeng E-mail: xfzheng@mail.ahnu.edu.cn; Yao, Guanxin; Zhang, Xianyi; Cui, Zhifeng

    2015-06-15

    Compared to single ion/electron-optics for velocity-map imaging, a double-focusing lens assembly designed not only allows for mapping velocity imaging of photoelectrons but also allows for investigating the vibrational structure of the intermediate states of neutral species in resonance enhanced multiphoton ionization (REMPI) spectra. In this presentation, in order to record REMPI and photoelectron spectra separately, we have constructed a compact photoelectron velocity-map imaging (VMI) apparatus combined with an opposite linear Wiley-Mclaren time-of-flight mass spectrometer (TOFMS). A mass resolution (m/Δm) of ∼1300 for TOFMS and electron energy resolution (ΔE/E) of 2.4% for VMI have been achieved upon three-photon ionization of Xe atom at 258.00 nm laser wavelength. As a benchmark, in combination of one-color (1 + 1) REMPI and photoelectron imaging of benzene via 6{sup 1} and 6{sup 1}1{sup 1} vibronic levels in the S{sub 1} state, the vibrational structures of the cation and photoelectron angular anisotropy are unraveled. In addition, two-color (1 + 1′) REMPI and photoelectron imaging of aniline was used to complete the accurate measurement of ionization potential (62 271 ± 3 cm{sup −1}). The results suggest that the apparatus is a powerful tool for studying photoionization dynamics in the photoelectron imaging using vibrational-state selected excitation to the intermediate states of neutrals based on REMPI technique.

  11. The design of double electrostatic-lens optics for resonance enhanced multiphoton ionization and photoelectron imaging experiments.

    PubMed

    Qu, Zehua; Li, Chunsheng; Qin, Zhengbo; Zheng, Xianfeng; Yao, Guanxin; Zhang, Xianyi; Cui, Zhifeng

    2015-06-01

    Compared to single ion/electron-optics for velocity-map imaging, a double-focusing lens assembly designed not only allows for mapping velocity imaging of photoelectrons but also allows for investigating the vibrational structure of the intermediate states of neutral species in resonance enhanced multiphoton ionization (REMPI) spectra. In this presentation, in order to record REMPI and photoelectron spectra separately, we have constructed a compact photoelectron velocity-map imaging (VMI) apparatus combined with an opposite linear Wiley-Mclaren time-of-flight mass spectrometer (TOFMS). A mass resolution (m/Δm) of ∼1300 for TOFMS and electron energy resolution (ΔE/E) of 2.4% for VMI have been achieved upon three-photon ionization of Xe atom at 258.00 nm laser wavelength. As a benchmark, in combination of one-color (1 + 1) REMPI and photoelectron imaging of benzene via 6(1) and 6(1)1(1) vibronic levels in the S1 state, the vibrational structures of the cation and photoelectron angular anisotropy are unraveled. In addition, two-color (1 + 1') REMPI and photoelectron imaging of aniline was used to complete the accurate measurement of ionization potential (62,271 ± 3 cm(-1)). The results suggest that the apparatus is a powerful tool for studying photoionization dynamics in the photoelectron imaging using vibrational-state selected excitation to the intermediate states of neutrals based on REMPI technique. PMID:26133827

  12. The design of double electrostatic-lens optics for resonance enhanced multiphoton ionization and photoelectron imaging experiments

    NASA Astrophysics Data System (ADS)

    Qu, Zehua; Li, Chunsheng; Qin, Zhengbo; Zheng, Xianfeng; Yao, Guanxin; Zhang, Xianyi; Cui, Zhifeng

    2015-06-01

    Compared to single ion/electron-optics for velocity-map imaging, a double-focusing lens assembly designed not only allows for mapping velocity imaging of photoelectrons but also allows for investigating the vibrational structure of the intermediate states of neutral species in resonance enhanced multiphoton ionization (REMPI) spectra. In this presentation, in order to record REMPI and photoelectron spectra separately, we have constructed a compact photoelectron velocity-map imaging (VMI) apparatus combined with an opposite linear Wiley-Mclaren time-of-flight mass spectrometer (TOFMS). A mass resolution (m/Δm) of ˜1300 for TOFMS and electron energy resolution (ΔE/E) of 2.4% for VMI have been achieved upon three-photon ionization of Xe atom at 258.00 nm laser wavelength. As a benchmark, in combination of one-color (1 + 1) REMPI and photoelectron imaging of benzene via 61 and 6111 vibronic levels in the S1 state, the vibrational structures of the cation and photoelectron angular anisotropy are unraveled. In addition, two-color (1 + 1') REMPI and photoelectron imaging of aniline was used to complete the accurate measurement of ionization potential (62 271 ± 3 cm-1). The results suggest that the apparatus is a powerful tool for studying photoionization dynamics in the photoelectron imaging using vibrational-state selected excitation to the intermediate states of neutrals based on REMPI technique.

  13. Resonance-enhanced multiphoton ionization time-of-flight mass spectrometry for detection of nitrogen containing aliphatic and aromatic compounds: resonance-enhanced multiphoton ionization spectroscopic investigation and on-line analytical application.

    PubMed

    Streibel, T; Hafner, K; Mühlberger, F; Adam, T; Zimmermann, R

    2006-01-01

    Resonance-enhanced multiphoton ionization (REMPI) combined with time-of-flight mass spectrometry (TOFMS) is an analytical method capable of on-line monitoring of trace compounds in complex matrices. A necessary prerequisite for substance selective detection is spectroscopic investigation of the target molecules. Several organic nitrogen compounds comprising aliphatic and aromatic amines, nitrogen heterocyclic compounds, and aromatic nitriles are spectroscopically investigated with a tunable narrow bandwidth optical parametric oscillator (OPO) laser system providing a scannable wavelength range between 220 and 340 nm. These species are known as possible precursors in fuel-NO formation from combustion of solid fuels such as biomass and waste. A newly conceived double inlet system was used in this study, which allows rapid change between effusive and supersonic molecular beams. The resulting REMPI spectra of the compounds are discussed with respect to electronic transitions that could be utilized for a selective ionization of these compounds in complex mixtures such as combustion and process gases. The practicability of this approach is demonstrated by wavelength selected on-line REMPI-TOFMS detection of aniline and cyanonaphthalene in the burning chamber of a waste incineration plant. REMPI mass spectra recorded at different excitation wavelengths as well as variations in time show the utilization of species-selective REMPI-TOFMS detection for on-line monitoring of crucial substances in pollutant formation.

  14. REAL TIME, ON-LINE CHARACTERIZATION OF DIESEL GENERATOR AIR TOXIC EMISSIONS BY RESONANCE ENHANCED MULTI-PHOTON IONIZATION TIME OF FLIGHT MASS SPECTROMETRY

    EPA Science Inventory

    The laser based resonance, enhanced multi-photon ionization time-of-flight mass spectrometry (REMPI-TOFMS) technique has been applied to the exhaust gas stream of a diesel generator to measure, in real time, concentration levels of aromatic air toxics. Volatile organic compounds ...

  15. Resonant two-photon ionization spectroscopy of jet-cooled OsN: 520-418 nm

    NASA Astrophysics Data System (ADS)

    Garcia, Maria A.; Morse, Michael D.

    2011-09-01

    The optical transitions of supersonically cooled OsN have been investigated in the range from 19 200 to 23 900 cm-1 using resonant two-photon ionization spectroscopy. More than 20 vibronic bands were observed, 17 of which were rotationally resolved and analyzed. The ground state is confirmed to be 2Δ5/2, deriving from the 1σ2 2σ2 1π4 1δ3 3σ2 electronic configuration. The X 2Δ5/2 ground state rotational constant for 192Os14N was found to be B0 = 0.491921(34) cm-1, giving r0 = 1.62042(6) Å (1σ error limits). The observed bands were grouped into three band systems with Ω' = 7/2 and four with Ω' = 3/2, corresponding to the three 2Φ7/2 and four 2Π3/2 states expected from the 1σ2 2σ2 1π4 1δ3 3σ1 2π1 and 1σ2 2σ2 1π4 1δ2 3σ2 2π1 electronic configurations. In addition, two interacting upper states with Ω' = 5/2 were observed, one of which is thought to correspond to a 1σ2 2σ2 1π3 1δ3 3σ2 2π1, 2Δ5/2 state. Spectroscopic constants are reported for all of the observed states, and comparisons to related molecules are made. The ionization energy of OsN is estimated as IE(OsN) = 8.80 ± 0.06 eV.

  16. Kinetic modeling of evolution of 3 + 1:Resonance enhanced multiphoton ionization plasma in argon at low pressures

    SciTech Connect

    Tholeti, Siva Sashank; Alexeenko, Alina A.; Shneider, Mikhail N.

    2014-06-15

    We present numerical kinetic modeling of generation and evolution of the plasma produced as a result of resonance enhanced multiphoton ionization (REMPI) in Argon gas. The particle-in-cell/Monte Carlo collision (PIC/MCC) simulations capture non-equilibrium effects in REMPI plasma expansion by considering the major collisional processes at the microscopic level: elastic scattering, electron impact ionization, ion charge exchange, and recombination and quenching for metastable excited atoms. The conditions in one-dimensional (1D) and two-dimensional (2D) formulations correspond to known experiments in Argon at a pressure of 5 Torr. The 1D PIC/MCC calculations are compared with the published results of local drift-diffusion model, obtained for the same conditions. It is shown that the PIC/MCC and diffusion-drift models are in qualitative and in reasonable quantitative agreement during the ambipolar expansion stage, whereas significant non-equilibrium exists during the first few 10 s of nanoseconds. 2D effects are important in the REMPI plasma expansion. The 2D PIC/MCC calculations produce significantly lower peak electron densities as compared to 1D and show a better agreement with experimentally measured microwave radiation scattering.

  17. New Rydberg states of gas-phase aluminum halides observed by resonance-enhanced multiphoton ionization spectroscopy

    SciTech Connect

    Hudgens, J.W.; Dearden, D.V.; Johnson, R.D. III

    1993-12-31

    The authors report detection and characterization of AlF and AlCl using 1+2, 2=1, 2+2, 3+1, and 3+2 resonance-enhanced multiphoton ionization (REMPI) spectroscopy. REMPI Spectra of AlF reveal 13 new Rydberg states that lie between 70,000 and 77,000 cm{sup {minus}1}. These new states, in combination with previously known states, form six Rydberg series. Least-squares fitting of the Rydberg series to the Rydberg equation yields the precise adiabatic ionization potential, IP{sub a}(AlF) = 9.729 {+-} 0.001 eV. Vibrational intervals of the new Rydberg states are about 25% greater than those of AlF (X {sup 1}{Sigma}{sup +}), with most lying between 930-980 cm{sup {minus}1}. REMPI spectra of AlCl reveal new Rydberg states that lie between 54000 and 60000 cm{sup {minus}1}. Vibrational intervals of these new Rydberg states are about 25% greater than those of AlCl (X {sup 1}{Sigma}{sup +}), with most lying between 570-600 cm{sup {minus}1}.

  18. Kinetic modeling of evolution of 3 + 1:Resonance enhanced multiphoton ionization plasma in argon at low pressures

    NASA Astrophysics Data System (ADS)

    Tholeti, Siva Sashank; Shneider, Mikhail N.; Alexeenko, Alina A.

    2014-06-01

    We present numerical kinetic modeling of generation and evolution of the plasma produced as a result of resonance enhanced multiphoton ionization (REMPI) in Argon gas. The particle-in-cell/Monte Carlo collision (PIC/MCC) simulations capture non-equilibrium effects in REMPI plasma expansion by considering the major collisional processes at the microscopic level: elastic scattering, electron impact ionization, ion charge exchange, and recombination and quenching for metastable excited atoms. The conditions in one-dimensional (1D) and two-dimensional (2D) formulations correspond to known experiments in Argon at a pressure of 5 Torr. The 1D PIC/MCC calculations are compared with the published results of local drift-diffusion model, obtained for the same conditions. It is shown that the PIC/MCC and diffusion-drift models are in qualitative and in reasonable quantitative agreement during the ambipolar expansion stage, whereas significant non-equilibrium exists during the first few 10 s of nanoseconds. 2D effects are important in the REMPI plasma expansion. The 2D PIC/MCC calculations produce significantly lower peak electron densities as compared to 1D and show a better agreement with experimentally measured microwave radiation scattering.

  19. Detection of NO and NO(2) by (2 + 2) resonance-enhanced multiphoton ionization and photoacoustic spectroscopy near 454 nm.

    PubMed

    Pastel, R L; Sausa, R C

    1996-07-20

    Trace concentrations of NO and NO(2) are detected with a dye laser operating near 454 nm. NO is detected by a (2 + 2) resonance-enhanced multiphoton ionization process by means of NO A(2)Σ+-X(2)Π(0, 0) transitions with miniature electrodes, and NO(2) is detected by a one-photon absorption photoacoustic process by means of NO(2)A¯' (2)B(1)(0, 8, 0)- X¯ (2)A(1)(0, 0, 0) transitions with a miniature microphone. Rotationally resolved excitation spectra show that the spectral resolution is sufficiently high to identify these species at 1 atm. The technique's analytical merits are evaluated as functions of concentration, pressure, and laser intensities. Low laser intensities favor NO(2) photoacoustic detection whereas high laser intensities favor NO ionization. Limits of detection (signal-to-noise ratio 3) of 160 parts in 10(9) for NO and 400 parts in 10(9) for NO(2) are determined at 1 atm for a 10-s integration time. Signal response and noise analyses show that three decades of NO/NO(2) mixtures can be measured with a computational relative error in concentration that is three times the relative error in measuring the NO and NO(2) signals.

  20. Rotationally Resolved Vacuum Ultraviolet Resonance-Enhanced Multiphoton Ionization (VUV REMPI) of Acetylene via the G̃ Rydberg State.

    PubMed

    Schmidt-May, Alice F; Grütter, Monika; Neugebohren, Jannis; Kitsopoulos, T N; Wodtke, Alec M; Harding, Dan J

    2016-07-14

    We present a 1 + 1' resonance-enhanced multiphoton ionization (REMPI) scheme for acetylene via the linear G̃ 4sσ (1)Πu Rydberg state, offering partial rotational resolution and the possibility to detect excitation in both the cis- and trans-bending modes. The resonant transition to the G̃ state is driven by a vacuum ultraviolet (VUV) photon, generated by resonant four-wave mixing (FWM) in krypton. Ionization from the short-lived G̃ state then occurs quickly, driven by the high intensity of the residual light from the FWM process. We have observed nine bands in the region between 79 200 cm(-1) and 80 500 cm(-1) in C2H2 and C2D2. We compare our results with published spectra in this region and suggest alternative assignments for some of the Renner-Teller split bands. Similar REMPI schemes should be applicable to other small molecules with picosecond lifetime Rydberg states. PMID:27073931

  1. Resonantly Enhanced Betatron Hard X-rays from Ionization Injected Electrons in a Laser Plasma Accelerator.

    PubMed

    Huang, K; Li, Y F; Li, D Z; Chen, L M; Tao, M Z; Ma, Y; Zhao, J R; Li, M H; Chen, M; Mirzaie, M; Hafz, N; Sokollik, T; Sheng, Z M; Zhang, J

    2016-06-08

    Ultrafast betatron x-ray emission from electron oscillations in laser wakefield acceleration (LWFA) has been widely investigated as a promising source. Betatron x-rays are usually produced via self-injected electron beams, which are not controllable and are not optimized for x-ray yields. Here, we present a new method for bright hard x-ray emission via ionization injection from the K-shell electrons of nitrogen into the accelerating bucket. A total photon yield of 8 × 10(8)/shot and 10(8 )photons with energy greater than 110 keV is obtained. The yield is 10 times higher than that achieved with self-injection mode in helium under similar laser parameters. The simulation suggests that ionization-injected electrons are quickly accelerated to the driving laser region and are subsequently driven into betatron resonance. The present scheme enables the single-stage betatron radiation from LWFA to be extended to bright γ-ray radiation, which is beyond the capability of 3(rd) generation synchrotrons.

  2. Resonantly Enhanced Betatron Hard X-rays from Ionization Injected Electrons in a Laser Plasma Accelerator

    PubMed Central

    Huang, K.; Li, Y. F.; Li, D. Z.; Chen, L. M.; Tao, M. Z.; Ma, Y.; Zhao, J. R.; Li, M. H.; Chen, M.; Mirzaie, M.; Hafz, N.; Sokollik, T.; Sheng, Z. M.; Zhang, J.

    2016-01-01

    Ultrafast betatron x-ray emission from electron oscillations in laser wakefield acceleration (LWFA) has been widely investigated as a promising source. Betatron x-rays are usually produced via self-injected electron beams, which are not controllable and are not optimized for x-ray yields. Here, we present a new method for bright hard x-ray emission via ionization injection from the K-shell electrons of nitrogen into the accelerating bucket. A total photon yield of 8 × 108/shot and 108 photons with energy greater than 110 keV is obtained. The yield is 10 times higher than that achieved with self-injection mode in helium under similar laser parameters. The simulation suggests that ionization-injected electrons are quickly accelerated to the driving laser region and are subsequently driven into betatron resonance. The present scheme enables the single-stage betatron radiation from LWFA to be extended to bright γ-ray radiation, which is beyond the capability of 3rd generation synchrotrons. PMID:27273170

  3. Resonantly Enhanced Betatron Hard X-rays from Ionization Injected Electrons in a Laser Plasma Accelerator.

    PubMed

    Huang, K; Li, Y F; Li, D Z; Chen, L M; Tao, M Z; Ma, Y; Zhao, J R; Li, M H; Chen, M; Mirzaie, M; Hafz, N; Sokollik, T; Sheng, Z M; Zhang, J

    2016-01-01

    Ultrafast betatron x-ray emission from electron oscillations in laser wakefield acceleration (LWFA) has been widely investigated as a promising source. Betatron x-rays are usually produced via self-injected electron beams, which are not controllable and are not optimized for x-ray yields. Here, we present a new method for bright hard x-ray emission via ionization injection from the K-shell electrons of nitrogen into the accelerating bucket. A total photon yield of 8 × 10(8)/shot and 10(8 )photons with energy greater than 110 keV is obtained. The yield is 10 times higher than that achieved with self-injection mode in helium under similar laser parameters. The simulation suggests that ionization-injected electrons are quickly accelerated to the driving laser region and are subsequently driven into betatron resonance. The present scheme enables the single-stage betatron radiation from LWFA to be extended to bright γ-ray radiation, which is beyond the capability of 3(rd) generation synchrotrons. PMID:27273170

  4. Resonantly Enhanced Betatron Hard X-rays from Ionization Injected Electrons in a Laser Plasma Accelerator

    NASA Astrophysics Data System (ADS)

    Huang, K.; Li, Y. F.; Li, D. Z.; Chen, L. M.; Tao, M. Z.; Ma, Y.; Zhao, J. R.; Li, M. H.; Chen, M.; Mirzaie, M.; Hafz, N.; Sokollik, T.; Sheng, Z. M.; Zhang, J.

    2016-06-01

    Ultrafast betatron x-ray emission from electron oscillations in laser wakefield acceleration (LWFA) has been widely investigated as a promising source. Betatron x-rays are usually produced via self-injected electron beams, which are not controllable and are not optimized for x-ray yields. Here, we present a new method for bright hard x-ray emission via ionization injection from the K-shell electrons of nitrogen into the accelerating bucket. A total photon yield of 8 × 108/shot and 108 photons with energy greater than 110 keV is obtained. The yield is 10 times higher than that achieved with self-injection mode in helium under similar laser parameters. The simulation suggests that ionization-injected electrons are quickly accelerated to the driving laser region and are subsequently driven into betatron resonance. The present scheme enables the single-stage betatron radiation from LWFA to be extended to bright γ-ray radiation, which is beyond the capability of 3rd generation synchrotrons.

  5. Observation of the 5p Rydberg states of sulfur difluoride radical by resonance-enhanced multiphoton ionization spectroscopy.

    PubMed

    Zhang, Qun; Zhou, Xiaoguo; Li, Quanxin; Yu, Shuqin; Ma, Xingxiao

    2008-04-14

    Sulfur difluoride radicals in their ground state have been produced by a "laser-free" pulsed dc discharge of the SF6Ar gas mixtures in a supersonic molecular beam and detected by mass-selective resonance-enhanced multilphoton ionization (REMPI) spectroscopy in the wavelength range of 408-420 nm. Analyses of the (3+1) REMPI excitation spectrum have enabled identification of three hitherto unknown Rydberg states of this radical. Following the Rydberg state labeling in our previous work [see J. Phys. Chem. A 102, 7233 (1998)], these we label the K(5p1) [nu 0-0=71 837 cm(-1), omega'1(a1 sym str)=915 cm(-1)], L(5p2) [nu 0-0=72 134 cm(-1), omega'1(a1 sym str)=912 cm(-1)], and M(5p3) [nu 0-0=72 336 cm(-1), omega'1(a1 sym str)=926 cm(-1)] Rydberg states, respectively. [Origins, relative to the lowest vibrational level of the X 1A1 ground state, and vibrational frequencies of the symmetric S-F stretching mode are suggested by the numbers in brackets.] Photofragmentation process of SF2+-->SF+ +F that relates to the REMPI spectrum was discussed. PMID:18412444

  6. Evaluating the Aging of Multiple Emulsions Using Resonance-Enhanced Multiphoton Ionization Time-of-Flight Mass Spectrometry.

    PubMed

    Tsuda, Yukihiro; Uchimura, Tomohiro

    2016-01-01

    Resonance-enhanced multiphoton ionization time-of-flight mass spectrometry was applied to measurements of multiple emulsions with no pretreatment; a method for the quantitative evaluation of aging was proposed. We prepared water-in-oil-in-water (W/O/W) multiple emulsions containing toluene and m-phenylenediamine. The samples were measured immediately following both preparation and after having been stirred for 24 h. Time profiles of the peak areas for each analyte species were obtained, and several intense spikes for toluene could be detected from each sample after stirring, which suggests that the concentration of toluene in the middle phase had increased during stirring. On the other hand, in the case of a W/O/W multiple emulsion containing phenol and m-phenylenediamine, spikes for m-phenylenediamine, rather than phenol, were detected after stirring. In the present study, the time-profile data were converted into a scatter plot in order to quantitatively evaluate the aging. As a result, the ratio of the plots where strong signal intensities of toluene were detected increased from 8.4% before stirring to 33.2% after stirring for 24 h. The present method could be a powerful tool for evaluating multiple emulsions, such as studies on the kinetics of the encapsulation and release of active ingredients. PMID:27396662

  7. Resonance Enhanced Multi-Photon Ionization (rempi) and Double Resonance Uv-Uv and Ir-Uv Spectroscopic Investigation Isocytosine

    NASA Astrophysics Data System (ADS)

    Lee, Seung Jun; Min, Ahreum; Ahn, Ahreum; Moon, Cheol Joo; Choi, Myong Yong; Ishiuchi, Shun-Ichi; Miyazaki, Mitsuhiko; Fujii, Masaaki

    2013-06-01

    Isocytosine(iC), 2-aminouracil, is a non-natural nucleobase and its functional group's positions resemble those of guanine; therefore, its spectroscopic investigation is worthy of attention especially for the natural/unnatural base pairs with guanine and isoguanine. In this study, resonance enhanced multi-photon ionization (REMPI) and UV/IR-UV double resonance spectra of iC in the gas phase are presented. The collaboration work between Tokyo Institute of Technology, Japan and Gyeongsang National University, Korea using laser ablation and thermal evaporation, respectively, for producing jet-cooled iC is presented and discussed. The REMPI spectrum of iC monomers is recorded in the spectral range of 35000 to 36400cm-1, showing very congested π-π* vibronic bands. UV-UV hole burning spectroscopy is further conducted to investigate the conformational landscapes of iC monomers. Moreover, the presence of free OH band from IR-UV double resonance spectroscopy in combination with quantum chemical calculations convinces that the iC monomer in free-jet expansion experiment is an enol tautomer. However, a possible presence of a keto tautomer of iC may be provided by employing a pico-second experiment on iC.

  8. Zero kinetic energy photoelectron spectroscopy of jet cooled benzo[a]pyrene from resonantly enhanced multiphoton ionization

    NASA Astrophysics Data System (ADS)

    Zhang, Jie; Harthcock, Colin; Han, Fangyuan; Kong, Wei

    2011-12-01

    We report zero kinetic energy (ZEKE) photoelectron spectroscopy of benzo[a]pyrene (BaP) via resonantly enhanced multiphoton ionization (REMPI). Our analysis concentrates on the vibrational modes of the first excited state (S1) and those of the ground cationic state (D0). Similar to pyrene, another peri-condensed polycyclic aromatic hydrocarbon we have investigated, the first two electronically excited states of BaP exhibit extensive configuration interactions. However, the two electronic states are of the same symmetry, hence vibronic coupling does not introduce any out-of-plane modes in the REMPI spectrum, and Franck-Condon analysis is qualitatively satisfactory. The ZEKE spectra from the in-plane modes observed in the REMPI spectrum demonstrate strong propensity in preserving the vibrational excitation of the intermediate state. Although several additional bands in combination with the vibrational mode of the intermediate state are identifiable, they are much lower in intensity. This observation implies that the molecular structure of BaP has a tremendous capability to accommodate changes in charge density. All observed bands of the cation are IR active, establishing the role of ZEKE spectroscopy in mapping out far infrared bands for astrophysical applications.

  9. Rotationally resolved photoelectron spectra in resonance enhanced multiphoton ionization of HCl via the F 1Δ2 Rydberg state

    NASA Astrophysics Data System (ADS)

    Wang, Kwanghsi; McKoy, V.

    1991-12-01

    Results of studies of rotational ion distributions in the X 2Π3/2 and X 2Π1/2 spin-orbit states of HCl+ resulting from (2+1') resonance enhanced multiphoton ionization (REMPI) via the S(0) branch of the F 1Δ2 Rydberg state are reported and compared with measured threshold-field-ionization zero-kinetic-energy spectra reported recently [K. S. Haber, Y. Jiang, G. Bryant, H. Lefebvre-Brion, and E. R. Grant, Phys. Rev. A (in press)]. These results show comparable intensities for J+=3/2 of the X 2Π3/2 ion and J+=1/2 of the X 2Π1/2 ion. Both transitions require an angular momentum change of ΔN=-1 upon photoionization. To provide further insight into the near-threshold dynamics of this process, we also show rotationally resolved photoelectron angular distributions, alignment of the ion rotational levels, and rotational distributions for the parity components of the ion rotational levels. About 18% population is predicted to occur in the (+) parity component, which would arise from odd partial-wave contributions to the photoelectron matrix element. This behavior is similar to that in (2+1) REMPI via the S(2) branch of the F 1Δ2 state of HBr and was shown to arise from significant l mixing in the electronic continuum due to the nonspherical molecular ion potential. Rotational ion distributions resulting from (2+1) REMPI via the S(10) branch of the F 1Δ2 state are also shown.

  10. Photoionization Dynamics and Ion State Distributions in Single-Photon and Resonance-Enhanced Multiphoton Ionization of Molecules.

    NASA Astrophysics Data System (ADS)

    Braunstein, Matthew

    This thesis presents results of theoretical studies of single-photon ionization and resonance enhanced multiphoton ionization (REMPI) of several small molecules. The first part of the thesis examines shape resonances in the photoionization of O_2. Studies reported here include investigations of branching ratios of electronic multiplet states in the 3sigma _{g} and 1pi_ {u} photoionization of O_2 and a comparison of photoionization of the singlet states, a ^1Delta_{g} and d ^1prod_{g } (3ssigma_{g} 1pi_{g}), with that of the ground state of O_2. These studies show that the electronic exchange interaction between the ion core and the photoelectron in shape resonant energy regions profoundly affects the electronic state distributions of the molecular ion. We also report vibrational branching ratios in the single-photon ionization of O_2 , and in REMPI of O_2 via the G^3prod_{g} Rydberg state. In these studies, we find that a shape resonance causes a dependence of the electronic transition moment on the molecular geometry leading to non-Franck -Condon ion vibrational distributions and a dependence of the rotational branch intensity on the ion vibrational state. The second part of this thesis examines shape resonances in other molecules, focusing on the more general aspects of the photoionization dynamics. Here we present studies of the vibrational state distributions in the 7 sigma photoionization of the polyatomic N_2O, where a shape resonance causes non-Franck-Condon vibrational state distributions, the degree of which depends on the nuclear displacements involved and whether the shape resonance is localized on a particular bond. We also study the photoionization dynamics of the valence shell of Cl_2, where a shape resonance is also seen. Finally, we present studies of the K-shell ionization of CO. Studies in this energy region have assumed a new importance with the development of tunable X-ray synchrotron sources. Here, electronic relaxation in the production of a K

  11. Alignment and pulse-duration effects in two-photon double ionization of H2 by femtosecond XUV laser pulses

    NASA Astrophysics Data System (ADS)

    Guan, Xiaoxu; Bartschat, Klaus; Schneider, Barry I.; Koesterke, Lars

    2014-10-01

    We present calculations for the dependence of the two-photon double ionization (DI) of H2 on the relative orientation of the linear laser polarization to the internuclear axis and the length of the pulse. We use the fixed-nuclei approximation at the equilibrium distance of 1.4 a0, where a0=0.529 ×10-10m is the Bohr radius. Central photon energies cover the entire direct DI domain from 26.5 to 34.0 eV. In contrast to the parallel geometry studied earlier [X. Guan, K. Bartschat, B. I. Schneider, and L. Koesterke, Phys. Rev. A 83, 043403 (2011), 10.1103/PhysRevA.83.043403], the effect of the pulse duration is almost negligible for the case when the two axes are perpendicular to each other. This is a consequence of the symmetry rules for dipole excitation in the two cases. In the parallel geometry, doubly excited states of 1Σu+ symmetry affect the cross section, while in the perpendicular geometry only much longer-lived 1Πu states are present. This accounts for the different convergence patterns observed in the calculated cross sections as a function of the pulse length. When the photon energy approaches the threshold of sequential DI, a sharp increase of the generalized total cross section (GTCS) with increasing pulse duration is also observed in the perpendicular geometry, very similar to the case of the molecular axis being oriented along the laser polarization direction. Our results differ from those of Colgan et al. [J. Colgan, M. S. Pindzola, and F. Robicheaux, J. Phys. B 41, 121002 (2008), 10.1088/0953-4075/41/12/121002] and Morales et al. [F. Morales, F. Martín, D. A. Horner, T. N. Rescigno, and C. W. McCurdy, J. Phys. B 42, 134013 (2009), 10.1088/0953-4075/42/13/134013], but are in excellent agreement with the GTCSs of Simonsen et al. [A. S. Simonsen, S. A. Sørngård, R. Nepstad, and M. Førre, Phys. Rev. A 85, 063404 (2012), 10.1103/PhysRevA.85.063404] over the entire domain of direct DI.

  12. Investigation of the photoionization properties of pharmaceutically relevant substances by resonance-enhanced multiphoton ionization spectroscopy and single-photon ionization spectroscopy using synchrotron radiation.

    PubMed

    Kleeblatt, Juliane; Ehlert, Sven; Hölzer, Jasper; Sklorz, Martin; Rittgen, Jan; Baumgärtel, Peter; Schubert, Jochen K; Zimmermann, Ralf

    2013-08-01

    The photoionization properties of the pharmaceutically relevant substances amantadine, diazepam, dimethyltryptamine, etomidate, ketamine, mescaline, methadone, and propofol were determined. At beamline U125/2-10m-NIM of the BESSY II synchrotron facility (Berlin, Germany) vacuum ultraviolet (VUV) photoionization spectra were recorded in the energy range 7.1 to 11.9 eV (174.6 to 104.2 nm), showing the hitherto unknown ionization energies and fragmentation appearance energies of the compounds under investigation. Furthermore, (1+1)-resonance-enhanced multiphoton ionization (REMPI) spectra of selected compounds (amantadine, diazepam, etomidate, ketamine, and propofol) were recorded by a continuous scan in the energy range between 3.6 and 5.7 eV (345 to 218 nm) using a tunable optical parametric oscillator (spectral resolution: 0.1 nm) laser system. The resulting REMPI wavelength spectra of these compounds are discussed and put into context with already known UV absorption data. Time-of-flight mass spectrometry was used for ion detection in both experiments. Finally, the implications of the obtained physical-chemical results for potential analytical applications are discussed. In this context, fast detection approaches for the considered compounds from breath gas using photoionization mass spectrometry and a rapid pre-concentration step (e.g., needle trap device) are of interest.

  13. Laser ablation with resonance-enhanced multiphoton ionization time-of-flight mass spectrometry for determining aromatic lignin volatilization products from biomass

    NASA Astrophysics Data System (ADS)

    Mukarakate, Calvin; Scheer, Adam M.; Robichaud, David J.; Jarvis, Mark W.; David, Donald E.; Ellison, G. Barney; Nimlos, Mark R.; Davis, Mark F.

    2011-03-01

    We have designed and developed a laser ablation/pulsed sample introduction/mass spectrometry platform that integrates pyrolysis (py) and/or laser ablation (LA) with resonance-enhanced multiphoton ionization (REMPI) reflectron time-of-flight mass spectrometry (TOFMS). Using this apparatus, we measured lignin volatilization products of untreated biomass materials. Biomass vapors are produced by either a custom-built hot stage pyrolysis reactor or laser ablation using the third harmonic of an Nd:YAG laser (355 nm). The resulting vapors are entrained in a free jet expansion of He, then skimmed and introduced into an ionization region. One color resonance-enhanced multiphoton ionization (1+1 REMPI) is used, resulting in highly selective detection of lignin subunits from complex vapors of biomass materials. The spectra obtained by py-REMPI-TOFMS and LA-REMPI-TOFMS display high selectivity and decreased fragmentation compared to spectra recorded by an electron impact ionization molecular beam mass spectrometer (EI-MBMS). The laser ablation method demonstrates the ability to selectively isolate and volatilize specific tissues within the same plant material and then detect lignin-based products from the vapors with enhanced sensitivity. The identification of select products observed in the LA-REMPI-TOFMS experiment is confirmed by comparing their REMPI wavelength scans with that of known standards.

  14. Laser ablation with resonance-enhanced multiphoton ionization time-of-flight mass spectrometry for determining aromatic lignin volatilization products from biomass.

    PubMed

    Mukarakate, Calvin; Scheer, Adam M; Robichaud, David J; Jarvis, Mark W; David, Donald E; Ellison, G Barney; Nimlos, Mark R; Davis, Mark F

    2011-03-01

    We have designed and developed a laser ablation∕pulsed sample introduction∕mass spectrometry platform that integrates pyrolysis (py) and∕or laser ablation (LA) with resonance-enhanced multiphoton ionization (REMPI) reflectron time-of-flight mass spectrometry (TOFMS). Using this apparatus, we measured lignin volatilization products of untreated biomass materials. Biomass vapors are produced by either a custom-built hot stage pyrolysis reactor or laser ablation using the third harmonic of an Nd:YAG laser (355 nm). The resulting vapors are entrained in a free jet expansion of He, then skimmed and introduced into an ionization region. One color resonance-enhanced multiphoton ionization (1+1 REMPI) is used, resulting in highly selective detection of lignin subunits from complex vapors of biomass materials. The spectra obtained by py-REMPI-TOFMS and LA-REMPI-TOFMS display high selectivity and decreased fragmentation compared to spectra recorded by an electron impact ionization molecular beam mass spectrometer (EI-MBMS). The laser ablation method demonstrates the ability to selectively isolate and volatilize specific tissues within the same plant material and then detect lignin-based products from the vapors with enhanced sensitivity. The identification of select products observed in the LA-REMPI-TOFMS experiment is confirmed by comparing their REMPI wavelength scans with that of known standards. PMID:21456715

  15. Laser induced avalanche ionization in gases or gas mixtures with resonantly enhanced multiphoton ionization or femtosecond laser pulse pre-ionization

    SciTech Connect

    Shneider, Mikhail N.; Miles, Richard B.

    2012-08-15

    The paper discusses the requirements for avalanche ionization in gas or gas mixtures initiated by REMPI or femtosecond-laser pre-ionization. Numerical examples of dependencies on partial composition for Ar:Xe gas mixture with REMPI of argon and subsequent classic avalanche ionization of Xe are presented.

  16. Fraunhofer-like diffracted lateral photoelectron momentum distributions of H2+ in charge-resonance-enhanced ionization in strong laser fields

    NASA Astrophysics Data System (ADS)

    Xin, Lin; Qin, Han-Cheng; Wu, Wan-Yang; He, Feng

    2015-12-01

    For H2+ at the critical internuclear distance where the charge-resonance-enhanced ionization is most prominent, the lateral photoelectron momentum distribution presents the Fraunhofer-like diffraction pattern: a central disk surrounded by one or more rings. We study this phenomenon by simulating the time-dependent Schrödinger equation and unveil the mechanism: the stretched molecule constructs an interatomic Coulomb potential, which works as a circular aperture and diffracts the electron when it travels between two nuclei. This distinct lateral photoelectron momentum distribution offers another perspective to look into molecular structures.

  17. Vibrations of the S{sub 1} state of fluorobenzene-h{sub 5} and fluorobenzene-d{sub 5} via resonance-enhanced multiphoton ionization (REMPI) spectroscopy

    SciTech Connect

    Harris, Joe P.; Andrejeva, Anna; Tuttle, William D.; Wright, Timothy G.; Pugliesi, Igor; Schriever, Christian

    2014-12-28

    We report resonance-enhanced multiphoton ionization spectra of the isotopologues fluorobenzene-h{sub 5} and fluorobenzene-d{sub 5}. By making use of quantum chemical calculations, the changes in the wavenumber of the vibrational modes upon deuteration are examined. Additionally, the mixing of vibrational modes both between isotopologues and also between the two electronic states is discussed. The isotopic shifts lead to dramatic changes in the appearance of the spectrum as vibrations shift in and out of Fermi resonance. Assignments of the majority of the fluorobenzene-d{sub 5} observed bands are provided, aided by previous results on fluorobenzene-h{sub 5}.

  18. 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.

  19. Two-photon double-ionization of the H2 molecule in light perpindicular to the internuclear axis: effects of pulse duration

    NASA Astrophysics Data System (ADS)

    Guan, Xiaoxu; Bartschat, Klaus; Schneider, Barry; Koesterke, Lars

    2014-05-01

    Earlier, we solved the time-dependent Schrödinger equation to calculate the two-photon double ionization of the hydrogen molecule induced by non-sequential absorption of photons with a central energy of 30 eV in a short laser pulse lasting for about 1.6 femtoseconds. The linear polarization of the radiation was aligned with the internuclear axis. At the equilibrium distance Req, several doubly excited 1Σg , u states, accessible through photon absorption,lie about 30 eV above the X1Σg ground state. These states are likely responsible for the significant disagreement seen in the literature for previous results on both angle-integrated and angle-differential cross sections. Here we continue to explore the fundamental role of doubly excited states on the two-photon break-up process,now for the even more difficult problem of laser polarization perpendicular to the internuclear axis. Such studies require relatively long laser pulses, thus making the calculations computationally very challenging.

  20. Fine- and hyperfine-structure effects in molecular photoionization. II. Resonance-enhanced multiphoton ionization and hyperfine-selective generation of molecular cations

    NASA Astrophysics Data System (ADS)

    Germann, Matthias; Willitsch, Stefan

    2016-07-01

    Resonance-enhanced multiphoton ionization (REMPI) is a widely used technique for studying molecular photoionization and producing molecular cations for spectroscopy and dynamics studies. Here, we present a model for describing hyperfine-structure effects in the REMPI process and for predicting hyperfine populations in molecular ions produced by this method. This model is a generalization of our model for fine- and hyperfine-structure effects in one-photon ionization of molecules presented in Paper I [M. Germann and S. Willitsch, J. Chem. Phys. 145, 044314 (2016)]. This generalization is achieved by covering two main aspects: (1) treatment of the neutral bound-bound transition including the hyperfine structure that makes up the first step of the REMPI process and (2) modification of our ionization model to account for anisotropic populations resulting from this first excitation step. Our findings may be used for analyzing results from experiments with molecular ions produced by REMPI and may serve as a theoretical background for hyperfine-selective ionization experiments.

  1. Angular and internal state distributions of H2 (+) generated by (2 + 1) resonance enhanced multiphoton ionization of H2 using time-of-flight mass spectrometry.

    PubMed

    Perreault, William E; Mukherjee, Nandini; Zare, Richard N

    2016-06-01

    We report direct measurement of the anisotropy parameter β for the angular distribution of the photoelectron and photoion in (2 + 1) resonance enhanced multiphoton ionization process of H2 X (1)Σg (+) (v = 0, J = 0) molecules through the intermediate H2 E,F (1)Σg (+) (v' = 0, J' = 0) level (λ = 201.684 nm) using a time-of-flight mass spectrometer. The time-of-flight spectra were recorded as the direction of polarization of the ionizing laser was varied with respect to the flight axis of the H2 molecular beam and were fitted to an angular distribution in an appropriately rotated coordinate system with the z-axis oriented along the time-of-flight axis. The anisotropy parameter β was found to be 1.72 ± 0.13 by fitting the time-of-flight spectra and agreed with previous measurements. Using secondary ionization with a delayed laser pulse of different wavelength, we also determined the vibrational energy distribution of the ions, showing that 98% ± 4% of the ions are generated in their ground vibrational state, in agreement with the calculated Franck-Condon factors between the H2 E,F (1)Σg (+) (v' = 0) and H2 (+) X (1)Σg (+) (v″) vibrational levels.

  2. Resonance enhanced multiphoton ionization photoelectron spectroscopy and pulsed field ionization via the F 1Delta 2(vscript=0) and f 3Delta 2(vscript=0) Rydberg states of HCl

    NASA Astrophysics Data System (ADS)

    de Beer, E.; Buma, W. J.; de Lange, C. A.

    1993-09-01

    In this paper, we report the first rotationally resolved one- and two-color resonance enhanced multiphoton ionization photoelectron spectroscopy (REMPI-PES) study of the HCl molecule. The agreement between our experimental branching ratios and theoretical investigations is excellent. We also report the first zero kinetic energy pulsed field ionization (ZEKE-PFI) experiments carried out in a ``magnetic bottle'' electron spectrometer. A direct comparison is made between ZEKE-PFI and REMPI-PES spectra for ionization via several rotational levels of the F 1Δ2(v'=0) and f 3Δ2(v'=0) Rydberg states of HCl. Large differences in both the spin-orbit and rotational branching ratios are found between the ZEKE-PFI and REMPI-PES spectra. These differences can be understood qualitatively on the basis of rotational and spin-orbit autoionization mechanisms.

  3. Observation of rotamers of m-aminobenzoic acid: Zero kinetic energy photoelectron and hole-burning resonantly enhanced multiphoton ionization spectroscopy

    NASA Astrophysics Data System (ADS)

    He, Yonggang; Wu, Chengyin; Kong, Wei

    2004-11-01

    We report studies of supersonically cooled m-aminobenzoic acid using two-color resonantly enhanced multiphoton ionization (REMPI) and two-color zero kinetic energy (ZEKE) photoelectron spectroscopy. Two conformers have been identified and characterized using the hole-burning method in the REMPI experiment. With the aid of ab initio and density functional calculations, vibrational modes of the first electronically excited state (S1) of the neutral species and those of the ground state cation (D0) have been assigned, and the adiabatic ionization potentials have been determined for both conformers. The REMPI spectra are dominated by in-plane motions of the substituents and ring deformation modes. A propensity of Δv=0, where Δv is the change in vibrational quantum number from the S1 to the D0 state, is observed in the ZEKE spectra. The origin of this behavior is discussed in the context of electron back donation from the two substituents in the excited state and in the cationic state. Comparisons of these results with those of p-aminobenzoic acid will be analyzed.

  4. Two-photon physics

    SciTech Connect

    Bardeen, W.A.

    1981-10-01

    A new experimental frontier has recently been opened to the study of two photon processes. The first results of many aspects of these reactions are being presented at this conference. In contrast, the theoretical development of research ito two photon processes has a much longer history. This talk reviews the many different theoretical ideas which provide a detailed framework for our understanding of two photon processes.

  5. Ionic rotational branching ratios in resonant enhanced multiphoton ionization of NO via the A2Sigma(+)(3s sigma) and D2Sigma(+)(3p sigma) states

    NASA Astrophysics Data System (ADS)

    Rudolph, H.; McKoy, V.; Dixit, S. N.; Huo, W. M.

    1988-01-01

    Results are presented for the rotationally resolved photoelectron spectra resulting from a (2 + 1) one-color resonant enhanced multiphoton ionization (REMPI) of NO via the rotationally clean S21(11.5) and mixed S11(15.5) + R21(15.5) branches of the 0-0 transition in the D-X band. The calculations were done in the fixed-nuclei frozen core approximation. The resulting photoionization spectra, convoluted with a Lorentzian detection function, agree qualitatively with experimental results of Viswanathan et al. (1986) and support their conclusion that the nonspherical nature of the molecular potential creates a substantial l-mixing in the continuum, which in turn leads to the intense Delta N = 0 peak. The rather strong photoelectron energy dependence of the rotational branching ratios of the D 2Sigma(+) S21(11.5) line was investigated and compared to the weak energy dependence of the A 2Sigma(+) R22(21.5) line.

  6. Two-color resonance-enhanced multiphoton ionization study of the lowest Rydberg p state of bis(ɛ6-benzene)chromium and its deuterated derivatives

    NASA Astrophysics Data System (ADS)

    Ketkov, Sergey Yu.; Selzle, Heinrich L.; Schlag, Edward W.

    2004-07-01

    Two-color resonance-enhanced multiphoton ionization (REMPI) spectra of jet-cooled (η6-C6H6)2Cr(1), (η6-C6D6)2Cr(2), and (η6-C6D6)(η6-C6D5H)Cr(3) have been measured with use of the 3dz2→R4px,y Rydberg transition as the first step of the electronic excitation. The 000 Rydberg component shifts by 59 and 54 cm-1 to red when one goes from 1 to 2 and 3, respectively. Surprisingly, the REMPI spectra of 1-3 show very rich vibronic structures revealing both totally symmetric vibrations and degenerate vibrational modes. Presence of intense peaks corresponding to the e2g modes in the spectra of 1 and 2 is indicative of Jahn-Teller coupling in the R4px,y Rydberg state. Additional REMPI resonances appear on going from 1 and 2 to 3 as a result of the symmetry reduction. The vibronic components in the spectra of 1-3 were assigned on the basis of the selection rules and comparison with the vibrational frequencies of the 1 and 2 ground-state molecules. The frequencies of over 10 normal vibrations have been determined for the gas-phase 1-3 Rydberg-state molecules from the REMPI experiment. The wavenumber corresponding to the lowest-energy mode (the ring torsion vibration) appears to be 40 cm-1 in 1 and 35 cm-1 in the deuterated complexes. The REMPI peaks are homogeneously broadened. The lower lifetime limits for the upper-state components increase on going from the vibrationless level to higher-lying vibronic states and on going from 1 to the deuterated derivatives.

  7. Resonance Enhanced Multi-photon Spectroscopy of DNA

    NASA Astrophysics Data System (ADS)

    Ligare, Marshall Robert

    For over 50 years DNA has been studied to better understand its connection to life and evolution. These past experiments have led to our understanding of its structure and function in the biological environment but the interaction of DNA with UV radiation at the molecular level is still not very well understood. Unique mechanisms in nucleobase chromaphores protect us from adverse chemical reactions after UV absorption. Studying these processes can help develop theories for prebiotic chemistry and the possibility of alternative forms of DNA. Using resonance enhanced multi-photon spectroscopic techniques in the gas phase allow for the structure and dynamics of individual nucleobases to be studied in detail. Experiments studying different levels of structure/complexity with relation to their biological function are presented. Resonant IR multiphoton dissociation spectroscopy in conjunction with molecular mechanics and DFT calculations are used to determine gas phase structures of anionic nucleotide clusters. A comparison of the identified structures with known biological function shows how the hydrogen bonding of the nucleotides and their clusters free of solvent create favorable structures for quick incorporation into enzymes such as DNA polymerase. Resonance enhanced multi-photon ionization (REMPI) spectroscopy techniques such as resonant two photon ionization (R2PI) and IR-UV double resonance are used to further elucidate the structure and excited state dynamics of the bare nucleobases thymine and uracil. Both exhibit long lived excited electronic states that have been implicated in DNA photolesions which can ultimately lead to melanoma and carcinoma. Our experimental data in comparison with many quantum chemical calculations suggest a new picture for the dynamics of thymine and uracil in the gas phase. A high probability of UV absorption from a vibrationally hot ground state to the excited electronic state shows that the stability of thymine and uracil comes from

  8. Capillary column gas chromatography, resonance enhanced multiphoton ionization, time-of-flight mass spectrometry, laser-induced fluorescence, flame ionization detection system for the determination of polynuclear aromatic compounds in complex mixtures

    SciTech Connect

    Dobson, R.L.M.

    1986-01-01

    A method is reached to fully characterize the polynuclear aromatic hydrocarbons (PAC) that have been deemed to be highly mutagenic or carcinogenic. A multidimensional, laser-based analytical instrument has been developed that, when utilized to the full extent of its capabilities could be the solution to this complex analytical problem. The overall technique is termed Capillary Column Gas Chromatography, Resonance Enhanced Multiphoton Ionization, Time-of-Flight Mass Spectrometry, Laser-induced Fluorescence, with parallel Flame Ionization Detection (CC/GC-REMPI-TOF/MS-LIF-FID). This system combines the selectivity of two complementary laser-based methods, REMPI and LIF, with an extremely powerful and proven analytical tool, GC/MS. The GC effluent passes through the ion source of a TOF/MS, where it is interrogated by a tunable ultraviolet laser beam. Thus, PAC and other absorbing species may be selectively excited and/or ionized in the presence of nonabsorbing components. All laser-analyte interaction products (actions, electrons, and photons) are simultaneously monitored utilizing the TOF/MS, a total electron current detector (TECD), and a LIF detector. The main advantage of this technique is that all analytically useful data for each absorbing chromatographic eluent may be collected on-the-fly. The simultaneous availability of this information simplifies the characterization task. The present absolute detection limits for several PAC have been determined to be low picogram range. Also, a linear dynamic range of approximately four orders of magnitude has been established for the TECD, indicating that this technique is both sensitive and quantitative. Further, the use of deuterated analogs, of selected PAC, as internal reference standards greatly assists in quantitation.

  9. Capillary column gas chromatography, resonance enhanced multiphoton ionization, time-of-flight mass spectrometry laser-induced fluorescence, flame ionization detection system for the determination of polynuclear aromatic compounds in complex mixtures

    SciTech Connect

    Dobson, R.L.M.

    1986-06-01

    Of the thousands of chemical compounds that have been deemed mutagenic or carcinogenic, it is generally agreed that the polynuclear aromatic hydrocarbons (PAC) are among the most potent. Because of the wide range of potency of PAC, even among geometric isomers and substitutional derivatives, it is important to fully characterize these samples. This task is a formidable one, usually requiring elaborate sample clean-up and fractionation prior to analysis. A multidimensional, laser-based analytical instrument has been developed that, when utilized to the full extent of its capabilities, could be the solution to this complex analytical problem. The overall technique is termed Capillary Column Gas Chromatography, Resonance Enhanced Multiphoton Ionization, Time-Of-Flight Mass Spectrometry, Laser-induced Fluorescence, with parallel Flame Ionization Detection (CC/GC-REMPI-TOF/MS-LIF-FID). This system combines the selectivity and sensitivity of two complementary laser-based methods, REMPI and LIF, with an extremely powerful and proven analytical tool, GC/MS. The GC effluent passes through the ion source of a TOF/MS, where it is interrogated by a tunable ultraviolet laser beam. All laser-analyte interaction products (cations, electrons, and photons) are simultaneously monitored utilizing the TOF/MS, a total electron current detector (TECD), and a LIF detector. The simultaneous availability of this information simplifies the characterization task. The present absolute detection limits for several PAC have been determined to be in the low picogram range. Also, a linear dynamic range of approximately four orders of magnitude has been established for the TECD, indicating that this technique is both sensitive and quantitative. Further, the use of deuterated analogs, of selected PAC, as internal reference standards greatly assists in quantitation. 219 refs., 37 figs., 13 tabs.

  10. Resonance enhanced tunneling

    NASA Astrophysics Data System (ADS)

    Matsumoto, S.; Yoshimura, M.

    2000-12-01

    Time evolution of tunneling in thermal medium is examined using the real-time semiclassical formalism previously developed. Effect of anharmonic terms in the potential well is shown to give a new mechanism of resonance enhanced tunneling. If the friction from environment is small enough, this mechanism may give a very large enhancement for the tunneling rate. The case of the asymmetric wine bottle potential is worked out in detail.

  11. A 1 + 1' resonance-enhanced multiphoton ionization scheme for rotationally state-selective detection of formaldehyde via the à (1)A2 ← X[combining tilde] (1)A1 transition.

    PubMed

    Park, G Barratt; Krüger, Bastian C; Meyer, Sven; Wodtke, Alec M; Schäfer, Tim

    2016-08-10

    The formaldehyde molecule is an important model system for understanding dynamical processes in small polyatomic molecules. However, prior to this work, there have been no reports of a resonance-enhanced multiphoton ionization (REMPI) detection scheme for formaldehyde suitable for rovibrationally state-selective detection in molecular beam scattering experiments. Previously reported tunable REMPI schemes are either non-rotationally resolved, involve multiple resonant steps, or involve many-photon ionization steps. In the current work, we present a new 1 + 1' REMPI scheme for formaldehyde. The first photon is tunable and provides rotational resolution via the vibronically allowed à (1)A2 ← X[combining tilde] (1)A1 transition. Molecules are then directly ionized from the à state by one photon of 157 nm. The results indicate that the ionization cross section from the 4(1) vibrational level of the à state is independent of the rotational level used as intermediate, to within experimental uncertainty. The 1 + 1' REMPI intensities are therefore directly proportional to the à ← X[combining tilde] absorption intensities and can be used for quantitative measurement of X[combining tilde]-state population distributions.

  12. Studies of structural isomers o-, m-, and p-fluorophenylacetylene by two-color resonant two-photon mass-analyzed threshold ionization spectroscopy.

    PubMed

    Shivatare, Vidya S; Kundu, Aniket; Patwari, G Naresh; Tzeng, Wen Bih

    2014-09-18

    We report the vibrational spectra of o-fluorophenylacetylene (OFPA), m-fluorophenylacetylene (MFPA), and p-fluorophenylacetylene (PFPA) in the electronically excited S1 and cationic ground D0 states. These new data show that the relative location of the fluorine atom with respect to the acetylenic group can influence the transition energy and molecular vibration. The adiabatic ionization energies of these structural isomers follow the order: PFPA < OFPA < MFPA. It is found that the molecular geometries of these molecules in the D0 state resemble those in the S1 state. Detailed spectral analysis suggests that the in-plane ring deformation vibrations are slightly "harder" in the D0 state than the corresponding ones in the S1 state.

  13. Feasibility of two-photon rotational spectroscopy on trapped HD+

    NASA Astrophysics Data System (ADS)

    Constantin, Florin L.

    2016-04-01

    Calculations of frequencies, transition rates, lineshapes and lightshifts of two-photon rotational transitions of HD+ in the ground vibrational state are presented. Two-photon rotational transitions can be addressed at high transition rates despite of the scarcity of sources of radiation in the THz spectral domain. A resonance-enhanced multiphoton dissociation detection scheme addresses the two-photon rotational transition (v,J)=(0,1)-<(0,2)-<(0,3) at 3.268 THz, the two-photon rovibrational transition (v,J)=(0,3)->4,2)->(9,3) at 1.4 μm and the photodissociation of (v,J)=(9,3) level at 512 nm on trapped and sympathetically cooled HD+ ions in the Lamb-Dicke regime. The photodissociated fraction of HD+ ions, modeled by rate equations, increases significantly at two-photon resonances when the rotational levels are coupled with the two-photon transition. A REMPD scheme with narrow-linewidth optical and THz sources may push the resolution of rotational spectroscopy at 4×10-13.

  14. Analysis of the (1)A' S1 ← (1)A' S0 and (2)A' D0 ← (1)A' S1 band systems in 1,2-dichloro-4-fluorobenzene by means of resonance-enhanced-multi-photon-ionization (REMPI) and mass-analyzed-threshold-ionization (MATI) spectroscopy.

    PubMed

    Krüger, Sascha; Grotemeyer, Jürgen

    2016-03-14

    Resonance enhanced multiphoton ionization (REMPI) and mass analyzed threshold ionization (MATI) spectroscopy have been applied in order to investigate the vibrational structure of 1,2-dichloro-4-fluorobenzene (1,2,4-DCFB) in its first excited state (S1) and the cationic ground state (D0). The selection of the state prior to ionization resulted in MATI spectra with different intensity distributions thus giving access to many vibrational levels. To support the experimental findings, geometry optimizations and frequency analyses at DFT (density functional) and TDDFT (time-dependent density functional) levels of theory have been applied. Additionally, a multidimensional Franck-Condon approach has been used to calculate the vibrational intensities from the DFT calculations. An excellent agreement between simulated and measured REMPI and MATI spectra allowed for a confident assignment of vibrational levels and mechanisms active during excitation and ionization. In order to avoid any ambiguity regarding the assignment of the vibrational bands to normal modes, Duschinsky normal mode analysis has been performed to correlate the ground state (S0) normal modes of 1,2,4-DCFB with the benzene derived Wilson nomenclature. From the REMPI spectra the electronic excitation energy (EE) of 1,2-dichloro-4-fluorobenzene could be determined to be 35 714 ± 2 cm(-1) while the MATI spectra yielded the adiabatic ionization energy (IE) of 1,2-dichloro-4-fluorobenzene which could be determined to be 73 332 ± 7 cm(-1).

  15. 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.

  16. Two Photon Polymerization of Ormosils

    NASA Astrophysics Data System (ADS)

    Matei, A.; Zamfirescu, M.; Jipa, F.; Luculescu, C.; Dinescu, M.; Buruiana, E. C.; Buruiana, T.; Sima, L. E.; Petrescu, S. M.

    2010-10-01

    In this work, 3D structures of hybrid polymers—ORMOSILS (organically modified silicates) were produced via Two Photon Polymerization (2PP) of hybrid methacrylates based on silane derivates. Synthetic routes have been used to obtain series of hybrid monomers, their structure and purity being checked by NMR Spectroscopy and Fourier Transform Infrared Spectroscopy. Two photon polymerization method (a relatively new technology which allows fast micro and nano processing of three-dimensional structures with application in medical devices, tissue scaffolds, photonic crystals etc) was used for monomers processing. As laser a Ti: Sapphire laser was used, with 200 fs pulse duration and 2 kHz repetition rate, emitting at 775 nm. A parametric study on the influence of the processing parameters (laser fluence, laser scanning velocity, photo initiator) on the written structures was carried out. The as prepared polymeric scaffolds were tested in mesenchymal stem cells and fibroblasts cell cultures, with the aim of further obtaining bone and dermal grafts. Cells morphology, proliferation, adhesion and alignment were analyzed for different experimental conditions.

  17. Two-photon excitation of aluminium phthalocyanines

    SciTech Connect

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

    1999-12-31

    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. (lasers in medicine)

  18. A velocity map imaging study of the one and two photon dissociations of state-selected DCl+ cations

    NASA Astrophysics Data System (ADS)

    Webb, Alexander D.; Nahler, N. Hendrik; Dixon, Richard N.; Ashfold, Michael N. R.

    2006-11-01

    DCl+(XΠ3/22,v+'=0) cations have been prepared by 2+1 resonance enhanced multiphoton ionization, and their subsequent fragmentation following excitation at numerous wavelengths in the range of 240-350nm studied by velocity map imaging of the resulting Cl+ products. This range of excitation wavelengths allows selective population of AΣ+2 state levels with all vibrational (v+') quantum numbers in the range 0⩽v+'⩽15. Image analysis yields wavelength dependent branching ratios and recoil anisotropies of the various D +Cl+ (PJ3, D1, and S1) product channels. Levels with 10⩽v+'⩽15 have sufficient energy to predissociate, forming D +Cl+(PJ3) products with perpendicular recoil anisotropies—consistent with the AΣ+2←XΠ2 parent excitation and subsequent fragmentation on a time scale that is fast compared with the parent rotational period. Branching into the various spin-orbit states of the Cl+(PJ3) product is found to depend sensitively upon v+' and, in the case of the v+'=13 level, to vary with the precise choice of excitation wavelength within the AΣ+2←XΠ2(13,0) band. Such variations have been rationalized qualitatively in terms of the differing contributions made to the overall predissociation rate of DCl+(A,v+') molecules by coupling to repulsive states of Π4, Σ-4, and Σ-2 symmetries, all of which are calculated to cross the outer limb of the AΣ+2 state potential at energies close to that of the v+'=10 level. Cl+(PJ3) fragments are detected weakly following excitation to AΣ+2 state levels with v+'=0 or 1, Cl+(D1) fragments dominate the ion yield when exciting via 2⩽v+'⩽6 and via v+'=9, while Cl+(S1) fragments dominate the Cl+ images obtained when exciting via levels with v+'=7 and 8. Analysis of wavelength resolved action spectra for forming these Cl+ ions and of the resulting Cl+ ion images shows that (i) these ions all arise via two photon absorption processes, resonance enhanced at the one photon energy by the various A(v+'<10) levels, (ii

  19. Two-Photon Physics in Hadronic Processes

    SciTech Connect

    Carl Carlson; Marc Vanderhaeghen

    2007-11-01

    Two-photon exchange contributions to elastic electron-scattering are reviewed. The apparent discrepancy in the extraction of elastic nucleon form factors between unpolarized Rosenbluth and polarization transfer experiments is discussed, as well as the understanding of this puzzle in terms of two-photon exchange corrections. Calculations of such corrections both within partonic and hadronic frameworks are reviewed. In view of recent spin-dependent electron scattering data, the relation of the two-photon exchange process to the hyperfine splitting in hydrogen is critically examined. The imaginary part of the two-photon exchange amplitude as can be accessed from the beam normal spin asymmetry in elastic electron-nucleon scattering is reviewed. Further extensions and open issues in this field are outlined.

  20. Two-Photon Laser Scanning Microscopy

    NASA Astrophysics Data System (ADS)

    Nimmerjahn, A.; Theer, P.; Helmchen, F.

    Since its inception more than 15 years ago, two-photon laser scanning microscopy (2PLSM) has found widespread use in biological and medical research. Two-photon microscopy is based on simultaneous absorption of two photons by fluorophores and subsequent fluorescence emission, a process which under normal illumination conditions is highly improbable. Theoretically described around 1930 by Maria Göppert-Mayer [1], the first experimental demonstration of two-photon excitation had to await the invention of the laser, which produced sufficiently high light intensities to observe two-photon absorption events [2]. Only after the development of ultrafast lasers providing subpicosecond light pulses with high peak power intensities, however, two-photon-excited fluorescence became practical in a laser-scanning microscope [3]. Since then 2PLSM has developed into the method of choice for high-resolution imaging in living animals (reviewed in [4,5]). One of the main reasons is the low sensitivity of 2PLSM to light scattering, which enables imaging relatively deep inside biological tissue and direct observation of the dynamic behavior of cells in their native environment. In this chapter, we introduce the physical principles governing 2PLSM and briefly describe the key instrument components. We give an overview of fluorescence labeling techniques and how they are combined with 2PLSM for functional imaging and photomanipulation in living tissue. Finally, we discuss limitations and provide some future perspectives.

  1. 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

  2. The two-photon Rydberg atom micromaser

    SciTech Connect

    Brune, M.; Raimond, J.M.; Goy, P.; Davidovich, L.; Haroche, S.

    1988-07-01

    The authors recently operated a Rydberg atom maser on a two-photon degenerate atomic transition. This device combines two interesting features: it is a quantum oscillator working on an intrinsically nonlinear effect and it is a micromaser, with only a few atoms and few tens of photons at a time in the cavity. In this paper, they discuss why Rydberg atom-superconducting cavity systems are well adapted for two-photon maser studies and the authors analyze the main properties of this new device by comparing it to Rydberg masers operating on one-photon transitions.

  3. 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. PMID:18596366

  4. Resonantly Enhanced Pair Production in a Simple Diatomic Model

    NASA Astrophysics Data System (ADS)

    Fillion-Gourdeau, François; Lorin, Emmanuel; Bandrauk, André D.

    2013-01-01

    A new mechanism for the production of electron-positron pairs from the interaction of a laser field and a fully ionized diatomic molecule in the tunneling regime is presented. When the laser field is turned off, the Dirac operator has resonances in both the positive and the negative energy continua while bound states are in the mass gap. When this system is immersed in a strong laser field, the resonances move in the complex energy plane: the negative energy resonances are pushed to higher energies while the bound states are Stark shifted [F. Fillion-Gourdeau , J. Phys. A 45, 215304 (2012)JPHAC50305-4470]. It is argued here that there is a pair production enhancement at the crossing of resonances by looking at a simple one-dimensional model: the nuclei are modeled simply by Dirac delta potential wells while the laser field is assumed to be static and of finite spatial extent. The average rate for the number of electron-positron pairs produced is evaluated and the results are compared to the one and zero nucleus cases. It is shown that positrons are produced by the resonantly enhanced pair production mechanism, which is analogous to the resonantly enhanced ionization of molecular physics. This phenomenon could be used to increase the number of pairs produced at low field strength, allowing the study of the Dirac vacuum.

  5. Resonantly enhanced pair production in a simple diatomic model.

    PubMed

    Fillion-Gourdeau, François; Lorin, Emmanuel; Bandrauk, André D

    2013-01-01

    A new mechanism for the production of electron-positron pairs from the interaction of a laser field and a fully ionized diatomic molecule in the tunneling regime is presented. When the laser field is turned off, the Dirac operator has resonances in both the positive and the negative energy continua while bound states are in the mass gap. When this system is immersed in a strong laser field, the resonances move in the complex energy plane: the negative energy resonances are pushed to higher energies while the bound states are Stark shifted [F. Fillion-Gourdeau et al., J. Phys. A 45, 215304 (2012)]. It is argued here that there is a pair production enhancement at the crossing of resonances by looking at a simple one-dimensional model: the nuclei are modeled simply by Dirac delta potential wells while the laser field is assumed to be static and of finite spatial extent. The average rate for the number of electron-positron pairs produced is evaluated and the results are compared to the one and zero nucleus cases. It is shown that positrons are produced by the resonantly enhanced pair production mechanism, which is analogous to the resonantly enhanced ionization of molecular physics. This phenomenon could be used to increase the number of pairs produced at low field strength, allowing the study of the Dirac vacuum.

  6. Determination of Hexachlorocyclohexane by Gas Chromatography Combined with Femtosecond Laser Ionization Mass Spectrometry

    NASA Astrophysics Data System (ADS)

    Yang, Xixiang; Imasaka, Tomoko; Li, Adan; Imasaka, Totaro

    2016-09-01

    Structural isomers and enantiomers of hexachlorocyclohexane (HCH) were separated using a chiral column by gas chromatography and quantitatively determined by multiphoton ionization mass spectrometry using an ultraviolet femtosecond laser (200 and 267 nm) as the ionization source. The order of elution of the enantiomers (i.e., (+)-α-HCH and (-)-α-HCH) was predicted from stabilization energies calculated for the complexes using permethylated γ-cyclodextrin as the stationary phase of the column, and the results were compared with the experimental data. The molecular ions observed for HCH were weak, even though they can be ionized through a process of resonance enhanced two-photon ionization at 200 nm. This unfavorable result can be attributed to the dissociation of the molecular ion, as predicted from quantum chemical calculations.

  7. Multicolored two-photon fluorescent microscopy and localized two-photon fluorescent spectroscopy in living cells

    NASA Astrophysics Data System (ADS)

    Bergey, Earl J.; Wang, Xiaopeng; Krebs, Linda J.; Pudavar, Haridas E.; Kapoor, Rakesh; Friend, Christopher S.; Liebow, Charles; Prasad, Paras N.

    2001-04-01

    Imaging in biological systems has become one of the most relied upon tools in the study of human disease. Two-photon excitation methodology in laser scanning microscopy has resulted in 3D-imaging capability not easily achieved in one- photon systems. Our Institute, in conjunction with Andrew Schally (Noble Laureate, Tulane University), has used two- photon laser scanning microscopy (TPLSM) to understand the real time cellular transport of the chemotherapeutic agent, Luteinizing Hormone-Releasing Hormone-Doxorubicin (AN152) covalently coupled to a novel two-photon fluorophore (C625). At the Institute, new and highly efficient two-photon fluorophores that fluoresce at different wavelengths have been developed. The coupling of LH-RH and AN152 with two-photon fluorophores having different spectroscopic profiles allows for the simultaneous determination of their cellular compartmentalization. Coupled with the two-photon microspectrofluorometer, we acquired localized fluorescence spectra from the inside of living cells to differentiate the cytoplasmic and nuclear localization of the LH-RH and AN152 respectively. The ability of these new dyes to fluoresce at different wavelengths using the same excitation wavelength provides a major advantage over single photon dyes. This technology has great promise in imaging the dynamic changes or events occurring in living cells over short periods of time. Another approach to bioimaging at the Institute is the integration of two-photon and nanosized technologies. Nanoclinics (20 - 30 nm silica bubbles) can be fabricated to contain these two photon fluorophores and the surface functionalized with biological agents which can target specific cells. These highly fluorescent nanoclinics are sufficiently small in size to allow for tissue penetration, allowing for the multiple probing for different cellular functions in normal and cancerous tissues.

  8. Resonance-enhanced multiphoton ionization (REMPI) spectroscopy of bromobenzene and its perdeuterated isotopologue: Assignment of the vibrations of the S{sub 0}, S{sub 1}, and D{sub 0}{sup +} states of bromobenzene and the S{sub 0} and D{sub 0}{sup +} states of iodobenzene

    SciTech Connect

    Andrejeva, Anna; Tuttle, William D.; Harris, Joe P.; Wright, Timothy G.

    2015-12-28

    We report vibrationally resolved spectra of the S{sub 1}←S{sub 0} transition of bromobenzene using resonance-enhanced multiphoton ionization spectroscopy. We study bromobenzene-h{sub 5} as well as its perdeuterated isotopologue, bromobenzene-d{sub 5}. The form of the vibrational modes between the isotopologues and also between the S{sub 0} and S{sub 1} electronic states is discussed for each species, allowing assignment of the bands to be achieved and the activity between states and isotopologues to be established. Vibrational bands are assigned utilizing quantum chemical calculations, previous experimental results, and isotopic shifts. Previous work and assignments of the S{sub 1} spectra are discussed. Additionally, the vibrations in the ground state cation, D{sub 0}{sup +}, are considered, since these have also been used by previous workers in assigning the excited neutral state spectra. We also examine the vibrations of iodobenzene in the S{sub 0} and D{sub 0}{sup +} states and comment on the previous assignments of these. In summary, we have been able to assign the corresponding vibrations across the whole monohalobenzene series of molecules, in the S{sub 0}, S{sub 1}, and D{sub 0}{sup +} states, gaining insight into vibrational activity and vibrational couplings.

  9. Two-Photon Small Molecule Enzymatic Probes.

    PubMed

    Qian, Linghui; Li, Lin; Yao, Shao Q

    2016-04-19

    Enzymes are essential for life, especially in the development of disease and on drug effects, but as we cannot yet directly observe the inside interactions and only partially observe biochemical outcomes, tools "translating" these processes into readable information are essential for better understanding of enzymes as well as for developing effective tools to fight against diseases. Therefore, sensitive small molecule probes suitable for direct in vivo monitoring of enzyme activities are ultimately desirable. For fulfilling this desire, two-photon small molecule enzymatic probes (TSMEPs) producing amplified fluorescent signals based on enzymatic conversion with better photophysical properties and deeper penetration in intact tissues and whole animals have been developed and demonstrated to be powerful in addressing the issues described above. Nonetheless, currently available TSMEPs only cover a small portion of enzymes despite the distinct advantages of two-photon fluorescence microscopy. In this Account, we would like to share design principles for TSMEPs as potential indicators of certain pathology-related biomarkers together with their applications in disease models to inspire more elegant work to be done in this area. Highlights will be addressed on how to equip two-photon fluorescent probes with features amenable for direct assessment of enzyme activities in complex pathological environments. We give three recent examples from our laboratory and collaborations in which TSMEPs are applied to visualize the distribution and activity of enzymes at cellular and organism levels. The first example shows that we could distinguish endogenous phosphatase activity in different organelles; the second illustrates that TSMEP is suitable for specific and sensitive detection of a potential Parkinson's disease marker (monoamine oxidase B) in a variety of biological systems from cells to patient samples, and the third identifies that TSMEPs can be applied to other enzyme

  10. Polymerized nanotips via two-photon photopolymerization

    NASA Astrophysics Data System (ADS)

    Qi, Fengjie; Li, Yan; Tan, Dengfeng; Yang, Hong; Gong, Qihuang

    2007-02-01

    We present new methods to produce polymerized nanotips via two-photon photopolymerization. By gradually changing the laser power, we fabricate a single polymerized tip with the size of 120nm. When two rectangle anchors with protuberances are close enough, lines with the slimmest part of about 20-30nm and tips with the widths of about 35nm are produced between anchors, which are the best resolution obtained with the resin SCR-500 to our knowledge. As the tips are adhered to larger polymerized structures, they can survive post processing in spite of their small sizes.

  11. 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.

  12. Two-photon spectroscopy in francium

    NASA Astrophysics Data System (ADS)

    Gomez, E.; Sprouse, G. D.; Aubin, S.; Orozco, L. A.

    2004-05-01

    Two-photon spectroscopy allows the study of excited states of the same parity as the ground state in francium. It makes possible the determination of their electronic properties, such as the lifetimes. A further benefit is the cascade process back down to the ground state that provides information about the intermediate states in the decay. We produce francium at the Superconducting LINAC at Stony Brook and trap it in our high efficiency magneto-optical trap. We prepare the atoms in the 9s level with two photon excitation. The direct decay of the atoms to the 7P_3/2 level gives the lifetime of the 9s level^1. We use the indirect decay through the 8p levels and detect the cascade decay from the 8p levels to the ground state. With the use of time-correlated single-photon counting techniques and appropriate interference filters we separate the contributions from different fine levels and obtain a lifetime measurement to better than 3% (2%) for the 8P_1/2 (8P_3/2) level. The corresponding result in rubidium reaches a precision below 1% for the 6p manifold. Work supported by NSF. E.G. acknowledges support from CONACYT. ^1 S. Aubin, E. Gomez, L.A. Orozco and G.D. Sprouse, Opt. Lett. 28, 2055 (2003)

  13. Optimizing ultrashort laser pulse compression by two photon absorption

    NASA Astrophysics Data System (ADS)

    Welch, G.; Frisch, J.; Smith, S.; Glownia, J. M.; Fry, A.

    2016-02-01

    Demonstrated is an approach for relative optimization of ultrashort pulses using two-photon generated photocurrent in a GaAsP photodiode. Two-photon absorption is a nonlinear process, allowing for highly sensitive tuning of ultrashort laser systems.

  14. Experimental realization of a two-photon Raman laser

    NASA Astrophysics Data System (ADS)

    Brown, William J.

    1999-11-01

    This thesis describes the development of a novel quantum oscillator known as a two-photon Raman laser. It is based on two-photon stimulated emission in strongly driven potassium atoms. Two-photon lasers were first proposed in the 1960's, but only recently have such devices been experimentally realized. The two-photon Raman laser is an important step forward as it provides the first opportunity to study the turn-on behavior, instabilities, and noise properties of a pure two-photon optical device. The necessary ingredients for a two-photon laser are a medium displaying two-photon laser beam amplification and an optical resonator. In my two-photon Raman laser the amplification arises from a multi-photon process in which state-prepared potassium atoms undergo two-photon Raman transitions. This amplification process was studied using a high-density, small-Doppler-width potassium atomic beam that was driven by a strong pump laser and probed by a weak probe laser. I observed two-photon Raman amplification for a range of pump laser frequencies, atomic beam number densities, and probe beam powers. The two-photon Raman gain is linearly dependent on the input probe power as expected for a two-photon process. This gain mechanism is also spectrally isolated from other mechanisms occurring in strongly driven potassium atoms. The optical resonator consists of a sub-confocal high finesse cavity. The cavity is constructed so that the two-photon Raman process will lase while all other processes are suppressed. The cavity buildup is sufficient to support lasing given the maximum two-photon Raman gain observed in the amplification experiment. Using this apparatus I have observed two-photon lasing. In agreement with theoretical predictions, an external photon source is required to initiate two-photon lasing. I initiated the two-photon laser using an externally injected pulse of light and using a frequency degenerate one-photon process. The two-photon Raman laser threshold was mapped as

  15. Atmospheric-pressure laser ionization: a novel ionization method for liquid chromatography/mass spectrometry.

    PubMed

    Constapel, M; Schellenträger, M; Schmitz, O J; Gäb, S; Brockmann, K J; Giese, R; Benter, Th

    2005-01-01

    We report on the development of a new laser-ionization (LI) source operating at atmospheric pressure (AP) for liquid chromatography/mass spectrometry (LC/MS) applications. APLI is introduced as a powerful addition to existing AP ionization techniques, in particular atmospheric-pressure chemical ionization (APCI), electrospray ionization (ESI), and atmospheric pressure photoionization (APPI). Replacing the one-step VUV approach in APPI with step-wise two-photon ionization strongly enhances the selectivity of the ionization process. Furthermore, the photon flux during an ionization event is drastically increased over that of APPI, leading to very low detection limits. In addition, the APLI mechanism generally operates primarily directly on the analyte. This allows for very efficient ionization even of non-polar compounds such as polycyclic aromatic hydrocarbons (PAHs). The APLI source was characterized with a MicroMass Q-Tof Ultima II analyzer. Both the effluent of an HPLC column containing a number of PAHs (benzo[a]pyrene, fluoranthene, anthracene, fluorene) and samples from direct syringe injection were analyzed with respect to selectivity and sensitivity of the overall system. The liquid phase was vaporized by a conventional APCI inlet (AP probe) with the corona needle removed. Ionization was performed through selective resonance-enhanced multi-photon ionization schemes using a high-repetition-rate fixed-frequency excimer laser operating at 248 nm. Detection limits well within the low-fmol regime are readily obtained for various aromatic hydrocarbons that exhibit long-lived electronic states at the energy level of the first photon. Only molecular ions are generated at the low laser fluxes employed ( approximately 1 MW/cm(2)). The design and performance of the laser-ionization source are presented along with results of the analysis of aromatic hydrocarbons.

  16. 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.

  17. Full Quantum Analysis of Two-Photon Absorption Using Two-Photon Wave Function: Comparison of Two-Photon Absorption with One-Photon Absorption

    NASA Astrophysics Data System (ADS)

    Nakanishi, Toshihiro; Kobayashi, Hirokazu; Sugiyama, Kazuhiko; Kitano, Masao

    2009-10-01

    For dissipation-free photon-photon interaction at the single photon level, we analyze one-photon and two-photon transitions induced by photon pairs in three-level atoms using two-photon wave functions. We show that two-photon absorption can be substantially enhanced by adjusting the time correlation of photon pairs. We study two typical cases: a Gaussian wave function and a rectangular wave function. In the latter, we find that under special conditions one-photon transition is completely suppressed, while two-photon transition is maintained with a high probability.

  18. Two-photon imaging of stem cells

    NASA Astrophysics Data System (ADS)

    Uchugonova, A.; Gorjup, E.; Riemann, I.; Sauer, D.; König, K.

    2008-02-01

    A variety of human and animal stem cells (rat and human adult pancreatic stem cells, salivary gland stem cells, dental pulpa stem cells) have been investigated by femtosecond laser 5D two-photon microscopy. Autofluorescence and second harmonic generation have been imaged with submicron spatial resolution, 270 ps temporal resolution, and 10 nm spectral resolution. In particular, NADH and flavoprotein fluorescence was detected in stem cells. Major emission peaks at 460nm and 530nm with typical mean fluorescence lifetimes of 1.8 ns and 2.0 ns, respectively, were measured using time-correlated single photon counting and spectral imaging. Differentiated stem cells produced the extracellular matrix protein collagen which was detected by SHG signals at 435 nm.

  19. Two-photon fluorescence anisotropy imaging

    NASA Astrophysics Data System (ADS)

    Li, Wei; Wang, Yi; Shao, Hanrong; He, Yonghong; Ma, Hui

    2006-09-01

    We have developed a novel method for imaging the fluorescence intensity and anisotropy by two-photon fluorescence microscopy and tested its capability in biological application. This method is applied to model sample including FITC and FITC-CD44 antibody solution and also FITC-CD44 stained cells. The fluorescence anisotropy (FA) of FITC-CD44ab solution is higher than the FITC solution with the same concentration. The fluorescence in cell sample has even higher FA than in solution because the rotation diffusion is restrained in membrane. The method is employed to study the effect of berberine a kind of Chinese medicine, on tumor metastasis. The results indicated that tumor cell membrane fluidity is decreasing with increasing the concentration of berberine in culture medium.

  20. Two photon annihilation operators and squeezed vacuum

    NASA Technical Reports Server (NTRS)

    Roy, Anil K.; Mehta, C. L.; Saxena, G. M.

    1993-01-01

    Inverses of the harmonic oscillator creation and annihilation operators by their actions on the number states are introduced. Three of the two photon annihilation operators, viz., a(sup +/-1)a, aa(sup +/-1), and a(sup 2), have normalizable right eigenstates with nonvanishing eigenvalues. The eigenvalue equation of these operators are discussed and their normalized eigenstates are obtained. The Fock state representation in each case separates into two sets of states, one involving only the even number states while the other involving only the odd number states. It is shown that the even set of eigenstates of the operator a(sup +/-1)a is the customary squeezed vacuum S(sigma) O greater than.

  1. Dynamics of two-photon paired superradiance

    NASA Astrophysics Data System (ADS)

    Yoshimura, M.; Sasao, N.; Tanaka, M.

    2012-07-01

    We develop for dipole-forbidden transition a dynamical theory of two-photon paired superradiance (PSR). This is a cooperative process characterized by two photons emitted back to back with equal energies. By irradiating the trigger laser from two target ends, with its frequency tuned at the half energy between two levels, a macroscopically coherent state of medium and fields dynamically emerges as time evolves, and a large signal of amplified output occurs with a time delay. The basic semiclassical equations in 1+1 space-time dimensions are derived for the field-plus-medium system to describe the space-time evolution of the entire system and are numerically solved to demonstrate the existence of both explosive and weak PSR phenomena in the presence of relaxation terms. The explosive PSR event terminates accompanying a sudden release of most of the energy stored in the target. Our numerical simulations are performed using the vibrational transition X1Σg+v=1→0 of a para-H2 molecule and taking many different excited atom number densities and different initial coherences between the metastable and the ground states. In an example with a number density close to O(1021 cm-3) and a high initial coherence, the explosive event terminates several nanoseconds after the trigger irradiation, when the phase relaxation time larger than O(10 ns) is taken. After PSR events the system is expected to follow a steady-state solution which is obtained by analytic means and is made of many objects of field condensates endowed with a topological stability.

  2. Two-photon-induced singlet fission in rubrene single crystal.

    PubMed

    Ma, Lin; Galstyan, Gegham; Zhang, Keke; Kloc, Christian; Sun, Handong; Soci, Cesare; Michel-Beyerle, Maria E; Gurzadyan, Gagik G

    2013-05-14

    The two-photon-induced singlet fission was observed in rubrene single crystal and studied by use of femtosecond pump-probe spectroscopy. The location of two-photon excited states was obtained from the nondegenerate two-photon absorption (TPA) spectrum. Time evolution of the two-photon-induced transient absorption spectra reveals the direct singlet fission from the two-photon excited states. The TPA absorption coefficient of rubrene single crystal is 52 cm∕GW at 740 nm, as obtained from Z-scan measurements. Quantum chemical calculations based on time-dependent density functional theory support our experimental data. PMID:23676057

  3. Resonantly enhanced four-wave mixing

    DOEpatents

    Begley, Richard F.; Kurnit, Norman A.

    1978-01-01

    A method and apparatus for achieving large susceptibilities and long interaction lengths in the generation of new wavelengths in the infrared spectral region. A process of resonantly enhanced four-wave mixing is employed, utilizing existing laser sources, such as the CO.sub.2 laser, to irradiate a gaseous media. The gaseous media, comprising NH.sub.3, CH.sub.3 F, D.sub.2, HCl, HF, CO, and H.sub.2 or some combination thereof, are of particular interest since they are capable of providing high repetition rate operation at high flux densities where crystal damage problems become a limitation.

  4. Resonantly-enhanced harmonic generation in Argon.

    PubMed

    Ackermann, P; Münch, H; Halfmann, T

    2012-06-18

    We present systematic investigations of harmonic generation in Argon, driven in the vicinity of a five-photon resonance by intense, tunable picosecond radiation pulses. When properly matching the laser frequency with the Stark-shifted multi-photon resonance, we observe a pronounced enhancement not only of the 5th, but also the 7th and 9th harmonic of the driving laser (i.e. at orders higher than the involved multi-photon resonance). We study the harmonic yield at different intensities and wavelengths of the driving laser to determine optimal conditions for resonantly-enhanced harmonic generation.

  5. Two-photon mapping of neocortical circuits

    NASA Astrophysics Data System (ADS)

    Nikolenko, Volodymyr

    The synaptic circuits of the cerebral cortex are still poorly understood, yet knowing their basic structure appears key for understanding their function (Lorente de No, 1949). While some argue that there is a basic modular circuit present in all cortical regions (Douglas et al., 1989; Hubel and Wiesel, 1977), others suggest that synaptic circuits could be randomly structured (Braitenberg and Schuz, 1998). To investigate the patterns of synaptic connections present in neocortex, I have developed a novel two-photon optical mapping method (Nikolenko et al., 2007) to systematically reveal cells that connect to four classes of neurons in slices of mouse primary sensory cortex. Inputs to these cells originated preferentially from specific cortical layers and often were laterally restricted, revealing functional columnar circuits with sharp boundaries. Moreover, many neurons extensively sampled particular territories, and, in some cases, virtually every cell from a particular layer was connected to the postsynaptic target. The results reveal circuits with dense columnar connectivity, approximating in some cases the complete sampling from every potential presynaptic cell in an input layer. I discuss the implications of these findings in the context of the computational strategies used by the cortex.

  6. Two-photon excitation energy transfer microscopy

    NASA Astrophysics Data System (ADS)

    Periasamy, Ammasi

    2000-04-01

    Fluorescence resonance energy transfer (FRET) imaging is a unique tool used to visualize the spaciotemporal dynamics of protein-protein interactions in living cells. We used FRET to study the dimerization of the pituitary-specific transcription factor of Pit-1 fused with blue flourescent protein and green fluorescent protein. Transcriptional activity of the GFP- and BFP-Pit-1 fusion proteins was demonstrated by their ability to activate the prolactin gene promoter. The energy transfer in the conventional fluorescence microscopy was less efficient due to photobleaching of the BFP-Pit-1 donor molecules. In our studies we developed two-photon excitation energy transfer microscopy, where the photobleaching of blue flourescent protein was considerably reduced. This 2p-FRET imaging system was used to acquire the donor and acceptor images for a living HeLa cell nucleus. We selected 732 nm from the tunable Verdi pumped ti:sapphire laser, in a way that only excites the BFP-Pit-1 and not the GFP-Pit-1 proteins. The efficiency of the 2p-FRET signal increased to 30 percent compared to the conventional FRET imaging, which clearly demonstrates that there is considerable reduction in photobleaching of donor molecules in the 2p-FRET microscopy.

  7. Ordering of azobenzenes by two-photon isomerization

    SciTech Connect

    Ishitobi, Hidekazu; Sekkat, Zouheir; Kawata, Satoshi

    2006-10-28

    We report on light induced orientation by two-photon isomerization of azobenzenes in films of polymer. The dynamics of isomerization and orientation by one-photon absorption and two-photon absorption (TPA) are similar, and TPA creates a degree of molecular orientation which is comparable to that achieved by single-photon isomerization, in agreement with the theoretical predictions of two-photon isomeric orientation.

  8. Two-photon absorption by a quantum dot pair

    NASA Astrophysics Data System (ADS)

    Scheibner, Michael; Economou, Sophia E.; Ponomarev, Ilya V.; Jennings, Cameron; Bracker, Allan S.; Gammon, Daniel

    2015-08-01

    The biexciton absorption spectrum of a pair of InAs/GaAs quantum dots is being studied by photoluminescence excitation spectroscopy. An absorption resonance with the characteristics of an instantaneous two-photon process reveals a coherent interdot two-photon transition. Pauli-selective tunneling is being used to demonstrate the transduction of the two-photon coherence into a nonlocal spin singlet state. The two-photon transition can be tuned spectrally by electric field, enabling amplification of its transition strength.

  9. Two-Photon Absorption by H2 Molecules: Origin of the 2175A Astronomical Band?

    NASA Astrophysics Data System (ADS)

    Sorokin, Peter P.; Glownia, James H.

    2007-04-01

    The near UV spectra of OB stars are often dominated by a broad extinction band peaking at 2175A. Forty years after its discovery, the origin of this band remains unknown, although it is usually attributed to linear scattering or linear absorption by interstellar dust particles. Here we report that two-photon absorption by H2 molecules in gaseous clouds enveloping OB stars should lead to a strong band peaking near 2175A. We first show that if the product of the H2 density in the gaseous cloud times the emitted stellar VUV flux is sufficiently great, the threshold for stimulated Rayleigh scattering will be exceeded, resulting in the generation of intense, monochromatic VUV light at the rest frame frequencies of H2 B- and C-state resonance lines originating from levels J''=0 and J''=1 of X0. This coherently generated light must necessarily propagate radially inwards towards the photosphere of the illuminating OB star, and therefore cannot be detected externally. However, this same light effectively constitutes intense ``first step'' monochromatic radiation that should induce continuum photons emitted by the OB star near 2175A to be strongly absorbed as ``second steps'' in resonantly-enhanced H2 two-photon transitions to two well known doubly-excited dissociative states of H2. Archival UV and VUV spectra of 185 OB stars strongly support our nonlinear model for the 2175A band.

  10. Production of narrowband tunable extreme-ultraviolet radiation by noncollinear resonance-enhanced four-wave mixing.

    PubMed

    Hannemann, S; Hollenstein, U; van Duijn, E J; Ubachs, W

    2005-06-15

    Fourier-transform-limited extreme-ultraviolet (XUV) radiation (bandwidth approximately < 300 MHz) tunable around 91 nm is produced by use of two-photon resonance-enhanced four-wave mixing on the Kr resonance at 94 093 cm(-1). Noncollinear phase matching ensures the generation of an XUV sum frequency 2 omega1 + omega2 that can be filtered from auxiliary laser beams and harmonics by an adjustable slit. Application of the generated XUV light is demonstrated in spectroscopic investigations of highly excited states in H2 and N2.

  11. Two-photon coherent states of the radiation field

    NASA Technical Reports Server (NTRS)

    Yuen, H. P.

    1976-01-01

    The concept of a two-photon coherent state is introduced for applications in quantum optics. It is a simple generalization of the well-known minimum-uncertainty wave packets. The detailed properties of two-photon coherent states are developed and distinguished from ordinary coherent states. These two-photon coherent states are mathematically generated from coherent states through unitary operators associated with quadratic Hamiltonians. Physically they are the radiation states of ideal two-photon lasers operating far above threshold, according to the self-consistent-field approximation. The mean-square quantum noise behavior of these states, which is basically the same as those of minimum-uncertainty states, leads to applications not obtainable from coherent states or one-photon lasers. The essential behavior of two-photon coherent states is unchanged by small losses in the system. The counting rates or distributions these states generate in photocount experiments also reveal their difference from coherent states.

  12. Synthesis of Two-Photon Materials and Two-Photon Liquid Crystals

    NASA Technical Reports Server (NTRS)

    Subramaniam, Girija

    2001-01-01

    The duration of the grant was interrupted by two major accidents that the PI met with-- an auto accident in Pasadena, CA during her second summer at JPL which took almost eight months for recovery and a second accident during Fall 2000 that left her in crutches for the entire semester. Further, the time released agreed by the University was not given in a timely fashion. The candidate has been given post-grant expire time off. In spite of all these problems, the PI synthesized a number of new two-photon materials and studied the structure-activity correlation to arrive at the best-optimized structure. The PI's design proved to be one of the best in the sense that these materials has a hitherto unreported two-photon absorption cross section. Many materials based on PI's design was later made by the NASA colleague. This is Phase 1. Phase II of this grant is to orate liquid crystalline nature into this potentially useful materials and is currently in progress. Recent observations of nano- and pico-second response time of homeotropically aligned liquid crystals suggest their inherent potentials to act as laser hardening materials, i.e., as protective devices against short laser pulses. The objective of the current project is to exploit this potential by the synthesis of liquid crystals with high optical nonlinearity and optimizing their performance. The PI is trying structural variations to bring in liquid crystalline nature without losing the high two-photon cross section. Both Phase I and Phase II led to many invited presentations and publications in reputed journals like 'Science' and 'Molecular Crystals'. The list of presentations and reprints are enclosed. Another important and satisfying outcome of this grant is the opportunity that this grant offered to the budding undergraduate scientists to get involved in a visible research of international importance. All the students had a chance to learn a lot during research, had the opportunity to present their work at

  13. Neutron elastic backscattering with resonance enhancement

    SciTech Connect

    Gomberg, H.J.; McEllistrem, M.T.

    1993-12-31

    Reliable detection of explosives and narcotics depends on generating signatures of compounds which characterize them. Major explosives and also alkaloid narcotics contain unique concentrations of Carbon, Oxygen, and Nitrogen which provide specific elemental ratios and chemical signatures. Neutron-induced reaction methods are rapid and non-invasive means of probing container interiors for special element-ratio signatures which signal the presence of significant amounts of contraband. Among these reactions the highest probabilities occur for neutron from different light elements, allowing determination of relative abundance of these elements. The authors have already demonstrated signature for simulated explosives and simulated narcotics in experimental tests at 1-4 MeV at the University of Kentucky accelerator labs. Intensities of neutron scatter at angles near 150{degrees} from three different elements, C, N, and O, were determined. Fast neutron time-of-flight detection methods enabled measurement of neutron energies, and thus separation of scattering from the different elements. Making measurements on and off strong resonances for specific elements, increases PFD and reduces PFA. Measurements illustrating this resonance enhancement technique will be presented.

  14. Resonant enhancement of absorption in the superlens

    NASA Astrophysics Data System (ADS)

    Alekseyev, Leonid; Jacob, Zubin; Narimanov, Evgenii

    2007-03-01

    The Veselago lens (also known as the super lens) [1], which is a slab made of left handed material with ɛ=-1 and μ=-1 has interesting properties like perfect lensing [2] and cloaking [3]. When a source is placed in front of it there are regions of high field intensity in such a lens , known as anomalously localized resonant regions [3]. For practical applications of the superlens taking advantage of these properties, the effect of finite loss on the device performance is critical [4] . We calculate the absorption loss of dipole radiation by an ɛ<0 and μ<0 slab and find resonant enhancement of absorption in the superlensing regime. [1] V. G. Veselago, ``The electrodynamics of substances with simultaneously negative values of permittivity and permeability,'' Sov. Phys. Usp. 10, 509 (1968). [2] J. B. Pendry, ``Negative refraction makes a perfect lens,'' Phys. Rev. Lett. 85, 3966-3969 (2000). [3] Graeme W. Milton and Nicolae-Alexandry P. Nicorovici ``On the cloaking effects associated with anomalous localized resonance,'' Proc. R. Soc. A (2006) 462, 3027-3059. [4] V. A. Podolskiy and E. E. Narimanov, ``Near-sighted superlens,'' Opt. Lett. 30, 75-77 (2005)

  15. Resonance enhancement of neutrinoless double electron capture

    NASA Astrophysics Data System (ADS)

    Krivoruchenko, M. I.; Šimkovic, Fedor; Frekers, Dieter; Faessler, Amand

    2011-06-01

    The process of neutrinoless double electron (0νECEC) capture is revisited for those cases where the two participating atoms are nearly degenerate in mass. The theoretical framework is the formalism of an oscillation of two atoms with different total lepton number (and parity), one of which can be in an excited state so that mass degeneracy is realized. In such a case and assuming light Majorana neutrinos, the two atoms will be in a mixed configuration with respect to the weak interaction. A resonant enhancement of transitions between such pairs of atoms will occur, which could be detected by the subsequent electromagnetic de-excitation of the excited state of the daughter atom and nucleus. Available data of atomic masses, as well as nuclear and atomic excitations are used to select the most likely candidates for the resonant transitions. Assuming an effective mass for the Majorana neutrino of 1 eV, some half-lives are predicted to be as low as 1022 years in the unitary limit. It is argued that, in order to obtain more accurate predictions for the 0νECEC half-lives, precision mass measurements of the atoms involved are necessary, which can readily be accomplished by today's high precision Penning traps. Further advancements also require a better understanding of high-lying excited states of the final nuclei (i.e. excitation energy, angular momentum and parity) and the calculation of the nuclear matrix elements.

  16. Two-photon interference of temporally separated photons

    NASA Astrophysics Data System (ADS)

    Kim, Heonoh; Lee, Sang Min; Moon, Han Seb

    2016-10-01

    We present experimental demonstrations of two-photon interference involving temporally separated photons within two types of interferometers: a Mach-Zehnder interferometer and a polarization-based Michelson interferometer. The two-photon states are probabilistically prepared in a symmetrically superposed state within the two interferometer arms by introducing a large time delay between two input photons; this state is composed of two temporally separated photons, which are in two different or the same spatial modes. We then observe two-photon interference fringes involving both the Hong-Ou-Mandel interference effect and the interference of path-entangled two-photon states simultaneously in a single interferometric setup. The observed two-photon interference fringes provide simultaneous observation of the interferometric properties of the single-photon and two-photon wavepackets. The observations can also facilitate a more comprehensive understanding of the origins of the interference phenomena arising from spatially bunched/anti-bunched two-photon states comprised of two temporally separated photons within the interferometer arms.

  17. Two-photon interference of temporally separated photons

    PubMed Central

    Kim, Heonoh; Lee, Sang Min; Moon, Han Seb

    2016-01-01

    We present experimental demonstrations of two-photon interference involving temporally separated photons within two types of interferometers: a Mach-Zehnder interferometer and a polarization-based Michelson interferometer. The two-photon states are probabilistically prepared in a symmetrically superposed state within the two interferometer arms by introducing a large time delay between two input photons; this state is composed of two temporally separated photons, which are in two different or the same spatial modes. We then observe two-photon interference fringes involving both the Hong-Ou-Mandel interference effect and the interference of path-entangled two-photon states simultaneously in a single interferometric setup. The observed two-photon interference fringes provide simultaneous observation of the interferometric properties of the single-photon and two-photon wavepackets. The observations can also facilitate a more comprehensive understanding of the origins of the interference phenomena arising from spatially bunched/anti-bunched two-photon states comprised of two temporally separated photons within the interferometer arms. PMID:27708380

  18. Two-Photon Fluorescence Microscopy for Biomedical Research

    NASA Technical Reports Server (NTRS)

    Fischer, David; Zimmerli, Greg; Asipauskas, Marius

    2007-01-01

    This viewgraph presentation gives an overview of two-photon microscopy as it applies to biomedical research. The topics include: 1) Overview; 2) Background; 3) Principles of Operation; 4) Advantages Over Confocal; 5) Modes of Operation; and 6) Applications.

  19. Photodamage of mesotetraphenylporphyrin under one- and two-photon excitation

    SciTech Connect

    Wen Yanan; Liu Yuqiang; Yang Zhenling; Yang Yanqiang; Guo Ximing

    2010-08-15

    Photoinduced damage behavior of mesotetraphenylporphyrin (TPP) under one- and two-photon excitation with femtosecond laser pulses is investigated in the present work. Quenching in the luminescent intensity is observed. Results suggest that laser irradiation on TPP mainly causes two simultaneously occurring photoprocesses: photodamage and formation of a porphine-type photoproduct. The damage rate exhibits a linear dependence on the incident light power in one-photon excitation, whereas in two-photon excitation, the power dependence of the damage rate turns out to be exponential. The photoproduct formed in one- and two-photon excitation is identical. This product, which is observed to possess superior photostability and two-photon absorbing ability compared with the original TPP sensitizer, is likely to be treated as a secondary photosensitizer in the activation process of photodynamic therapy (PDT). This work might be helpful for the drug evaluation in the practical application of PDT.

  20. Two-photon directed evolution of green fluorescent proteins

    PubMed Central

    Stoltzfus, Caleb R.; Barnett, Lauren M.; Drobizhev, Mikhail; Wicks, Geoffrey; Mikhaylov, Alexander; Hughes, Thomas E.; Rebane, Aleksander

    2015-01-01

    Directed evolution has been used extensively to improve the properties of a variety of fluorescent proteins (FPs). Evolutionary strategies, however, have not yet been used to improve the two-photon absorption (2PA) properties of a fluorescent protein, properties that are important for two-photon imaging in living tissues, including the brain. Here we demonstrate a technique for quantitatively screening the two-photon excited fluorescence (2PEF) efficiency and 2PA cross section of tens of thousands of mutant FPs expressed in E. coli colonies. We use this procedure to move EGFP through three rounds of two-photon directed evolution leading to new variants showing up to a 50% enhancement in peak 2PA cross section and brightness within the near-IR tissue transparency wavelength range. PMID:26145791

  1. Pulse-shaping based two-photon FRET stoichiometry.

    PubMed

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

    2015-02-01

    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.

  2. Two-photon directed evolution of green fluorescent proteins

    NASA Astrophysics Data System (ADS)

    Stoltzfus, Caleb R.; Barnett, Lauren M.; Drobizhev, Mikhail; Wicks, Geoffrey; Mikhaylov, Alexander; Hughes, Thomas E.; Rebane, Aleksander

    2015-07-01

    Directed evolution has been used extensively to improve the properties of a variety of fluorescent proteins (FPs). Evolutionary strategies, however, have not yet been used to improve the two-photon absorption (2PA) properties of a fluorescent protein, properties that are important for two-photon imaging in living tissues, including the brain. Here we demonstrate a technique for quantitatively screening the two-photon excited fluorescence (2PEF) efficiency and 2PA cross section of tens of thousands of mutant FPs expressed in E. coli colonies. We use this procedure to move EGFP through three rounds of two-photon directed evolution leading to new variants showing up to a 50% enhancement in peak 2PA cross section and brightness within the near-IR tissue transparency wavelength range.

  3. Two-photon absorption spectroscopy of rubrene single crystals

    NASA Astrophysics Data System (ADS)

    Irkhin, Pavel; Biaggio, Ivan

    2014-05-01

    We determine the wavelength dependence of the two-photon absorption cross section in rubrene single crystals both by direct measurement of nonlinear transmission and from the two-photon excitation spectrum of the photoluminescence. The peak two-photon absorption coefficient for b-polarized light was found to be (4.6±1)×10-11 m/W at a wavelength of 850±10 nm. It is 2.3 times larger for c-polarized light. The lowest energy two-photon excitation peak corresponds to an excited state energy of 2.92±0.04 eV and it is followed by a vibronic progression of higher energy peaks separated by ˜0.14 eV.

  4. Coherence revivals in two-photon frequency combs

    SciTech Connect

    Torres-Company, Victor; Lancis, Jesus; Lajunen, Hanna; Friberg, Ari T.

    2011-09-15

    We describe and theoretically analyze the self-imaging Talbot effect of entangled photon pairs in the time domain. Rich phenomena are observed in coherence propagation along dispersive media of mode-locked two-photon states with frequency entanglement exhibiting a comblike correlation function. Our results can be used to remotely transfer frequency standards through optical fiber networks with two-photon light, avoiding the requirement of dispersion compensation.

  5. The use of CNDO in spectroscopy. XV. Two photon absorption

    NASA Astrophysics Data System (ADS)

    Marchese, Francis T.; Seliskar, C. J.; Jaffé, H. H.

    1980-04-01

    Two-photon absorptivities have been calculated within the CNDO/S-CI molecular orbital framework of Del Bene and Jaffé utilizing the second order time dependent perturbation equations of Göppert-Mayer and polarization methods of McClain. Good agreement is found between this theory and experiment for transition energies, symmetries, and two-photon absorptivities for the following molecules: biphenyl, terphenyl, 2,2'-difluorobiphenyl, 2,2'-bipyridyl, phenanthrene, and the isoelectronic series: fluorene, carbazole, dibenzofuran.

  6. Voigt spectral profiles in two-photon resonance fluorescence

    SciTech Connect

    Alexanian, Moorad; Bose, Subir K.

    2007-11-15

    A recent work on two-photon fluorescence is extended by considering the pump field to be a coherent state, which represents a laser field operating well above threshold. The dynamical conditions are investigated under which the two-photon spectrum gives rise, in addition to a Lorentzian line shape at the pump frequency, to two Voigt spectral sideband profiles. Additional conditions are found under which the Voigt profile behaves like either a Gaussian or a Lorentzian line shape.

  7. Two-photon photovoltaic effect in gallium arsenide.

    PubMed

    Ma, Jichi; Chiles, Jeff; Sharma, Yagya D; Krishna, Sanjay; Fathpour, Sasan

    2014-09-15

    The two-photon photovoltaic effect is demonstrated in gallium arsenide at 976 and 1550 nm wavelengths. A waveguide-photodiode biased in its fourth quadrant harvests electrical power from the optical energy lost to two-photon absorption. The experimental results are in good agreement with simulations based on nonlinear wave propagation in waveguides and the drift-diffusion model of carrier transport in semiconductors. Power efficiency of up to 8% is theoretically predicted in optimized devices.

  8. Multicolor two-photon tissue imaging by wavelength mixing.

    PubMed

    Mahou, Pierre; Zimmerley, Maxwell; Loulier, Karine; Matho, Katherine S; Labroille, Guillaume; Morin, Xavier; Supatto, Willy; Livet, Jean; Débarre, Delphine; Beaurepaire, Emmanuel

    2012-08-01

    We achieve simultaneous two-photon excitation of three chromophores with distinct absorption spectra using synchronized pulses from a femtosecond laser and an optical parametric oscillator. The two beams generate separate multiphoton processes, and their spatiotemporal overlap provides an additional two-photon excitation route, with submicrometer overlay of the color channels. We report volume and live multicolor imaging of 'Brainbow'-labeled tissues as well as simultaneous three-color fluorescence and third-harmonic imaging of fly embryos. PMID:22772730

  9. Two photon couplings of the lightest isoscalars from BELLE data

    SciTech Connect

    Dai, Ling -Yun; Pennington, Michael R.

    2014-07-07

    Amplitude Analysis of two photon production of ππ and K¯K, using S-matrix constraints and fitting all available data, including the latest precision results from Belle, yields a single partial wave solution up to 1.4 GeV. The two photon couplings of the σ/f0(500), f0(980) and f2(1270) are determined from the residues of the resonance poles.

  10. Multicolor two-photon tissue imaging by wavelength mixing.

    PubMed

    Mahou, Pierre; Zimmerley, Maxwell; Loulier, Karine; Matho, Katherine S; Labroille, Guillaume; Morin, Xavier; Supatto, Willy; Livet, Jean; Débarre, Delphine; Beaurepaire, Emmanuel

    2012-07-08

    We achieve simultaneous two-photon excitation of three chromophores with distinct absorption spectra using synchronized pulses from a femtosecond laser and an optical parametric oscillator. The two beams generate separate multiphoton processes, and their spatiotemporal overlap provides an additional two-photon excitation route, with submicrometer overlay of the color channels. We report volume and live multicolor imaging of 'Brainbow'-labeled tissues as well as simultaneous three-color fluorescence and third-harmonic imaging of fly embryos.

  11. Two photon couplings of the lightest isoscalars from BELLE data

    DOE PAGES

    Dai, Ling -Yun; Pennington, Michael R.

    2014-07-07

    Amplitude Analysis of two photon production of ππ and K¯K, using S-matrix constraints and fitting all available data, including the latest precision results from Belle, yields a single partial wave solution up to 1.4 GeV. The two photon couplings of the σ/f0(500), f0(980) and f2(1270) are determined from the residues of the resonance poles.

  12. In Vivo Cell Tracking Using Two-Photon Microscopy.

    PubMed

    Malide, Daniela

    2016-01-01

    Recently we have explored and developed approaches imaging using confocal/two-photon microscopy, which enables simultaneous high-resolution assessment of specifically fluorescently marked cells in conjunction with structural components of the tissues visualized via harmonic generated signals. This approach uses commercially available confocal and two-photon laser microscope and automated user-interactive image analysis methods based on commercially available software packages allowing easy implementation in usual microscopy facilities. PMID:27283422

  13. Two-photon photovoltaic effect in gallium arsenide.

    PubMed

    Ma, Jichi; Chiles, Jeff; Sharma, Yagya D; Krishna, Sanjay; Fathpour, Sasan

    2014-09-15

    The two-photon photovoltaic effect is demonstrated in gallium arsenide at 976 and 1550 nm wavelengths. A waveguide-photodiode biased in its fourth quadrant harvests electrical power from the optical energy lost to two-photon absorption. The experimental results are in good agreement with simulations based on nonlinear wave propagation in waveguides and the drift-diffusion model of carrier transport in semiconductors. Power efficiency of up to 8% is theoretically predicted in optimized devices. PMID:26466255

  14. Uniform silica nanoparticles encapsulating two-photon absorbing fluorescent dye

    SciTech Connect

    Wu Weibing; Liu Chang; Wang Mingliang; Huang Wei; Zhou Shengrui; Jiang Wei; Sun Yueming; Cui Yiping; Xu Chunxinag

    2009-04-15

    We have prepared uniform silica nanoparticles (NPs) doped with a two-photon absorbing zwitterionic hemicyanine dye by reverse microemulsion method. Obvious solvatochromism on the absorption spectra of dye-doped NPs indicates that solvents can partly penetrate into the silica matrix and then affect the ground and excited state of dye molecules. For dye-doped NP suspensions, both one-photon and two-photon excited fluorescence are much stronger and recorded at shorter wavelength compared to those of free dye solutions with comparative overall dye concentration. This behavior is possibly attributed to the restricted twisted intramolecular charge transfer (TICT), which reduces fluorescence quenching when dye molecules are trapped in the silica matrix. Images from two-photon laser scanning fluorescence microscopy demonstrate that the dye-doped silica NPs can be actively uptaken by Hela cells with low cytotoxicity. - Graphical abstract: Water-soluble silica NPs doped with a two-photon absorbing zwitterionic hemicyanine dye were prepared. They were found of enhanced one-photon and two-photon excited fluorescence compared to free dye solutions. Images from two-photon laser scanning fluorescence microscopy demonstrate that the dye-doped silica NPs can be actively uptaken by Hela cells.

  15. Two Photon Polymerization of Microneedles for Transdermal Drug Delivery

    PubMed Central

    Gittard, Shaun D.; Ovsianikov, Aleksandr; Chichkov, Boris N.; Doraiswamy, Anand; Narayan, Roger J.

    2010-01-01

    Importance of the field Microneedles are small-scale devices that are finding use for transdermal delivery of protein-based pharmacologic agents and nucleic acid-based pharmacologic agents; however, microneedles prepared using conventional microelectronics-based technologies have several shortcomings, which have limited translation of these devices into widespread clinical use. Areas covered in this review Two photon polymerization is a laser-based rapid prototyping technique that has been recently used for direct fabrication of hollow microneedles with a wide variety of geometries. In addition, an indirect rapid prototyping method that involves two photon polymerization and polydimethyl siloxane micromolding has been used for fabrication of solid microneedles with exceptional mechanical properties. What the reader will gain In this review, the use of two photon polymerization for fabricating in-plane and out-of-plane hollow microneedle arrays is described. The use of two photon polymerization-micromolding for fabrication of solid microneedles is also reviewed. In addition, fabrication of microneedles with antimicrobial properties is discussed; antimicrobial microneedles may reduce the risk of infection associated with formation of channels through the stratum corneum. Take home message It is anticipated that the use of two photon polymerization as well as two photon polymerization-micromolding for fabrication of microneedles and other microstructured drug delivery devices will increase over the coming years. PMID:20205601

  16. Functional polymers by two-photon 3D lithography

    NASA Astrophysics Data System (ADS)

    Infuehr, Robert; Pucher, Niklas; Heller, Christian; Lichtenegger, Helga; Liska, Robert; Schmidt, Volker; Kuna, Ladislav; Haase, Anja; Stampfl, Jürgen

    2007-12-01

    In the presented work, two-photon 3D lithography and selective single-photon photopolymerization in a prefabricated polydimethylsiloxane matrix is presented as an approach with potential applicability of waveguide writing in 3D by two-photon polymerization. Photopolymers based on acrylate chemistry were used in order to evaluate the optical capabilities of the available two-photon system. Several photoinitiators, tailored for two-photon absorption, were tested in a mixture of trimethylolpropane triacrylate and ethoxylated trimethylolpropane triacrylate. Best results were obtained with a recently synthesized diynone-based photoinitiator. Feature resolutions in the range of 300 nm were achieved. Due to the cross-conjugated nature of that donor-π-acceptor-π-donor system a high two-photon absorption activity was achieved. Therefore, a resin mixture containing only 0.025 wt% of photoinitiator was practical for structuring by two-photon polymerization. The required initiator content was therefore a factor of 100 lower than in traditional one-photon lithography. The aim of the second part of this work was to fabricate optical waveguides by selectively irradiating a polymer network, which was swollen by a monomer. The monomer was polymerized by conventional single-photon polymerization and the uncured monomer was removed by evaporation at elevated temperatures. This treatment leads to a local change in refractive index. Refractive index changes in the range of Δ n = 0.01 (Δ n/ n = 0.7%) were achieved, which is sufficient for structuring waveguides for optoelectronic applications.

  17. Resonance enhanced laser mass spectrometry for process- and environmental-analysis: Applications and perspectives

    NASA Astrophysics Data System (ADS)

    Zimmermann, Ralf; Heger, Hans Jörg; Dorfner, Ralph; Boesl, Ulrich; Kettrup, Antonius

    1998-12-01

    Laser induced Resonance-Enhanced Multi-Photon Ionization Time-Of-Flight Mass Spectrometry (REMPI TOFMS) is a highly selective as well as sensitive analytical technique, well suited for species selective, on-line monitoring of trace-substances. In this contribution some analytical applications of a mobile REMPI-TOFMS are presented. This includes REMPI-TOMS on-line analysis of coffee roasting gas and waste incineration flue gas as well as headspace measurements of pulp processing lye or rapid analysis of polycyclic aromatic hydrocarbons from soil samples via thermal desorption.

  18. Calculation of the spatial resolution in two-photon absorption spectroscopy applied to plasma diagnosis

    SciTech Connect

    Garcia-Lechuga, M.; Fuentes, L. M.; Grützmacher, K.; Pérez, C. Rosa, M. I. de la

    2014-10-07

    We report a detailed characterization of the spatial resolution provided by two-photon absorption spectroscopy suited for plasma diagnosis via the 1S-2S transition of atomic hydrogen for optogalvanic detection and laser induced fluorescence (LIF). A precise knowledge of the spatial resolution is crucial for a correct interpretation of measurements, if the plasma parameters to be analysed undergo strong spatial variations. The present study is based on a novel approach which provides a reliable and realistic determination of the spatial resolution. Measured irradiance distribution of laser beam waists in the overlap volume, provided by a high resolution UV camera, are employed to resolve coupled rate equations accounting for two-photon excitation, fluorescence decay and ionization. The resulting three-dimensional yield distributions reveal in detail the spatial resolution for optogalvanic and LIF detection and related saturation due to depletion. Two-photon absorption profiles broader than the Fourier transform-limited laser bandwidth are also incorporated in the calculations. The approach allows an accurate analysis of the spatial resolution present in recent and future measurements.

  19. Confocal and Two-Photon Microscopy: Foundations, Applications and Advances

    NASA Astrophysics Data System (ADS)

    Diaspro, Alberto

    2001-11-01

    Confocal and Two-Photon Microscopy Foundations, Applications, and Advances Edited by Alberto Diaspro Confocal and two-photon fluorescence microscopy has provided researchers with unique possibilities of three-dimensional imaging of biological cells and tissues and of other structures such as semiconductor integrated circuits. Confocal and Two-Photon Microscopy: Foundations, Applications, and Advances provides clear, comprehensive coverage of basic foundations, modern applications, and groundbreaking new research developments made in this important area of microscopy. Opening with a foreword by G. J. Brakenhoff, this reference gathers the work of an international group of renowned experts in chapters that are logically divided into balanced sections covering theory, techniques, applications, and advances, featuring: In-depth discussion of applications for biology, medicine, physics, engineering, and chemistry, including industrial applications Guidance on new and emerging imaging technology, developmental trends, and fluorescent molecules Uniform organization and review-style presentation of chapters, with an introduction, historical overview, methodology, practical tips, applications, future directions, chapter summary, and bibliographical references Companion FTP site with full-color photographs The significant experience of pioneers, leaders, and emerging scientists in the field of confocal and two-photon excitation microscopy Confocal and Two-Photon Microscopy: Foundations, Applications, and Advances is invaluable to researchers in the biological sciences, tissue and cellular engineering, biophysics, bioengineering, physics of matter, and medicine, who use these techniques or are involved in developing new commercial instruments.

  20. Two-photon excitation in laser scanning fluorescence microscopy

    NASA Astrophysics Data System (ADS)

    Strickler, James H.; Webb, Watt W.

    1991-04-01

    Simultaneous absorption of two red photons from a strongly focused subpicosecond colliding pulse mode4ocked dye laser stimulates visible fluorescence emission from fluorophores having their normal absorption in the ultraviolet1. The quadratic increase of the two-photon excitation rate with excitation intensity restricts fluorescence emission to the focal volume thus providing the same depth resolution as does confocal microscopy. Image degradation due to out of focus backround is thus avoided. Photobleaching and most cellular photodamage are similarly confined to the focus thereby minimizing sample degredation during acquisition of the multiple sections required for 3-d image reconstruction. Fluorescence images of living cells and other thick photolabile fluorescence labled assemblies illustrate the depth discrimination of both two-photon fluorescence excitation and photobleaching. The quadratic intensity dependence of two-photon excitation allows 3-d spatially resolved photochemistry in particular the photolytic release of caged compounds such as neurotransmitters nucleotides fluorescent dyes and second messengers such as 1P3 and Ca. The two-photon release of cased ATP has been measured and release of a caged fluorescent dye has been shown. Point photobleaching and a 3-d " write once read many" optical memory have been demonstrated. Two-photon excitation of photo-initiated polymerization with a sharply focused single beam allows microfabrication of complex structures of arbitrary form. By scanning the focused beam through a liquid polymer with a UV excited initiator it is possible to harden the polymer only at the focus thereby creating

  1. Three-dimensional two-photon memory materials and systems

    NASA Astrophysics Data System (ADS)

    Ford, Joseph E.; Hunter, Susan; Piyaket, Ram; Fainman, Yeshaiahu; Esener, Sadik C.; Dvornikov, Alexander S.; Rentzepis, Peter M.

    1993-04-01

    We have been developing a two-photon 3-D memory expected to provide a Tbit storage capacity and a 1 ms access time for secondary storage. Even with this new technology, there still exists a four order of magnitude gap in access times between electronic RAMS and secondary storage. In addition to the existing permanent storage approach, we have begun working on systems, key components, and materials for a dynamic parallel-access 3-D two photon memories that will bridge the gap in primary memory technologies. Over the past three years our team has been developing a write-once mass-storage memory based on two-photon bond dissociation of spirobenzopyran molecules for long lifetime storage. A cache memory must have fast write-erase capability. To achieve this we are beginning to investigate highly sensitive two-photon materials which spontaneous decay (self-erase) to the off state. These materials will be incorporated into dynamic memory systems which continually refresh the memory contents, as in an electronic DRAM. The resulting memory is expected to provide a data capacity of 1 Gbit/cm3 with a 10 ns to 1 microsecond(s) access time and a 10 Tbit/s data rate. In this presentation the latest results of the parallel-access 3-D volume memory using two-photon storage is discussed. We cover material and system considerations for both types of parallel-access memories: fast-access primary storage and large-capacity secondary storage.

  2. Two-photon flow cytometer with laser scanning Bessel beams

    NASA Astrophysics Data System (ADS)

    Wang, Yongdong; Ding, Yu; Ray, Supriyo; Paez, Aurelio; Xiao, Chuan; Li, Chunqiang

    2016-03-01

    Flow cytometry is an important technique in biomedical discovery for cell counting, cell sorting and biomarker detection. In vivo flow cytometers, based on one-photon or two-photon excited fluorescence, have been developed for more than a decade. One drawback of laser beam scanning two-photon flow cytometer is that the two-photon excitation volume is fairly small due to the short Rayleigh range of a focused Gaussian beam. Hence, the sampling volume is much smaller than one-photon flow cytometry, which makes it challenging to count or detect rare circulating cells in vivo. Bessel beams have narrow intensity profiles with an effective spot size (FWHM) as small as several wavelengths, making them comparable to Gaussian beams. More significantly, the theoretical depth of field (propagation distance without diffraction) can be infinite, making it an ideal solution as a light source for scanning beam flow cytometry. The trade-off of using Bessel beams rather than a Gaussian beam is the fact that Bessel beams have small concentric side rings that contribute to background noise. Two-photon excitation can reduce this noise, as the excitation efficiency is proportional to intensity squared. Therefore, we developed a two-photon flow cytometer using scanned Bessel beams to form a light sheet that intersects the micro fluidic channel.

  3. Two-photon interference between disparate sources for quantum networking

    PubMed Central

    McMillan, A. R.; Labonté, L.; Clark, A. S.; Bell, B.; Alibart, O.; Martin, A.; Wadsworth, W. J.; Tanzilli, S.; Rarity, J. G.

    2013-01-01

    Quantum networks involve entanglement sharing between multiple users. Ideally, any two users would be able to connect regardless of the type of photon source they employ, provided they fulfill the requirements for two-photon interference. From a theoretical perspective, photons coming from different origins can interfere with a perfect visibility, provided they are made indistinguishable in all degrees of freedom. Previous experimental demonstrations of such a scenario have been limited to photon wavelengths below 900 nm, unsuitable for long distance communication, and suffered from low interference visibility. We report two-photon interference using two disparate heralded single photon sources, which involve different nonlinear effects, operating in the telecom wavelength range. The measured visibility of the two-photon interference is 80 ± 4%, which paves the way to hybrid universal quantum networks. PMID:23783585

  4. Relative fine-structure intensities in two-photon excitation

    NASA Technical Reports Server (NTRS)

    Crosley, D. R.; Bischel, W. K.

    1984-01-01

    A discrepancy is pointed out between experimental determinations of the relative intensities for different fine-structure components of the two-photon transitions 2p3P 3p3P in oxygen and 2p3 4S0 - 2p2 3p4D0 in nitrogen, which agreed well with calculations involving a single virtual intermediate level, and a two-photon selection rule dJ not equal to one, derived in a purely theoretical and erroneous treatment of these transitions. Five other experiments are also briefly examined, with the conclusion that relative fine-structure intensities in two-photon transitions are well understood as straightforward extensions of angular momentum coupling in single-photon cases, in accordance with allowed dJ = 0, + or -1, and + or -2 transitions.

  5. Interference and complementarity for two-photon hybrid entangled states

    SciTech Connect

    Nogueira, W. A. T.; Santibanez, M.; Delgado, A.; Saavedra, C.; Neves, L.; Lima, G.; Padua, S.

    2010-10-15

    In this work we generate two-photon hybrid entangled states (HESs), where the polarization of one photon is entangled with the transverse spatial degree of freedom of the second photon. The photon pair is created by parametric down-conversion in a polarization-entangled state. A birefringent double-slit couples the polarization and spatial degrees of freedom of these photons, and finally, suitable spatial and polarization projections generate the HES. We investigate some interesting aspects of the two-photon hybrid interference and present this study in the context of the complementarity relation that exists between the visibility of the one-photon and that of the two-photon interference patterns.

  6. Two-photon excitation laser scanning microscopy: applications in neuroscience

    NASA Astrophysics Data System (ADS)

    Denk, Winfried

    1996-05-01

    High resolution fluorescence imaging in intact tissues faces special challenges posed by scattering of excitation and fluorescence light and the need to avoid photodynamic damage. Significant improvements over conventional widefield and confocal imaging are provided when two-photon excitation is used. Applications to the functional imaging of the calcium dynamics in synaptic spines, small invertebrate neurites, and auditory hair cells are shown. Two-photon absorption induced photolysis can also be used for scanning photochemical microscopy and for high resolution measurements of diffusional coupling between cellular compartments.

  7. Two-photon interference with non-identical photons

    NASA Astrophysics Data System (ADS)

    Liu, Jianbin; Zhou, Yu; Zheng, Huaibin; Chen, Hui; Li, Fu-li; Xu, Zhuo

    2015-11-01

    Two-photon interference with non-identical photons is studied based on the superposition principle in Feynman's path integral theory. The second-order temporal interference pattern is observed by superposing laser and pseudothermal light beams with different spectra. The reason why there is two-photon interference for photons of different spectra is that non-identical photons can be indistinguishable for the detection system when Heisenberg's uncertainty principle is taken into account. These studies are helpful to understand the second-order interference of light in the language of photons.

  8. Spatial solitons in two-photon photorefractive media

    SciTech Connect

    Hou Chunfeng; Pei Yanbo; Zhou Zhongxiang; Sun Xiudong

    2005-05-15

    We provide a theory for spatial solitons due to the two-photon photorefractive effect based on the Castro-Camus model [Opt. Lett. 28, 1129 (2003)]. We present the evolution equation of one-dimensional spatial solitons in two-photon photorefractive media. In steady state and under appropriate external bias conditions, we obtain the dark and bright soliton solutions of the optical wave evolution equation, and also discuss the self-deflection of the bright solitons theoretically by taking into account the diffusion effect.

  9. Spatial solitons in two-photon photorefractive media

    NASA Astrophysics Data System (ADS)

    Hou, Chunfeng; Pei, Yanbo; Zhou, Zhongxiang; Sun, Xiudong

    2005-05-01

    We provide a theory for spatial solitons due to the two-photon photorefractive effect based on the Castro-Camus model [Opt. Lett. 28, 1129 (2003)]. We present the evolution equation of one-dimensional spatial solitons in two-photon photorefractive media. In steady state and under appropriate external bias conditions, we obtain the dark and bright soliton solutions of the optical wave evolution equation, and also discuss the self-deflection of the bright solitons theoretically by taking into account the diffusion effect.

  10. Two-photon Compton process in pulsed intense laser fields

    NASA Astrophysics Data System (ADS)

    Seipt, Daniel; Kämpfer, Burkhard

    2012-05-01

    Based on strong-field QED in the Furry picture we use the Dirac-Volkov propagator to derive a compact expression for the differential emission probability of the two-photon Compton process in a pulsed intense laser field. The relation of real and virtual intermediate states is discussed, and the natural regularization of the on-shell contributions due to the finite laser pulse is highlighted. The inclusive two-photon spectrum is 2 orders of magnitude stronger than expected from a perturbative estimate.

  11. Relativistic Calculation of the Two-Photon Bremsstrahlung Process

    NASA Astrophysics Data System (ADS)

    Fedorova, T. A.; Korol, A. V.; Solovjev, I. A.

    We present analytical and numerical results on the relativistic calculation of the two-photon bremsstrahlung process. For the approximate calculation of relativistic free-free two-photon matrix elements in the central field, we applied the method based on the accurate treatment of the diagonal singularities in the relativistic free-free single-photon matrix elements. Numerical calculations are carried out with the Furry-Sommerfeld-Maue wave functions. The obtained results are compared with the results of the relativistic Born approximation.

  12. Resonantly enhanced method for generation of tunable, coherent vacuum ultraviolet radiation

    DOEpatents

    Glownia, James H.; Sander, Robert K.

    1985-01-01

    Carbon Monoxide vapor is used to generate coherent, tunable vacuum ultraviolet radiation by third-harmonic generation using a single tunable dye laser. The presence of a nearby electronic level resonantly enhances the nonlinear susceptibility of this molecule allowing efficient generation of the vuv light at modest pump laser intensities, thereby reducing the importance of a six-photon multiple-photon ionization process which is also resonantly enhanced by the same electronic level but to higher order. By choosing the pump radiation wavelength to be of shorter wavelength than individual vibronic levels used to extend tunability stepwise from 154.4 to 124.6 nm, and the intensity to be low enough, multiple-photon ionization can be eliminated. Excitation spectra of the third-harmonic emission output exhibit shifts to shorter wavelength and broadening with increasing CO pressure due to phase matching effects. Increasing the carbon monoxide pressure, therefore, allows the substantial filling in of gaps arising from the stepwise tuning thereby providing almost continuous tunability over the quoted range of wavelength emitted.

  13. Resonantly enhanced method for generation of tunable, coherent vacuum-ultraviolet radiation

    DOEpatents

    Glownia, J.H.; Sander, R.K.

    1982-06-29

    Carbon Monoxide vapor is used to generate coherent, tunable vacuum ultraviolet radiation by third-harmonic generation using a single tunable dye laser. The presence of a nearby electronic level resonantly enhances the nonlinear susceptibility of this molecule allowing efficient generation of the vuv light at modest pump laser intensities, thereby reducing the importance of a six-photon multiple-photon ionization process which is also resonantly enhanced by the same electronic level but no higher order. By choosing the pump radiation wavelength to be of shorter wavelength than individual vibronic levels used to extend tunability stepwise from 154.4 to 124.6 nm, and the intensity to be low enough, multiple-photon ionization can be eliminated. Excitation spectra of the third-harmonic emission output exhibit shifts to shorter wavelength and broadening with increasing CO pressure due to phase matching effects. Increasing the carbon monoxide pressure, therefore, allows the substantial filling in of gaps arising from the stepwise tuning thereby providing almost continuous tunability over the quoted range of wavelength emitted.

  14. Two-photon absorbing porphyrins for oxygen microscopy (Conference Presentation)

    NASA Astrophysics Data System (ADS)

    Esipova, Tatiana V.; Vinogradov, Sergei A.

    2016-03-01

    The ability to quantify oxygen in vivo in 3D with high spatial and temporal resolution is invaluable for many areas of the biomedical science, including ophthalmology, neuroscience, cancer and stem biology. An optical method based on oxygen-dependent quenching of phosphorescence is being developed, that allows quantitative minimally invasive real-time imaging of partial pressure of oxygen (pO2) in tissue. In the past, dendritically protected phosphorescent oxygen probes with controllable quenching parameters and defined bio-distributions have been developed. More recently our probe strategy has extended to encompass two-photon excitable oxygen probes, which brought about first demonstrations of two-photon phosphorescence lifetime microscopy (2PLM) of oxygen in vivo, providing new valuable information for neuroscience and stem cell biology. However, current two-photon oxygen probes suffer from a number of limitations, such as low brightness and high cost of synthesis, which dramatically reduce imaging performance and limit usability of the method. Here we present an approach to new bright phosphorescent chromophores with internally enhanced two-photon absorption cross-sections, which pave a way to novel proves for 2PLM. In addition to substantial increase in performance, the new probes can be synthesized by much more efficient methods, thereby greatly reducing the cost of the synthesis and making the technique accessible to a broader range of researchers across different fields.

  15. Theory of the Rydberg-atom two-photon micromaser

    SciTech Connect

    Brune, M.; Raimond, J.M.; Haroche, S.

    1987-01-01

    A continuous-wave maser operating on a two-photon transition between Rydberg levels is expected to oscillate with about one atom and a few tens of microwave photons at any time in its superconducting cavity. We analyze in detail the characteristics of this new microscopic quantum electronics device presently under construction in our laboratory.

  16. An Interactive Approach to Two-Photon Microscopy

    NASA Astrophysics Data System (ADS)

    So, Peter T. C.; Yu, Weiming; Ragan, Tim; Gratton, Enrico

    1996-03-01

    Typical fluorescence microscopy is a method for passive observation. Novel two-photon microscopy has typical excitation volume on the order of 0.1 femtoliter. This ability to selectively excite a small region in a sample has opened new opportunities for interactive experimentation. Two emerging interactive two-photon techniques will be described. Single particle tracking has been applied to the study of protein diffusion and interaction. The traditional approach is limited to monitoring two dimensional motions with video rate time resolution. We have developed a 3-D two-photon particle tracking instrument. Using a real-time feedback system, we can interactively follow the position of the diffusing fluorescent particle by maximizing detected intensity. This system has been used to study the process of antigen endocytosis of macrophage. (2) There are no reliable manipulation methods for objects, such as virus particles, of sizes below 0.1 micrometer but larger than atomic dimensions. Two-photon excitation can initiate localized chemical reaction for nanomanipulation. Consider the diffusion of an object in a photo-polymerizable medium. By locally polymerizing the medium adjacent to the object, we can break the spatial symmetry of the diffusion of the object and interactively direct its motion. [Supported by NIH grant RR03155.

  17. Multimodal dyes: toward correlative two-photon and electron microscopy

    NASA Astrophysics Data System (ADS)

    Bolze, Frédéric; Ftouni, Hussein; Nicoud, Jean-François; Leoni, Piero; Schwab, Yannick; Rehspringer, Jean-Luc; Mafouana, Rodrigues R.

    2013-03-01

    Nowadays, many crucial biological questions involve the observation of biological samples at different scales. Thus, optical microscopy can be associated to magnetic nuclear imaging allowing access to data from the cellular to the organ level, or can be associated to electron microscopy to reach the sub cellular level. We will describe here the design, synthesis and characterization of new bimodal probes, which can be used as dye in two-photon excited microscopy (TPEM) and electron dense markers in scanning and transmission electron microscopy (EM). In a first part, we will describe new molecular dyes with small organic systems grafted on metal atoms (Pt, Au). Such systems show good twophoton induced fluorescence and two-photon images of HeLa cells will be presented. In a second part, we will present hybrid organic-inorganic fluorescent systems with diketopyrrolopyrole-based dye grafted on iron oxide-silica core shell nanoparticles by peptide bond. Such systems present high two-photon absorption cross sections and good fluorescence quantum yields. These nanoparticles are rapidly internalized in HeLa cells and high quality two-photon images were performed with low laser power. Then we will present our results on correlative light-electron microscopy were twophoton and electron microscopy (both scanning and transmission) images were obtained on the same biological sample.

  18. Four new two-photon polymerization initiators with varying donor and conjugated bridge: Synthesis and two-photon activity

    NASA Astrophysics Data System (ADS)

    Hao, Fuying; Liu, Zhaodi; Zhang, Mingliang; Liu, Jie; Zhang, Shengyi; Wu, Jieying; Zhou, Hongping; Tian, YuPeng

    2014-01-01

    A specific series of dumbbell-shaped bis-carbazoles or bis-phenothiazines dyes (1, 2, 3 and 4) constructed with styrene or biphenylethyne as the π-bridge have been synthesized and characterized. Detailed spectral properties including linear absorption, one and two-photon fluorescence properties were investigated. The results show that extending conjugated chain and introducing donors have substantial effect on their photophysical properties. Among them, two-photon absorption cross sections (σ) of the four dyes in DMF determined by the Z-scan technique are successively increased from 1 to 4 with enhancing electron-donating ability and extending conjugated chain, but electron-donating ability has larger contribution to the σ values than extending conjugated chain based on the comparison of small molecules (D-π-D). Two-photon initiation polymerization (TPIP) microfabrication experiments have been carried out using compound 4 as an initiator under irradiation of 200 fs, 76 MHz femtosecond laser at 760 nm. The results confirm that the four dyes can be effectively used as organic two-photon photopolymerization initiators.

  19. Ultrafast Laser Studies of Two-Photon Excited Fluorescence Intermittency in Single CdSe/ZnS Quantum Dots.

    PubMed

    Early, Kevin T; Nesbitt, David J

    2015-12-01

    Two-photon fluorescence microscopy of single quantum dots conditions has been reported by several groups, with contrasting observations regarding the kinetics and dynamics of fluorescence intermittency or "blinking". Here, we investigate the power dependence, kinetics, and statistics of two photon-excited fluorescence intermittency from single CdSe/ZnS quantum dots in a solid PMMA film as a function of sub-bandgap laser intensity at 800 nm. Fluorescence intermittency is observed at all excitation powers and a quadratic (n = 1.97(3)) dependence of the shot noise-limited fluorescence intensity on the incident laser power is verified, confirming essentially zero background contribution from one-photon excitation processes. Such analyses permit two photon absorption cross sections for single quantum dots to be extracted quantitatively from the data, which reveal good agreement with those obtained from previous two-photon FCS measurements. Strictly inverse power law-distributed off-state dwell times are observed for all excitation powers, with a mean power law exponent ⟨m(off)⟩ = 1.65(4) in excellent agreement with the behavior observed under one-photon excitation conditions. Finally, a superquadratic (n = 2.3(2)) rather than quartic (n = 4) power dependence is observed for the on-state blinking dwell times, which we kinetically analyze and interpret in terms of a novel 2 + 1 "hot" exciton ionization/blinking mechanism due to partially saturated 1-photon sub-bandgap excitation out of the two-photon single exciton state. The kinetic results are consistent with quantum dot photoionization quantum yields from "hot" exciton states (4(1) × 10(-6)) comparable with experimental estimates (10(-6)-10(-5)) of Auger ionization efficiencies out of the biexcitonic state.

  20. Meson production in two-photon interactions at LHC energies

    SciTech Connect

    Da Silva, D. T.; Goncalves, V. P.; Sauter, W. K.

    2013-03-25

    The LHC opens a new kinematical regime at high energy, where several questions related to the description of the high-energy regime of the Quantum Chromodynamics (QCD) remain without satisfactory answers. Some open questions are the search for non-q-bar q resonances, the determination of the spectrum of q-bar q states and the identification of states with anomalous {gamma}{gamma} couplings. A possible way to study these problems is the study of meson production in two-photon interactions. In this contribution we calculate the meson production in two-photon interactions at LHC energies considering proton - proton collisions and estimate the total cross section for the production of the mesons {pi}, a, f, {eta} and {chi}.

  1. One- and two-photon detachment of O-

    NASA Astrophysics Data System (ADS)

    Génévriez, Matthieu; Urbain, Xavier; Dochain, Arnaud; Cyr, Alain; Dunseath, Kevin M.; Terao-Dunseath, Mariko

    2016-08-01

    Cross sections for one- and two-photon detachment of O-(1 s22 s22 p5P2o) have been determined in a joint experimental and theoretical study. The absolute measurement is based on the animated-crossed-beam technique, which is extended to the case of pulsed lasers, pulsed ion beams, and multiphoton detachment. The ab initio calculations employ R -matrix Floquet theory, with simple descriptions of the initial bound state and the residual oxygen atom which reproduce well the electron affinity and ground-state polarizability. For one-photon detachment, the measured and computed cross sections are in good mutual agreement, departing significantly from previous reference experiments and calculations. The generalized two-photon detachment cross section, measured at the Nd:YAG laser wavelength, is in good agreement with the R -matrix Floquet calculations. Long-standing discrepancies between theory and experiment are thus resolved.

  2. 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.

  3. Integrated photoacoustic, confocal, and two-photon microscope.

    PubMed

    Rao, Bin; Soto, Florentina; Kerschensteiner, Daniel; Wang, Lihong V

    2014-03-01

    The invention of green fluorescent protein and other molecular fluorescent probes has promoted applications of confocal and two-photon fluorescence microscopy in biology and medicine. However, exogenous fluorescence contrast agents may affect cellular structure and function, and fluorescence microscopy cannot image nonfluorescent chromophores. We overcome this limitation by integrating optical-resolution photoacoustic microscopy into a modern Olympus IX81 confocal, two-photon, fluorescence microscope setup to provide complementary, label-free, optical absorption contrast. Automatically coregistered images can be generated from the same sample. Imaging applications in ophthalmology, developmental biology, and plant science are demonstrated. For the first time, in a familiar microscopic fluorescence imaging setting, this trimodality microscope provides a platform for future biological and medical discoveries.

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

    PubMed Central

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

    2016-01-01

    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. PMID:27446680

  5. Direct frequency comb two-photon laser cooling and trapping

    NASA Astrophysics Data System (ADS)

    Long, Xueping; Jayich, Andrew; Campbell, Wesley C.

    2016-05-01

    Generating and manipulating high energy photons for spectroscopy on electric dipole transitions of atoms and molecules with deeply bound valence electrons is difficult. Further, laser cooling of such species is even more challenging for lack of laser power. A possible solution is to drive two-photon transitions. This may alleviate the photon energy problem and open the door to cold, trapped samples of highly desirable species with tightly bound electrons. We perform a proof of principle experiment with rubidium by driving a two-photon transition with an optical frequency comb. We perform optical cooling and extend this technique to trapping, where we are able to make a magneto-optical trap in one dimension. This work is supported by the National Science Foundation CAREER program.

  6. Two-photon-induced cycloreversion reaction of chalcone photodimers

    NASA Astrophysics Data System (ADS)

    Träger, J.; Härtner, S.; Heinzer, J.; Kim, H.-C.; Hampp, N.

    2008-04-01

    The photocleavage reaction of chalcone photodimers has been studied using a two-photon process. For this purpose, a novel chalcone dimer has been synthesized as a low molecular weight model substance for polymer bound chalcones and its photochemistry triggered by two-photon-absorption (2PA) has been investigated using a pulsed frequency-doubled Nd:YAG-laser. The 2PA-induced cycloreversion reaction selectively leads to the cleavage of the chalcone photodimers resulting in the formation of monomeric chalcone molecules. Hence, as an application chalcones can be used as a photosensitive linker which can be cleaved beyond an UV-absorbing barrier. The 2PA cross section of the chalcone photodimer was determined to be of 1.1 × 10 -49 cm 4 s photon -1 (11 GM).

  7. Combinatorial discovery of two-photon photoremovable protecting groups.

    PubMed

    Pirrung, Michael C; Pieper, Wolfgang H; Kaliappan, Krishna P; Dhananjeyan, Mugunthu R

    2003-10-28

    A design principle for a two-photon photochemically removable protecting group based on sequential one-photon processes has been established. The expected performance of such groups in spatially directed photoactivation/photodeprotection has been shown by a kinetic analysis. One particular molecular class fitting into this design, the nitrobenzyl ethers of o-hydroxycinnamates, has been presented. An initial demonstration of two-photon deprotection of one such group prompted further optimization with respect to photochemical deprotection rate. This was accomplished by the preparation and screening of a 135-member indexed combinatorial library. Optimum performance for lambda >350 nm deprotection in organic solvent was found with 4,5-dialkoxy and -cyano substitution in the nitrobenzyl group and 4-methoxy substitution in the cinnamate. PMID:14557545

  8. Multiple pulse resonantly enhanced laser plasma wakefield acceleration

    SciTech Connect

    Corner, L.; Walczak, R.; Nevay, L. J.; Dann, S.; Hooker, S. M.; Bourgeois, N.; Cowley, J.

    2012-12-21

    We present an outline of experiments being conducted at Oxford University on multiple-pulse, resonantly-enhanced laser plasma wakefield acceleration. This method of laser plasma acceleration uses trains of optimally spaced low energy short pulses to drive plasma oscillations and may enable laser plasma accelerators to be driven by compact and efficient fibre laser sources operating at high repetition rates.

  9. Simultaneous two-photon excitation of photodynamic therapy agents

    SciTech Connect

    Wachter, E.A.; Fisher, W.G. |; Partridge, W.P.; Dees, H.C.; Petersen, M.G.

    1998-01-01

    The spectroscopic and photochemical properties of several photosensitive compounds are compared using conventional single-photon excitation (SPE) and simultaneous two-photon excitation (TPE). TPE is achieved using a mode-locked titanium:sapphire laser, the near infrared output of which allows direct promotion of non-resonant TPE. Excitation spectra and excited state properties of both type 1 and type 2 photodynamic therapy (PDT) agents are examined.

  10. Light-Meson Two-Photon Decays in Full QCD

    SciTech Connect

    Cohen, Saul; Lin, Huey-Wen; Dudek, Jozef; Edwards, Robert

    2008-12-01

    We present a study of two-photon decays of light mesons, focusing on the neutral pion decay. This important process highlights the effects of the axial anomaly in QCD but has been little studied on the lattice. By applying the Lehmann-Symanzik-Zimmermann (LSZ) reduction formula, we reconstruct the electromagnetic matrix elements from three-point vector-vector Green functions calculated on 2+1-flavor isotropic clover lattices.

  11. Chirping a two-photon transition in a multistate ladder

    SciTech Connect

    Merkel, Wolfgang; Mack, Holger; Schleich, Wolfgang P.; Lutz, Eric; Paulus, Gerhard G.; Girard, Bertrand

    2007-08-15

    We consider a two-photon transition in a specific ladder system driven by a chirped laser pulse. In the weak field limit, we find that the excited state probability amplitude arises due to interference of multiple quantum paths which are weighted by quadratic phase factors. The excited state population has the form of a Gauss sum which plays a prominent role in number theory.

  12. Two-photon exchange and elastic electron-proton scattering

    SciTech Connect

    Peter Blunden; Wally Melnitchouk; John Tjon

    2003-06-01

    Two-photon exchange contributions to elastic electron-proton scattering cross sections are evaluated in a simple hadronic model including the finite size of the proton. The corrections are found to be small, but with a strong angular dependence at fixed Q{sup 2}. This is significant for the Rosenbluth technique for determining the ratio of electric and magnetic form factors of the proton, and partly reconciles the apparent discrepancy with the results of the polarization transfer technique.

  13. 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.

  14. Two-Photon Absorption in Organometallic Bromide Perovskites.

    PubMed

    Walters, Grant; Sutherland, Brandon R; Hoogland, Sjoerd; Shi, Dong; Comin, Riccardo; Sellan, Daniel P; Bakr, Osman M; Sargent, Edward H

    2015-09-22

    Organometallic trihalide perovskites are solution-processed semiconductors that have made great strides in third-generation thin film light-harvesting and light-emitting optoelectronic devices. Recently, it has been demonstrated that large, high-purity single crystals of these perovskites can be synthesized from the solution phase. These crystals' large dimensions, clean bandgap, and solid-state order have provided us with a suitable medium to observe and quantify two-photon absorption in perovskites. When CH3NH3PbBr3 single crystals are pumped with intense 800 nm light, we observe band-to-band photoluminescence at 572 nm, indicative of two-photon absorption. We report the nonlinear absorption coefficient of CH3NH3PbBr3 perovskites to be 8.6 cm GW(-1) at 800 nm, comparable to epitaxial single-crystal semiconductors of similar bandgap. We have leveraged this nonlinear process to electrically autocorrelate a 100 fs pulsed laser using a two-photon perovskite photodetector. This work demonstrates the viability of organometallic trihalide perovskites as a convenient and low-cost nonlinear absorber for applications in ultrafast photonics.

  15. Localizable and photoactivatable fluorophore for spatiotemporal two-photon bioimaging.

    PubMed

    Zhou, Liyi; Zhang, Xiaobing; Lv, Yifan; Yang, Chao; Lu, Danqing; Wu, Yuan; Chen, Zhuo; Liu, Qiaoling; Tan, Weihong

    2015-06-01

    Photoactivatable probe-based fluorescent imaging has become an efficient and attractive technique for spatiotemporal microscopic studies of biological events. However, almost all previously reported photoactivatable organic probes have been based on hydrosoluble precursors, which have produced water-soluble active fluorophores able to readily diffuse away from the photocleavage site, thereby dramatically reducing spatial resolution. Hydroxyphenylquinazolinone (HPQ), a small organic dye known for its classic luminescence mechanism through excited-state intramolecular proton transfer (ESIPT), shows strong light emission in the solid state, but no emission in solution. In this work, HPQ was employed as a precursor to develop a localizable, photoactivatable two-photon probe (PHPQ) for spatiotemporal bioimaging applications. After photocleavage, PHPQ releases a precipitating HPQ fluorophore which shows both one-photon and two-photon excited yellow-green fluorescence, thereby producing a localizable fluorescence signal that affords high spatial resolution for bioimaging, with more than 200-fold one-photon and 150-fold two-photon fluorescence enhancement.

  16. 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.

  17. 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

  18. Near-threshold photoelectron angular distributions from two-photon resonant photoionization of He

    NASA Astrophysics Data System (ADS)

    O'Keeffe, P.; Mihelič, A.; Bolognesi, P.; Žitnik, M.; Moise, A.; Richter, R.; Avaldi, L.

    2013-01-01

    Two-photon resonant photoionization of helium is investigated both experimentally and theoretically. Ground state helium atoms are excited to the 1s4p, 1s5p and 1s6p 1P states by synchrotron radiation and ionized by a synchronized infrared pulsed picosecond laser. The photoelectron angular distributions of the emitted electrons are measured using a velocity map imaging (VMI) spectrometer. The measured asymmetry parameters of the angular distribution allow the phase differences and the ratios of the dipole matrix elements of the 1sɛs and 1sɛd channels to be determined. The experimental results agree with the calculated values obtained in a configuration-interaction calculation with a Coulomb-Sturmian basis set. The effects of the radiative decay of the intermediate state and the static electric field of the VMI spectrometer on the measurements are discussed.

  19. Cross sections of one- and two-photon detachment of the hydrogen negative ion

    NASA Astrophysics Data System (ADS)

    Pazdzersky, V. A.; Usachenko, V. I.; Ushnurtsev, A. V.

    2000-03-01

    The model non-local separable Yamaguchi potential is proposed as being particularly appropriate for the description of the interaction of a detached electron with its parent residual atomic core in a theoretical treatment of the processes of H- negative ion multiphoton detachment in a monochromatic electromagnetic (EM) field of both linear and circular polarization. Within the framework of that model we derive exact analytical expressions for the cross sections of the one- and two-photon H- detachment processes in the lowest orders of perturbation theory on EM interaction of the detached electron with an ionizing field and studied the effect of various values of the problem parameters. We show that both obtained cross sections are in good agreement with the values measured in relevant experiments and the best results calculated by other authors with different (but much more sophisticated and complicated) approaches and methods.

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

    SciTech Connect

    Sinclair, Michael B.; Melgaard, David Kennett; Reichardt, Thomas A.; Timlin, Jerilyn Ann; Garcia, Omar Fidel; Luk, Ting Shan; Jones, Howland D. T.; Collins, Aaron M.

    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 we 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 two-photon

  1. Two-Photon Fluorescence Microscopy Developed for Microgravity Fluid Physics

    NASA Technical Reports Server (NTRS)

    Fischer, David G.; Zimmerli, Gregory A.; Asipauskas, Marius

    2004-01-01

    Recent research efforts within the Microgravity Fluid Physics Branch of the NASA Glenn Research Center have necessitated the development of a microscope capable of high-resolution, three-dimensional imaging of intracellular structure and tissue morphology. Standard optical microscopy works well for thin samples, but it does not allow the imaging of thick samples because of severe degradation caused by out-of-focus object structure. Confocal microscopy, which is a laser-based scanning microscopy, provides improved three-dimensional imaging and true optical sectioning by excluding the out-of-focus light. However, in confocal microscopy, out-of-focus object structure is still illuminated by the incoming beam, which can lead to substantial photo-bleaching. In addition, confocal microscopy is plagued by limited penetration depth, signal loss due to the presence of a confocal pinhole, and the possibility of live-cell damage. Two-photon microscopy is a novel form of laser-based scanning microscopy that allows three-dimensional imaging without many of the problems inherent in confocal microscopy. Unlike one-photon microscopy, it utilizes the nonlinear absorption of two near-infrared photons. However, the efficiency of two-photon absorption is much lower than that of one-photon absorption because of the nonlinear (i.e., quadratic) electric field dependence, so an ultrafast pulsed laser source must typically be employed. On the other hand, this stringent energy density requirement effectively localizes fluorophore excitation to the focal volume. Consequently, two-photon microscopy provides optical sectioning and confocal performance without the need for a signal-limiting pinhole. In addition, there is a reduction in photo-damage because of the longer excitation wavelength, a reduction in background fluorescence, and a 4 increase in penetration depth over confocal methods because of the reduction in Rayleigh scattering.

  2. Two-photon imaging and analysis of neural network dynamics

    NASA Astrophysics Data System (ADS)

    Lütcke, Henry; Helmchen, Fritjof

    2011-08-01

    The glow of a starry night sky, the smell of a freshly brewed cup of coffee or the sound of ocean waves breaking on the beach are representations of the physical world that have been created by the dynamic interactions of thousands of neurons in our brains. How the brain mediates perceptions, creates thoughts, stores memories and initiates actions remains one of the most profound puzzles in biology, if not all of science. A key to a mechanistic understanding of how the nervous system works is the ability to measure and analyze the dynamics of neuronal networks in the living organism in the context of sensory stimulation and behavior. Dynamic brain properties have been fairly well characterized on the microscopic level of individual neurons and on the macroscopic level of whole brain areas largely with the help of various electrophysiological techniques. However, our understanding of the mesoscopic level comprising local populations of hundreds to thousands of neurons (so-called 'microcircuits') remains comparably poor. Predominantly, this has been due to the technical difficulties involved in recording from large networks of neurons with single-cell spatial resolution and near-millisecond temporal resolution in the brain of living animals. In recent years, two-photon microscopy has emerged as a technique which meets many of these requirements and thus has become the method of choice for the interrogation of local neural circuits. Here, we review the state-of-research in the field of two-photon imaging of neuronal populations, covering the topics of microscope technology, suitable fluorescent indicator dyes, staining techniques, and in particular analysis techniques for extracting relevant information from the fluorescence data. We expect that functional analysis of neural networks using two-photon imaging will help to decipher fundamental operational principles of neural microcircuits.

  3. Two-Photon Exchange in (Semi-)Inclusive DIS

    SciTech Connect

    Schlegel, Marc; Metz, Andreas

    2009-01-01

    In this note we consider effects of a Two-Photon Exchange (TPE) in inclusive DIS and semi-inclusive DIS (SIDIS). In particular, transverse single spin asymmetries are generated in inclusive DIS if more than one photon is exchanged between the lepton and the hadron. We briefly summarize the TPE in DIS in the parton model and extend our approach to SIDIS, where a new leading twist $\\sin(2\\phi)$ contribution to the longitudinal beam spin asymmetry shows up. Possible TPE effects for the Sivers and the Collins asymmetries in SIDIS are power-suppressed.

  4. Two-photon physics as a probe of hadron dynamics

    SciTech Connect

    Brodsky, S.J.

    1981-05-01

    Two-photon collisions provide an ideal laboratory for testing many features of quantum chromodynamics, especially the interplay between the vector-meson-dominated and point-like hadronic interactions of the photon. A number of QCD applications are discussed, including: jet and single-particle production at large transverse momentum; the photon structure function and its relationship to the ..gamma.. ..-->.. q anti q wave function; and the possible role of gluonium states in the ..gamma gamma.. ..-->.. rho/sup 0/rho/sup 0/ channel. Evidence that even low momentum transfer photon-hadron interactions are sensitive to the point-like ..gamma.. ..-->.. q anti q coupling is discussed.

  5. Two-photon exclusive processes in quantum chromodynamics

    SciTech Connect

    Brodsky, S.J.

    1986-07-01

    QCD predictions for ..gamma gamma.. annihilation into single mesons, meson pairs, and baryon pairs are reviewed. Two-photon exclusive processes provide the most sensitive and practical measure of the distribution amplitudes, and thus a critical confrontation between QCD and experiment. Both the angular distribution and virtual photon mass dependence of these amplitudes are sensitive to the shapes of the phi (chi, Q). Novel effects involving the production of qq anti q anti q states at threshold are also discussed, and a new method is presented for systematically incorporating higher-order QCD corrections in ..gamma gamma.. reactions.

  6. Rate for annihilation of galactic dark matter into two photons

    SciTech Connect

    Giudice, G.F.; Griest, K.

    1989-04-01

    A calculation of the cross section for neutralino-neutralino annihilation into two photons is performed and applied to dark matter in the galactic halo to find the counting rate in a large gamma ray detector such as EGRET (Energetic Gamma Ray Experiment Telescope) or ASTROGAM. Combining constraints from particle accelerators with the requirement that the neutralinos make up the dark matter, it is found that rates of over a few dozen events per year are unlikely. The assumptions that go into these conclusions are listed. Other particle dark matter candidates which could give larger and perhaps observable signals are suggested.

  7. Rate for annihilation of galactic dark matter into two photons

    SciTech Connect

    Giudice, G.F. ); Griest, K.

    1989-10-15

    We perform a calculation of the cross section for neutralino-neutralino annihilation into two photons and apply it to dark matter in the galactic halo to find the counting rate in a large {gamma}-ray detector such as EGRET or ASTROGAM. Combining constraints from particle accelerators with the requirement that the neutralinos make up the dark matter we find that rates over a few dozen events per year are unlikely. We list the assumptions that go into our conclusions and suggest other particle dark-matter candidates which could give larger and perhaps observable signals.

  8. Rate for annihilation of galactic dark matter into two photons

    NASA Technical Reports Server (NTRS)

    Giudice, Gian F.; Griest, Kim

    1989-01-01

    A calculation of the cross section for neutralino-neutralino annihilation into two photons is performed and applied to dark matter in the galactic halo to find the counting rate in a large gamma ray detector such as EGRET (Energetic Gamma Ray Experiment Telescope) or ASTROGAM. Combining constraints from particle accelerators with the requirement that the neutralinos make up the dark matter, it is found that rates of over a few dozen events per year are unlikely. The assumptions that go into these conclusions are listed. Other particle dark matter candidates which could give larger and perhaps observable signals are suggested.

  9. Two-photon microscopy of nanoparticles and biotissues

    NASA Astrophysics Data System (ADS)

    Rivera, Judith Noemi

    Biomedical Imaging is an important tool in medical research and clinical practice. From understanding the fundamental processes involved in our biological makeup to its use in diagnostics in helping determine what ails us, the advancements in imaging and microscopy have helped shape our view of the world and nature. Microscopy in particular is often used to study the smallest of cells and their dynamical properties while attempting to minimally change the sample being studied. My research objective is largely divided into two parts. The first part consists of designing a video-rate raster scanning two-photon microscope that is faster than current commercially available two-photon microscopes, while maintaining the high-quality optical resolution of the system. This fast scanning mechanism proves to be an essential component in biomedical imaging due to the fact that many biological processes are dynamic and require the use of imaging systems with a high degree of temporal resolution in order to study. The second objective of my research is to implement the microscope, building it up component by component, and then demonstrating its high speed imaging capabilities, in which I have been largely successful. Current commercially available two-photon microscopes have imaging speeds on the order of 2 frames per second; however, our imaging system currently has a video-rate imaging speed at 30 frames per second. In addition, with further improvements and changes to the electronics that control our mirrors, we hope to soon achieve imaging speeds of up to 300 frames per second. Since my goal is to increase the temporal resolvability of images while imaging a fast moving, dynamic biological system, I also helped design and construct a second two-photon microscope that theoretically has the ability to temporally resolve the images on the order of several thousand of frames per second. However, given the high image acquisition period of our relatively low peak power laser, we

  10. Combined two-photon microscopy and angiographic optical coherence tomography

    NASA Astrophysics Data System (ADS)

    Kim, Bumju; Wang, Tae Jun; Li, Qingyun; Nam, Jutaek; Hwang, Sekyu; Chung, Euiheon; Kim, Sungjee; Kim, Ki Hean

    2013-08-01

    A combined two-photon microscopy (TPM) and angiographic optical coherence tomography (OCT) is developed, which can provide molecular, cellular, structural, and vascular information of tissue specimens in vivo. This combined system is implemented by adding an OCT vasculature visualization method to the previous combined TPM and OCT, and then is applied to in vivo tissue imaging. Two animal models, a mouse brain cranial window model and a mouse ear cancer model, are used. Both molecular, cellular information at local regions of tissues, and structural, vascular information at relatively larger regions are visualized in the same sections. In vivo tissue microenvironments are better elucidated by the combined TPM and angiographic OCT.

  11. Combined two-photon microscopy and angiographic optical coherence tomography.

    PubMed

    Kim, Bumju; Wang, Tae Jun; Li, Qingyun; Nam, Jutaek; Hwang, Sekyu; Chung, Euiheon; Kim, Sungjee; Kim, Ki Hean

    2013-08-01

    A combined two-photon microscopy (TPM) and angiographic optical coherence tomography (OCT) is developed, which can provide molecular, cellular, structural, and vascular information of tissue specimens in vivo. This combined system is implemented by adding an OCT vasculature visualization method to the previous combined TPM and OCT, and then is applied to in vivo tissue imaging. Two animal models, a mouse brain cranial window model and a mouse ear cancer model, are used. Both molecular, cellular information at local regions of tissues, and structural, vascular information at relatively larger regions are visualized in the same sections. In vivo tissue microenvironments are better elucidated by the combined TPM and angiographic OCT.

  12. Two-photon photoassociative spectroscopy of ultracold Sr88

    NASA Astrophysics Data System (ADS)

    Martinez de Escobar, Y. N.; Mickelson, P. G.; Pellegrini, P.; Nagel, S. B.; Traverso, A.; Yan, M.; Côté, R.; Killian, T. C.

    2008-12-01

    We present results from two-photon photoassociative spectroscopy of the least-bound vibrational level of the XΣg+1 state of the Sr288 dimer. Measurement of the binding energy allows us to determine the s -wave scattering length a88=-1.4(6)a0 . For the intermediate state, we use a bound level on the metastable S01-P13 potential, which provides large Franck-Condon transition factors and narrow one-photon photoassociative lines that are advantageous for observing quantum-optical effects such as Autler-Townes resonance splittings.

  13. Two-photon entanglement in multiqubit bidirectional-waveguide QED

    NASA Astrophysics Data System (ADS)

    Mirza, Imran M.; Schotland, John C.

    2016-07-01

    We study entanglement generation and control in bidirectional-waveguide QED driven by a two-photon Gaussian wave packet. In particular, we focus on how increasing the number of qubits affects the overall average pairwise entanglement in the system. We also investigate how the presence of a second photon can introduce nonlinearities, thereby manipulating the generated entanglement. In addition, we show that, through the introduction of chirality and small decay rates, entanglement can be stored and enhanced up to factors of 2 and 3, respectively. Finally, we analyze the influence of finite detunings and time-delays on the generated entanglement.

  14. Polarization rotation under two-photon Raman resonance for magnetometry

    SciTech Connect

    Pradhan, S.; Behera, R.; Das, A. K.

    2012-04-23

    The polarization rotation and coherent population trapping signal arising due to two photon process using linearly polarized light are found to be significantly enhanced for a Zeeman degenerate system. The zero crossing of the dispersive profile is found to be shifting proportional to the applied magnetic field, albeit the absorptive profile position remains invariant for a slightly imbalanced orthogonal circular polarization component. It provides an alternative method for precise measurement of vector magnetic field without requirement of a bias field. The use of polarization rotation signal for magnetic field measurement offers added advantage due to improved signal to noise ratio.

  15. Imaging of spatial correlations of two-photon states

    NASA Astrophysics Data System (ADS)

    Bobrov, Ivan B.; Kalashnikov, Dmitry A.; Krivitsky, Leonid A.

    2014-04-01

    We use a fiber-based double-slit Young interferometer for studying the far-field spatial distribution of the two-photon coincidence rate (coincidence pattern) for various quantum states with different degree of spatial entanglement. The realized experimental approach allows us to characterize coincidence patterns for different states without any modifications of the setup. Measurements were carried out with path-entangled and separable states. The dependence of the coincidence pattern on the phase of the interferometer for superposition and separable states was studied. The results have implications for using of nonclassical light in multiphoton imaging, quantum lithography, and studies of phase decoherence.

  16. Two-photon spectroscopy of excitons with entangled photons.

    PubMed

    Schlawin, Frank; Mukamel, Shaul

    2013-12-28

    The utility of quantum light as a spectroscopic tool is demonstrated for frequency-dispersed pump-probe, integrated pump-probe, and two-photon fluorescence signals which show Ramsey fringes. Simulations of the frequency-dispersed transmission of a broadband pulse of entangled photons interacting with a three-level model of matter reveal how the non-classical time-bandwidth properties of entangled photons can be used to disentangle congested spectra, and reveal otherwise unresolved features. Quantum light effects are most pronounced at weak intensities when entangled photon pairs are well separated, and are gradually diminished at higher intensities when different photon pairs overlap.

  17. Chromophore design for large two-photon absorption

    NASA Astrophysics Data System (ADS)

    Dudley, Christopher

    2014-11-01

    Conjugated oligothiophene chromophores are compared and studied for designing large linear and nonlinear absorption cross-sections. Optical properties of chromophores synthesized by the Naval Research Laboratory are modeled to construct a design factor of merit to predict and understand two-photon absorption (TPA) designs. Computer modeling to optimize parameters to produce photo active chromophores is conducted. Geometry, π-center (electron relay) and the electron donor or acceptor groups attached to the π-centers are considered for importance in TPA. This work could serve equally well as guide for quick back of the envelop research or industrial design verifications as well as an outline for introducing computation methods to students.

  18. Two-photon interferences with degenerate and nondegenerate paired photons

    NASA Astrophysics Data System (ADS)

    Liu, Chang; Chen, J. F.; Zhang, Shanchao; Zhou, Shuyu; Kim, Yoon-Ho; Loy, M. M. T.; Wong, G. K. L.; Du, Shengwang

    2012-02-01

    We generate narrow-band frequency-tunable entangled photon pairs from spontaneous four-wave mixing in three-level cold atoms and study their two-photon quantum interference after a beam splitter. We find that the path-exchange symmetry plays a more important role in the Hong-Ou-Mandel interference than the temporal or frequency indistinguishability, and observe coalescence interference for both degenerate and nondegenerate photons. We also observe a quantum beat in the same experimental setup using either slow or fast detectors.

  19. Two-photon tomography using on-chip quantum walks

    NASA Astrophysics Data System (ADS)

    Titchener, James G.; Solntsev, Alexander S.; Sukhorukov, Andrey A.

    2016-09-01

    We present a conceptual approach to quantum tomography based on first expanding a quantum state across extra degrees of freedom and then exploiting the introduced sparsity to perform reconstruction. We formulate its application to photonic circuits, and show that measured spatial photon correlations at the output of a specially tailored discrete-continuous quantum-walk can enable full reconstruction of any two-photon spatially entangled and mixed state at the input. This approach does not require any tunable elements, so is well suited for integration with on-chip superconducting photon detectors.

  20. Two-photon tomography using on-chip quantum walks.

    PubMed

    Titchener, James G; Solntsev, Alexander S; Sukhorukov, Andrey A

    2016-09-01

    We present an approach to quantum tomography based on first expanding a quantum state across extra degrees of freedom and then exploiting the introduced sparsity to perform reconstruction. We formulate its application to photonic circuits and show that measured spatial photon correlations at the output of a specially tailored discrete-continuous quantum walk can enable full reconstruction of any two-photon spatially entangled and mixed state at the input. This approach does not require any tunable elements, so it is well suited for integration with on-chip superconducting photon detectors. PMID:27607977

  1. Two-photon spectroscopy of excitons with entangled photons

    SciTech Connect

    Schlawin, Frank; Mukamel, Shaul

    2013-12-28

    The utility of quantum light as a spectroscopic tool is demonstrated for frequency-dispersed pump-probe, integrated pump-probe, and two-photon fluorescence signals which show Ramsey fringes. Simulations of the frequency-dispersed transmission of a broadband pulse of entangled photons interacting with a three-level model of matter reveal how the non-classical time-bandwidth properties of entangled photons can be used to disentangle congested spectra, and reveal otherwise unresolved features. Quantum light effects are most pronounced at weak intensities when entangled photon pairs are well separated, and are gradually diminished at higher intensities when different photon pairs overlap.

  2. Imaging nanowire plasmon modes with two-photon polymerization

    SciTech Connect

    Gruber, Christian; Trügler, Andreas; Hohenester, Ulrich; Ditlbacher, Harald; Hohenau, Andreas; Krenn, Joachim R.; Hirzer, Andreas; Schmidt, Volker

    2015-02-23

    Metal nanowires sustain propagating surface plasmons that are strongly confined to the wire surface. Plasmon reflection at the wire end faces and interference lead to standing plasmon modes. We demonstrate that these modes can be imaged via two-photon (plasmon) polymerization of a thin film resist covering the wires and subsequent electron microscopy. Thereby, the plasmon wavelength and the phase shift of the nanowire mode picked up upon reflection can be directly retrieved. In general terms, polymerization imaging is a promising tool for the imaging of propagating plasmon modes from the nano- to micro-scale.

  3. Nonlocal Pancharatnam phase in two-photon interferometry

    SciTech Connect

    Mehta, Poonam; Samuel, Joseph; Sinha, Supurna

    2010-09-15

    We propose a polarized intensity interferometry experiment, which measures the nonlocal Pancharatnam phase acquired by a pair of Hanbury-Brown-Twiss photons. The setup involves two polarized thermal sources illuminating two polarized detectors. Varying the relative polarization angle of the detectors introduces a two-photon geometric phase. Local measurements at either detector do not reveal the effects of the phase, which is an optical analog of the multiparticle Aharonov-Bohm effect. The geometric phase sheds light on the three-slit experiment and suggests ways of tuning entanglement.

  4. Resonance enhanced neutron standing waves in thin films

    SciTech Connect

    Satija, S.K.; Gallagher, P.D.; Lindstrom, R.M.; Paul, R.L.; Zhang, H. |; Russell, T.P.; Lambooy, P.; Kramer, E.J.

    1995-12-31

    Simultaneous measurements of neutron reflectivity and prompt gamma ray emission, from samples with buried Gd layers, are shown to be of significant aid in determining the depth profile of the entire sample. Because of resonant enhancement of the neutron standing waves in the sample, the gamma ray signals are considerably enhanced making these experiments possible. A possible application of this technique to study grazing angle neutron diffraction is also mentioned.

  5. Two-Photon-Induced Fluorescence of Isomorphic Nucleobase Analogs

    PubMed Central

    Lane, Richard S. K.; Jones, Rosemary; Sinkeldam, Renatus W.

    2014-01-01

    Five isomorphic fluorescent uridine mimics have been subjected to two-photon (2P) excitation analysis to investigate their potential applicability as non-perturbing probes for the single-molecule detection of nucleic acids. We find that small structural differences can cause major changes in the two-photon excitation probability, with the 2P cross sections varying by over one order of magnitude. Two of the probes, both furan-modified uridine analogs, have the highest 2P cross sections (3.8 GM and 7.6 GM) reported for nucleobase analogs, using a conventional Ti:sapphire laser for excitation at 690 nm; they also have the lowest emission quantum yields. In contrast, the analogs with the highest reported quantum yields have the lowest 2P cross sections. The structure-photophysical property relationship presented here is a first step towards the rational design of emissive nucleobase analogs with controlled 2P characteristics. The results demonstrate the potential for major improvements through judicious structural modifications. PMID:24604669

  6. Temperature dependence of the two photon absorption in indium arsenide

    SciTech Connect

    Berryman, K.W.; Rella, C.W.

    1995-12-31

    Nonlinear optical processes in semiconductors have long been a source of interesting physics. Two photon absorption (TPA) is one such process, in which two photons provide the energy for the creation of an electron-hole pair. Researchers at other FEL centers have studied room temperature TPA in InSb, InAs, and HgCdTe. Working at the Stanford Picosecond FEL Center, we have extended and refined this work by measuring the temperature dependence of the TPA coefficient in InAs over the range from 80 to 350 K at four wavelengths: 4.5, 5.06, 6.01, and 6.3 microns. The measurements validate the functional dependence of recent band structure calculations with enough precision to discriminate parabolic from non-parabolic models, and to begin to observe smaller effects, such as contributions due to the split-off band. These experiments therefore serve as a strong independent test of the Kane band theory, as well as providing a starting point for detailed observations of other nonlinear absorption mechanisms.

  7. Two-photon single particle tracking in 3D

    NASA Astrophysics Data System (ADS)

    So, Peter T. C.; Ragan, Timothy; Gratton, Enrico; Carerro, Jenny; Voss, Edward

    1997-05-01

    Transport processes are important in biology and medicine. Examples include virus docking and infection, endocytosis of extracellular protein and phagocytosis of antigenic material. Trafficking driven by molecular motors inside a complex 3D environment is a shared common theme. The complex sequence of these events are difficult to resolve with conventional techniques where the action of many cells are asynchronously averaged. Single particle tracking (SPT) was developed by Ghosh and Webb to address this problem and has proven to be a powerful technique in understanding membrane- protein interaction. Since the traditional SPT method uses wide field illumination and area detectors, it is limited to the study of 2D systems. In this presentation, we report the development of a 3D single particle tracking technique using two-photon excitation. Using a real-time feedback system, we can dynamically position the sub-femtoliter two-photon excitation volume to follow the fluorescent particle under transport by maximizing the detected fluorescent intensity. Further, fluorescence spectroscopy can be performed in real time along the particle trajectory to monitor the underlying biochemical signals driving this transport process. The first application of this instrument will focus on the study of antigen endocytosis process of macrophages.

  8. Multidimensional two-photon imaging of diseased skin

    NASA Astrophysics Data System (ADS)

    Cicchi, R.; Sestini, S.; De Giorgi, V.; Massi, D.; Lotti, T.; Pavone, F. S.

    2008-02-01

    We used combined two photon intrinsic fluorescence (TPE), second harmonic generation microscopy (SHG), fluorescence lifetime imaging microscopy (FLIM), and multispectral two photon emission detection (MTPE) to investigate different kinds of human cutaneous ex-vivo skin lesions. Morphological and spectroscopic analyses allowed to characterize both healthy and pathological skin samples, including tumors, as well as to discriminate between healthy and diseased tissue, in a good agreement with common routine histology. In particular, we examined tissue samples from normal and pathological scar tissue (keloid), and skin tumors, including basal cell carcinoma (BCC) and malignant melanoma (MM). By using combined TPE-SHG microscopy we investigated morphological features of different skin regions, as BCC, tumor-stroma interface, healthy dermis, fibroblastic proliferation, and keloids. The SHG to autofluorescence aging index of dermis (SAAID) score was used to characterize each region, finding differences between BCC, healthy skin, tumor-stroma interface, keloids, and fibroblastic proliferation. Further comparative analysis of healthy skin and neoplastic samples was performed using FLIM. In particular, BCC showed a blue-shifted fluorescence emission, a higher absorption at 800 nm excitation wavelength, and a slightly longer mean fluorescence lifetime. MM showed a lifetime distribution similar to the corresponding melanocytic nevus (MN) lifetime distribution for the slow lifetime component, and different for the fast lifetime component.

  9. Double-Pomeron and two-photon processes at RHIC

    SciTech Connect

    Chung, S.U.; Weygand, D.P.; Willutzki, H.J.

    1991-11-01

    Double-Pomeron processes have been shown to be an important and novel source of hadron production at moderate energies at the ISR. These processes are expected to provide glue-rich hadrons from 1 GeV to 10 GeV or more, encompassing the states consisting of u, d, s and b quarks. The double-pomeron cross sections for central hadroproduction are calculated for p {times} p and Au {times} Au at RHIC. Two-photon production of hadrons in the central region begins to dominate or at least become comparable to the double-Pomeron processes as the Z of the beams increases from p to Au. Since photons couple to charge, these hadroproductions involve mainly quarkonia and multiquark states. Therefore, a comparative study of these processes is expected to provide new insights into the constituents of hadronic matter. The two-photon processes are calculated following the recipe given by Cahn and Jackson. The paper starts out with a thorough discussion of the relevant kinematics, phase space and Regge amplitudes.

  10. Two-Photon Holographic Stimulation of ReaChR

    PubMed Central

    Chaigneau, Emmanuelle; Ronzitti, Emiliano; Gajowa, Marta A.; Soler-Llavina, Gilberto J.; Tanese, Dimitrii; Brureau, Anthony Y. B.; Papagiakoumou, Eirini; Zeng, Hongkui; Emiliani, Valentina

    2016-01-01

    Optogenetics provides a unique approach to remotely manipulate brain activity with light. Reaching the degree of spatiotemporal control necessary to dissect the role of individual cells in neuronal networks, some of which reside deep in the brain, requires joint progress in opsin engineering and light sculpting methods. Here we investigate for the first time two-photon stimulation of the red-shifted opsin ReaChR. We use two-photon (2P) holographic illumination to control the activation of individually chosen neurons expressing ReaChR in acute brain slices. We demonstrated reliable action potential generation in ReaChR-expressing neurons and studied holographic 2P-evoked spiking performances depending on illumination power and pulse width using an amplified laser and a standard femtosecond Ti:Sapphire oscillator laser. These findings provide detailed knowledge of ReaChR's behavior under 2P illumination paving the way for achieving in depth remote control of multiple cells with high spatiotemporal resolution deep within scattering tissue. PMID:27803649

  11. Animal model for two-photon excitation in the eye

    NASA Astrophysics Data System (ADS)

    Bird, Mark; Campbell, Melanie C. W.

    2006-09-01

    We wish to deliver Two-Photon Excitation (TPE) to the in vivo retina and to image its effects in order to understand and treat eye disease. A schematic model of the rat eye with a gradient refractive index in the crystalline lens is reconstructed in ZEMAX TM. This model predicts the monochromatic aberrations as a function of pupil size and field angle and the change in the Point Spread Function (PSF) at best focus. A simple water model of the nonlinear pulse broadening effect has been used to predict the minimal temporal pulse width that will propagate to the retina. In a rat eye uncorrected for monochromatic aberrations, a pupil between 1mm and 1.8mm diameter delivers a peak intensity acceptable for two-photon effects. A somewhat larger diameter pupil (1.35-2.0mm) gives an optimum optical quality for imaging on the optical axis. Correction of the monochromatic aberrations with adaptive optics would improve both imaging and peak intensity. The effect of second order dispersion is dependent on the form of the dispersion relation used. Based on experimental results of second order dispersion, the minimum pulse width to reach the retina is approximately 30fs for the rat eye and approximately 60fs for the human eye.

  12. Nonresonant two-photon transitions in length and velocity gauges

    NASA Astrophysics Data System (ADS)

    Jentschura, U. D.

    2016-08-01

    We reexamine the invariance of two-photon transition matrix elements and corresponding two-photon Rabi frequencies under the "gauge" transformation from the length to the velocity gauge. It is shown that gauge invariance, in the most general sense, only holds at exact resonance, for both one-color as well as two-color absorption. The arguments leading to this conclusion are supported by analytic calculations which express the matrix elements in terms of hypergeometric functions, and ramified by a "master identity" which is fulfilled by off-diagonal matrix elements of the Schrödinger propagator under the transformation from the velocity to the length gauge. The study of the gauge dependence of atomic processes highlights subtle connections between the concept of asymptotic states, the gauge transformation of the wave function, and infinitesimal damping parameters for perturbations and interaction Hamiltonians that switch off the terms in the infinite past and future [of the form exp(-ɛ |t |)] . We include a pertinent discussion.

  13. Two-photon multiplane imaging of neural circuits (Conference Presentation)

    NASA Astrophysics Data System (ADS)

    Yang, Weijian; Miller, Jae-eun K.; Carrillo-Reid, Luis; Pnevmatikakis, Eftychios; Paninski, Liam; Peterka, Darcy S.; Yuste, Rafael

    2016-03-01

    Imaging the neuronal activity throughout the brain with high temporal and spatial resolution is an important step in understanding how the brain works. Two-photon laser scanning microscopy with fluorescent calcium indicators has enabled this type of experiments in vivo. Most of these microscopes acquire images serially, with a single laser beam, limiting the overall imaging speed. To overcome this limit, multiple beamlets can be used to image in parallel multiple regions. Here, we demonstrate a novel scheme of a two-photon laser-scanning microscope that can simultaneously record neuronal activity at multiple planes of the sample with a single photomultiplier tube. A spatial light modulator is used to generate the designated multiple beamlets, and a constrained non-negative matrix factorization algorithm is used to demix the signals from multiple scanned planes. We simultaneously record neuronal activity of multiple layers of a mouse cortex at 10 fps in vivo. This novel imaging scheme provides a powerful tool for mapping the brain activity.

  14. Interpreting two-photon imaging data of lymphocyte motility.

    PubMed

    Meyer-Hermann, Michael E; Maini, Philip K

    2005-06-01

    Recently, using two-photon imaging it has been found that the movement of B and T cells in lymph nodes can be described by a random walk with persistence of orientation in the range of 2 minutes. We interpret this new class of lymphocyte motility data within a theoretical model. The model considers cell movement to be composed of the movement of subunits of the cell membrane. In this way movement and deformation of the cell are correlated to each other. We find that, indeed, the lymphocyte movement in lymph nodes can best be described as a random walk with persistence of orientation. The assumption of motility induced cell elongation is consistent with the data. Within the framework of our model the two-photon data suggest that T and B cells are in a single velocity state with large stochastic width. The alternative of three different velocity states with frequent changes of their state and small stochastic width is less likely. Two velocity states can be excluded. PMID:16089770

  15. Two-Photon Photochemistry of CdSe Quantum Dots.

    PubMed

    Zeng, Youhong; Kelley, David F

    2015-10-27

    The two-photon photochemistry of CdSe quantum dots (QDs) has been systematically studied. We find that upon intense irradiation CdSe quantum dots that absorb two or more visible photons undergo photodarkening. The quantum yield for this process is on the order of 6% in chloroform and much smaller in nonpolar solvents, such as octane. An analysis of the energetics indicates that, following two-photon excitation, the biexciton undergoes an Auger process producing a hot hole. This hot hole is ejected to a surface-bound TOP ligand, forming a QD(-)/TOP(+) contact ion pair that separates in chloroform, but not in octane. The charged and deligated QD is dark, resulting in the overall photodarkening. This photodarkening reaction may or may not be reversible, depending on what other chemical components are in the irradiated solution. The quantum dot concentration dependence and PL decay kinetics indicate that charge recombination occurs rapidly, followed by ligand reattachment and reorganization on a longer (tens of minutes) time scale. The relation of this mechanism to one-photon photochemistry is also discussed.

  16. Single-organelle tracking by two-photon conversion

    NASA Astrophysics Data System (ADS)

    Watanabe, Wataru; Shimada, Tomoko; Matsunaga, Sachihiro; Kurihara, Daisuke; Fukui, Kiichi; Shin-Ichi Arimura, Shin-Ichi; Tsutsumi, Nobuhiro; Isobe, Keisuke; Itoh, Kazuyoshi

    2007-03-01

    Spatial and temporal information about intracellular objects and their dynamics within a living cell are essential for dynamic analysis of such objects in cell biology. A specific intracellular object can be discriminated by photoactivatable fluorescent proteins that exhibit pronounced light-induced spectral changes. Here, we report on selective labeling and tracking of a single organelle by using two-photon conversion of a photoconvertible fluorescent protein with near-infrared femtosecond laser pulses. We performed selective labeling of a single mitochondrion in a living tobacco BY-2 cell using two-photon photoconversion of Kaede. Using this technique, we demonstrated that, in plants, the directed movement of individual mitochondria along the cytoskeletons was mediated by actin filaments, whereas microtubules were not required for the movement of mitochondria. This single-organelle labeling technique enabled us to track the dynamics of a single organelle, revealing the mechanisms involved in organelle dynamics. The technique has potential application in direct tracking of selective cellular and intracellular structures.

  17. The CLAS Two Photon Exchange Experiment: Analysis Methods

    NASA Astrophysics Data System (ADS)

    Rimal, Dipak; Raue, Brian; Khetarpal, Puneet; CLAS Collaboration

    2011-04-01

    The two photon exchange contribution to the elastic electron proton scattering has been suggested as the most likely explanation for the discrepancy observed between Rosenbluth and the polarization transfer methods in the measurement of proton electric-to-magnetic form factor ratio of the proton (GEp /GMp). The Two Photon Exchange (TPE) experiment recently completed data taking in Jefferson Lab's Hall-B and will directly measure, with high precision, the TPE contribution to elastic scattering by comparing the ratio of cross sections for electron-proton to positron-proton elastic scattering. The data were collected using a primary electron beam of 5.6 GeV to produce a photon beam, which in turn was used to produce a mixed e+ /e- beam that was incident upon an LH2 target. The CEBAF Large Acceptance Spectrometer (CLAS) was used to detect both the scattered leptons and protons. The resulting data span Q2 up to 2.5 GeV2 and nearly the entire epsilon range. The analysis techniques will be discussed along with some preliminary results. Supported in part by the U.S. D.O.E.

  18. Conformational Change of Self-Assembled DNA Nanotubes Induced by Two-Photon Excitation.

    PubMed

    Dai, Ziwen; Tam, Dick Yan; Xu, Hailiang; Chan, Miu Shan; Liu, Ling Sum; Bolze, Frédéric; Sun, Xiao Hua; Lo, Pik Kwan

    2015-09-01

    Two-photon-regulated, shape-changing DNA nanostructures are demonstrated by integrating a DNA nanotube with a two-photon photocleavable module that enables the opening of the cavities of tube, and becomes partially single-stranded in response to two-photon excitation under 800 nm fs laser pulses.

  19. Fluorescent Pluronic nanodots for in vivo two-photon imaging

    NASA Astrophysics Data System (ADS)

    Maurin, Mathieu; Vurth, Laeticia; Vial, Jean-Claude; Baldeck, Patrice; Marder, Seth R.; Sanden, Boudewijn Van der; Stephan, Olivier

    2009-06-01

    We report the synthesis of new nanosized fluorescent probes based on bio-compatible polyethylene-polypropylene glycol (Pluronic) materials. In aqueous solution, mini-emulsification of Pluronic with a high fluorescent di-stryl benzene-modified derivative, exhibiting a two-photon absorption cross section as high as 2500 Goeppert-Mayer units at 800 nm, leads to nanoparticles exhibiting a hydrodynamic radius below 100 nm. We have demonstrated that these new probes with luminescence located in the spectral region of interest for bio-imaging (the yellow part of the visible spectrum) allow deep (500 µm) bio-imaging of the mice brain vasculature. The dose injected during our experiments is ten times lower when compared to the classical commercial rhodamine-B isothicyanate-Dextran system but gives similar results to homogeneous blood plasma staining. The mean fluorescent signal intensity stayed constant during more than 1 h.

  20. Fluorescent Pluronic nanodots for in vivo two-photon imaging.

    PubMed

    Maurin, Mathieu; Vurth, Laeticia; Vial, Jean-Claude; Baldeck, Patrice; Marder, Seth R; Van der Sanden, Boudewijn; Stephan, Olivier

    2009-06-10

    We report the synthesis of new nanosized fluorescent probes based on bio-compatible polyethylene-polypropylene glycol (Pluronic) materials. In aqueous solution, mini-emulsification of Pluronic with a high fluorescent di-stryl benzene-modified derivative, exhibiting a two-photon absorption cross section as high as 2500 Goeppert-Mayer units at 800 nm, leads to nanoparticles exhibiting a hydrodynamic radius below 100 nm. We have demonstrated that these new probes with luminescence located in the spectral region of interest for bio-imaging (the yellow part of the visible spectrum) allow deep (500 microm) bio-imaging of the mice brain vasculature. The dose injected during our experiments is ten times lower when compared to the classical commercial rhodamine-B isothicyanate-Dextran system but gives similar results to homogeneous blood plasma staining. The mean fluorescent signal intensity stayed constant during more than 1 h.

  1. RESONANCE PRODUCTION BY TWO-PHOTON INTERACTIONS AT SPEAR

    SciTech Connect

    Jenni, P.; Burke, D.L.; Telnov, V.; Alam, M.S.; Boyarski, A.M.; Breidenbach, M.; Dorenbosch, J.; Dorfan, J.M.; Feldman, G.J.; Franklin, M.E.B.; Hanson, G.; Hayes, K.G.; Himel, T.; Hitlin, D.G.; Hollebeek, R.J.; Innes, W.R.; Jaros, J.A.; Larsen, R.R.; Luth, V.; Perl, M.L.; Richter, B.; Roussarie, A.; Scharre, D.L.; Schindler, R.H.; Schwitters, R.F.; Siegrist, J.L.; Taureg, H.; Tonutti, M.; Vidal, R.A.; Weiss, J.M.; Zaccone, H.

    1981-06-01

    Two-photon interactions have been studied with the SLAC-LBL Mark II magnetic detector at SPEAR. The cross section for {eta}' production by the reaction e{sup +}e{sup -} {yields} e{sup +}e{sup -}{eta}' has been measured at beam energies from 2.0 GeV to 3.7 GeV. The radiative width {Lambda}{sub {gamma}{gamma}}({eta}') has been determined to be 5.8 {+-} 1.1 keV ({+-}20% systematic uncertainty). Upper limits on the radiative widths of the f(1270), A{sub 2}(1310) and f'(1515) tensor mesons have been determined. A search has been made for production of the E(1420) by {gamma}{gamma} collisions, but no signal is observed.

  2. Fluorescent Pluronic nanodots for in vivo two-photon imaging.

    PubMed

    Maurin, Mathieu; Vurth, Laeticia; Vial, Jean-Claude; Baldeck, Patrice; Marder, Seth R; Van der Sanden, Boudewijn; Stephan, Olivier

    2009-06-10

    We report the synthesis of new nanosized fluorescent probes based on bio-compatible polyethylene-polypropylene glycol (Pluronic) materials. In aqueous solution, mini-emulsification of Pluronic with a high fluorescent di-stryl benzene-modified derivative, exhibiting a two-photon absorption cross section as high as 2500 Goeppert-Mayer units at 800 nm, leads to nanoparticles exhibiting a hydrodynamic radius below 100 nm. We have demonstrated that these new probes with luminescence located in the spectral region of interest for bio-imaging (the yellow part of the visible spectrum) allow deep (500 microm) bio-imaging of the mice brain vasculature. The dose injected during our experiments is ten times lower when compared to the classical commercial rhodamine-B isothicyanate-Dextran system but gives similar results to homogeneous blood plasma staining. The mean fluorescent signal intensity stayed constant during more than 1 h. PMID:19448291

  3. Whole Brain Imaging with Serial Two-Photon Tomography

    PubMed Central

    Amato, Stephen P.; Pan, Feng; Schwartz, Joel; Ragan, Timothy M.

    2016-01-01

    Imaging entire mouse brains at submicron resolution has historically been a challenging undertaking and largely confined to the province of dedicated atlasing initiatives. This has limited systematic investigations into important areas of neuroscience, such as neural circuits, brain mapping and neurodegeneration. In this article, we describe in detail Serial Two-Photon (STP) tomography, a robust, reliable method for imaging entire brains with histological detail. We provide examples of how the basic methodology can be extended to other imaging modalities, such as Optical Coherence Tomography (OCT), in order to provide unique contrast mechanisms. Furthermore, we provide a survey of the research that STP tomography has enabled in the field of neuroscience, provide examples of how this technology enables quantitative whole brain studies, and discuss the current limitations of STP tomography-based approaches. PMID:27047350

  4. Rapid three dimensional two photon neural population scanning.

    PubMed

    Schuck, Renaud; Quicke, Peter; Copeland, Caroline; Garasto, Stefania; Annecchino, Luca A; Hwang, June Kyu; Schultz, Simon R

    2015-08-01

    Recording the activity of neural populations at high sampling rates is a fundamental requirement for understanding computation in neural circuits. Two photon microscopy provides one promising approach towards this. However, neural circuits are three dimensional, and functional imaging in two dimensions fails to capture the 3D nature of neural dynamics. Electrically tunable lenses (ETLs) provide a simple and cheap method to extend laser scanning microscopy into the relatively unexploited third dimension. We have therefore incorporated them into our Adaptive Spiral Scanning (SSA) algorithm, which calculates kinematically efficient scanning strategies using radially modulated spiral paths. We characterised the response of the ETL, incorporated its dynamics using MATLAB models of the SSA algorithm and tested the models on populations of Izhikevich neurons of varying size and density. From this, we show that our algorithms can theoretically at least achieve sampling rates of 36.2Hz compared to 21.6Hz previously reported for 3D scanning techniques. PMID:26737626

  5. Anomalous two-photon spectral features in warm rubidium vapor

    NASA Astrophysics Data System (ADS)

    Perrella, C.; Light, P. S.; Milburn, T. J.; Kielpinski, D.; Stace, T. M.; Luiten, A. N.

    2016-09-01

    We report observation of anomalous fluorescence spectral features in the environs of a two-photon transition in a rubidium vapor when excited with two different wavelength lasers that are both counterpropagating through the vapor. These features are characterized by an unusual trade-off between the detunings of the driving fields. Three different hypothetical processes are presented to explain the observed spectra: a simultaneous three-atom and four-photon collision, a four-photon excitation involving a light field produced via amplified spontaneous emission, and population pumping perturbing the expected steady-state spectra. Numerical modeling of each hypothetical process is presented, supporting the population pumping process as the most plausible mechanism.

  6. Two-photon exchange effect studied with neural networks

    SciTech Connect

    Graczyk, Krzysztof M.

    2011-09-15

    An approach to the extraction of the two-photon exchange (TPE) correction from elastic ep scattering data is presented. The cross-section, polarization transfer (PT), and charge asymmetry data are considered. It is assumed that the TPE correction to the PT data is negligible. The form factors and TPE correcting term are given by one multidimensional function approximated by the feedforward neural network (NN). To find a model-independent approximation, the Bayesian framework for the NNs is adapted. A large number of different parametrizations is considered. The most optimal model is indicated by the Bayesian algorithm. The obtained fit of the TPE correction behaves linearly in {epsilon} but it has a nontrivial Q{sup 2} dependence. A strong dependence of the TPE fit on the choice of parametrization is observed.

  7. High contrast two-photon imaging of fingermarks

    PubMed Central

    Stoltzfus, Caleb R.; Rebane, Aleksander

    2016-01-01

    Optically-acquired fingermarks are widely used as evidence across law enforcement agencies as well as in the courts of law. A common technique for visualizing latent fingermarks on nonporous surfaces consists of cyanoacrylate fuming of the fingerprint material, followed by impregnation with a fluorescent dye, which under ultra violet (UV) illumination makes the fingermarks visible and thus accessible for digital recording. However, there exist critical circumstances, when the image quality is compromised due to high background scattering, high auto-fluorescence of the substrate material, or other detrimental photo-physical and photo-chemical effects such as light-induced damage to the sample. Here we present a novel near-infrared (NIR), two-photon induced fluorescence imaging modality, which significantly enhances the quality of the fingermark images, especially when obtained from highly reflective and/or scattering surfaces, while at the same time reducing photo-damage to sensitive forensic samples. PMID:27053515

  8. Two-Photon Fluorescence Tracking of Colloidal Clusters.

    PubMed

    Roy, Debjit; Mondal, Dipankar; Goswami, Debabrata

    2016-07-01

    In situ dynamics of colloidal cluster formation from nanoparticles is yet to be addressed. Using two-photon fluorescence (TPF) that has been amply used for single particle tracking, we demonstrate in situ measurement of effective three-dimensional optical trap stiffness of nanoparticles and their aggregates without using any position sensitive detector. Optical trap stiffness is an essential measure of the strength of an optical trap. TPF is a zero-background detection scheme and has excellent signal-to-noise-ratio, which can be easily extended to study the formation of colloidal cluster of nanospheres in the optical trapping regime. TPF tracking can successfully distinguish colloidal cluster from its monomer. PMID:27165039

  9. Quantum theory of a two-photon micromaser

    SciTech Connect

    Davidovich, L.; Raimond, J.M.; Brune, M.; Haroche, S.

    1987-10-15

    We present the quantum theory of a microscopic maser operating on a degenerate two-photon transition between levels of the same parity. We derive both a master equation and a Fokker-Planck equation for this system, and show that quantum effects may have a substantial influence on the behavior of the maser. They modify the oscillation threshold and make external triggering of this maser unnecessary, whereas, according to semiclassical theory, such a triggering is required to start up the maser oscillation. We derive the phase-diffusion properties of the field and show that the diffusion coefficient is complex in this case, its imaginary part being associated with a frequency shift of the field inside the cavity. We show that, in steady state, the photon-number statistics is sub-Poissonian for a wide range of pumping rates.

  10. Exploring Entangled Two-Photon Absorption in Molecules

    NASA Astrophysics Data System (ADS)

    Caraher, John

    2014-05-01

    Goodson and colleagues have reported anomalously large cross-sections (of order σ =10-17 cm2) for the two-photon absorption of entangled photons in a number of molecules. This poster reports on attempts to replicate and expand upon their results for one of these, zinc tetraphenylporphyrin (Zn TPP) in chloroform solution. It will also discuss the interpretation of the Goodson group's experimental data, particularly their results regarding entanglement area and entanglement time (the spatial and temporal widths of the fourth-order coherence functions, respectively). Results of direct measurement of entanglement time (via a Hong-Ou-Mandel interferometer) for a laser and optical system essentially identical to the one used in Goodson's work will be presented and compared with their reported values. Supported by the DePauw University Faculty Development Committee.

  11. Four-dimensional multi-site two-photon excitation

    NASA Astrophysics Data System (ADS)

    Daria, Vincent R.; Stricker, Christian; Bowman, Richard; Bachor, Hans-A.; Redman, Stephen

    2010-02-01

    We use the holographic method to project an arbitrary array of diffraction-limited focal spots suitable for multi-site twophoton excitation. The spot array can be projected arbitrarily within a three-dimensional (3D) volume, while the fourth dimension in time is attributed to high temporal resolution via high-speed non-iterative calculation of the hologram using a video graphics accelerator board. We show that the spots have sufficient energy and spatiotemporal photon density for localized two-photon excitation at individual spots in the array. The significance of this work points to 3D microscopy, non-linear micro-fabrication, volume holographic optical storage and biomedical instrumentation. In neuroscience, timecritical release of neurotransmitters at multiple sites within complex dendritic trees of neurons can lead to insights on the mechanisms of information processing in the brain.

  12. Two-photon quantum walk in a multimode fiber

    PubMed Central

    Defienne, Hugo; Barbieri, Marco; Walmsley, Ian A.; Smith, Brian J.; Gigan, Sylvain

    2016-01-01

    Multiphoton propagation in connected structures—a quantum walk—offers the potential of simulating complex physical systems and provides a route to universal quantum computation. Increasing the complexity of quantum photonic networks where the walk occurs is essential for many applications. We implement a quantum walk of indistinguishable photon pairs in a multimode fiber supporting 380 modes. Using wavefront shaping, we control the propagation of the two-photon state through the fiber in which all modes are coupled. Excitation of arbitrary output modes of the system is realized by controlling classical and quantum interferences. This report demonstrates a highly multimode platform for multiphoton interference experiments and provides a powerful method to program a general high-dimensional multiport optical circuit. This work paves the way for the next generation of photonic devices for quantum simulation, computing, and communication. PMID:27152325

  13. Two-photon quantum walk in a multimode fiber.

    PubMed

    Defienne, Hugo; Barbieri, Marco; Walmsley, Ian A; Smith, Brian J; Gigan, Sylvain

    2016-01-01

    Multiphoton propagation in connected structures-a quantum walk-offers the potential of simulating complex physical systems and provides a route to universal quantum computation. Increasing the complexity of quantum photonic networks where the walk occurs is essential for many applications. We implement a quantum walk of indistinguishable photon pairs in a multimode fiber supporting 380 modes. Using wavefront shaping, we control the propagation of the two-photon state through the fiber in which all modes are coupled. Excitation of arbitrary output modes of the system is realized by controlling classical and quantum interferences. This report demonstrates a highly multimode platform for multiphoton interference experiments and provides a powerful method to program a general high-dimensional multiport optical circuit. This work paves the way for the next generation of photonic devices for quantum simulation, computing, and communication.

  14. Two-photon quantum walk in a multimode fiber.

    PubMed

    Defienne, Hugo; Barbieri, Marco; Walmsley, Ian A; Smith, Brian J; Gigan, Sylvain

    2016-01-01

    Multiphoton propagation in connected structures-a quantum walk-offers the potential of simulating complex physical systems and provides a route to universal quantum computation. Increasing the complexity of quantum photonic networks where the walk occurs is essential for many applications. We implement a quantum walk of indistinguishable photon pairs in a multimode fiber supporting 380 modes. Using wavefront shaping, we control the propagation of the two-photon state through the fiber in which all modes are coupled. Excitation of arbitrary output modes of the system is realized by controlling classical and quantum interferences. This report demonstrates a highly multimode platform for multiphoton interference experiments and provides a powerful method to program a general high-dimensional multiport optical circuit. This work paves the way for the next generation of photonic devices for quantum simulation, computing, and communication. PMID:27152325

  15. Two-Photon Voltmeter for Measuring a Molecular Electric Field**

    PubMed Central

    Rebane, Aleksander; Wicks, Geoffrey; Drobizhev, Mikhail; Cooper, Thomas; Trummal, Aleksander; Uudsemaa, Merle

    2015-01-01

    We present a new approach for determining the strength of the dipolar solute-induced reaction field, along with the ground- and excited-state electrostatic dipole moments and polarizability of a solvated chromophore, using exclusively one-photon and two-photon absorption measurements. We verify the approach on two benchmark chromophores N,N-dimethyl-6-propionyl-2-naphthylamine (prodan) and coumarin 153 (C153) in a series of toluene/dimethyl sulfoxide (DMSO) mixtures and find that the experimental values show good quantitative agreement with literature and our quantum-chemical calculations. Our results indicate that the reaction field varies in a surprisingly broad range, 0–107 V cm−1, and that at close proximity, on the order of the chromophore radius, the effective dielectric constant of the solute–solvent system displays a unique functional dependence on the bulk dielectric constant, offering new insight into the close-range molecular interaction. PMID:25958849

  16. High contrast two-photon imaging of fingermarks

    NASA Astrophysics Data System (ADS)

    Stoltzfus, Caleb R.; Rebane, Aleksander

    2016-04-01

    Optically-acquired fingermarks are widely used as evidence across law enforcement agencies as well as in the courts of law. A common technique for visualizing latent fingermarks on nonporous surfaces consists of cyanoacrylate fuming of the fingerprint material, followed by impregnation with a fluorescent dye, which under ultra violet (UV) illumination makes the fingermarks visible and thus accessible for digital recording. However, there exist critical circumstances, when the image quality is compromised due to high background scattering, high auto-fluorescence of the substrate material, or other detrimental photo-physical and photo-chemical effects such as light-induced damage to the sample. Here we present a novel near-infrared (NIR), two-photon induced fluorescence imaging modality, which significantly enhances the quality of the fingermark images, especially when obtained from highly reflective and/or scattering surfaces, while at the same time reducing photo-damage to sensitive forensic samples.

  17. Resonantly enhanced Bragg-scattering spectroscopy of an atomic transition

    NASA Astrophysics Data System (ADS)

    Yang, Xudong; Qiao, Cuifang; Li, Chuanliang; Chen, Fenghua

    2016-07-01

    A novel resonantly enhanced Bragg-scattering (REBS) spectroscopy from a population difference grating (PDG) is reported. The PDG is formed by a standing-wave (SW) pump field, which periodically modulates the space population distributions of two levels in the 87Rb D1 line. Then, a probe beam, having identical frequency and orthogonal polarization with the SW pump field, is Bragg-scattered by the PDG. The research achievement shows that the Bragg-scattered light is strongest at an atomic transition, and forms an REBS spectrum with a high signal-to-noise ratio and sub-natural linewidth. The observed REBS can be applied in precise frequency measurements.

  18. Photosensitizer-doped conjugated polymer nanoparticles for simultaneous two-photon imaging and two-photon photodynamic therapy in living cells.

    PubMed

    Shen, Xiaoqin; Li, Lin; Wu, Hao; Yao, Shao Q; Xu, Qing-Hua

    2011-12-01

    Photosensitizer doped conjugated polymer nanoparticles have been prepared by incorporating polyoxyethylene nonylphenylether (CO-520) into the nanoparticles using a re-precipitation method. The conjugated polymer, poly[9,9-dibromohexylfluorene-2,7-ylenethylene-alt-1,4-(2,5-dimethoxy)phenylene] (PFEMO), was used as the host matrix to disperse tetraphenylporphyrin (TPP) and an energy donor to enhance the two-photon excitation properties of TPP. These CO-520 incorporated, TPP-doped PFEMO nanoparticles are stable and have low cytotoxicity in the dark. The TPP emission of the nanoparticles was found to be enhanced by about 20 times by PFEMO under two-photon excitation. The nanoparticles showed significantly enhanced two-photon excitation singlet oxygen generation efficiency and two-photon photodynamic therapy activity in cancer cells. These composite nanoparticles display features required for ideal photosensitizers, such as low cytotoxicity in the dark and efficient two-photon photodynamic activity under laser radiation. In addition, these novel nano-photosensitizers allow simultaneous in vivo monitoring by two-photon fluorescence imaging during two-photon photodynamic treatment. These photosensitizer-doped conjugated polymer nanoparticles can act as novel photosensitizing agents for two-photon photodynamic therapy and related applications.

  19. Frequency upconversion and two-photon absorption of salicylaldehyde azine 1

    NASA Astrophysics Data System (ADS)

    Souza, A. B.; Alencar, M. A. R. C.; Cardoso, S. H.; Valle, M. S.; Diniz, R.; Hickmann, J. M.

    2013-10-01

    Two-photon absorption and two-photon excitation fluorescence of salicylaldehyde azine 1 crystals were investigated. It was observed an intense visible fluorescence when this material was excited with a laser tuned at the near infrared region. Varying the laser intensity we characterized this phenomenon as a simultaneous two-photon laser absorption process. Using open aperture Z-scan measurements we characterized this two-photon absorption phenomenon and measured the value of the two-photon absorption cross-section of this molecule to be equal to 87 GM. Our results indicate that this is a promising organic material aiming nonlinear photonics applications.

  20. Classes of two-photon states defined by linear interactions and destructive two-photon quantum interference in a single mode

    NASA Astrophysics Data System (ADS)

    Lund, A. P.

    2015-11-01

    We describe a two-photon quantum interference effect which differs from the Hong-Ou-Mandel effect in that the destructive quantum inference occurs on a component of the state where two photons are in a single output mode while maintaining the two-photon events in the alternative mode. This effect is manifestly nonclassical but requires more sophisticated technology to observe than the Hong-Ou-Mandel effect. The theory outlined in this paper can also be used to classify two-photon states into classes which are related by the ability to transform the states within the class by using only linear optical interactions. This theory shows that there is an infinite number of these classes of two photon states when there are two or more modes which can support the photons.

  1. A Dipolar Anthracene Dye: Synthesis, Optical Properties and Two-photon Tissue Imaging.

    PubMed

    Moon, Hyunsoo; Jun, Yong Woong; Kim, Dokyoung; Ryu, Hye Gun; Wang, Taejun; Kim, Ki Hean; Huh, Youngbuhm; Jung, Junyang; Ahn, Kyo Han

    2016-09-20

    Two-photon microscopy is a powerful tool for studying biological systems. In search of novel two-photon absorbing dyes for bioimaging, we synthesized a new anthracene-based dipolar dye (anthradan) and evaluated its two-photon absorbing and imaging properties. The new anthradan, 9,10-bis(o-dimethoxy-phenyl)-anthradan, absorbs and emits at longer wavelengths than acedan, a well-known two-photon absorbing dye. It is also stable under two-photon excitation conditions and biocompatible, and thus used for two-photon imaging of mouse organ tissues to show bright, near-red fluorescence along with negligible autofluorescence. Such an anthradan thus holds promise as a new class of two-photon absorbing dyes for the development of fluorescent probes and tags for biological systems. PMID:27535006

  2. A Dipolar Anthracene Dye: Synthesis, Optical Properties and Two-photon Tissue Imaging.

    PubMed

    Moon, Hyunsoo; Jun, Yong Woong; Kim, Dokyoung; Ryu, Hye Gun; Wang, Taejun; Kim, Ki Hean; Huh, Youngbuhm; Jung, Junyang; Ahn, Kyo Han

    2016-09-20

    Two-photon microscopy is a powerful tool for studying biological systems. In search of novel two-photon absorbing dyes for bioimaging, we synthesized a new anthracene-based dipolar dye (anthradan) and evaluated its two-photon absorbing and imaging properties. The new anthradan, 9,10-bis(o-dimethoxy-phenyl)-anthradan, absorbs and emits at longer wavelengths than acedan, a well-known two-photon absorbing dye. It is also stable under two-photon excitation conditions and biocompatible, and thus used for two-photon imaging of mouse organ tissues to show bright, near-red fluorescence along with negligible autofluorescence. Such an anthradan thus holds promise as a new class of two-photon absorbing dyes for the development of fluorescent probes and tags for biological systems.

  3. Two-Photon Ghost Image and Interference-Diffraction

    NASA Technical Reports Server (NTRS)

    Shih, Y. H.; Sergienko, A. V.; Pittman, T. B.; Strekalov, D. V.; Klyshko, D. N.

    1996-01-01

    One of the most surprising consequences of quantum mechanics is entanglement of two or more distance particles. The two-particle entangled state was mathematically formulated by Schrodinger. Based on this unusual quantum behavior, EPR defined their 'physical reality' and then asked the question: 'Can Quantum-Mechanical Description of Physical Reality Be Considered Complete?' One may not appreciate EPR's criterion of physical reality and insist that 'no elementary quantum phenomenon is a phenomenon until it is a recorded phenomenon'. Optical spontaneous parametric down conversion (SPDC) is the most effective mechanism to generate an EPR type entangled two-photon state. In SPDC, an optical beam, called the pump, is incident on a birefringent crystal. The pump is intense enough so that nonlinear effects lead to the conversion of pump photons into pairs of photons, historically called signal and idler. Technically, the SPDC is said to be type-1 or type-2, depending on whether the signal and idler beams have parallel or orthogonal polarization. The SPDC conversion efficiency is typically on the order of 10(exp -9) to 10(exp -11), depending on the SPDC nonlinear material. The signal and idler intensities are extremely low, only single photon detection devices can register them. The quantum entanglement nature of SPDC has been demonstrated in EPR-Bohm experiments and Bell's inequality measurements. The following two experiments were recently performed in our laboratory, which are more closely related to the original 1935 EPR gedankenezperiment. The first experiment is a two-photon optical imaging type experiment, which has been named 'ghost image' by the physics community. The signal and idler beams of SPDC are sent in different directions, so that the detection of the signal and idler photons can be performed by two distant photon counting detectors. An aperture object (mask) is placed in front of the signal photon detector and illuminated by the signal beam through a

  4. Review of two-photon exchange in electron scattering

    SciTech Connect

    J. Arrington, P. G. Blunden, W. Melnitchouk

    2011-10-01

    We review the role of two-photon exchange (TPE) in electron-hadron scattering, focusing in particular on hadronic frameworks suitable for describing the low and moderate Q^2 region relevant to most experimental studies. We discuss the effects of TPE on the extraction of nucleon form factors and their role in the resolution of the proton electric to magnetic form factor ratio puzzle. The implications of TPE on various other observables, including neutron form factors, electroproduction of resonances and pions, and nuclear form factors, are summarized. Measurements seeking to directly identify TPE effects, such as through the angular dependence of polarization measurements, nonlinear epsilon contributions to the cross sections, and via e+p to e-p cross section ratios, are also outlined. In the weak sector, we describe the role of TPE and gamma-Z interference in parity-violating electron scattering, and assess their impact on the extraction of the strange form factors of the nucleon and the weak charge of the proton.

  5. Higgs decay into two photons in a warped extra dimension

    NASA Astrophysics Data System (ADS)

    Hahn, Juliane; Hörner, Clara; Malm, Raoul; Neubert, Matthias; Novotny, Kristiane; Schmell, Christoph

    2014-05-01

    A detailed five-dimensional calculation of the Higgs-boson decay into two photons is performed in both the minimal and the custodially protected Randall-Sundrum (RS) model, where the Standard Model (SM) fields propagate in the bulk and the scalar sector lives on or near the IR brane. It is explicitly shown that the gauge invariance of the sum of diagrams involving bosonic fields in the SM also applies to the case of these RS scenarios. An exact expression for the amplitude in terms of the five-dimensional (5D) gauge-boson and fermion propagators is presented, which includes the full dependence on the Higgs-boson mass. Closed expressions for the 5D -boson propagators in the minimal and the custodial RS model are derived, which are valid to all orders in . In contrast to the fermion case, the result for the bosonic contributions to the amplitude is insensitive to the details of the localization of the Higgs profile on or near the IR brane. The various RS predictions for the rate of the process are compared with the latest LHC data, and exclusion regions for the RS model parameters are derived.

  6. Two-Photon Absorption in Conjugated Energetic Molecules.

    PubMed

    Bjorgaard, Josiah A; Sifain, Andrew E; Nelson, Tammie; Myers, Thomas W; Veauthier, Jacqueline M; Chavez, David E; Scharff, R Jason; Tretiak, Sergei

    2016-07-01

    Time-dependent density functional theory (TD-DFT) was used to investigate the relationship between molecular structure and the one- and two-photon absorption (OPA and TPA, respectively) properties of novel and recently synthesized conjugated energetic molecules (CEMs). The molecular structures of CEMs can be strategically altered to influence the heat of formation and oxygen balance, two factors that can contribute to the sensitivity and strength of an explosive material. OPA and TPA are sensitive to changes in molecular structure as well, influencing the optical range of excitation. We found calculated vertical excitation energies to be in good agreement with experiment for most molecules. Peak TPA intensities were found to be significant and on the order of 10(2) GM. Natural transition orbitals for essential electronic states defining TPA peaks of relatively large intensity were used to examine the character of relevant transitions. Modification of molecular substituents, such as additional oxygen or other functional groups, produces significant changes in electronic structure, OPA, and TPA and improves oxygen balance. The results show that certain molecules are apt to undergo nonlinear absorption, opening the possibility for controlled, direct optical initiation of CEMs through photochemical pathways. PMID:27257984

  7. Two-Photon-Absorption Scheme for Optical Beam Tracking

    NASA Technical Reports Server (NTRS)

    Ortiz, Gerardo G.; Farr, William H.

    2011-01-01

    A new optical beam tracking approach for free-space optical communication links using two-photon absorption (TPA) in a high-bandgap detector material was demonstrated. This tracking scheme is part of the canonical architecture described in the preceding article. TPA is used to track a long-wavelength transmit laser while direct absorption on the same sensor simultaneously tracks a shorter-wavelength beacon. The TPA responsivity was measured for silicon using a PIN photodiode at a laser beacon wavelength of 1,550 nm. As expected, the responsivity shows a linear dependence with incident power level. The responsivity slope is 4.5 x 10(exp -7) A/W2. Also, optical beam spots from the 1,550-nm laser beacon were characterized on commercial charge coupled device (CCD) and complementary metal-oxide semiconductor (CMOS) imagers with as little as 13.7 microWatts of optical power (see figure). This new tracker technology offers an innovative solution to reduce system complexity, improve transmit/receive isolation, improve optical efficiency, improve signal-to-noise ratio (SNR), and reduce cost for free-space optical communications transceivers.

  8. Synergistic Two-Photon Absorption Enhancement in Photosynthetic Light Harvesting

    NASA Astrophysics Data System (ADS)

    Chen, Kuo-Mei; Chen, Yu-Wei; Gao, Ting-Fong

    2012-06-01

    The grand scale fixation of solar energies into chemical substances by photosynthetic reactions of light-harvesting organisms provides Earth's other life forms a thriving environment. Scientific explorations in the past decades have unraveled the fundamental photophysical and photochemical processes in photosynthesis. Higher plants, green algae, and light-harvesting bacteria utilize organized pigment-protein complexes to harvest solar power efficiently and the resultant electronic excitations are funneled into a reaction center, where the first charge separation process takes place. Here we show experimental evidences that green algae (Chlorella vulgaris) in vivo display a synergistic two-photon absorption enhancement in their photosynthetic light harvesting. Their absorption coefficients at various wavelengths display dramatic dependence on the photon flux. This newly found phenomenon is attributed to a coherence-electronic-energy-transfer-mediated (CEETRAM) photon absorption process of light-harvesting pigment-protein complexes of green algae. Under the ambient light level, algae and higher plants can utilize this quantum mechanical mechanism to create two entangled electronic excitations adjacently in their light-harvesting networks. Concerted multiple electron transfer reactions in the reaction centers and oxygen evolving complexes can be implemented efficiently by the coherent motion of two entangled excitons from antennae to the charge separation reaction sites. To fabricate nanostructured, synthetic light-harvesting apparatus, the paramount role of the CEETRAM photon absorption mechanism should be seriously considered in the strategic guidelines.

  9. Two-photon autofluorescence spectroscopy of oral mucosa tissue

    NASA Astrophysics Data System (ADS)

    Edward, Kert; Shilagard, Tuya; Qiu, Suimin; Vargas, Gracie

    2011-03-01

    The survival rate for individuals diagnosed with oral cancer is correlated with the stage of detection. Thus the development of novel techniques for the earliest possible detection of malignancies is of critical importance. Single photon (1P) autofluorescence spectroscopy has proven to be a powerful diagnostic tool in this regard, but 2P (two photon) spectroscopy remains essentially unexplored. In this investigation, a spectroscopic system was incorporated into a custom-built 2P laser scanning microscope. Oral cancer was induced in the buccal pouch of Syrian Golden hamsters by tri-weekly topical application of 9,10-dimethyl-1,2-benzanthracene (DMBA).Three separated sites where investigated in each hamster at four excitation wavelengths from 780 nm to 890 nm. A Total of 8 hamsters were investigated (4 normal and 4 DMBA treated). All investigated sites were imaged via 2p imaging, marked for biopsy, processed for histology and H&E staining, and graded by a pathologist. The in vivo emission spectrum for normal, mild/high grade dysplasia and squamous cell carcinoma is presented. It is shown that the hamsters with various stages of dysplasia are characterized by spectral differences as a function of depth and excitation wavelength, compared to normal hamsters.

  10. 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.

  11. Two photon absorption in high power broad area laser diodes

    NASA Astrophysics Data System (ADS)

    Dogan, Mehmet; Michael, Christopher P.; Zheng, Yan; Zhu, Lin; Jacob, Jonah H.

    2014-03-01

    Recent advances in thermal management and improvements in fabrication and facet passivation enabled extracting unprecedented optical powers from laser diodes (LDs). However, even in the absence of thermal roll-over or catastrophic optical damage (COD), the maximum achievable power is limited by optical non-linear effects. Due to its non-linear nature, two-photon absorption (TPA) becomes one of the dominant factors that limit efficient extraction of laser power from LDs. In this paper, theoretical and experimental analysis of TPA in high-power broad area laser diodes (BALD) is presented. A phenomenological optical extraction model that incorporates TPA explains the reduction in optical extraction efficiency at high intensities in BALD bars with 100μm-wide emitters. The model includes two contributions associated with TPA: the straightforward absorption of laser photons and the subsequent single photon absorption by the holes and electrons generated by the TPA process. TPA is a fundamental limitation since it is inherent to the LD semiconductor material. Therefore scaling the LDs to high power requires designs that reduce the optical intensity by increasing the mode size.

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

    PubMed Central

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

    2016-01-01

    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. PMID:27029524

  13. Two-photon polymerization for fabrication of biomedical devices

    NASA Astrophysics Data System (ADS)

    Ovsianikov, Aleksandr; Doraiswamy, Anand; Narayan, R.; Chichkov, B. N.

    2007-01-01

    Two-photon polymerization (2PP) is a novel technology which allows the fabrication of complex three-dimensional (3D) microstructures and nanostructures. The number of applications of this technology is rapidly increasing; it includes the fabrication of 3D photonic crystals [1-4], medical devices, and tissue scaffolds [5-6]. In this contribution, we discuss current applications of 2PP for microstructuring of biomedical devices used in drug delivery. While in general this sector is still dominated by oral administration of drugs, precise dosing, safety, and convenience are being addressed by transdermal drug delivery systems. Currently, main limitations arise from low permeability of the skin. As a result, only few types of pharmacological substances can be delivered in this manner [7]. Application of microneedle arrays, whose function is to help overcome the barrier presented by the epidermis layer of the skin, provides a very promising solution. Using 2PP we have fabricated arrays of hollow microneedles with different geometries. The effect of microneedle geometry on skin penetration is examined. Our results indicate that microneedles created using 2PP technique are suitable for in vivo use, and for integration with the next generation of MEMS- and NEMS-based drug delivery devices.

  14. Photodynamic therapy by nonresonant two-photon excitation

    NASA Astrophysics Data System (ADS)

    Koenig, Karsten; Riemann, Iris; Fischer, Peter

    1999-07-01

    Intracellular photodynamic reactions by nonlinear excitation of porphyrin photosensitizers have been induced using near infrared ultrashort laser pulses at 200 fs pulse width, 80 MHz pulse repetition rate and 2 mW mean laser power. In particular, a highly focused 780 nm pulsed laser scanning beam was employed at a frame rate of 1/16 s-1 (60 microsecond(s) pixel dwell time) to expose Photofrin-labeled and aminolevulinic acid (ALA)-labeled Chinese hamster ovary cells. Intracellular accumulation and photobleaching of the fluorescent photosensitizers protoporphyrin IX and Photofrin have been studied by non-resonant two-photon fluorescence excitation. Subsequent scanning of the sensitizer-labeled cells resulted in reduced cloning efficiency of 50% and 0% after about 13 scans (approximately equals 10 mJ) and 50 scans, respectively, in the case of Photofrin accumulation (5 (mu) g/ml) and after about 24 scans and 100 scans in the case of ALA administration (1.5 mg/ml). Live/dead assays revealed the loss of vitality of most of cells after 50 scans for Photofrin-labeled cells and 100 scans for ALA-labeled cells. Sensitizer-free control cells could be scanned more than 250 times (1.1 h) without impact on the reproduction behavior, morphology, and vitality.

  15. Characterization of two-photon polymerization process using Raman microspectroscopy

    NASA Astrophysics Data System (ADS)

    Jiang, L. J.; Zhou, Y. S.; Xiong, W.; Gao, Y.; Baldacchini, T.; Silvain, J.-F.; Jiang, L.; Lu, Y. F.

    2014-03-01

    Two-photon polymerization (TPP) is a promising micro/nanofabrication technique, which is capable of fabricating 3D micro/nanostructures beyond the diffraction limit of light. However, the study of TPP process with a focus on the dependence of degree of conversion on TPP parameters using a non-destructive and efficient method is still lacking. We studied the quantitative relationships between the TPP parameters and the cross-linking of an acrylic-based IP-L 780 photoresist via systematic Raman characterization. The differences in the Raman spectra between the non-polymerized and the polymerized IP-L 780 photoresists were observed by probing the excitation of carbon-carbon double bond (C=C) vibrations. We obtained the relationship between the degree of conversion in TPP and the Raman spectra of the IP-L 780 resin, in which the intensity of the characteristic Raman peak of IP-L 780 at 1635 cm-1 decreases with the increase of the TPP laser dose. A mathematic model of the degree of conversion with respective to the TPP parameters, including laser average power and writing speed, has been established. The method provides a simple and effective way to characterize and optimize the TPP micro/nanofabrication processes. The established model for the degree of conversion as the function of TPP parameters will contribute to the advanced 3D TPP micro/nanofabrication by providing a guidance to optimize the laser doses, voxel sizes, and the mechanical strength of the polymers.

  16. Two-photon holographic optogenetics of neural circuits (Conference Presentation)

    NASA Astrophysics Data System (ADS)

    Yang, Weijian; Carrillo-Reid, Luis; Peterka, Darcy S.; Yuste, Rafael

    2016-03-01

    Optical manipulation of in vivo neural circuits with cellular resolution could be important for understanding cortical function. Despite recent progress, simultaneous optogenetic activation with cellular precision has either been limited to 2D planes, or a very small numbers of neurons over a limited volume. Here we demonstrate a novel paradigm for simultaneous 3D activation using a low repetition rate pulse-amplified fiber laser system and a spatial light modulator (SLM) to project 3D holographic excitation patterns on the cortex of mice in vivo for targeted volumetric 3D photoactivation. This method is compatible with two-photon imaging, and enables the simultaneous activation of multiple cells in 3D, using red-shifted opsins, such as C1V1 or ReaChR, while simultaneously imaging GFP-based sensors such as GCaMP6. This all-optical imaging and 3D manipulation approach achieves simultaneous reading and writing of cortical activity, and should be a powerful tool for the study of neuronal circuits.

  17. Method for universal detection of two-photon polarization entanglement

    NASA Astrophysics Data System (ADS)

    Bartkiewicz, Karol; Horodecki, Paweł; Lemr, Karel; Miranowicz, Adam; Życzkowski, Karol

    2015-03-01

    Detecting and quantifying quantum entanglement of a given unknown state poses problems that are fundamentally important for quantum information processing. Surprisingly, no direct (i.e., without quantum tomography) universal experimental implementation of a necessary and sufficient test of entanglement has been designed even for a general two-qubit state. Here we propose an experimental method for detecting a collective universal witness, which is a necessary and sufficient test of two-photon polarization entanglement. It allows us to detect entanglement for any two-qubit mixed state and to establish tight upper and lower bounds on its amount. A different element of this method is the sequential character of its main components, which allows us to obtain relatively complicated information about quantum correlations with the help of simple linear-optical elements. As such, this proposal realizes a universal two-qubit entanglement test within the present state of the art of quantum optics. We show the optimality of our setup with respect to the minimal number of measured quantities.

  18. R-matrix study of ionization in barium via two-photon interfering routes

    NASA Astrophysics Data System (ADS)

    Aymar, M.; Luc-Koenig, E.; Lecomte, J. M.; Millet, M.; Lyras, A.

    2000-02-01

    A quantitative analysis of part of the experimental data reported by Wang, Chen and Elliott [1,3] who studied in barium coherent control through two-color resonant interfering paths is reported. Dynamics of the two-color photoionization process, described as an adiabatic process in the rotating wave approximation, is governed by the coherent excitation of the 6s6p and 6s7p 1P1 intermediate states. Interference effects are found to play a minor role. The required atomic parameters are obtained from a theoretical approach based on a combination of jj-coupled eigenchannel R-matrix and Multichannel Quantum Defect Theory.

  19. A package for the ab-initio calculation of one- and two-photon cross sections of two-electron atoms, using a CI B-splines method

    NASA Astrophysics Data System (ADS)

    Nikolopoulos, L. A. A.

    2003-02-01

    A package is presented for the fully ab-initio calculation of one- and two-photon ionization cross sections for two-electron atomic systems (H -, He, Mg, Ca, …) under strong laser fields, within lowest-order perturbation theory (LOPT) and in the dipole approximation. The atomic structure is obtained through configuration interaction (CI) of antisymmetrized two-electron states expanded in a B-spline finite basis. The formulation of the theory and the relevant codes presented here represent the accumulation of work over the last ten years [1-11,13-15]. Extensions to more than two-photon ionization is straightforward. Calculation is possible for both the length and velocity form of the laser-atom interaction operator. The package is mainly, written in standard FORTRAN language and uses the publicly available libraries SLATEC, LAPACK and BLAS.

  20. Two photon microscopy for studies of xenobiotics in human skin

    NASA Astrophysics Data System (ADS)

    Simonsson, Carl; Smedh, Maria; Jonson, Charlotte; Karlberg, Ann-Therese; Ericson, Marica B.

    2007-07-01

    For successful uptake and distribution of drugs from transdermal formulations, it is important to understand the skin barrier function. Innovative advances in modern microscopy have provided valuable tools to study the interaction between the skin and xenobiotics. Two-photon microscopy (TPM) allows non-invasive visualization of fluorescent compounds in the skin. The advantages of TPM over conventional confocal microscopy are better light penetration into highly scattering and absorbing tissue such as human skin, improved detection efficiency, limited out of focus photobleaching and reduced phototoxic effects. We present TPM as an alternative non-invasive in vitro method to study chemical penetration enhancement of fluorescent model drugs. The permeability of sulforhodamine B (SRB) through human epidermis was measured with vertical diffusion cells. The absorption was visualized using TPM after 24 h passive diffusion. We have evaluated variations in physicochemical parameters controlling dermal drug uptake induced by the penetration enhancer oleic acid according to methods previously described by Yu et al. Optical sectioning by TPM was compared with cryosectioning. Oleic acid significantly increased penetration of sulforhodamine. TPM images demonstrate a four-fold increase in the partition coefficient. In addition, a six-fold increase in the concentration gradient was found over stratum corneum. Better light penetration and detection efficiency increase maximum imaging depth in TPM compared to conventional confocal microscopy, however loss of signal due to scattering and absorption is still significant and will affect distribution profiles generated by optical sectioning. A true concentration profile cannot be established without better knowledge about signal losses in the skin.

  1. 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.

  2. Reaction-based two-photon probes for mercury ions: fluorescence imaging with dual optical windows.

    PubMed

    Rao, Alla Sreenivasa; Kim, Dokyoung; Wang, Taejun; Kim, Ki Hean; Hwang, Sekyu; Ahn, Kyo Han

    2012-05-18

    For fluorescent imaging of mercury ions in living species, two-photon probes with dual optical windows are in high demand but remain unexplored. Several dithioacetals were evaluated, and a probe was found, which, upon reaction with mercury species, yielded a two-photon dye; this conversion accompanies ratiometric emission changes with a 97-nm shift, enabling fluorescent imaging of both the probe and mercury ions in cells by one- and two-photon microscopy for the first time.

  3. Transitional behavior between self-Kerr and cross-Kerr effects by two photons

    SciTech Connect

    Koshino, Kazuki

    2007-06-15

    The transitional behavior of the two-photon Kerr effect between the self-Kerr and cross-Kerr cases is investigated. To this end, we have developed a semiclassical method for evaluating the two-photon Kerr effect that is applicable to any two-photon input state. It is revealed that the maximum Kerr effect is obtained when the second photon is input with a delay time that corresponds to the absorption time of the first photon by the optical material.

  4. Two-photon vibrational spectroscopy for biosciences based on surface-enhanced hyper-Raman scattering

    PubMed Central

    Kneipp, Janina; Kneipp, Harald; Kneipp, Katrin

    2006-01-01

    Two-photon excitation is gaining rapidly in interest and significance in spectroscopy and microscopy. Here we introduce a new approach that suggests versatile optical labels suitable for both one- and two-photon excitation and also two-photon-excited ultrasensitive, nondestructive chemical probing. The underlying spectroscopic effect is the incoherent inelastic scattering of two photons on the vibrational quantum states called hyper-Raman scattering (HRS). The rather weak effect can be strengthened greatly if HRS takes place in the local optical fields of gold and silver nanostructures. This so-called surface-enhanced HRS (SEHRS) is the two-photon analogue to surface-enhanced Raman scattering (SERS). SEHRS provides structurally sensitive vibrational information complementary to those obtained by SERS. SEHRS combines the advantages of two-photon spectroscopy with the structural information of vibrational spectroscopy and the high-sensitivity and nanometer-scale local confinement of plasmonics-based spectroscopy. We infer effective two-photon cross-sections for SEHRS on the order of 10−46 to 10−45 cm4·s, similar to or higher than the best “action” cross-sections (product of the two-photon absorption cross-section and fluorescence quantum yield) for two-photon fluorescence, and we demonstrate HRS on biological structures such as single cells after incubation with gold nanoparticles. PMID:17088534

  5. Synthesis and blue-violet two-photon excited fluorescence of a new organoboron compound

    NASA Astrophysics Data System (ADS)

    Cao, Duxia; Liu, Zhiqiang; Li, Guozhong; Liu, Guoqun; Zhang, Guohui

    2008-02-01

    A new A-π-D-π-A type organoboron compound, 3,6-bis(dimesitylboryl)- N-butyl-carbazole (abbreviated as BBC), with trivalent boron as electron acceptor and carbazole as electron donor and π-conjugated core, has been synthesized and its single and two-photon related photophysical properties experimentally investigated. Pumped by 720 nm laser pulses in femtosecond regime, it showed strong two-photon excited blue-violet fluorescence at 393 nm in toluene and 403 nm in THF. The measured two-photon absorption cross-section by two-photon fluorescence method in toluene and THF is 34 GM and 38 GM, respectively.

  6. A ratiometric two-photon fluorescent probe for fluoride ion imaging in living cells and zebrafish.

    PubMed

    Hu, Wei; Zeng, Lingyu; Wang, Yanying; Liu, Zhihong; Ye, Xiaoxue; Li, Chunya

    2016-09-21

    Using 6-hydroxyl-quinoline-2-benzothiazole (HQB) as a two-photon fluorophore and tert-butyldiphenylsilyl as a recognition domain for F(-), a ratiometric two-photon fluorescent fluoride probe, QF, was synthesized and fully characterized. QF displays both one- and two-photon ratiometric responses towards fluoride ions in aqueous solution. QF was enabled to detect exogenous fluoride ions in living cells by a ratiometric method. Two-photon microscopic imaging of fluoride ions in living HeLa cells and zebrafish has also been achieved. QF has been demonstrated to be an excellent fluorescent probe with high selectivity, low cytotoxicity and good photostability.

  7. Two-photon absorption and spectroscopy of the lowest two-photon transition in small donor-acceptor-substituted organic molecules

    NASA Astrophysics Data System (ADS)

    Beels, Marten T.; Biaggio, Ivan; Reekie, Tristan; Chiu, Melanie; Diederich, François

    2015-04-01

    We determine the dispersion of the third-order polarizability of small donor-acceptor substituted organic molecules using wavelength-dependent degenerate four-wave mixing experiments in solutions with varying concentrations. We find that donor-acceptor-substituted molecules that are characterized by extremely efficient off-resonant nonlinearities also have a correspondingly high two-photon absorption cross section. The width and shape of the first two-photon resonance for these noncentrosymmetric molecules follows what is expected from their longest wavelength absorption peak, and the observed two-photon absorption cross sections are record high when compared to the available literature data, the size of the molecule, and the fundamental limit for two-photon absorption to the lowest excited state, which is essentially determined by the number of conjugated electrons and the excited-state energies. The two-photon absorption of the smallest molecule, which only has 16 electrons in its conjugated system, is one order of magnitude larger than for the molecule called AF-50, a reference molecule for two-photon absorption [O.-K. Kim et al., Chem. Mater. 12, 284 (2000), 10.1021/cm990662r].

  8. Photodissociation-ionization dynamics of molecular chlorine Rydberg states using velocity map imaging

    NASA Astrophysics Data System (ADS)

    Parker, D. H.; Bakker, B. L. G.; Samartzis, P. C.; Kitsopoulos, T. N.

    2001-07-01

    Velocity map images are reported for photoelectrons and atomic chlorine ions produced during one-color REMPI (resonance enhanced multiphoton ionization) of molecular chlorine via the v=0-15 vibrational levels of the 2 1Πg(4s) Rydberg state. Previous magnetic bottle photoelectron studies by Koenders et al. of the same process have shown that REMPI proceeds by two-photon resonant excitation, followed by core-excitation to a super-excited Rydberg state at the three-photon level. This state undergoes (auto)-ionization, resulting in the formation of ground-state molecular chlorine ions, and/or dissociation to neutral products, resulting in the production of electronically excited neutral chlorine atoms. Photoelectrons arise from ionization of Cl2 and electronically excited Cl atoms, while Cl+ ions arise from the dissociation of Cl2+ and from ionization of the excited Cl atoms. The chlorine ion velocity map images reveal new information on the dissociation-ionization dynamics of superexcited Cl2 and the dissociation dynamics of the subsequently formed Cl2+ ions. In the latter case an unexpected low-energy Σ←Π (perpendicular) dissociation pathway to Cl+(1D)+Cl(3P) product atoms is observed. Results from the photoelectron images are compared with those from the magnetic bottle studies. While the imaging kinetic-energy resolution is less than that of the magnetic bottle spectrometer, the angular distribution information and lack of velocity bias of imaging is advantageous. Most of the trends observed in the electron and Cl+ images can be rationalized in terms of single-electron excitation processes and the known molecular orbital structure of the electronic states involved.

  9. Hybrid Theranostic Platform for Second Near-IR Window Light Triggered Selective Two-Photon Imaging and Photothermal Killing of Targeted Melanoma Cells.

    PubMed

    Tchounwou, Christine; Sinha, Sudarson Sekhar; Viraka Nellore, Bhanu Priya; Pramanik, Avijit; Kanchanapally, Rajashekhar; Jones, Stacy; Chavva, Suhash Reddy; Ray, Paresh Chandra

    2015-09-23

    Despite advances in the medical field, even in the 21st century cancer is one of the leading causes of death for men and women in the world. Since the second near-infrared (NIR) biological window light between 950 and 1350 nm offers highly efficient tissue penetration, the current article reports the development of hybrid theranostic platform using anti-GD2 antibody attached gold nanoparticle (GNP) conjugated, single-wall carbon nanotube (SWCNT) for second near-IR light triggered selective imaging and efficient photothermal therapy of human melanoma cancer cell. Reported results demonstrate that due to strong plasmon-coupling, two-photon luminescence (TPL) intensity from theranostic GNP attached SWCNT materials is 6 orders of magnitude higher than GNP or SWCNT alone. Experimental and FDTD simulation data indicate that the huge enhancement of TPL intensity is mainly due to strong resonance enhancement coupled with the stronger electric field enhancement. Due to plasmon coupling, the theranostic material serves as a local nanoantennae to enhance the photothermal capability via strong optical energy absorption. Reported data show that theranostic SWCNT can be used for selective two-photon imaging of melanoma UACC903 cell using 1100 nm light. Photothermal killing experiment with 1.0 W/cm(2) 980 nm laser light demonstrates that 100% of melanoma UACC903 cells can be killed using theranostic SWCNT bind melanoma cells after just 8 min of exposure. These results demonstrate that due to plasmon coupling, the theranostic GNP attached SWCNT material serves as a two-photon imaging and photothermal source for cancer cells in biological window II.

  10. Hybrid Theranostic Platform for Second Near-IR Window Light Triggered Selective Two-Photon Imaging and Photothermal Killing of Targeted Melanoma Cells.

    PubMed

    Tchounwou, Christine; Sinha, Sudarson Sekhar; Viraka Nellore, Bhanu Priya; Pramanik, Avijit; Kanchanapally, Rajashekhar; Jones, Stacy; Chavva, Suhash Reddy; Ray, Paresh Chandra

    2015-09-23

    Despite advances in the medical field, even in the 21st century cancer is one of the leading causes of death for men and women in the world. Since the second near-infrared (NIR) biological window light between 950 and 1350 nm offers highly efficient tissue penetration, the current article reports the development of hybrid theranostic platform using anti-GD2 antibody attached gold nanoparticle (GNP) conjugated, single-wall carbon nanotube (SWCNT) for second near-IR light triggered selective imaging and efficient photothermal therapy of human melanoma cancer cell. Reported results demonstrate that due to strong plasmon-coupling, two-photon luminescence (TPL) intensity from theranostic GNP attached SWCNT materials is 6 orders of magnitude higher than GNP or SWCNT alone. Experimental and FDTD simulation data indicate that the huge enhancement of TPL intensity is mainly due to strong resonance enhancement coupled with the stronger electric field enhancement. Due to plasmon coupling, the theranostic material serves as a local nanoantennae to enhance the photothermal capability via strong optical energy absorption. Reported data show that theranostic SWCNT can be used for selective two-photon imaging of melanoma UACC903 cell using 1100 nm light. Photothermal killing experiment with 1.0 W/cm(2) 980 nm laser light demonstrates that 100% of melanoma UACC903 cells can be killed using theranostic SWCNT bind melanoma cells after just 8 min of exposure. These results demonstrate that due to plasmon coupling, the theranostic GNP attached SWCNT material serves as a two-photon imaging and photothermal source for cancer cells in biological window II. PMID:26327304

  11. TWO-PHOTON EXCHANGE IN ELECTRON-PROTON ELASTIC SCATTERING: THEORY UPDATE

    SciTech Connect

    Andrei Afanasev

    2007-05-21

    Recent theoretical developments in the studies of two-photon exchange effects in elastic electron-proton scattering are reviewed. Two-photon exchange mechanism is considered a likely source of discrepancy between polarized and unpolarized experimental measurements of the proton electric form factor at momentum transfers of several GeV$^2$. This mechanism predicts measurable effects that are currently studied experimentally.

  12. Effect of morphology and solvent on two-photon absorption of nano zinc oxide

    SciTech Connect

    Kavitha, M.K.; Haripadmam, P.C.; Gopinath, Pramod; Krishnan, Bindu; John, Honey

    2013-05-15

    Highlights: ► ZnO nanospheres and triangular structures synthesis by novel precipitation technique. ► The effect of precursor concentration on the size and shape of nano ZnO. ► Open aperture Z-scan measurements of the ZnO nanoparticle dispersions. ► Nanospheres exhibit higher two photon absorption coefficient than triangular nanostructures. ► Nanospheres dispersed in water exhibit higher two photon absorption coefficient than its dispersion in 2-propanol. - Abstract: In this paper, we report the effect of morphology and solvent on the two-photon absorption of nano zinc oxide. Zinc oxide nanoparticles in two different morphologies like nanospheres and triangular nanostructures are synthesized by novel precipitation technique and their two-photon absorption coefficient is measured using open aperture Z-scan technique. Experimental results show that the zinc oxide nanospheres exhibit higher two-photon absorption coefficient than the zinc oxide triangular nanostructures. The zinc oxide nanospheres dispersed in water exhibit higher two-photon absorption coefficient than that of its dispersion in 2-propanol. The zinc oxide nanospheres dispersed in water shows a decrease in two-photon absorption coefficient with an increase in on-axis irradiance. The result confirms the dependence of shape and solvent on the two-photon absorption of nano zinc oxide.

  13. Quantum correlation of path-entangled two-photon states in waveguide arrays with defects

    SciTech Connect

    Dou, Yiling; Xu, Lei; Han, Bin; Bo, Fang; Xu, Jingjun; Zhang, Guoquan

    2014-04-15

    We study the quantum correlation of path-entangled states of two photons in coupled one-dimensional waveguide arrays with lattice defects. Both off-diagonal and diagonal defects are considered, which show different effects on the quantum correlation of path-entangled two-photon states. Two-photon bunching or anti-bunching effects can be observed and controlled. The two photons are found to have a tendency to bunch at the side lobes with a repulsive off-diagonal defect, and the path-entanglement of the input two-photon state can be preserved during the propagation. We also found that defect modes may play an important role on the two-photon correlation of path-entangled states in the waveguide arrays. Due to the quantum interference effect, intriguing evolution dynamics of the two-photon correlation matrix elements with oscillation frequencies being either twice of or the same as that of a classical light wave, depending on the position of the correlation matrix element, is observed. Our results show that it is possible to manipulate the two-photon correlation properties of path-entangled states in waveguide arrays with lattice defects.

  14. 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

  15. Resonantly Enhanced Emission from a Luminescent Nanostructured Waveguide

    NASA Astrophysics Data System (ADS)

    Inada, Yasuhisa; Hashiya, Akira; Nitta, Mitsuru; Tomita, Shogo; Tsujimoto, Akira; Suzuki, Masa-Aki; Yamaki, Takeyuki; Hirasawa, Taku

    2016-09-01

    Controlling the characteristics of photon emission represents a significant challenge for both fundamental science and device technologies. Research on microcavities, photonic crystals, and plasmonic nanocavities has focused on controlling spontaneous emission by way of designing a resonant structure around the emitter to modify the local density of photonic states. In this work, we demonstrate resonantly enhanced emission using luminescent nanostructured waveguide resonance (LUNAR). Our concept is based on coupling between emitters in the luminescent waveguide and a resonant waveguide mode that interacts with a periodic nanostructure and hence outcouples via diffraction. We show that the enhancement of resonance emission can be controlled by tuning the design parameters. We also demonstrate that the enhanced emission is attributable to the accelerated spontaneous emission rate that increases the probability of photon emission in the resonant mode, accompanied by enhanced the local density of photonic states. This study demonstrates that nanostructured luminescent materials can be designed to exhibit functional and enhanced emission. We anticipate that our concept will be used to improve the performance of a variety of photonic and optical applications ranging from bio/chemical sensors to lighting, displays and projectors.

  16. Resonantly Enhanced Emission from a Luminescent Nanostructured Waveguide

    PubMed Central

    Inada, Yasuhisa; Hashiya, Akira; Nitta, Mitsuru; Tomita, Shogo; Tsujimoto, Akira; Suzuki, Masa-aki; Yamaki, Takeyuki; Hirasawa, Taku

    2016-01-01

    Controlling the characteristics of photon emission represents a significant challenge for both fundamental science and device technologies. Research on microcavities, photonic crystals, and plasmonic nanocavities has focused on controlling spontaneous emission by way of designing a resonant structure around the emitter to modify the local density of photonic states. In this work, we demonstrate resonantly enhanced emission using luminescent nanostructured waveguide resonance (LUNAR). Our concept is based on coupling between emitters in the luminescent waveguide and a resonant waveguide mode that interacts with a periodic nanostructure and hence outcouples via diffraction. We show that the enhancement of resonance emission can be controlled by tuning the design parameters. We also demonstrate that the enhanced emission is attributable to the accelerated spontaneous emission rate that increases the probability of photon emission in the resonant mode, accompanied by enhanced the local density of photonic states. This study demonstrates that nanostructured luminescent materials can be designed to exhibit functional and enhanced emission. We anticipate that our concept will be used to improve the performance of a variety of photonic and optical applications ranging from bio/chemical sensors to lighting, displays and projectors. PMID:27682993

  17. Two-Photon Probes for Lysosomes and Mitochondria: Simultaneous Detection of Lysosomes and Mitochondria in Live Tissues by Dual-Color Two-Photon Microscopy Imaging.

    PubMed

    Lim, Chang Su; Hong, Seung Taek; Ryu, Seong Shick; Kang, Dong Eun; Cho, Bong Rae

    2015-10-01

    Novel two-photon (TP) probes were developed for lysosomes (PLT-yellow) and mitochondria (BMT-blue and PMT-yellow). These probes emitted strong TP-excited fluorescence in cells at widely separated wavelength regions and displayed high organelle selectivity, good cell permeability, low cytotoxicity, and pH insensitivity. The BMT-blue and PLT-yellow probes could be utilized to detect lysosomes and mitochondria simultaneously in live tissues by using dual-color two-photon microscopy, with minimum interference from each other.

  18. Correlated two-photon generation by diamond atomic system in Yb atoms

    NASA Astrophysics Data System (ADS)

    Yoon, Tai Hyun; Song, Minsoo

    2011-05-01

    We study a non-degenerate correlated two-photon generation with narrow bandwidths of 50 MHz by using a diamond atomic system in the collimated Yb atomic beam. We excited the 6s2 1S0 atoms into the 6s7s 1S0 excited state by the resonant two-photon transition via the intermediate 6s6p 1P1 state. Then, the excited atoms decay spontaneously into the 6s2 1S0 ground state via the inter-combination 6s6p 3P1 state. We are focusing on the closed-loop two-photon absorption/excitation path through which correlated two photons having the wavelengths of 611.3 nm (Stokes) and 556.8 nm (anti-Stokes) can be generated efficiently. We performed first a two-photon absorption spectroscopy for the 1S0-1P1-1S0 two-photon transitions. An ECDL at 399 nm was used to excite the 1S0-1P1 transition and another ECDL at 1077 nm was used to excite the 1P1-1S0 transition. From the spontaneous two-photon emission process, we were able to detect correlated two-photons at 611.3 nm and 555.8 nm at the plane perpendicular to the excitation beams, and parallel to the Yb atomic beam. We detected a few times of 106 photons per second both at the idler and signal beams at the condition of two-photon resonance with the detection solid angle of only 0.01 sr. We also performed an optical switching and modulation experiments of the photon-pair by optically switching and frequency modulation of the 399-nm driving field.

  19. A Two-Photon Fluorescent Probe for Lysosomal Thiols in Live Cells and Tissues

    PubMed Central

    Fan, Jiangli; Han, Zhichao; Kang, Yao; Peng, Xiaojun

    2016-01-01

    Lysosome-specific fluorescent probes are exclusive to elucidate the functions of lysosomal thiols. Moreover, two-photon microscopy offers advantages of less phototoxicity, better three dimensional spatial localization, deeper penetration depth and lower self-absorption. However, such fluorescent probes for thiols are still rare. In this work, an efficient two-photon fluorophore 1,8-naphthalimide-based probe conjugating a 2,4-dinitrobenzenesulfonyl chloride and morpholine was designed and synthesized, which exhibited high selectivity and sensitivity towards lysosomal thiols by turn-on fluorescence method quantitatively and was successfully applied to the imaging of thiols in live cells and tissues by two-photon microscopy. PMID:26794434

  20. {Delta} resonance contribution to two-photon exchange in electron-proton scattering

    SciTech Connect

    S. Kondratyuk; P. G. Blunden; W. Melnitchouk; J. A. Tjon

    2005-06-01

    We calculate the effects on the elastic electron-proton scattering cross section of the two-photon exchange contribution with an intermediate {Delta} resonance. The {Delta} two-photon exchange contribution is found to be smaller in magnitude than the previously evaluated nucleon contribution, with an opposite sign at backward scattering angles. The sum of the nucleon and {Delta} two-photon exchange corrections has the angular dependence compatible with both the polarization transfer and the Rosenbluth methods of measuring the nucleon electromagnetic form factors.

  1. Evaluation of the exothermicity of the chemi-ionization reaction Sm + O → SmO(+) + e(.).

    PubMed

    Cox, Richard M; Kim, JungSoo; Armentrout, P B; Bartlett, Joshua; VanGundy, Robert A; Heaven, Michael C; Ard, Shaun G; Melko, Joshua J; Shuman, Nicholas S; Viggiano, Albert A

    2015-04-01

    The exothermicity of the chemi-ionization reaction Sm + O → SmO(+) + e(-) has been re-evaluated through the combination of several experimental methods. The thermal reactivity (300-650 K) of Sm(+) and SmO(+) with a range of species measured using a selected ion flow tube-mass spectrometer apparatus is reported and provides limits for the bond strength of SmO(+), 5.661 eV ≤ D0(Sm(+)-O) ≤ 6.500 eV. A more precise value is measured to be 5.725 ± 0.07 eV, bracketed by the observed reactivity of Sm(+) and SmO(+) with several species using a guided ion beam tandem mass spectrometer (GIBMS). Combined with the established Sm ionization energy (IE), this value indicates an exothermicity of the title reaction of 0.08 ± 0.07 eV, ∼0.2 eV smaller than previous determinations. In addition, the ionization energy of SmO has been measured by resonantly enhanced two-photon ionization and pulsed-field ionization zero kinetic energy photoelectron spectroscopy to be 5.7427 ± 0.0006 eV, significantly higher than the literature value. Combined with literature bond energies of SmO, this value indicates an exothermicity of the title reaction of 0.14 ± 0.17 eV, independent from and in agreement with the GIBMS result presented here. The evaluated thermochemistry also suggests that D0(SmO) = 5.83 ± 0.07 eV, consistent with but more precise than the literature values. Implications of these results for interpretation of chemical release experiments in the thermosphere are discussed.

  2. Note: Derivation of two-photon circular dichroism--Addendum to "Two-photon circular dichroism" [J. Chem. Phys. 62, 1006 (1975)].

    PubMed

    Friese, Daniel H

    2015-09-01

    This addendum shows the detailed derivation of the fundamental equations for two-photon circular dichroism which are given in a very condensed form in the original publication [I. Tinoco, J. Chem. Phys. 62, 1006 (1975)]. In addition, some minor errors are corrected and some of the derivations in the original publication are commented.

  3. An Amphiphilic BODIPY-Porphyrin Conjugate: Intense Two-Photon Absorption and Rapid Cellular Uptake for Two-Photon-Induced Imaging and Photodynamic Therapy.

    PubMed

    Zhang, Tao; Lan, Rongfeng; Gong, Longlong; Wu, Baoyan; Wang, Yuzhi; Kwong, Daniel W J; Wong, Wai-Kwok; Wong, Ka-Leung; Xing, Da

    2015-11-01

    The new amphiphilic BODPY-porphyrin conjugate BZnPP and its precursor BZnPH were synthesised, and their linear and two-photon photophysical properties, together with their cellular uptake and photo-cytotoxicity, were studied. This amphiphilic conjugate consists of a hydrophobic BODIPY moiety and a hydrophilic tetra(ethylene glycol) chain bridging a cationic triphenylphosphonium group to an amphiphilic porphyrin ZnP through acetylide linkers at its meso positions. A large two-photon absorption cross-section (σ=1725 GM) and a high singlet oxygen quantum yield (0.52) were recorded. Intense linear- and two-photon-induced red emissions were also observed for both BZnPP and BZnPH. Further in vitro studies showed that BZnPP exhibited very efficient cellular uptake and strong photocytotoxic but weak dark cytotoxic properties towards human breast carcinoma MCF-7 cells. In summary, the two-photon-induced emission and the potent photo-cytotoxicity of BZnPP make it an efficacious dual-purpose tumour-imaging and photodynamic therapeutic agent in the tissue-transparent spectral windows.

  4. Note: Derivation of two-photon circular dichroism—Addendum to “Two-photon circular dichroism” [J. Chem. Phys. 62, 1006 (1975)

    SciTech Connect

    Friese, Daniel H.

    2015-09-07

    This addendum shows the detailed derivation of the fundamental equations for two-photon circular dichroism which are given in a very condensed form in the original publication [I. Tinoco, J. Chem. Phys. 62, 1006 (1975)]. In addition, some minor errors are corrected and some of the derivations in the original publication are commented.

  5. Observation of Nondegenerate Two-Photon Gain in GaAs

    NASA Astrophysics Data System (ADS)

    Reichert, Matthew; Smirl, Arthur L.; Salamo, Greg; Hagan, David J.; Van Stryland, Eric W.

    2016-08-01

    Two-photon lasers require materials with large two-photon gain (2PG) coefficients and low linear and nonlinear losses. Our previous demonstration of large enhancement of two-photon absorption in semiconductors for very different photon energies translates directly into enhancement of 2PG. We experimentally demonstrate nondegenerate 2PG in optically excited bulk GaAs via femtosecond pump-probe measurements. 2PG is isolated from other pump induced effects through the difference between measurements performed with parallel and perpendicular polarizations of pump and probe. An enhancement in the 2PG coefficient of nearly 2 orders of magnitude is reported. The results point a possible way toward two-photon semiconductor lasers.

  6. Measurement of Two-Photon Absorption Cross Section of Metal Ions by a Mass Sedimentation Approach

    PubMed Central

    Ma, Zhuo-Chen; Chen, Qi-Dai; Han, Bing; Liu, Xue-Qing; Song, Jun-Feng; Sun, Hong-Bo

    2015-01-01

    The photo-reduction of metal ions in solution induced by femtosecond laser is an important and novel method for fabricating three-dimensional metal microstructures. However, the nonlinear absorption cross section of metal ions remains unknown because its measurement is difficult. In the present study, a method based on Two-Photon Excited Sedimentation (TPES) is proposed to measure the two-photon absorption cross section (TPACS) of metal ions in solution. The power-squared dependence of the amount of sediment on the excitation intensity was confirmed, revealing that 800 nm femtosecond laser induced reduction of metal ions was a two photon absorption process. We believe that the proposed method may be applied to measure the TPACS of several metal ions, thereby opening a new avenue towards future analysis of two-photon absorption materials. PMID:26657990

  7. Two-photon fluorescence correlation spectroscopy with high count rates and low background using dielectric microspheres

    PubMed Central

    Aouani, Heykel; Schön, Peter; Brasselet, Sophie; Rigneault, Hervé; Wenger, Jérôme

    2010-01-01

    Two-photon excitation fluorescence is a powerful technique commonly used for biological imaging. However, the low absorption cross section of this non-linear process is a critical issue for performing biomolecular spectroscopy at the single molecule level. Enhancing the two-photon fluorescence signal would greatly improve the effectiveness of this technique, yet current methods struggle with medium enhancement factors and/or high background noise. Here, we show that the two-photon fluorescence signal from single Alexa Fluor 488 molecules can be enhanced up to 10 times by using a 3 µm diameter latex sphere while adding almost no photoluminescence background. We report a full characterization of the two-photon fluorescence enhancement by a single microsphere using fluorescence correlation spectroscopy. This opens new routes to enhance non-linear optical signals and extend biophotonic applications. PMID:21258531

  8. Observation of Nondegenerate Two-Photon Gain in GaAs.

    PubMed

    Reichert, Matthew; Smirl, Arthur L; Salamo, Greg; Hagan, David J; Van Stryland, Eric W

    2016-08-12

    Two-photon lasers require materials with large two-photon gain (2PG) coefficients and low linear and nonlinear losses. Our previous demonstration of large enhancement of two-photon absorption in semiconductors for very different photon energies translates directly into enhancement of 2PG. We experimentally demonstrate nondegenerate 2PG in optically excited bulk GaAs via femtosecond pump-probe measurements. 2PG is isolated from other pump induced effects through the difference between measurements performed with parallel and perpendicular polarizations of pump and probe. An enhancement in the 2PG coefficient of nearly 2 orders of magnitude is reported. The results point a possible way toward two-photon semiconductor lasers. PMID:27563962

  9. Fluorescence upconversion properties of a class of improved pyridinium dyes induced by two-photon absorption

    NASA Astrophysics Data System (ADS)

    Xu, Guibao; Hu, Dawei; Zhao, Xian; Shao, Zongshu; Liu, Huijun; Tian, Yupeng

    2007-06-01

    We report the fluorescence upconversion properties of a class of improved pyridinium toluene- p-sulfonates having donor- π-acceptor (D- π-A) structure under two-photon excitation at 1064 nm. The experimental results show that both the two-photon excited (TPE) fluorescence lifetime and the two-photon pumped (TPP) energy upconversion efficiency were increased with the enhancement of electron-donating capability of the donor in the molecule. It is also indicated that an overlong alkyl group tends to result in a weakened molecular conjugation, leading to a decreased two-photon absorption (TPA) cross section. By choosing the donor, we can obtain a longest fluorescence lifetime of 837 ps, a highest energy upconversion efficiency of ˜6.1%, and a maximum TPA cross-section of 8.74×10 -48 cm 4 s/photon in these dyes.

  10. Resolution enhancement of two-photon microscopy via intensity-modulated laser scanning structured illumination.

    PubMed

    Yeh, Chia-Hua; Chen, Szu-Yu

    2015-03-20

    Conventional structured illumination microscopy (SIM) with wide-field illumination is an applicable tool to provide resolution enhancement. And yet its applications in thick specimens are still full of challenges. By combing the structured illumination concept with two-photon excitation, a laser scanning two-photon structured illumination microscope (LSTP-SIM) was constructed to gain ∼1.42-fold lateral resolution enhancement in contrast to two-photon fluorescence microscopy. With a point-scanning geometry, an acoustic-optical modulator was used to modulate temporally the excitation intensity in order to produce the structured illumination pattern. The theoretical models of image formation and image reconstruction were clearly established. Simulation and experiments were both performed to show the capability of this system to enhance the lateral resolution. Combined with the inherent optical sectioning power of the two-photon excitation, LSTP-SIM would have the potential for applications in optically-thick specimens. PMID:25968516

  11. Observation of Two-Photon Photoemission Optogalvanic Effect Using Copper Target Electrode

    NASA Astrophysics Data System (ADS)

    Ajithprasad, K. C.; Sasikumar, P. R.; Harilal, S. S.; Nampoori, V. P. N.; Vallabhan, C. P. G.

    Two-photon-induced photoemission optogalvanic effect using copper as the target electrode has been observed in a nitrogen discharge cell using 532 nm radiation from a frequency-doubled Nd:YAG laser as the pump source.

  12. Chirp measurement of large-bandwidth femtosecond optical pulses using two-photon absorption

    NASA Astrophysics Data System (ADS)

    Albrecht, T. F.; Seibert, K.; Kurz, H.

    1991-08-01

    We describe a novel method for accurate chirp measurement of broadband femtosecond pulses over their entire bandwidth based on two-photon absorption. These chirp measurements are applied for the optimization of a fiber-grating-prism pulse compressor.

  13. Anticancer phototherapy using activation of E-combretastatins by two-photon-induced isomerization

    NASA Astrophysics Data System (ADS)

    Scherer, Kathrin M.; Bisby, Roger H.; Botchway, Stanley W.; Hadfield, John A.; Parker, Anthony W.

    2015-05-01

    The photoisomerization of relatively nontoxic E-combretastatins to clinically active Z-isomers is shown to occur in solution through both one- and two-photon excitations at 340 and 625 nm, respectively. The photoisomerization is also demonstrated to induce mammalian cell death by a two-photon absorption process at 625 nm. Unlike conventional photodynamic therapy (PDT), the mechanism of photoisomerization is oxygen-independent and active in hypoxic environments such as in tumors. The use of red or near-infrared (NIR) light for two-photon excitation allows greater tissue penetration than conventional UV one-photon excitation. The results provide a baseline for the development of a novel phototherapy that overcomes nondiscriminative systemic toxicity of Z-combretastatins and the limitations of PDT drugs that require the presence of oxygen to promote their activity, with the added benefits of two-photon red or NIR excitation for deeper tissue penetration.

  14. 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.

  15. 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.

  16. Y-shaped two-photon absorbing molecules with an imidazole-thiazole core

    NASA Technical Reports Server (NTRS)

    Feng, Ke; De Boni, Leonardo; Misoguti, Lino; Mendonca, C. R.; Meador, Michael; Hsu, Fu-Lian; Bu, Xiu R.

    2004-01-01

    Two new classes of two-photon absorbing Y-shaped molecules have been developed to possess an imidazole-thiazole core and a stilbene-type conjugation pathway with either nitro or sulfonyl as terminal electron-accepting group.

  17. Two-photon vibrational excitation of air by long-wave infrared laser pulses

    NASA Astrophysics Data System (ADS)

    Palastro, J. P.; Peñano, J.; Johnson, L. A.; Hafizi, B.; Wahlstrand, J. K.; Milchberg, H. M.

    2016-08-01

    Ultrashort long-wave infrared (LWIR) laser pulses can resonantly excite vibrations in N2 and O2 through a two-photon transition. The absorptive vibrational component of the ultrafast optical nonlinearity grows in time, starting smaller than but quickly surpassing the electronic, rotational, and vibrational refractive components. The growth of the vibrational component results in a novel mechanism of third-harmonic generation, providing an additional two-photon excitation channel, fundamental + third harmonic. The original and emergent two-photon excitations drive the resonance exactly out of phase, causing spatial decay of the absorptive vibrational nonlinearity. This nearly eliminates two-photon vibrational absorption. Here we present simulations and analytical calculations demonstrating how these processes modify the ultrafast optical nonlinearity in air. The results reveal nonlinear optical phenomena unique to the LWIR regime of ultrashort pulse propagation in the atmosphere.

  18. Two-photon-exchange effects in the electro-excitation of the $\\Delta$ resonance

    SciTech Connect

    Vladimir Pascalutsa; Carl E. Carlson; Marc Vanderhaghen

    2005-09-15

    We evaluate the two-photon exchange contribution to the eN {yields} e{Delta}(1232) {yields} e{pi}N process at large momentum transfer with the aim of a precision study of the ratios of electric quadrupole (E2) and Coulomb quadrupole (C2) to the magnetic dipole (M1) {gamma}* N{Delta} transitions. We relate the two-photon exchange amplitude to the N {yields} {Delta} generalized parton distributions and obtain a quantitative estimate of the two-photon effects. The two-photon exchange corrections to the C2/M1 ratio depend strongly on whether this quantity is obtained from an interference cross section or from the Rosenbluth-type cross sections, in similarity with the elastic, eN {yields} eN, process.

  19. Super-resolution two-photon microscopy via scanning patterned illumination

    NASA Astrophysics Data System (ADS)

    Urban, Ben E.; Yi, Ji; Chen, Siyu; Dong, Biqin; Zhu, Yongling; DeVries, Steven H.; Backman, Vadim; Zhang, Hao F.

    2015-04-01

    We developed two-photon scanning patterned illumination microscopy (2P-SPIM) for super-resolution two-photon imaging. Our approach used a traditional two-photon microscopy setup with temporally modulated excitation to create patterned illumination fields. Combing nine different illuminations and structured illumination reconstruction, super-resolution imaging was achieved in two-photon microscopy. Using 2P-SPIM we achieved a lateral resolution of 141 nm, which represents an improvement by a factor of 1.9 over the corresponding diffraction limit. We further demonstrated super-resolution cellular imaging by 2P-SPIM to image actin cytoskeleton in mammalian cells and three-dimensional imaging in highly scattering retinal tissue.

  20. Experimental observation of sub-Rayleigh quantum imaging with a two-photon entangled source

    SciTech Connect

    Xu, De-Qin; Song, Xin-Bing; Li, Hong-Guo; Zhang, De-Jian; Wang, Hai-Bo; Xiong, Jun Wang, Kaige

    2015-04-27

    It has been theoretically predicted that N-photon quantum imaging can realize either an N-fold resolution improvement (Heisenberg-like scaling) or a √(N)-fold resolution improvement (standard quantum limit) beyond the Rayleigh diffraction bound, over classical imaging. Here, we report the experimental study on spatial sub-Rayleigh quantum imaging using a two-photon entangled source. Two experimental schemes are proposed and performed. In a Fraunhofer diffraction scheme with a lens, two-photon Airy disk pattern is observed with subwavelength diffraction property. In a lens imaging apparatus, however, two-photon sub-Rayleigh imaging for an object is realized with super-resolution property. The experimental results agree with the theoretical prediction in the two-photon quantum imaging regime.

  1. Two-photon interference with continuous-wave multi-mode coherent light.

    PubMed

    Kim, Yong-Su; Slattery, Oliver; Kuo, Paulina S; Tang, Xiao

    2014-02-10

    We report two-photon interference with continuous-wave multi-mode coherent light. We show that the two-photon interference, in terms of the detection time difference, reveals two-photon beating fringes with the visibility V = 0.5. While scanning the optical delay of the interferometer, Hong-Ou-Mandel dips or peaks are measured depending on the chosen detection time difference. The HOM dips/peaks are repeated when the optical delay and the first-order coherence revival period of the multi-mode coherent light are the same. These results help to understand the nature of two-photon interference and also can be useful for quantum information science.

  2. The two-photon excitation cross section of 6MAP, a fluorescent adenine analogue.

    PubMed

    Stanley, Robert J; Hou, Zhanjia; Yang, Aiping; Hawkins, Mary E

    2005-03-01

    6MAP is a fluorescent analogue of adenine that undergoes Watson-Crick base pairing and base stacking in double-stranded DNA. The one-photon absorption spectrum of 6MAP is characterized by a maximum around 330 nm with moderate quantum yield fluorescence centered at about 420 nm. To take advantage of this probe for confocal and single-molecule microscopy, it would be advantageous to be able to excite the analogue via two photons. We report the first determination of the two-photon excitation cross section and spectrum for 6MAP from 614 to 700 nm. The power dependence of the fluorescence indicates that emission results from the absorption of two photons. The one-photon and two-photon emission line shapes are identical within experimental error. A study of the concentration dependence of the fluorescence yield for one-photon excitation shows no measurable quenching up to about 5 microM. The maximum in the two-photon excitation spectrum gives a two-photon cross section, delta(TPE), of 3.4 +/- 0.1 Goeppert-Mayer (G.M.) at 659 nm, which correlates well with the one-photon absorption maximum. This compares quite favorably with cross sections of various naturally fluorescent biological molecules such as flavins and nicotiamide. In addition, we have also obtained the two-photon-induced fluorescence emission spectrum of quinine sulfate. It is approximately the same as that for one-photon excitation, suggesting that two-photon excitation of quinine sulfate may be used for calibration purposes.

  3. The two-photon excitation cross section of 6MAP, a fluorescent adenine analogue.

    PubMed

    Stanley, Robert J; Hou, Zhanjia; Yang, Aiping; Hawkins, Mary E

    2005-03-01

    6MAP is a fluorescent analogue of adenine that undergoes Watson-Crick base pairing and base stacking in double-stranded DNA. The one-photon absorption spectrum of 6MAP is characterized by a maximum around 330 nm with moderate quantum yield fluorescence centered at about 420 nm. To take advantage of this probe for confocal and single-molecule microscopy, it would be advantageous to be able to excite the analogue via two photons. We report the first determination of the two-photon excitation cross section and spectrum for 6MAP from 614 to 700 nm. The power dependence of the fluorescence indicates that emission results from the absorption of two photons. The one-photon and two-photon emission line shapes are identical within experimental error. A study of the concentration dependence of the fluorescence yield for one-photon excitation shows no measurable quenching up to about 5 microM. The maximum in the two-photon excitation spectrum gives a two-photon cross section, delta(TPE), of 3.4 +/- 0.1 Goeppert-Mayer (G.M.) at 659 nm, which correlates well with the one-photon absorption maximum. This compares quite favorably with cross sections of various naturally fluorescent biological molecules such as flavins and nicotiamide. In addition, we have also obtained the two-photon-induced fluorescence emission spectrum of quinine sulfate. It is approximately the same as that for one-photon excitation, suggesting that two-photon excitation of quinine sulfate may be used for calibration purposes. PMID:16851408

  4. Serial two-photon tomography: an automated method for ex-vivo mouse brain imaging

    PubMed Central

    Ragan, Timothy; Kadiri, Lolahon R.; Venkataraju, Kannan Umadevi; Bahlmann, Karsten; Sutin, Jason; Taranda, Julian; Arganda-Carreras, Ignacio; Kim, Yongsoo; Seung, H. Sebastian

    2011-01-01

    Here we describe an automated method, which we call serial two-photon (STP) tomography, that achieves high-throughput fluorescence imaging of mouse brains by integrating two-photon microscopy and tissue sectioning. STP tomography generates high-resolution datasets that are free of distortions and can be readily warped in 3D, for example, for comparing multiple anatomical tracings. This method opens the door to routine systematic studies of neuroanatomy in mouse models of human brain disorders. PMID:22245809

  5. Two-Photon Neuronal and Astrocytic Stimulation with Azobenzene-Based Photoswitches

    PubMed Central

    2015-01-01

    Synthetic photochromic compounds can be designed to control a variety of proteins and their biochemical functions in living cells, but the high spatiotemporal precision and tissue penetration of two-photon stimulation have never been investigated in these molecules. Here we demonstrate two-photon excitation of azobenzene-based protein switches and versatile strategies to enhance their photochemical responses. This enables new applications to control the activation of neurons and astrocytes with cellular and subcellular resolution. PMID:24857186

  6. Observation of Two-Photon Excitation for Three-Level Atoms in a Squeezed Vacuum

    NASA Technical Reports Server (NTRS)

    Edamatsu, K.; Georgiades, N. Ph.; Polzik, E. S.; Kimble, H. J.; Parkins, A. S.

    1996-01-01

    The two-photon transition (6S(sub 1/2) yields 6D(sub 5/2)) of atomic Cesium is investigated for excitation with squeezed vacuum generated via nondegenerate parametric down conversion. The two-photon excitation rate (R) is observed to have a non-quadratic dependence of R = aI(exp 2) + bI on the incident photon flux (I), reflecting the nonclassical correlations of the squeezed vacuum field.

  7. Highly Selective Two-Photon Fluorescent Probe for Ratiometric Sensing and Imaging Cysteine in Mitochondria.

    PubMed

    Niu, Weifen; Guo, Lei; Li, Yinhui; Shuang, Shaomin; Dong, Chuan; Wong, Man Shing

    2016-02-01

    A novel ratiometric mitochondrial cysteine (Cys)-selective two-photon fluorescence probe has been developed on the basis of a merocyanine as the fluorophore and an acrylate moiety as the biothiol reaction site. The biocompatible and photostable acrylate-functionalized merocyanine probe shows not only a mitochondria-targeting property but also highly selective detection and monitoring of Cys over other biothiols such as homocysteine (Hcy) and glutathione (GSH) and hydrogen sulfide (H2S) in live cells. In addition, this probe exhibits ratiometric fluorescence emission characteristics (F518/F452), which are linearly proportional to Cys concentrations in the range of 0.5-40 μM. More importantly, the probe and its released fluorophore, merocyanine, exhibit strong two-photon excited fluorescence (TPEF) with two-photon action cross-section (Φσmax) of 65.2 GM at 740 nm and 72.6 GM at 760 nm in aqueous medium, respectively, which is highly desirable for high contrast and brightness ratiometric two-photon fluorescence imaging of the living samples. The probe has been successfully applied to ratiometrically image and detect mitochondrial Cys in live cells and intact tissues down to a depth of 150 μm by two-photon fluorescence microscopy. Thus, this ratiometric two-photon fluorescent probe is practically useful for an investigation of Cys in living biological systems. PMID:26717855

  8. Two-Photon and Second Harmonic Microscopy in Clinical and Translational Cancer Research

    PubMed Central

    PERRY, SETH W.; BURKE, RYAN M.; BROWN, EDWARD B.

    2012-01-01

    Application of two-photon microscopy (TPM) to translational and clinical cancer research has burgeoned over the last several years, as several avenues of pre-clinical research have come to fruition. In this review, we focus on two forms of TPM—two-photon excitation fluorescence microscopy, and second harmonic generation microscopy—as they have been used for investigating cancer pathology in ex vivo and in vivo human tissue. We begin with discussion of two-photon theory and instrumentation particularly as applicable to cancer research, followed by an overview of some of the relevant cancer research literature in areas that include two-photon imaging of human tissue biopsies, human skin in vivo, and the rapidly developing technology of two-photon microendoscopy. We believe these and other evolving two-photon methodologies will continue to help translate cancer research from the bench to the bedside, and ultimately bring minimally invasive methods for cancer diagnosis and treatment to therapeutic reality. PMID:22258888

  9. Two-photon fluorescent probes for biological Mg(2+) detection based on 7-substituted coumarin.

    PubMed

    Yin, Haijing; Zhang, Buchang; Yu, Haizhu; Zhu, Lin; Feng, Yan; Zhu, Manzhou; Guo, Qingxiang; Meng, Xiangming

    2015-05-01

    Two novel water-soluble coumarin-based compounds (OC7, NC7) were designed and synthesized as two-photon fluorescent probes for biological Mg(2+) detection. The compounds feature a β-keto acid as a high selective binding site for Mg(2+) and the coumarin framework as the two-photon fluorophore. OC7 and NC7 show significant "off-on" detecting signals (9.05-fold and 23.8-fold fluorescence enhancement) and lower detection limits compared with previous reported two-photon fluorescent probes for Mg(2+). Moreover, OC7-Mg(2+) and NC7-Mg(2+) exhibit large two-photon absorption cross sections (340 and 615 GM) at the near-infrared wavelengths (740 and 860 nm), which indicates that the probes are very suitable for detection of Mg(2+) in vivo. Both OC7 and NC7 are pH-insensitive and of low cytotoxicity and can be applied to image intracellular Mg(2+) under two-photon microscopy (TPM). Our results provide a strategy to modify the coumarin fluorophore to get better two-photon fluorescent properties. And the results also suggest that electronic density of β-keto acid plays a very important role in the recognition of Mg(2+).

  10. Highly Selective Two-Photon Fluorescent Probe for Ratiometric Sensing and Imaging Cysteine in Mitochondria.

    PubMed

    Niu, Weifen; Guo, Lei; Li, Yinhui; Shuang, Shaomin; Dong, Chuan; Wong, Man Shing

    2016-02-01

    A novel ratiometric mitochondrial cysteine (Cys)-selective two-photon fluorescence probe has been developed on the basis of a merocyanine as the fluorophore and an acrylate moiety as the biothiol reaction site. The biocompatible and photostable acrylate-functionalized merocyanine probe shows not only a mitochondria-targeting property but also highly selective detection and monitoring of Cys over other biothiols such as homocysteine (Hcy) and glutathione (GSH) and hydrogen sulfide (H2S) in live cells. In addition, this probe exhibits ratiometric fluorescence emission characteristics (F518/F452), which are linearly proportional to Cys concentrations in the range of 0.5-40 μM. More importantly, the probe and its released fluorophore, merocyanine, exhibit strong two-photon excited fluorescence (TPEF) with two-photon action cross-section (Φσmax) of 65.2 GM at 740 nm and 72.6 GM at 760 nm in aqueous medium, respectively, which is highly desirable for high contrast and brightness ratiometric two-photon fluorescence imaging of the living samples. The probe has been successfully applied to ratiometrically image and detect mitochondrial Cys in live cells and intact tissues down to a depth of 150 μm by two-photon fluorescence microscopy. Thus, this ratiometric two-photon fluorescent probe is practically useful for an investigation of Cys in living biological systems.

  11. A two-photon ratiometric fluorescent probe enables spatial coordinates determination of intracellular pH.

    PubMed

    Wang, Junjie; Sun, Yuming; Zhang, Weijia; Liu, Yong; Yu, Xiaoqiang; Zhao, Ning

    2014-11-01

    We reported a two-photon ratiometric fluorescent probe for detecting intracellular pH. When excited with 800 nm laser, an optimal output of laser as the routine equipment of two-photon fluorescence microscopy, the two-photon excited fluorescence of this probe showed distinct emission peak shift as large as 109 nm upon the change of pH values in vitro. Very importantly, the experiment results show that this probe has large two-photon absorption cross-section at pH 4.5 at 800 nm of 354 g, which ranks it as one of the best two-photon ratiometric fluorescent pH probes, and its working pH value is between 4.0 and 8.0 which could fit the intracellular pH range. Moreover, utilizing this probe, the two-photon ratiometric fluorescent images in living cells have been obtained, and the spatial coordinates of intracellular pH can be mapped. At the same time, the probe also exhibited selectivity, photostability and membrane permeability. And the photophysical properties of this probe in various solvents indicated that these photophysical properties variations are due to an intramolecular charge transfer process. At last, the imaging depth of the probe in liver biopsy slices was investigated. The experimental results demonstrated the maximum imaging depth can arrive 66 µm in living rat liver tissues.

  12. Photo-click construction of a targetable and activatable two-photon probe imaging protease in apoptosis.

    PubMed

    Zhou, Mi; Hu, Jing; Zheng, Mengmeng; Song, Qinhua; Li, Jinbo; Zhang, Yan

    2016-02-01

    A photo-click reaction was used as an efficient method to construct two-photon fluorescent probes bearing two functional peptides for targeting and for protease cleavage respectively. The activatable two-photon probe constructed by this method was applied to two-photon imaging of caspase-3 both in cellular apoptosis and in tumor tissue.

  13. Piezoelectric resonance enhanced microwave and optoelectronic interactive devices

    NASA Astrophysics Data System (ADS)

    McIntosh, Robert

    Electro-optic (EO) devices that modulate optical signals by electric fields are an integrative part of the photonics industry and device optimization is an important area of research. As applications move to large bandwidth and higher frequency, low electro-optic effects and the requirement for large dimension become restrictive for microwave-optical devices. Both experimental and computational evaluations indicate that strain and polarization distribution have a significant impact on electromagnetic wave propagation resulting from a resonant structure; however, no systematic study or fundamental understandings are available. This dissertation research has been carried out to study and further develop the subject of piezoelectric resonance enhanced electro-acoustic-optic process, in order to improve the sensitivity and efficiency of electro-optic sensors and to explore novel applications. Many finite element models have been constructed for evaluating the mechanisms of the phenomena and the effectiveness of the device structure. The enhancement in transmission is found to be directly related to the strain-coupled local polarization. At piezoelectric resonance oscillating dipoles or local polarizations become periodic in the material and have the greatest impact on transmission. Results suggest that the induced charge distribution by a piezoelectric material at certain resonant frequencies is effective for aiding or impeding the transmission of a propagating wave. The behavior of both piezoelectric-defined (or intrinsic piezoelectric materials) and engineered periodic structures are reported. The piezoelectric response of the surface displacement of samples is investigated using an ultra-high frequency laser Doppler vibrometer. A two dimensional view of the surface is obtained and the surface displacement, velocity and acceleration are compared to the electro-optic response under the resonant condition. A study of the acousto-optic (AO) effect in a family of oxide

  14. 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

  15. Titanium: Sapphire laser as an excitation source in two-photon spectroscopy

    SciTech Connect

    Fisher, W.G.; Wachter, E.A.; Armas, M.; Seaton, C.

    1997-02-01

    The passively mode-locked titanium:sapphire laser provides new opportunities for acquiring two-photon spectral data in the near-infrared, a region not commonly accessible to synchronously pumped dye lasers. This source generates pulses with peak powers near 100 kW at average powers over 1 W and is capable of yielding two-photon signals roughly two orders of magnitude larger than is possible with synchronously pumped dye lasers. However, the multimode output of this laser exhibits significant temporal and spectral pulse profile variations as the laser wavelength is tuned. As a consequence, peak powers of the titanium:sapphire laser can vary independently from average power across the tuning range. This wavelength dependence, coupled with the quadratic dependence of the two-photon signal upon the instantaneous power of the laser, precludes simple average power correction of nonlinear spectral band shapes. Here, we investigate the key properties of the titanium:sapphire laser as an excitation source for two-photon spectroscopy. We also identify a chemical reference suitable for obtaining source-corrected excitation spectra in the near-infrared using a double-beam, ratiometric approach; this is based on a source-independent two-photon excitation spectrum for the laser dye coumarin-480 that has been obtained with a single-frequency titanium:sapphire laser. From these data, correction factors are generated for correction of multimode source data. {copyright} {ital 1997} {ital Society for Applied Spectroscopy}

  16. Pseudopotential calculations and photothermal lensing measurements of two-photon absorption in solids

    SciTech Connect

    White, W.T. III

    1985-11-04

    We have studied two-photon absorption in solids theoretically and experimentally. We have shown that it is possible to use accurate band structure techniques to compute two-photon absorption spectra within 15% of measured values in a wide band-gap material, ZnS. The empirical pseudopotential technique that we used is significantly more accurate than previous models of two-photon absorption in zinc blende materials, including present tunneling theories (which are essentially parabolic-band results in disguise) and the nonparabolic-band formalism of Pidgeon et al. and Weiler. The agreement between our predictions and previous measurements allowed us to use ZnS as a reference material in order to validate a technique for measuring two-photon absorption that was previously untried in solids, pulsed dual-beam thermal lensing. With the validated technique, we examined nonlinear absorption in one other crystal (rutile) and in several glasses, including silicates, borosilicates, and one phosphate glass. Initially, we believed that the absorption edges of all the materials were comparable; however, subsequent evidence suggested that the effective band-gap energies of the glasses were above the energy of two photons in our measurement. Therefore, we attribute the nonlinear absorption that we observed in glasses to impurities or defects. The measured nonlinear absorption coefficients were of the order of a few cm/TW in the glasses and of the order of 10 cm/GW in the crystals, four orders of magnitude higher than in glasses. 292 refs.

  17. A multidimensional screening method for the selection of two-photon enhanced fluorescent proteins

    NASA Astrophysics Data System (ADS)

    Stoltzfus, Caleb; Barnett, Lauren; Rebane, Aleksander; Hughes, Thomas; Drobizhev, Mikhail; Wicks, Geoffrey; Mikhailov, Alexandr

    2014-03-01

    Two-photon excitation of fluorescent proteins (FPs) is widely used in imaging whole organisms or living tissues. Many different FPs are now available but these proteins have only been optimized for their one-photon properties. We have developed a technique for screening entire libraries of E. coli colonies expressing FPs that utilizes multiple wavelengths of linear excitation as well as two-photon excitation. Single mutations in a particular protein that affect one or twophoton properties are easily identified, providing new views of structure/function relationships. An amplified femtosecond Ti:sapphire laser and a spectrally filtered lamp source are used to acquire the fluorescence signals of up to ~1000 E. coli colonies on a standard Petri dish. Automation of the analysis and acquisition of the fluorescent signals makes it feasible to rapidly screen tens of thousands of colonies. In a proof of principle experiment with the commonly used EGFP, we used two rounds of error prone PCR and selection to evolve new proteins with shifted absorption and increased two-photon cross sections at 790nm. This method of screening, coupled with careful measurements of photo bleaching dynamics and two-photon cross sections, should make it possible to optimize a wide variety of fluorescent proteins and biosensors for use in two-photon microscopes.

  18. A theoretical investigation of two typical two-photon pH fluorescent probes.

    PubMed

    Xu, Zhong; Ren, Ai-Min; Guo, Jing-Fu; Liu, Xiao-Ting; Huang, Shuang; Feng, Ji-Kang

    2013-01-01

    Intracellular pH plays an important role in many cellular events, such as cell growth, endocytosis, cell adhesion and so on. Some pH fluorescent probes have been reported, but most of them are one-photon fluorescent probes, studies about two-photon fluorescent probes are very rare. In this work, the geometrical structure, electronic structure and one-photon properties of a series of two-photon pH fluorescent probes have been theoretically studied by using density functional theory (DFT) method. Their two-photon absorption (TPA) properties are calculated using the method of ZINDO/sum-over-states method. Two types of two-photon pH fluorescent probes have been investigated by theoretical methods. The mechanisms of the Photoinduced Charge Transfer (PCT) probes and the Photoinduced Electron Transfer (PET) probes are verified specifically. Some designed strategies of good two-photon pH fluorescent probes are suggested on the basis of the investigated results of two mechanisms. For the PCT probes, substituting a stronger electron-donating group for the terminal methoxyl group is an advisable choice to increase the TPA cross section. For the PET probes, the TPA cross sections increase upon protonation.

  19. Construction of a two-photon microscope and optimisation of illumination pulse duration.

    PubMed

    Soeller, C; Cannell, M B

    1996-07-01

    The construction of a two-photon/confocal microscope system is described in detail. For two-photon illumination, a Ti:sapphire modelocked laser generating 62-fs pulses at 715 nm was used. The effect of the optical train on illumination pulse width was examined and the observed increase in pulse duration was almost completely removed by the addition/adjustment of a prism compressor system. The imaging capabilities of the two-photon microscope are demonstrated and it is shown that the imaging performance of the two-photon microscope is similar to that of a conventional confocal microscope. With two-photon illumination, the resolution (full width at half-maximum intensity) was 0.42 microM (x-y) and 0.81 microM axially, while with single-photon illumination (at 488 nm in the same instrument with a confocal pinhole detector) the resolution was 0.3 microM (x-y) and 0.75 microM axially. The results are discussed with regard to the general problem of femtosecond pulse distortion in an optical system and a simple procedure for optimal pulse restoration is described. PMID:8766017

  20. Water-soluble two-photon absorbing nitrosyl complex for light-activated therapy through nitric oxide release.

    PubMed

    Zheng, Qingdong; Bonoiu, Adela; Ohulchanskyy, Tymish Y; He, Guang S; Prasad, Paras N

    2008-01-01

    A water-soluble nitrosyl complex with large two-photon absorption was synthesized by incorporating a two-photon absorbing chromophore with tetra(ethylene glycol) units, into the Roussin's red salt. The nitrosyl complex exhibits quenched emission due to energy transfer from the two-photon chromophore to the Roussin's red salt. The nitric oxide (NO) release induced by one- or two-photon irradiation was detected by EPR spectroscopy with a chemical probe, the Fe(II)- N-(dithiocarbamoyl)- N-methyl- d-glucamine (Fe-MGD) complex. Increased one- or two-photon excited fluorescence, with a concomitant photochemical release of NO, was observed upon one- or two-photon light irradiation. With the observed light-dependent cytotoxicity against cancer cells of the water-soluble nitrosyl complex, it was demonstrated that two-photon-functionalized nitrosyl complexes can be effective NO donors for light-activated treatment.

  1. Multiphoton ionization spectra of radical products in the F(2P)+ketene system: Spectral assignments and formation reaction for CH2F, observation of CF and CH

    NASA Astrophysics Data System (ADS)

    Hudgens, Jeffrey W.; Dulcey, C. S.; Long, George R.; Bogan, Denis J.

    1987-10-01

    The reactions of F(2P)+ketene and F(2P)+ketene-d2 were studied in a flow reactor. Spectra of the radical products CH2F, CD2F, CH, CF, and atomic carbon were detected between 292-395 nm by resonance enhanced multiphoton ionization (REMPI) mass spectrometry. Fluoromethyl radicals were identified as a major product of the F+ketene elementary reaction. REMPI spectra of fluoromethyl radicals originated from two-photon preparation of 3p, 4p, and 5p Rydberg states (quantum defect ˜0.6). Absorption of a third laser photon ionized the radicals, a 2+1 REMPI mechanism. Rydberg band origins were observed in CH2F at ν00=52 863, 63 275, and 67 265 cm-1 and in CD2F at ν00=52 786, 63 195, and 67 186 cm-1. A normal mode analysis revealed the vibrational frequencies of the C-F stretch, CH2 scissors, and out-of-plane bending modes in the Rydberg states. The ground state out-of-plane bending frequency in CH2F is 260(30) cm-1 and in CD2F it is 170(30) cm-1. CH radicals were generated by the photolysis of ketene and observed at ˜311 nm by two-photon excitation through the D 2Π(v'=2) ←←X 2Πr band. The reaction mechanism that generated the CF radicals was not determined. The REMPI CF radical spectrum generated by a 2+1 photon mechanism appeared as a series of bandheads described by the constants ν00=˜52 572 cm-1, ωe =1820 cm-1, and ωexe =-18.2 cm-1.

  2. Evaluation of the exothermicity of the chemi-ionization reaction Sm + O → SmO{sup +} + e{sup −}

    SciTech Connect

    Cox, Richard M; Kim, JungSoo; Armentrout, P. B. E-mail: mheaven@emory.edu; Bartlett, Joshua; VanGundy, Robert A.; Heaven, Michael C. E-mail: mheaven@emory.edu; Ard, Shaun G.; Shuman, Nicholas S.; Viggiano, Albert A. E-mail: mheaven@emory.edu; Melko, Joshua J.

    2015-04-07

    The exothermicity of the chemi-ionization reaction Sm + O → SmO{sup +} + e{sup −} has been re-evaluated through the combination of several experimental methods. The thermal reactivity (300–650 K) of Sm{sup +} and SmO{sup +} with a range of species measured using a selected ion flow tube-mass spectrometer apparatus is reported and provides limits for the bond strength of SmO{sup +}, 5.661 eV ≤ D{sub 0}(Sm{sup +}-O) ≤ 6.500 eV. A more precise value is measured to be 5.72{sub 5} ± 0.07 eV, bracketed by the observed reactivity of Sm{sup +} and SmO{sup +} with several species using a guided ion beam tandem mass spectrometer (GIBMS). Combined with the established Sm ionization energy (IE), this value indicates an exothermicity of the title reaction of 0.08 ± 0.07 eV, ∼0.2 eV smaller than previous determinations. In addition, the ionization energy of SmO has been measured by resonantly enhanced two-photon ionization and pulsed-field ionization zero kinetic energy photoelectron spectroscopy to be 5.7427 ± 0.0006 eV, significantly higher than the literature value. Combined with literature bond energies of SmO, this value indicates an exothermicity of the title reaction of 0.14 ± 0.17 eV, independent from and in agreement with the GIBMS result presented here. The evaluated thermochemistry also suggests that D{sub 0}(SmO) = 5.83 ± 0.07 eV, consistent with but more precise than the literature values. Implications of these results for interpretation of chemical release experiments in the thermosphere are discussed.

  3. Two-Photon Frequency Comb Excitation of Rubidium Atoms in External Magnetic Field

    NASA Astrophysics Data System (ADS)

    Vujičić, N.; Ban, T.; Skenderović, H.; Vdović, S.; Pichler, G.

    2008-10-01

    In the present experiment the 5S-5D two-photon transitions in 85Rb and 87Rb atoms as a result of the interaction of the femtosecond frequency comb with atomic levels of both rubidium isotopes are investigated. The main problem in studying of two-photon transitions is in optimization of the excitation efficiency of the desired state. There are two general cases: those transition with an intermediate resonance those in which the pulse spectrum is far detuned from an intermediate resonance. In order to investigate the dependence of the two-photon fluorescence signal as a result of interaction of the frequency comb with perturbed energy-level pattern an external magnetic field was applied.

  4. Two-Color, Two-Photon Imaging at Long Excitation Wavelengths Using a Diamond Raman Laser.

    PubMed

    Trägårdh, Johanna; Murtagh, Michelle; Robb, Gillian; Parsons, Maddy; Lin, Jipeng; Spence, David J; McConnell, Gail

    2016-08-01

    We demonstrate that the second-Stokes output from a diamond Raman laser, pumped by a femtosecond Ti:Sapphire laser, can be used to efficiently excite red-emitting dyes by two-photon excitation at 1,080 nm and beyond. We image HeLa cells expressing red fluorescent protein, as well as dyes such as Texas Red and Mitotracker Red. We demonstrate the potential for simultaneous two-color, two-photon imaging with this laser by using the residual pump beam for excitation of a green-emitting dye. We demonstrate this for the combination of Alexa Fluor 488 and Alexa Fluor 568. Because the Raman laser extends the wavelength range of the Ti:Sapphire laser, resulting in a laser system tunable to 680-1,200 nm, it can be used for two-photon excitation of a large variety and combination of dyes. PMID:27492283

  5. 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. PMID:26258885

  6. Two-photon imaging of spatially extended neuronal network dynamics with high temporal resolution

    PubMed Central

    Lillis, Kyle P.; Eng, Alfred; White, John A.; Mertz, Jerome

    2008-01-01

    We describe a simple two-photon fluorescence imaging strategy, called targeted path scanning (TPS), to monitor the dynamics of spatially extended neuronal networks with high spatiotemporal resolution. Our strategy combines the advantages of mirror-based scanning, minimized dead time, ease of implementation, and compatibility with high-resolution low-magnification objectives. To demonstrate the performance of TPS, we monitor the calcium dynamics distributed across an entire juvenile rat hippocampus (>1.5mm), at scan rates of 100Hz, with single cell resolution and single action potential sensitivity. Our strategy for fast, efficient two-photon microscopy over spatially extended regions provides a particularly attractive solution for monitoring neuronal population activity in thick tissue, without sacrificing the signal to noise ratio or high spatial resolution associated with standard two-photon microscopy. Finally, we provide the code to make our technique generally available. PMID:18539336

  7. Visible-wavelength two-photon excitation microscopy for fluorescent protein imaging

    NASA Astrophysics Data System (ADS)

    Yamanaka, Masahito; Saito, Kenta; Smith, Nicholas I.; Arai, Yoshiyuki; Uegaki, Kumiko; Yonemaru, Yasuo; Mochizuki, Kentaro; Kawata, Satoshi; Nagai, Takeharu; Fujita, Katsumasa

    2015-10-01

    The simultaneous observation of multiple fluorescent proteins (FPs) by optical microscopy is revealing mechanisms by which proteins and organelles control a variety of cellular functions. Here we show the use of visible-light based two-photon excitation for simultaneously imaging multiple FPs. We demonstrated that multiple fluorescent targets can be concurrently excited by the absorption of two photons from the visible wavelength range and can be applied in multicolor fluorescence imaging. The technique also allows simultaneous single-photon excitation to offer simultaneous excitation of FPs across the entire range of visible wavelengths from a single excitation source. The calculation of point spread functions shows that the visible-wavelength two-photon excitation provides the fundamental improvement of spatial resolution compared to conventional confocal microscopy.

  8. 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.

  9. Images of photoreceptors in living primate eyes using adaptive optics two-photon ophthalmoscopy

    PubMed Central

    Hunter, Jennifer J.; Masella, Benjamin; Dubra, Alfredo; Sharma, Robin; Yin, Lu; Merigan, William H.; Palczewska, Grazyna; Palczewski, Krzysztof; Williams, David R.

    2011-01-01

    In vivo two-photon imaging through the pupil of the primate eye has the potential to become a useful tool for functional imaging of the retina. Two-photon excited fluorescence images of the macaque cone mosaic were obtained using a fluorescence adaptive optics scanning laser ophthalmoscope, overcoming the challenges of a low numerical aperture, imperfect optics of the eye, high required light levels, and eye motion. Although the specific fluorophores are as yet unknown, strong in vivo intrinsic fluorescence allowed images of the cone mosaic. Imaging intact ex vivo retina revealed that the strongest two-photon excited fluorescence signal comes from the cone inner segments. The fluorescence response increased following light stimulation, which could provide a functional measure of the effects of light on photoreceptors. PMID:21326644

  10. Enhanced-locality fiber-optic two-photon-fluorescence live-brain interrogation

    SciTech Connect

    Fedotov, I. V.; Doronina-Amitonova, L. V.; Sidorov-Biryukov, D. A.; Fedotov, A. B.; Anokhin, K. V.; Kilin, S. Ya.; Sakoda, K.; Zheltikov, A. M.

    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.

  11. Up-conversion dynamics for temporally entangled two-photon pulses

    SciTech Connect

    Nakatani, Masatoshi; Shimizu, Ryosuke; Koshino, Kazuki

    2011-01-15

    We analyze the up conversion of a two-photon pulse having temporal entanglement on the basis of a full quantum formalism that treats both photons and optical media quantum mechanically. We derive a formula of the up-converted photon wave function, which is applicable to arbitrary input two-photon states for a three-level system, as the simplest second-order nonlinear optical system. As the input, we employ three kinds of temporally entangled two-photon pulses: correlated, uncorrelated, and anticorrelated. We observe the up-conversion efficiency and the temporal profile of the up-converted photon. Our results reveal the crossover behavior of the up conversion from anticorrelation to correlation and show how the temporal correlation in the input is reflected in the up-conversion process.

  12. Two-photon polymerization with variable repetition rate bursts of femtosecond laser pulses.

    PubMed

    Baldacchini, Tommaso; Snider, Scott; Zadoyan, Ruben

    2012-12-31

    We describe fabrication of microstructures by two-photon polymerization using bursts of femtosecond laser pulses. With the aid of an acousto-optic modulator driven by a function generator, two-photon polymerization is performed at variable burst repetition rates. We investigate how the time between the bursts of laser pulses influences the ultimate dimensions of lines written in a photosensitive resin. We observe that when using the same laser fluence, polymer lines fabricated at different burst repetition rates have different dimensions. In particular, the widths of two-photon polymerized lines become smaller with decreasing burst repetition rates. Based on the thermal properties of the resin and experimental writing conditions, we attribute this effect to localized heat accumulation. PMID:23388815

  13. 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.

  14. Fluorogenic, two-photon-triggered photoclick chemistry in live mammalian cells.

    PubMed

    Yu, Zhipeng; Ohulchanskyy, Tymish Y; An, Peng; Prasad, Paras N; Lin, Qing

    2013-11-13

    The tetrazole-based photoclick chemistry has provided a powerful tool to image proteins in live cells. To extend photoclick chemistry to living organisms with improved spatiotemporal control, here we report the design of naphthalene-based tetrazoles that can be efficiently activated by two-photon excitation with a 700 nm femtosecond pulsed laser. A water-soluble, cell-permeable naphthalene-based tetrazole was identified that reacts with acrylamide with the effective two-photon cross-section for the cycloaddition reaction determined to be 3.8 GM. Furthermore, the use of this naphthalene-tetrazole for real-time, spatially controlled imaging of microtubules in live mammalian cells via the fluorogenic, two-photon-triggered photoclick chemistry was demonstrated.

  15. Quantum random walk of two photons in separable and entangled states

    SciTech Connect

    Pathak, P. K.; Agarwal, G. S.

    2007-03-15

    We discuss quantum random walk of two photons using linear optical elements. We analyze the quantum random walk using photons in a variety of quantum states including entangled states. We find that for photons initially in separable Fock states, the final state is entangled. For polarization entangled photons produced by type-II downconverter, we calculate the joint probability of detecting two photons at a given site. We show the remarkable dependence of the two photon detection probability on the quantum nature of the state. In order to understand the quantum random walk, we present exact analytical results for small number of steps such as five. We present in detail numerical results for a number of cases and supplement the numerical results with asymptotic analytical results.

  16. Stimulated Rayleigh-Bragg scattering in two-photon absorbing media

    SciTech Connect

    He, Guang S.; Lu Changgui; Zheng Qingdong; Prasad, Paras N.; Zerom, Petros; Boyd, Robert W.; Samoc, Marek

    2005-06-15

    The origin and mechanism of backward stimulated Rayleigh scattering in two-photon absorbing media are studied theoretically and experimentally. This type of stimulated scattering has the unusual features of no frequency shift and low pump threshold requirement compared to all other known stimulated scattering effects. This frequency-unshifted stimulated Rayleigh scattering effect can be well explained by a two-photon-excitation-enhanced Bragg grating reflection model. The reflection of the forward pump beam from this stationary Bragg grating may substantially enhance the backward Rayleigh scattering beam, providing a positive feedback mechanism without causing any frequency shift. A two-counterpropagating-beam-formed grating experiment in a two-photon absorbing dye solution is conducted. The measured dynamic behavior of Bragg grating formation and reflectivity properties are basically consistent with the predictions from the proposed model.

  17. Source-corrected two-photon excited fluorescence measurements between 700 and 880 nm

    SciTech Connect

    Fisher, W.G.; Wachter, E.A.; Lytle, F.E.; Armas, M.; Seaton, C.

    1998-04-01

    Passively mode-locked titanium:sapphire (Ti:S) lasers are capable of generating a high-frequency train of transform-limited subpico-second pulses, producing peak powers near 10{sup 5}thinspW at moderate average powers. The low energy per pulse ({lt}20 nJ) permits low fluence levels to be maintained in tightly focused beams, reducing the possibility of saturating fluorescence transitions. These properties, combined with a wavelength tunability from approximately 700 nm to 1 {mu}m, provide excellent opportunities for studying simultaneous two-photon excitation (TPE). However, pulse formation is very sensitive to a variety of intracavity parameters, including group velocity dispersion compensation, which leads to wavelength-dependent pulse profiles as the wavelength is scanned. This wavelength dependence can seriously distort band shapes and apparent peak heights during collection of two-photon spectral data. Since two-photon excited fluorescence is proportional to the product of the peak and average powers, it is not possible to obtain source-independent spectra by using average power correction schemes alone. Continuous-wave, single-mode lasers can be used to generate source-independent two-photon data, but these sources are four to five orders of magnitude less efficient than the mode-locked Ti:S laser and are not practical for general two-photon measurements. Hence, a continuous-wave, single-mode Ti:S laser has been used to collect a source-independent excitation spectrum for the laser dye Coumarin 480. This spectrum may be used to correct data collected with multimode sources; this possibility is demonstrated by using a simple ratiometric method to collect accurate TPE spectra with the mode-locked Ti:S laser. An approximate value of the two-photon cross section for Coumarin 480 is also given. {copyright} {ital 1998} {ital Society for Applied Spectroscopy}

  18. Ruthenium(II) polypyridyl complexes as mitochondria-targeted two-photon photodynamic anticancer agents.

    PubMed

    Liu, Jiangping; Chen, Yu; Li, Guanying; Zhang, Pingyu; Jin, Chengzhi; Zeng, Leli; Ji, Liangnian; Chao, Hui

    2015-07-01

    Clinical acceptance of photodynamic therapy is currently hindered by poor depth efficacy and inefficient activation of the cell death machinery in cancer cells during treatment. To address these issues, photoactivation using two-photon absorption (TPA) is currently being examined. Mitochondria-targeted therapy represents a promising approach to target tumors selectively and may overcome the resistance in current anticancer therapies. Herein, four ruthenium(II) polypyridyl complexes (RuL1-RuL4) have been designed and developed to act as mitochondria-targeted two-photon photodynamic anticancer agents. These complexes exhibit very high singlet oxygen quantum yields in methanol (0.74-0.81), significant TPA cross sections (124-198 GM), remarkable mitochondrial accumulation, and deep penetration depth. Thus, RuL1-RuL4 were utilized as one-photon and two-photon absorbing photosensitizers in both monolayer cells and 3D multicellular spheroids (MCSs). These Ru(II) complexes were almost nontoxic towards cells and 3D MCSs in the dark and generate sufficient singlet oxygen under one- and two-photon irradiation to trigger cell death. Remarkably, RuL4 exhibited an IC50 value as low as 9.6 μM in one-photon PDT (λirr = 450 nm, 12 J cm(-2)) and 1.9 μM in two-photon PDT (λirr = 830 nm, 800 J cm(-2)) of 3D MCSs; moreover, RuL4 is an order of magnitude more toxic than cisplatin in the latter test system. The combination of mitochondria-targeting and two-photon activation provides a valuable paradigm to develop ruthenium(II) complexes for PDT applications.

  19. Activation of porphyrin photosensitizers by semiconductor quantum dots via two-photon excitation

    SciTech Connect

    Wen Yanan; Song Weisi; Liu Yuqiang; Wang Yinghui; Yang Yanqiang; An Limin

    2009-10-05

    Energy transfer from water-soluble quantum dots (QDs) to porphyrinlike sensitizers is studied by time-resolved spectroscopy of two-photon excitation with femtosecond laser pulses. Evident transfer results are observed. Electron exchange is found to be the dominant transfer mechanism. Relative intensity change between excitonic and trapping emission implies that nonradiative energy transfer occurs through the trapping state of QDs, which presents a way of raising energy transfer efficiency in this type of donor-acceptor pairs. This study underlines the potential of QD-porphyrin model system for applications in two-photon excitation photodynamic therapy.

  20. 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. PMID:27446677

  1. Two-photon fluorescence properties of curcumin as a biocompatible marker for confocal imaging

    NASA Astrophysics Data System (ADS)

    Kumar, Abhishek; Li, Lian; Chaturvedi, Akanksha; Brzostowski, Joseph; Chittigori, Joshna; Pierce, Susan; Samuelson, Lynne A.; Sandman, Daniel; Kumar, Jayant

    2012-05-01

    Two-photon (TP) fluorescence properties of an antioxidant and anti-tumor molecule, curcumin, were investigated. The two-photon absorption (TPA) action cross-section was measured in organic solvents and found to be 6 GM in tetrahydrofuran and 2 GM in dimethyl sulfoxide. The measured TPA cross-section is comparable to that of rhodamine 6G. One-photon and TP confocal microscopy has demonstrated that curcumin is internalized in cells and can be used for imaging applications. Our investigation indicates that curcumin is a viable biocompatible TP fluorescent marker.

  2. Repair of the (6-4) photoproduct by DNA photolyase requires two photons.

    PubMed

    Yamamoto, Junpei; Martin, Ryan; Iwai, Shigenori; Plaza, Pascal; Brettel, Klaus

    2013-07-15

    It takes two (photons) to tango: Single-turnover flash experiments showed that the flavoenzyme (6-4) photolyase uses a successive two-photon mechanism to repair the UV-induced T(6-4)T lesion in DNA (see picture). The intermediate (X) formed by the first photoreaction is likely to be the oxetane-bridged dimer T(ox)T. The enzyme could stabilize the normally short-lived T(ox)T, allowing repair to be completed by the second photoreaction. PMID:23761226

  3. Measurement of Electron Beam Polarization from Unstrained Bulk GaAs via Two Photon Photoemission

    SciTech Connect

    J L McCarter, T J Gay, J Hansknecht, M Poelker, M L Stutzman

    2011-06-01

    This paper describes measurements of the beam polarization and quantum efficiency for photoemission using two-photon excitation from unstrained bulk GaAs illuminated with pulsed, high intensity 1560nm laser light. Quantum efficiency is linearly proportional to 1560nm peak laser intensity, which was varied in three independent ways, indicating that the emitted electrons are promoted from the valence to the conduction band via two-photon absorption. Beam polarization was measured using a microMott polarimeter, with a value of 16.8(4)% polarization at 1560nm, which is roughly half the measured value of 33.4(8)% using 778 nm light.

  4. TWO-PHOTON TISSUE IMAGING: SEEING THE IMMUNE SYSTEM IN A FRESH LIGHT

    PubMed Central

    Cahalan, Michael D.; Parker, Ian; Wei, Sindy H.; Miller, Mark J.

    2009-01-01

    Many lymphocyte functions, such as antigen recognition, take place deep in densely populated lymphoid organs. Because direct in vivo observation was not possible, the dynamics of immune-cell interactions have been inferred or extrapolated from in vitro studies. Two-photon fluorescence excitation uses extremely brief (<1 picosecond) and intense pulses of light to ‘see’ directly into living tissues, to a greater depth and with less phototoxicity than conventional imaging methods. Two-photon microscopy, in combination with newly developed indicator molecules, promises to extend single-cell approaches to the in vivo setting and to reveal in detail the cellular collaborations that underlie the immune response. PMID:12415310

  5. Non-degenerate two photon absorption enhancement for laser dyes by precise lock-in detection

    SciTech Connect

    Xue, B.; Katan, C.; Bjorgaard, J. A.; Kobayashi, T.

    2015-12-15

    This study demonstrates a measurement system for a non-degenerate two-photon absorption (NDTPA) spectrum. The NDTPA light sources are a white light super continuum beam (WLSC, 500 ∼ 720 nm) and a fundamental beam (798 nm) from a Ti:Sapphire laser. A reliable broadband NDTPA spectrum is acquired in a single-shot detection procedure using a 128-channel lock-in amplifier. The NDTPA spectra for several common laser dyes are measured. Two photon absorption cross section enhancements are found in the experiment and validated by theoretical calculation for all of the chromophores.

  6. Two-photon excitation of atoms by ultrashort electromagnetic pulses in a discrete spectrum

    NASA Astrophysics Data System (ADS)

    Astapenko, V. A.; Sakhno, S. V.

    2016-07-01

    The paper is devoted to the theoretical investigation of two-photon excitation of atom in a discrete energy spectrum by ultrashort electromagnetic pulses of femto- and subfemtosecond ranges of durations. An analytical expression for the total probability of the process is derived. Numerical simulations are made for hydrogen and sodium atoms. It is shown that the total probability of the process is nonlinear function of pulse duration and character of this function depends strongly on the frequency detuning of pulse carrier frequency from two-photon resonance.

  7. 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.

  8. Photon structure functions and azimuthal asymmetries in two-photon processes

    SciTech Connect

    Higuchi, A.; Matsuda, S.; Kodaira, J.

    1981-09-01

    Based on the recently developed framework of Curci, Furmanski, and Petronzio, we derive the photon structure functions in quantum chromodynamics (QCD). Then we perform QCD calculations for the azimuthal asymmetries of jets in two-photon processes. We find that in contrast to the case of lepton-hadron scatterings, the deep-inelastic e/sup +/e/sup -/ reaction via two-photon exchange is expected to show cleaner signatures for the azimuthal asymmetries as a result of enhanced QCD effects. We suggest that these will serve as useful tests of QCD.

  9. Teleportation of entangled states without Bell-state measurement via a two-photon process

    NASA Astrophysics Data System (ADS)

    dSouza, A. D.; Cardoso, W. B.; Avelar, A. T.; Baseia, B.

    2011-02-01

    In this letter we propose a scheme using a two-photon process to teleport an entangled field state of a bimodal cavity to another one without Bell-state measurement. The quantum information is stored in a zero- and two-photon entangled state. This scheme requires two three-level atoms in a ladder configuration, two bimodal cavities, and selective atomic detectors. The fidelity and success probability do not depend on the coefficients of the state to be teleported. For convenient choices of interaction times, the teleportation occurs with fidelity close to the unity.

  10. Demonstration of a programmable source of two-photon multiqubit entangled states

    SciTech Connect

    Cialdi, Simone; Brivio, Davide; Paris, Matteo G. A.

    2010-04-15

    We suggest and demonstrate a novel source of two-photon multipartite entangled states which exploits the transverse spatial structure of spontaneous parametric down-conversion together with a programmable spatial light modulator (SLM). The one-dimensional SLM is used to perform polarization entanglement purification and to realize arbitrary phase gates between polarization and momentum degrees of freedom of photons. We experimentally demonstrate our scheme by generating two-photon three-qubit linear cluster states with high fidelity using a diode laser pump with a limited coherence time and power on the crystal as low as {approx}2.5 mW.

  11. Non-degenerate two photon absorption enhancement for laser dyes by precise lock-in detection

    NASA Astrophysics Data System (ADS)

    Xue, B.; Katan, C.; Bjorgaard, J. A.; Kobayashi, T.

    2015-12-01

    This study demonstrates a measurement system for a non-degenerate two-photon absorption (NDTPA) spectrum. The NDTPA light sources are a white light super continuum beam (WLSC, 500 ˜ 720 nm) and a fundamental beam (798 nm) from a Ti:Sapphire laser. A reliable broadband NDTPA spectrum is acquired in a single-shot detection procedure using a 128-channel lock-in amplifier. The NDTPA spectra for several common laser dyes are measured. Two photon absorption cross section enhancements are found in the experiment and validated by theoretical calculation for all of the chromophores.

  12. 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

  13. Insights into esophagus tissue architecture using two-photon confocal microscopy

    NASA Astrophysics Data System (ADS)

    Liu, Nenrong; Wang, Yue; Feng, Shangyuan; Chen, Rong

    2013-08-01

    In this paper, microstructures of human esophageal mucosa were evaluated using the two-photon laser scanning confocal microscopy (TPLSCM), based on two-photon excited fluorescence (TPEF) and second harmonic generation (SHG). The distribution of epithelial cells, muscle fibers of muscularis mucosae has been distinctly obtained. Furthermore, esophageal submucosa characteristics with cancer cells invading into were detected. The variation of collagen, elastin and cancer cells is very relevant to the pathology in esophagus, especially early esophageal cancer. Our experimental results indicate that the MPM technique has the much more advantages for label-free imaging, and has the potential application in vivo in the clinical diagnosis and monitoring of early esophageal cancer.

  14. 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.

  15. Plasmon-coupled gold nanospheres for two-photon imaging and photoantibacterial activity.

    PubMed

    Yuan, Peiyan; Ding, Xin; Guan, Zhenping; Gao, Nengyue; Ma, Rizhao; Jiang, Xiao-Fang; Yang, Yi Yan; Xu, Qing-Hua

    2015-04-01

    Positively charged Au nanospheres are found to form aggregates on the bacterial surface, resulting in significantly enhanced two-photon photoluminescence (TPPL). The enhanced TPPL is successfully utilized to image bacterial cells in the NIR region. In addition, these Au nanospheres effectively eradicate the bacterial cells by laser pulses in the same NIR region due to the photothermal effect.

  16. Rapid Prototyping of Chemical Microsensors Based on Molecularly Imprinted Polymers Synthesized by Two-Photon Stereolithography.

    PubMed

    Gomez, Laura Piedad Chia; Spangenberg, Arnaud; Ton, Xuan-Anh; Fuchs, Yannick; Bokeloh, Frank; Malval, Jean-Pierre; Tse Sum Bui, Bernadette; Thuau, Damien; Ayela, Cédric; Haupt, Karsten; Soppera, Olivier

    2016-07-01

    Two-photon stereolithography is used for rapid prototyping of submicrometre molecularly imprinted polymer-based 3D structures. The structures are evaluated as chemical sensing elements and their specific recognition properties for target molecules are confirmed. The 3D design capability is exploited and highlighted through the fabrication of an all-organic molecularly imprinted polymeric microelectromechanical sensor.

  17. New long-wave and highly efficient two-photon fluorophores for multiphoton microscopy

    NASA Astrophysics Data System (ADS)

    Gvishi, Raz; Berkovic, Garry; Kotler, Zvi; Krief, P.; Becker, J. Y.; Khodorkovsky, Vladimir

    2001-04-01

    An important ingredient in improving Multi Photon Laser Scanning Microscopy, MPLSM, is the development of efficient exogenous two-photon fluorescent (TPF) probes. Here we report on a new class of two-photon fluorophores, specifically designed in order to maximize their efficiency in potential MPLSM applications. The fluorophores possess a symmetric Donor-Acceptor-Donor (D-n-A-n-D) structure with varying conjugation length and have strong donors and acceptors. We have studied the two-photon excitation (TPE) properties of these fluorophores and found the following properties: (1) Very large two-photon absorption coefficients (6 > 1000 GM); (2) Peak TP excitation wavelength which are strongly shifted to the red ((lambda) 1 micrometer); (3) Large fluorescence quantum efficiency; (4) Large Stokes shifts of the fluorescence bands. These properties make them particularly suitable for imaging thicker samples, relying on the large improvement in TPE cross-sections and the reduced attenuation at both the excitation and emission wavelengths. We also describe TPE fluorescence anisotropy experiments revealing the tensorial shape of the fluorophores.

  18. Phosphorescent probes for two-photon microscopy of oxygen (Conference Presentation)

    NASA Astrophysics Data System (ADS)

    Vinogradov, Sergei A.; Esipova, Tatiana V.

    2016-03-01

    The ability to quantify oxygen in vivo in 3D with high spatial and temporal resolution is much needed in many areas of biological research. Our laboratory has been developing the phosphorescence quenching technique for biological oximetry - an optical method that possesses intrinsic microscopic capability. In the past we have developed dendritically protected oxygen probes for quantitative imaging of oxygen in tissue. More recently we expanded our design on special two-photon enhanced phosphorescent probes. These molecules brought about first demonstrations of the two-photon phosphorescence lifetime microscopy (2PLM) of oxygen in vivo, providing new information for neouroscience and stem cell biology. However, current two-photon oxygen probes suffer from a number of limitations, such as sub-optimal brightness and high cost of synthesis, which dramatically reduce imaging performance and limit usability of the method. In this paper we discuss principles of 2PLM and address the interplay between the probe chemistry, photophysics and spatial and temporal imaging resolution. We then present a new approach to brightly phosphorescent chromophores with internally enhanced two-photon absorption cross-sections, which pave a way to a new generation of 2PLM probes.

  19. In Vivo Two-Photon Fluorescence Kinetics of Primate Rods and Cones

    PubMed Central

    Sharma, Robin; Schwarz, Christina; Williams, David R.; Palczewska, Grazyna; Palczewski, Krzysztof; Hunter, Jennifer J.

    2016-01-01

    Purpose The retinoid cycle maintains vision by regenerating bleached visual pigment through metabolic events, the kinetics of which have been difficult to characterize in vivo. Two-photon fluorescence excitation has been used previously to track autofluorescence directly from retinoids and pyridines in the visual cycle in mouse and frog retinas, but the mechanisms of the retinoid cycle are not well understood in primates. Methods We developed a two-photon fluorescence adaptive optics scanning light ophthalmoscope dedicated to in vivo imaging in anesthetized macaques. Using pulsed light at 730 nm, two-photon fluorescence was captured from rods and cones during light and dark adaptation through the eye's pupil. Results The fluorescence from rods and cones increased with light exposure but at different rates. During dark adaptation, autofluorescence declined, with cone autofluorescence decreasing approximately 4 times faster than from rods. Rates of autofluorescence decrease in rods and cones were approximately 4 times faster than their respective rates of photopigment regeneration. Also, subsets of sparsely distributed cones were less fluorescent than their neighbors immediately following bleach at 565 nm and they were comparable with the S cone mosaic in density and distribution. Conclusions Although other molecules could be contributing, we posit that these fluorescence changes are mediated by products of the retinoid cycle. In vivo two-photon ophthalmoscopy provides a way to monitor noninvasively stages of the retinoid cycle that were previously inaccessible in the living primate eye. This can be used to assess objectively photoreceptor function in normal and diseased retinas. PMID:26903225

  20. Two-photon photoemission from a copper cathode in an X -band photoinjector

    NASA Astrophysics Data System (ADS)

    Li, H.; Limborg-Deprey, C.; Adolphsen, C.; McCormick, D.; Dunning, M.; Jobe, K.; Raubenheimer, T.; Vrielink, A.; Vecchione, T.; Wang, F.; Weathersby, S.

    2016-02-01

    This paper presents two-photon photoemission from a copper cathode in an X -band photoinjector. We experimentally verified that the electron bunch charge from photoemission out of a copper cathode scales with laser intensity (I) square for 400 nm wavelength photons. We compare this two-photon photoemission process with the single photon process at 266 nm. Despite the high reflectivity (R ) of the copper surface for 400 nm photons (R =0.48 ) and higher thermal energy of photoelectrons (two-photon at 200 nm) compared to 266 nm photoelectrons, the quantum efficiency of the two-photon photoemission process (400 nm) exceeds the single-photon process (266 nm) when the incident laser intensity is above 300 GW /cm2 . At the same laser pulse energy (E ) and other experimental conditions, emitted charge scales inversely with the laser pulse duration. A thermal emittance of 2.7 mm-mrad per mm root mean square (rms) was measured on our cathode which exceeds by sixty percent larger compared to the theoretical predictions, but this discrepancy is similar to previous experimental thermal emittance on copper cathodes with 266 nm photons. The damage of the cathode surface of our first-generation X -band gun from both rf breakdowns and laser impacts mostly explains this result. Using a 400 nm laser can substantially simplify the photoinjector system, and make it an alternative solution for compact pulsed electron sources.

  1. Atomic Dipole Squeezing in the Correlated Two-Mode Two-Photon Jaynes-Cummings Model

    NASA Technical Reports Server (NTRS)

    Dong, Zhengchao; Zhao, Yonglin

    1996-01-01

    In this paper, we study the atomic dipole squeezing in the correlated two-mode two-photon JC model with the field initially in the correlated two-mode SU(1,1) coherent state. The effects of detuning, field intensity and number difference between the two field modes are investigated through numerical calculation.

  2. Rapid Prototyping of Chemical Microsensors Based on Molecularly Imprinted Polymers Synthesized by Two-Photon Stereolithography.

    PubMed

    Gomez, Laura Piedad Chia; Spangenberg, Arnaud; Ton, Xuan-Anh; Fuchs, Yannick; Bokeloh, Frank; Malval, Jean-Pierre; Tse Sum Bui, Bernadette; Thuau, Damien; Ayela, Cédric; Haupt, Karsten; Soppera, Olivier

    2016-07-01

    Two-photon stereolithography is used for rapid prototyping of submicrometre molecularly imprinted polymer-based 3D structures. The structures are evaluated as chemical sensing elements and their specific recognition properties for target molecules are confirmed. The 3D design capability is exploited and highlighted through the fabrication of an all-organic molecularly imprinted polymeric microelectromechanical sensor. PMID:27145145

  3. Dynamics and two-photon absorption properties of chromophore functionalized semiconductor nanoparticles

    NASA Astrophysics Data System (ADS)

    Varaganti, Shankar; Gessesse, Mathias; Obare, Sherine O.; Ramakrishna, Guda

    2009-08-01

    Two photon absorption cross-sections and fluorescence dynamics of Riboflavin, Fluorescein 548, Coumarin 519 and Quinizarin adsorbed onto reactive (TiO2) and non-reactive (ZrO2) semiconductor nanoparticles have been investigated. These dye molecules are chosen because of their inherently different anchoring groups with which they can bind to semiconductor nanoparticles giving a handle to probe the influence of anchoring group as well as molecule-nanoparticle electronic coupling on the two-photon absorption and nonlinear optical properties. Two-photon excited fluorescence technique has been utilized to monitor the two photon absorption cross-sections and the dynamics of singlet states are followed with femto second fluorescence upconversion. Interesting cross-section trends have been observed where the TPA cross-section of chromophore on ZrO2 surface is similar or lower to that of the free dye while the cross-sections seem to be higher on the surface of reactive TiO2 nanoparticle surface. Fluorescence upconversion investigations were able to probe the electronic interactions of the chromophore with semiconductor nanoparticle and also the adsorption of the chromophores on the surface of the nanoparticle.

  4. 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...

  5. Evaluation of two-photon exchange graphs for the helium isoelectronic sequence

    NASA Astrophysics Data System (ADS)

    Sapirstein, J.

    1989-06-01

    Two-photon exchange graph contributions to the ground state energy of two-electron ions are evaluated in Furry picture QED. The natural separation of correlation effects from negative energy state effects is demonstrated. Some of these latter effects are evaluated both analytically and numerically, and shown to contribute at the level (Zα)3 a.u.

  6. Probing carrier lifetimes in photovoltaic materials using subsurface two-photon microscopy

    NASA Astrophysics Data System (ADS)

    Barnard, Edward S.; Hoke, Eric T.; Connor, Stephen T.; Groves, James R.; Kuykendall, Tevye; Yan, Zewu; Samulon, Eric C.; Bourret-Courchesne, Edith D.; Aloni, Shaul; Schuck, P. James; Peters, Craig H.; Hardin, Brian E.

    2013-06-01

    Accurately measuring the bulk minority carrier lifetime is one of the greatest challenges in evaluating photoactive materials used in photovoltaic cells. One-photon time-resolved photoluminescence decay measurements are commonly used to measure lifetimes of direct bandgap materials. However, because the incident photons have energies higher than the bandgap of the semiconductor, most carriers are generated close to the surface, where surface defects cause inaccurate lifetime measurements. Here we show that two-photon absorption permits sub-surface optical excitation, which allows us to decouple surface and bulk recombination processes even in unpassivated samples. Thus with two-photon microscopy we probe the bulk minority carrier lifetime of photovoltaic semiconductors. We demonstrate how the traditional one-photon technique can underestimate the bulk lifetime in a CdTe crystal by 10× and show that two-photon excitation more accurately measures the bulk lifetime. Finally, we generate multi-dimensional spatial maps of optoelectronic properties in the bulk of these materials using two-photon excitation.

  7. Two-photon imaging and spectroscopy of fresh human colon biopsies

    NASA Astrophysics Data System (ADS)

    Cicchi, R.; Sturiale, A.; Nesi, G.; Tonelli, F.; Pavone, F. S.

    2012-03-01

    Two-photon fluorescence (TPEF) microscopy is a powerful tool to image human tissues up to 200 microns depth without any exogenously added probe. TPEF can take advantage of the autofluorescence of molecules intrinsically contained in a biological tissue, as such NADH, elastin, collagen, and flavins. Two-photon microscopy has been already successfully used to image several types of tissues, including skin, muscles, tendons, bladder. Nevertheless, its usefulness in imaging colon tissue has not been deeply investigated yet. In this work we have used combined two-photon excited fluorescence (TPEF), second harmonic generation microscopy (SHG), fluorescence lifetime imaging microscopy (FLIM), and multispectral two-photon emission detection (MTPE) to investigate different kinds of human ex-vivo fresh biopsies of colon. Morphological and spectroscopic analyses allowed to characterize both healthy mucosa, polyp, and colon samples in a good agreement with common routine histology. Even if further analysis, as well as a more significant statistics on a large number of samples would be helpful to discriminate between low, mild, and high grade cancer, our method is a promising tool to be used as diagnostic confirmation of histological results, as well as a diagnostic tool in a multiphoton endoscope or colonoscope to be used in in-vivo imaging applications.

  8. Quantum Authencryption with Two-Photon Entangled States for Off-Line Communicants

    NASA Astrophysics Data System (ADS)

    Ye, Tian-Yu

    2016-02-01

    In this paper, a quantum authencryption protocol is proposed by using the two-photon entangled states as the quantum resource. Two communicants Alice and Bob share two private keys in advance, which determine the generation of two-photon entangled states. The sender Alice sends the two-photon entangled state sequence encoded with her classical bits to the receiver Bob in the manner of one-step quantum transmission. Upon receiving the encoded quantum state sequence, Bob decodes out Alice's classical bits with the two-photon joint measurements and authenticates the integrity of Alice's secret with the help of one-way hash function. The proposed protocol only uses the one-step quantum transmission and needs neither a public discussion nor a trusted third party. As a result, the proposed protocol can be adapted to the case where the receiver is off-line, such as the quantum E-mail systems. Moreover, the proposed protocol provides the message authentication to one bit level with the help of one-way hash function and has an information-theoretical efficiency equal to 100 %.

  9. Two-Photon Autofluorescence Imaging Reveals Cellular Structures Throughout the Retina of the Living Primate Eye

    PubMed Central

    Sharma, Robin; Williams, David R.; Palczewska, Grazyna; Palczewski, Krzysztof; Hunter, Jennifer J.

    2016-01-01

    Purpose Although extrinsic fluorophores can be introduced to label specific cell types in the retina, endogenous fluorophores, such as NAD(P)H, FAD, collagen, and others, are present in all retinal layers. These molecules are a potential source of optical contrast and can enable noninvasive visualization of all cellular layers. We used a two-photon fluorescence adaptive optics scanning light ophthalmoscope (TPF-AOSLO) to explore the native autofluorescence of various cell classes spanning several layers in the unlabeled retina of a living primate eye. Methods Three macaques were imaged on separate occasions using a custom TPF-AOSLO. Two-photon fluorescence was evoked by pulsed light at 730 and 920 nm excitation wavelengths, while fluorescence emission was collected in the visible range from several retinal layers and different locations. Backscattered light was recorded simultaneously in confocal modality and images were postprocessed to remove eye motion. Results All retinal layers yielded two-photon signals and the heterogeneous distribution of fluorophores provided optical contrast. Several structural features were observed, such as autofluorescence from vessel walls, Müller cell processes in the nerve fibers, mosaics of cells in the ganglion cell and other nuclear layers of the inner retina, as well as photoreceptor and RPE layers in the outer retina. Conclusions This in vivo survey of two-photon autofluorescence throughout the primate retina demonstrates a wider variety of structural detail in the living eye than is available through conventional imaging methods, and broadens the use of two-photon imaging of normal and diseased eyes. PMID:26903224

  10. Fluorescence detection of camptothecin anticancer drugs by two-photon excitation

    NASA Astrophysics Data System (ADS)

    Burke, Thomas G.; Malak, Magda; Bom, David; Curran, Dennis P.; Malak, Henryk M.; Gryczynski, Ignacy; Lakowicz, Joseph R.

    1998-04-01

    Hycamtin is a camptothecin anticancer analogue containing a dimethylaminomethyl substituent at position 9 and a hydroxy functionality at position 10. Using an excitation wavelength of 800 nm we have compared the two-photon cross sections and excited-state lifetimes from several camptothecins in phosphate buffered saline solution with and without the presence of human serum albumin (HSA). Drug and HSA concentrations of 10 (mu) M and 46 (mu) M were employed in our studies. In phosphate buffered saline solution containing HSA the following excited-state lifetimes (ns) and two- photon cross-sections (10-50 cm4 s/photon), respectively, were determined: hycamtin (4.3 nm, 36); camptothecin (1.3 ns, 1); 7-t-butyldimethylsilyl-10- hydroxycamptothecin (1.7 ns, 3.7); 7-t-butyldimethylsilyl- camptothecin (1.9 ns, 1.9); 7-trimethylsilyl-10- aminocamptothecin (6.3 ns; 35); and 7-trimethylsilyl-10- hydroxycamptothecin (1.8 ns; 2.2). Our results indicate that Hycamtin exhibits a high cross-section relative to the parent camptothecin molecule and represents one of the best camptothecin analogues to detect using two-photon excitation. Hycamtin was detected at concentrations as low as 0.05 (mu) M and 1 (mu) M in plasma and whole blood, respectively. The newly synthesized analogue 7- trimethylsilyl-10-aminocamptothecin was found to display similar lifetime and two-photon cross section values relative to Hycamtin. Thus, fluorescence detection with two- photon excitation may prove to be of advantage in the development of this promising new experimental therapeutic.

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

    PubMed Central

    2008-01-01

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

  12. L(alpha)-induced two-photon absorption of visible light emitted from an O-type star by H2(+) ions located near the surface of the Stromgren sphere surrounding the star: A possible explanation for the diffuse interstellar absorption bands (DIDs)

    NASA Technical Reports Server (NTRS)

    Glownia, James H.; Sorokin, Peter P.

    1994-01-01

    In this paper, a new model is proposed to account for the DIB's (Diffuse Interstellar Bands). In this model, the DIB's result from a non-linear effect: resonantly-enhanced two-photon absorption of H(2+) ions located near the surface of the Stromgren sphere that surrounds an O- or B- type star. The strong light that is required to 'drive' the two-photon transition is provided by L(alpha) light emerging from the Stromgren sphere that bounds the H II region surrounding the star. A value of approximately 100 micro W/sq cm is estimated for the L(alpha) flux at the Stromgren radius, R(s), of a strong (O5) star. It is shown that a c.w. L(alpha) flux of this intensity should be sufficient to induce a few percent absorption for visible light radiated by the same star at a frequency (omega2) that completes an allowed two-photon transition, provided (1) the L(alpha) radiation happens to be nearly resonant with the frequency of a fully-allowed absorber transition that effectively represents the first step in the two-photon transition, and (2) an effective column density approximately 10(sup18)/sq cm of the absorber is present near the Stromgren sphere radius, R(sub s).

  13. Readily Accessible and Predictable Naphthalene-Based Two-Photon Fluorophore with Full Visible-Color Coverage.

    PubMed

    Koo, Ja Young; Heo, Cheol Ho; Shin, Young-Hee; Kim, Dahahm; Lim, Chang Su; Cho, Bong Rae; Kim, Hwan Myung; Park, Seung Bum

    2016-09-26

    Herein we report 22 acedan-derived, two-photon fluorophores with synthetic feasibility and full coverage of visible wavelength emission. The emission wavelengths were predicted by computational analysis, which enabled us to visualize multicolor images by two-photon excitation with single wavelength, and to design a turn-on, two-photon fluorescence sensor for endogenous H2 O2 in Raw 264.7 macrophage and rat brain hippocampus ex vivo. PMID:27471103

  14. Readily Accessible and Predictable Naphthalene-Based Two-Photon Fluorophore with Full Visible-Color Coverage.

    PubMed

    Koo, Ja Young; Heo, Cheol Ho; Shin, Young-Hee; Kim, Dahahm; Lim, Chang Su; Cho, Bong Rae; Kim, Hwan Myung; Park, Seung Bum

    2016-09-26

    Herein we report 22 acedan-derived, two-photon fluorophores with synthetic feasibility and full coverage of visible wavelength emission. The emission wavelengths were predicted by computational analysis, which enabled us to visualize multicolor images by two-photon excitation with single wavelength, and to design a turn-on, two-photon fluorescence sensor for endogenous H2 O2 in Raw 264.7 macrophage and rat brain hippocampus ex vivo.

  15. Two-photon photodetector in a multiquantum well GaAs laser structure at 1.55 microm.

    PubMed

    Duchesne, D; Razzari, L; Halloran, L; Morandotti, R; SpringThorpe, A J; Christodoulides, D N; Moss, D J

    2009-03-30

    We report two-photon photocurrent in a GaAs/AlGaAs multiple quantum well laser at 1.55 microm. Using 1ps pulses, a purely quadratic photocurrent is observed. We measure the device efficiency, sensitivity, as well as the two-photon absorption coefficient. The results show that the device has potential for signal processing, autocorrelation and possibly two-photon source applications at sub-Watt power levels.

  16. A note on approximate teleportation of an unknown atomic state in the two-photon Jaynes-Cummings model

    NASA Astrophysics Data System (ADS)

    dSouza, A. D.; Cardoso, W. B.; Avelar, A. T.; Baseia, B.

    2009-04-01

    We consider recent schemes [J.M. Liu, B. Weng, Physica A 367 (2006) 215] to teleport unknown atomic states and superposition of zero- and two-photon states using the two-photon Jaynes-Cummings model. Here we do the same using the “full two-photon Jaynes-Cumming”, valid for arbitrary average number of photons. The success probability and fidelity of this teleportation are also considered.

  17. Study of the Effect of the Pulse Width of the Excitation Source on the Two-Photon Absorption and Two-Photon Circular Dichroism Spectra of Biaryl Derivatives.

    PubMed

    Vesga, Yuly; Hernandez, Florencio E

    2016-09-01

    Herein we report on the expanded theoretical calculations and the experimental measurements of the two-photon absorption (TPA) and two-photon circular dichroism (TPCD) spectra of a series of optically active biaryl derivatives (R-BINOL, R-VANOL, and R-VAPOL) using femtosecond pulses. The comparative analysis of the experimental TPCD spectra obtained with our tunable amplified femtosecond system with those previously measured in our group on the same series of compounds in the picosecond regime reveals a decrease in the amplitude of the signal and an improvement in matching with the theory in the former. These results can be explained based on the negligible contribution of excited state absorption (ESA) using femtosecond pulses compared to the picosecond regime. We show how ESA affects both the strength of the signal and the shape of the TPA and TPCD spectra. TPA and TPCD spectra were obtained using the double L-scan technique over a broad spectral range (450-750 nm) using 90 fs pulses at 50 Hz repetition rate produced by an amplified femtosecond system. The theoretical calculations were performed using modern analytical response theory within the time-dependent density functional theory (TD-DFT) approach using CAM-B3LYP and 6-311++G(d,p) basis sets. PMID:27525702

  18. The Correlated Two-Photon Transport in a One-Dimensional Waveguide Coupling to a Hybrid Atom-Optomechanical System

    NASA Astrophysics Data System (ADS)

    Liu, Jingyi; Zhang, Wenzhao; Li, Xun; Yan, Weibin; Zhou, Ling

    2016-10-01

    We investigate the two-photon transport properties inside one-dimensional waveguide side coupled to an atom-optomechanical system, aiming to control the two-photon transport by using the nonlinearity. By generalizing the scheme of Phys. Rev. A 90, 033832, we show that Kerr nonlinearity induced by the four-level atoms is remarkable and can make the photons antibunching, while the nonlinear interaction of optomechanical coupling participates in both the single photon and the two photon processes so that it can make the two photons exhibiting bunching and antibunching.

  19. In vivo characterization of early-stage radiation skin injury in a mouse model by two-photon microscopy

    PubMed Central

    Jang, Won Hyuk; Shim, Sehwan; Wang, Taejun; Yoon, Yeoreum; Jang, Won-Suk; Myung, Jae Kyung; Park, Sunhoo; Kim, Ki Hean

    2016-01-01

    Ionizing radiation (IR) injury is tissue damage caused by high energy electromagnetic waves such as X-ray and gamma ray. Diagnosis and treatment of IR injury are difficult due to its characteristics of clinically latent post-irradiation periods and the following successive and unpredictable inflammatory bursts. Skin is one of the many sensitive organs to IR and bears local injury upon exposure. Early-stage diagnosis of IR skin injury is essential in order to maximize treatment efficiency and to prevent the aggravation of IR injury. In this study, early-stage changes of the IR injured skin at the cellular level were characterized in an in vivo mouse model by two-photon microscopy (TPM). Various IR doses were applied to the mouse hind limbs and the injured skin regions were imaged daily for 6 days after IR irradiation. Changes in the morphology and distribution of the epidermal cells and damage of the sebaceous glands were observed before clinical symptoms. These results showed that TPM is sensitive to early-stage changes of IR skin injury and may be useful for its diagnosis. PMID:26755422

  20. In vivo characterization of early-stage radiation skin injury in a mouse model by two-photon microscopy.

    PubMed

    Jang, Won Hyuk; Shim, Sehwan; Wang, Taejun; Yoon, Yeoreum; Jang, Won-Suk; Myung, Jae Kyung; Park, Sunhoo; Kim, Ki Hean

    2016-01-01

    Ionizing radiation (IR) injury is tissue damage caused by high energy electromagnetic waves such as X-ray and gamma ray. Diagnosis and treatment of IR injury are difficult due to its characteristics of clinically latent post-irradiation periods and the following successive and unpredictable inflammatory bursts. Skin is one of the many sensitive organs to IR and bears local injury upon exposure. Early-stage diagnosis of IR skin injury is essential in order to maximize treatment efficiency and to prevent the aggravation of IR injury. In this study, early-stage changes of the IR injured skin at the cellular level were characterized in an in vivo mouse model by two-photon microscopy (TPM). Various IR doses were applied to the mouse hind limbs and the injured skin regions were imaged daily for 6 days after IR irradiation. Changes in the morphology and distribution of the epidermal cells and damage of the sebaceous glands were observed before clinical symptoms. These results showed that TPM is sensitive to early-stage changes of IR skin injury and may be useful for its diagnosis. PMID:26755422

  1. Parametric resonance enhancement in neutron interferometry and application for the search for non-Newtonian gravity

    SciTech Connect

    Gudkov, Vladimir; Shimizu, Hirohiko M.; Greene, Geoffrey L.

    2011-02-15

    The parametric resonance enhancement of the phase of neutrons due to non-Newtonian anomalous gravitation is considered. The existence of such resonances is confirmed by numerical calculations. A possible experimental scheme for observing this effect is discussed based on an existing neutron interferometer design.

  2. Parametric resonance enhancement in neutron interferometry and application for the search for non-Newtonian gravity

    SciTech Connect

    Greene, Geoffrey L; Gudkov, Vladimir; Shimizu, Hirohiko M.

    2011-01-01

    The parametric resonance enhancement of the phase of neutrons due to non-Newtonian anomalous gravitation is considered. The existence of such resonances is confirmed by numerical calculations. A possible experimental scheme for observing this effect is discussed based on an existing neutron interferometer design.

  3. Ultrashort Two-Photon-Absorption Laser-Induced Fluorescence in Nanosecond-Duration, Repetitively Pulsed Discharges

    NASA Astrophysics Data System (ADS)

    Schmidt, Jacob Brian

    Absolute number densities of atomic species produced by nanosecond duration, repetitively pulsed electric discharges are measured by two-photon absorption laser-induced fluorescence (TALIF). Relatively high plasma discharge pulse energies (=1 mJ/pulse) are used to generate atomic hydrogen, oxygen, and nitrogen in a variety of discharge conditions and geometries. Unique to this work is the development of femtosecond-laser-based TALIF (fs-TALIF). Fs-TALIF offers a number of advantages compared to more conventional ns-pulse-duration laser systems, including better accuracy of direct quenching measurements in challenging environments, significantly reduced photolytic interference including photo-dissociation and photo-ionization, higher signal and increased laser-pulse bandwidth, the ability to collect two-dimensional images of atomic species number densities with far greater spatial resolution compared with more conventional diagnostics, and much higher laser repetition rates allowing for more efficient and accurate measurements of atomic species number densities. In order to fully characterize the fs-TALIF diagnostic and compare it with conventional ns-TALIF, low pressure (100 Torr) ns-duration pulsed discharges are operated in mixtures of H2, O2, and N2 with different buffer gases including argon, helium, and nitrogen. These discharge conditions are used to demonstrate the capability for two-dimensional imaging measurements. The images produced are the first of their kind and offer quantitative insight into spatially and temporally resolved kinetics and transport in ns-pulsed discharge plasmas. The two-dimensional images make possible comparison with high-fidelity plasma kinetics models of the presented data. The comparison with the quasi-one-dimensional kinetic model show good spatial and temporal agreement. The same diagnostics are used at atmospheric pressure, when atomic oxygen fs-TALIF is performed in an atmospheric-pressure plasma jet (APPJ). Here, the

  4. Conjugated polymers with pyrrole as the conjugated bridge: synthesis, characterization, and two-photon absorption properties.

    PubMed

    Li, Qianqian; Zhong, Cheng; Huang, Jing; Huang, Zhenli; Pei, Zhiguo; Liu, Jun; Qin, Jingui; Li, Zhen

    2011-07-14

    The synthesis, one- and two-photon absorption (2PA) and emission properties of two novel pyrrole-based conjugated polymers (P1 and P2) are reported. They emitted strong yellow-green and orange fluorescence with fluorescent quantum yields (Φ) of 46 and 33%, respectively. Their maximal 2PA cross sections (δ) measured by the two-photon-induced fluorescence method using femtosecond laser pulses in THF were 2392 and 1938 GM per repeating unit, respectively, indicating that the 2PA chromophores consisting of the triphenylamine with nonplanar structure as the donor and electron-rich pyrrole as the conjugated bridge could be the effective repeating units to enhance the δ values.

  5. 3D fabrication of all-polymer conductive microstructures by two photon polymerization.

    PubMed

    Kurselis, Kestutis; Kiyan, Roman; Bagratashvili, Victor N; Popov, Vladimir K; Chichkov, Boris N

    2013-12-16

    A technique to fabricate electrically conductive all-polymer 3D microstructures is reported. Superior conductivity, high spatial resolution and three-dimensionality are achieved by successive application of two-photon polymerization and in situ oxidative polymerization to a bi-component formulation, containing a photosensitive host matrix and an intrinsically conductive polymer precursor. By using polyethylene glycol diacrylate (PEG-DA) and 3,4-ethylenedioxythiophene (EDOT), the conductivity of 0.04 S/cm is reached, which is the highest value for the two-photon polymerized all-polymer microstructures to date. The measured electrical conductivity dependency on the EDOT concentration indicates percolation phenomenon and a three-dimensional nature of the conductive pathways. Tunable conductivity, biocompatibility, and environmental stability are the characteristics offered by PEG-DA/EDOT blends which can be employed in biomedicine, MEMS, microfluidics, and sensorics.

  6. Continuous wave two-photon scanning near-field optical microscopy.

    PubMed Central

    Kirsch, A K; Subramaniam, V; Striker, G; Schnetter, C; Arndt-Jovin, D J; Jovin, T M

    1998-01-01

    We have implemented continuous-wave two-photon excitation of near-UV absorbing fluorophores in a scanning near-field optical microscope (SNOM). The 647-nm emission of an Ar-Kr mixed gas laser was used to excite the UV-absorbing DNA dyes DAPI, the bisbenzimidazole Hoechst 33342, and ethidium bromide in a shared aperture SNOM with uncoated fiber tips. Polytene chromosomes of Drosophila melanogaster and the nuclei of 3T3 Balb/c cells labeled with these dyes were readily imaged. The fluorescence intensity showed the expected nonlinear (second order) dependence on the excitation power in the range of 8-180 mW. We measured the fluorescence intensity as a function of the tip-sample displacement in the direction normal to the sample surface in the single- and two-photon excitation modes (SPE, TPE). The fluorescence intensity decayed faster in TPE than in SPE. PMID:9726953

  7. Efficient simultaneous dense coding and teleportation with two-photon four-qubit cluster states

    NASA Astrophysics Data System (ADS)

    Zhang, Cai; Situ, Haozhen; Li, Qin; He, Guang Ping

    2016-08-01

    We firstly propose a simultaneous dense coding protocol with two-photon four-qubit cluster states in which two receivers can simultaneously get their respective classical information sent by a sender. Because each photon has two degrees of freedom, the protocol will achieve a high transmittance. The security of the simultaneous dense coding protocol has also been analyzed. Secondly, we investigate how to simultaneously teleport two different quantum states with polarization and path degree of freedom using cluster states to two receivers, respectively, and discuss its security. The preparation and transmission of two-photon four-qubit cluster states is less difficult than that of four-photon entangled states, and it has been experimentally generated with nearly perfect fidelity and high generation rate. Thus, our protocols are feasible with current quantum techniques.

  8. Two-photon exchange between two three-level atoms in separate cavities

    SciTech Connect

    Alexanian, Moorad

    2011-02-15

    The temporal evolution of two coupled cavities, each containing a single three-level atom, is studied when the cavities exchange two coherent photons. The general state of the system is a linear superposition of symmetric and antisymmetric states with the symmetric states controlled by two of the four eigenfrequencies and the antisymmetric states by the other two. The system undergoes Rabi oscillations between the two symmetric (antisymmetric) states. There is state transfer between the cavities when both atoms are in the ground state and two photons are exchanged. In addition, there is also Rabi ''flopping'' whereby one atom is in the excited state and the other in the ground state and the roles are reversed in a periodic fashion by the exchange of two photons. The generation of entanglement can be explicitly given as a function of time. Models of coupled cavities are of interest in distributed quantum information and computation.

  9. In vivo reactive neural plasticity investigation by means of correlative two photon: electron microscopy

    NASA Astrophysics Data System (ADS)

    Allegra Mascaro, A. L.; Cesare, P.; Sacconi, L.; Grasselli, G.; Mandolesi, G.; Maco, B.; Knott, G.; Huang, L.; De Paola, V.; Strata, P.; Pavone, F. S.

    2013-02-01

    In the adult nervous system, different populations of neurons correspond to different regenerative behavior. Although previous works showed that olivocerebellar fibers are capable of axonal regeneration in a suitable environment as a response to injury1, we have hitherto no details about the real dynamics of fiber regeneration. We set up a model of singularly axotomized climbing fibers (CF) to investigate their reparative properties in the adult central nervous system (CNS) in vivo. Time lapse two-photon imaging has been combined to laser nanosurgery2, 3 to define a temporal pattern of the degenerative event and to follow the structural rearrangement after injury. To characterize the damage and to elucidate the possible formation of new synaptic contacts on the sprouted branches of the lesioned CF, we combined two-photon in vivo imaging with block face scanning electron microscopy (FIB-SEM). Here we describe the approach followed to characterize the reactive plasticity after injury.

  10. Accuracy of different DFT formalisms for prediction of two-photon absorption properties of conjugated polymers

    NASA Astrophysics Data System (ADS)

    Nayyar, Iffat; Mikhailov, Ivan; Masunov, Artem

    2010-03-01

    The importance of organic molecules with large two-photon absorption (2PA) is realized for deep-tissue fluorescence microscopy, photodynamic therapy, three-dimensional microfabrication and optical data storage. Computer predictions provide understanding of structure/activity relationships and assist in the rational design of polymer materials as an alternative to trial and error methods. In this contribution, we compare various density functional theory (DFT) formalisms to predict two-photon absorption spectra in a series of large donor-acceptor substituted conjugated molecules. We conclude that the accuracy of a posteriori Tamm-Dancoff approximation [1] is close to the exact results obtained in Coupled Electronic Oscillators formalism [2]. Adjusting fraction of exact exchange in XC functionals allow for improved agreement with experiment. [1] Mikhailov, I.A.; Tafur, S.; Masunov, A.E., Phys. Rev. A 77, 01250 (2008) [2] Masunov, A.M.; Tretiak, S., J. Phys. Chem. B 108, 899 (2004)

  11. Two-photon physics and the coming generation of heavy ion colliders

    SciTech Connect

    Rhoades-Brown, M.J.

    1992-07-01

    The possibilities for two-photon physics at the coming generation of heavy ion colliders is discussed. Particular attention is given to both e{sup +}, e{sup {minus}} production and resonance production of the Higgs particle. For e{sup +},e{sup {minus}} production the inadequacy of traditional perturbation theory is outlined, and through of the introduction of approximations valid for heavy ions it is shown how to sum a class of non-perturbative diagrams. The role of the nuclear form factor in suppressing the cross section for the heaviest resonances is also discussed. It is shown how this latter point affects the two-photon cross sections for W{sup +},W{sup {minus}} and Higgs production at RHIC, LHC and SSC energies.

  12. Two-photon physics and the coming generation of heavy ion colliders

    SciTech Connect

    Rhoades-Brown, M.J.

    1992-01-01

    The possibilities for two-photon physics at the coming generation of heavy ion colliders is discussed. Particular attention is given to both e{sup +}, e{sup {minus}} production and resonance production of the Higgs particle. For e{sup +},e{sup {minus}} production the inadequacy of traditional perturbation theory is outlined, and through of the introduction of approximations valid for heavy ions it is shown how to sum a class of non-perturbative diagrams. The role of the nuclear form factor in suppressing the cross section for the heaviest resonances is also discussed. It is shown how this latter point affects the two-photon cross sections for W{sup +},W{sup {minus}} and Higgs production at RHIC, LHC and SSC energies.

  13. Two-photon excitation cross-section in light and intermediate atoms

    NASA Technical Reports Server (NTRS)

    Omidvar, K.

    1980-01-01

    The method of explicit summation over the intermediate states is used along with LS coupling to derive an expression for two-photon absorption cross section in light and intermediate atoms in terms of integrals over radial wave functions. Two selection rules, one exact and one approximate, are also derived. In evaluating the radial integrals, for low-lying levels, the Hartree-Fock wave functions, and for high-lying levels, hydrogenic wave functions obtained by the quantum defect method are used. A relationship between the cross section and the oscillator strengths is derived. Cross sections due to selected transitions in nitrogen, oxygen, and chlorine are given. The expression for the cross section is useful in calculating the two-photon absorption in light and intermediate atoms.

  14. Two-photon triggered drug delivery system: a new way to prevent posterior capsule opacification

    NASA Astrophysics Data System (ADS)

    Kim, H.-C.; Härtner, S.; Hampp, N.

    2006-02-01

    One of the major complications of cataract surgery is posterior capsule opacification caused by proliferation and migration of residual lens epithelial cells into the visual axis. In this study we present a novel approach to treat posterior capsule opacification in a non-invasive manner. A polymer-drug conjugate has been developed which is suitable for manufacturing functional intraocular lenses equipped with a drug delivery system. The therapeutic molecules, 5-fluorouracil, were attached through a photolabile linkage to the acrylic polymer backbone of the intraocular lens material. The controlled release of 5-fluorouracil is accomplished by two-photon induced cleavage of the linkage which is stable in ordinary conditions. The properties of the therapeutic system are characterized and the function is demonstrated in in vitro tests. The utilization of two-photon-absorption processes in drug delivery may provide a powerful tool to prevent posterior capsule opacification.

  15. Ultra-low shrinkage hybrid photosensitive material for two-photon polymerization microfabrication.

    PubMed

    Ovsianikov, Aleksandr; Viertl, Jacques; Chichkov, Boris; Oubaha, Mohamed; MacCraith, Brian; Sakellari, Ioanna; Giakoumaki, Anastasia; Gray, David; Vamvakaki, Maria; Farsari, Maria; Fotakis, Costas

    2008-11-25

    Investigations into the structuring by two-photon polymerization of a nonshrinking, photosensitive, zirconium sol-gel material are presented. This hybrid material can be photostructured even when it contains up to 30 mol % of zirconium propoxide (ZPO); by varying the material's inorganic content, it is possible to modify and tune its refractive index. The introduction of ZPO significantly increases the photosensitivity of the resulting photopolymer. The fabricated three-dimensional photonic crystal structures demonstrate high resolution and a clear band-stop in the near-IR region. In contrast to common practice, no additional effort is required to precompensate for shrinkage or to improve the structural stability of the fabricated photonic crystals; this, combined with the possibility of tuning this material's optical, mechanical, and chemical properties, makes it suitable for a variety of applications by two-photon polymerization manufacturing.

  16. Cationic Two-Photon Lanthanide Bioprobes Able to Accumulate in Live Cells.

    PubMed

    Bui, Anh Thy; Beyler, Maryline; Liao, Yuan-Yuan; Grichine, Alexei; Duperray, Alain; Mulatier, Jean-Christophe; Guennic, Boris Le; Andraud, Chantal; Maury, Olivier; Tripier, Raphaël

    2016-07-18

    An original cationic water-soluble cyclen-based Eu(III) complex [EuL(1)](+) featuring a chromophore-functionalized antenna to increase the two-photon (2P) absorption properties was synthesized. The photophysical properties were thoroughly studied in various solvents and rationalized with the help of theoretical calculations. The complex exhibits an optimized 2P absorption cross section. Finally, 2P microscopy imaging experiments on living T24 human cancer cells highlighted the spontaneous internalization and the biological stability of this 2P bioprobe in vitro. Macrocyclic-based antennas open new perspectives for future optimization of the photophysical properties and allows envisaging the design of Eu, Tb, Yb, and Sm bioprobes. This result also opens the way for the design of functional two-photon Ln complexes able to monitor intracellular physicochemical parameters. PMID:27367598

  17. Two-Photon or Higher-Order Absorbing Optical Materials for Generation of Reactive Species

    NASA Technical Reports Server (NTRS)

    Cumpston, Brian (Inventor); Lipson, Matthew (Inventor); Marder, Seth R. (Inventor); Perry, Joseph W. (Inventor)

    2013-01-01

    Disclosed are highly efficient multiphoton absorbing compounds and methods of their use. The compounds generally include a bridge of pi-conjugated bonds connecting electron donating groups or electron accepting groups. The bridge may be substituted with a variety of substituents as well. Solubility, lipophilicity, absorption maxima and other characteristics of the compounds may be tailored by changing the electron donating groups or electron accepting groups, the substituents attached to or the length of the pi-conjugated bridge. Numerous photophysical and photochemical methods are enabled by converting these compounds to electronically excited states upon simultaneous absorption of at least two photons of radiation. The compounds have large two-photon or higher-order absorptivities such that upon absorption, one or more Lewis acidic species, Lewis basic species, radical species or ionic species are formed.

  18. Two-photon or higher-order absorbing optical materials for generation of reactive species

    NASA Technical Reports Server (NTRS)

    Cumpston, Brian (Inventor); Lipson, Matthew (Inventor); Marder, Seth R. (Inventor); Perry, Joseph W. (Inventor)

    2003-01-01

    Disclosed are highly efficient multiphoton absorbing compounds and methods of their use. The compounds generally include a bridge of pi-conjugated bonds connecting electron donating groups or electron accepting groups. The bridge may be substituted with a variety of substituents as well. Solubility, lipophilicity, absorption maxima and other characteristics of the compounds may be tailored by changing the electron donating groups or electron accepting groups, the substituents attached to or the length of the pi-conjugated bridge. Numerous photophysical and photochemical methods are enabled by converting these compounds to electronically excited states upon simultaneous absorption of at least two photons of radiation. The compounds have large two-photon or higher-order absorptivities such that upon absorption, one or more Lewis acidic species, Lewis basic species, radical species or ionic species are formed.

  19. Measurement of electron beam polarization from unstrained GaAs via two-photon photoemission

    SciTech Connect

    McCarter, James L.; Afanasev, A.; Gay, T. J.; Hansknecht, John C.; Kechiantz, A.; Poelker, B. Matthew

    2014-02-01

    Two-photon absorption of 1560 nm light was used to generate polarized electron beams from unstrained GaAs photocathodes of varying thickness: 625 {mu}m, 0.32 {mu}m, and 0.18 {mu}m. For each photocathode, the degree of spin polarization of the photoemitted beam was less than 50%, contradicting earlier predictions based on simple quantum mechanical selection rules for spherically-symmetric systems but consistent with the more sophisticated model of Bhat et al. (Phys. Rev. B 71 (2005) 035209). Polarization via two-photon absorption was the highest from the thinnest photocathode sample and comparable to that obtained via one-photon absorption (using 778 nm light), with values 40.3 +- 1.0% and 42.6 +- 1.0%, respectively.

  20. Non-resonant below-bandgap two-photon absorption in quantum dot solar cells

    SciTech Connect

    Li, Tian; Dagenais, Mario

    2015-04-27

    We study the optically nonlinear sub-bandgap photocurrent generation facilitated by an extended tailing distribution of states in an InAs/GaAs quantum dots (QDs) solar cell. The tailing states function as both the energy states for low energy photon absorption and the photocarriers extraction pathway. One of the biggest advantages of our method is that it can clearly differentiate the photocurrent due to one-photon absorption (1PA) process and two-photon absorption (2PA) process. Both 1PA and 2PA photocurrent generation efficiency in an InAs/GaAs QD device operated at 1550 nm have been quantitatively evaluated. A two-photon absorption coefficient β = 5.7 cm/GW is extracted.

  1. 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

  2. Two-photon microscopy of oxygen: polymersomes as probe carrier vehicles

    PubMed Central

    Sinks, Louise E.; Robbins, Gregory P.; Roussakis, Emmanuel; Troxler, Thomas; Hammer, Daniel A.; Vinogradov, Sergei A.

    2010-01-01

    Oxygen concentration distributions in biological systems can be imaged by the phosphorescence quenching method in combination with two-photon laser scanning microscopy. In this paper we identified the excitation regime in which the signal of a two-photon-enhanced phosphorescent probe1 is dependent quadratically on the excitation power (quadratic regime), and performed simulations that relate the photophysical properties of the probe to the imaging resolution. Further, we characterized polymersomes as a method of probe encapsulation and delivery. Photo-physical and oxygen sensing properties of the probe were found unchanged when the probe is encapsulated in polymersomes. Polymersomes were found capable of sustaining high probe concentrations, thereby serving to improve the signal-to-noise ratios for oxygen detection compared to the previously employed probe delivery methods. Imaging of polymersomes loaded with the probe was used as a test-bed for a new method. PMID:20462225

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

    PubMed

    Han, Meng; Bindewald-Wittich, Almut; Holz, Frank G; Giese, Guenter; 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.

  4. Coherence gated wavefront sensorless adaptive optics for two photon excited fluorescence retinal imaging (Conference Presentation)

    NASA Astrophysics Data System (ADS)

    Jian, Yifan; Cua, Michelle; Bonora, Stefano; Pugh, Edward N.; Zawadzki, Robert J.; Sarunic, Marinko V.

    2016-03-01

    We present a novel system for adaptive optics two photon imaging. We utilize the bandwidth of the femtosecond excitation beam to perform coherence gated imaging (OCT) of the sample. The location of the focus is directly observable in the cross sectional OCT images, and adjusted to the desired depth plane. Next, using real time volumetric OCT, we perform Wavefront Sensorless Adaptive Optics (WSAO) aberration correction using a multi-element adaptive lens capable of correcting up to 4th order Zernike polynomials. The aberration correction is performed based on an image quality metric, for example intensity. The optimization time is limited only by the OCT acquisition rate, and takes ~30s. Following aberration correction, two photon fluorescence images are acquired, and compared to results without adaptive optics correction. This technique is promising for multiphoton imaging in multi-layered, scattering samples such as eye and brain, in which traditional wavefront sensing and guide-star sensorless adaptive optics approaches may not be suitable.

  5. Enhanced two-photon absorption in a hollow-core photonic-band-gap fiber

    SciTech Connect

    Saha, Kasturi; Venkataraman, Vivek; Londero, Pablo; Gaeta, Alexander L.

    2011-03-15

    We show that two-photon absorption (TPA) in rubidium atoms can be greatly enhanced by the use of a hollow-core photonic-band-gap fiber. We investigate off-resonant, degenerate Doppler-free TPA on the 5S{sub 1/2{yields}}5D{sub 5/2} transition and observe 1% absorption of a pump beam with a total power of only 1 mW in the fiber. These results are verified by measuring the amount of emitted blue fluorescence and are consistent with the theoretical predictions which indicate that transit-time effects play an important role in determining the two-photon absorption cross section in a confined geometry.

  6. Selective two-photon absorptive resonance femtosecond-laser electronic-excitation tagging velocimetry.

    PubMed

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

    2016-05-15

    Selective two-photon absorptive resonance femtosecond-laser electronic-excitation tagging (STARFLEET), a nonseeded ultrafast-laser-based velocimetry technique, is demonstrated in reactive and nonreactive 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 nonreactive), 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. PMID:27176968

  7. Two-Photon Imaging of Lymphocyte Motility and Antigen Response in Intact Lymph Node

    NASA Astrophysics Data System (ADS)

    Miller, Mark J.; Wei, Sindy H.; Parker, Ian; Cahalan, Michael D.

    2002-06-01

    Lymphocyte motility is vital for trafficking within lymphoid organs and for initiating contact with antigen-presenting cells. Visualization of these processes has previously been limited to in vitro systems. We describe the use of two-photon laser microscopy to image the dynamic behavior of individual living lymphocytes deep within intact lymph nodes. In their native environment, T cells achieved peak velocities of more than 25 micrometers per minute, displaying a motility coefficient that is five to six times that of B cells. Antigenic challenge changed T cell trajectories from random walks to ``swarms'' and stable clusters. Real-time two-photon imaging reveals lymphocyte behaviors that are fundamental to the initiation of the immune response.

  8. Coincidence in the two-photon spectra of Li and Li2 at 735 nm

    NASA Astrophysics Data System (ADS)

    DeGraffenreid, W.; Sansonetti, Craig J.

    2005-02-01

    A coincidence between the 22S1/2-32S1/2 two-photon transition in the atomic spectrum of 6Li and the X 1Σ+g→ E 1Σ+g two-photon ro-vibrational series of 7Li2 was observed near 735 nm in a heat pipe oven using a tunable laser and thermionic diode detection scheme. The molecular transition obscures one component of the 6Li atomic transition. Selective detection of the atomic transition was obtained by adding an intensity-modulated laser that drives atoms from the 3S to 16P state. The coincident molecular transition and four nearby molecular lines were identified using previously determined Dunham coefficients.

  9. Rational Design of Fluorescent Phthalazinone Derivatives for One- and Two-Photon Imaging.

    PubMed

    Yang, Lingfei; Zhu, Yuanjun; Shui, Mengyang; Zhou, Tongliang; Cai, Yuanbo; Wang, Wei; Xu, Fengrong; Niu, Yan; Wang, Chao; Zhang, Jun-Long; Xu, Ping; Yuan, Lan; Liang, Lei

    2016-08-22

    Phthalazinone derivatives were designed as optical probes for one- and two-photon fluorescence microscopy imaging. The design strategy involves stepwise extension and modification of pyridazinone by 1) expansion of pyridazinone to phthalazinone, a larger conjugated system, as the electron acceptor, 2) coupling of electron-donating aromatic groups such as N,N-diethylaminophenyl, thienyl, naphthyl, and quinolyl to the phthalazinone, and 3) anchoring of an alkyl chain to the phthalazinone with various terminal substituents such as triphenylphosphonio, morpholino, triethylammonio, N-methylimidazolio, pyrrolidino, and piperidino. Theoretical calculations were utilized to verify the initial design. The desired fluorescent probes were synthesized by two different routes in considerable yields. Twenty-two phthalazinone derivatives were synthesized and their photophysical properties were measured. Selected compounds were applied in cell imaging, and valuable information was obtained. Furthermore, the designed compounds showed excellent performance in two-photon microscopic imaging of mouse brain slices.

  10. Resonant two-photon annihilation of an electron-positron pair in a pulsed electromagnetic wave

    NASA Astrophysics Data System (ADS)

    Voroshilo, A. I.; Roshchupkin, S. P.; Nedoreshta, V. N.

    2016-09-01

    Two-photon annihilation of an electron-positron pair in the field of a plane low-intensity circularly polarized pulsed electromagnetic wave was studied. The conditions for resonance of the process which are related to an intermediate particle that falls within the mass shell are studied. In the resonant approximation the probability of the process was obtained. It is demonstrated that the resonant probability of two-photon annihilation of an electron-positron pair may be several orders of magnitude higher than the probability of this process in the absence of the external field. The obtained results may be experimentally verified by the laser facilities of the international megaprojects, for example, SLAC (National Accelerator Laboratory), FAIR (Facility for Antiproton and Ion Research), and XFEL (European X-Ray Free-Electron Laser).

  11. Demonstration of an Exposed-Core Fiber Platform for Two-Photon Rubidium Spectroscopy

    NASA Astrophysics Data System (ADS)

    Perrella, C.; Griesser, H. P.; Light, P. S.; Kostecki, R.; Stace, T. M.; Ebendorff-Heidepriem, H.; Monro, T. M.; White, A. G.; Luiten, A. N.

    2015-07-01

    We demonstrate a promising fiber architecture for generating strong photon-photon interactions. Exposed-core silica optical fibers possess low-loss guidance between 400 and 1700 nm crucial for quantum-logic applications. The potential of this fiber is demonstrated by exciting a two-photon transition within a rubidium vapor using an exposed-core silica optical fiber. Transit-time broadened spectral features enable measurement of the evanescent-field scale length of (120 ±20 ) nm which shows excellent agreement with the characteristics of the modeled fiber mode (118 ±2 ) nm . We observe a two-photon absorption coefficient of 8.3 cm-1 for one optical mode in response to a transmitted power of 1.3 mW in the second mode. A clear pathway to an exposed-core fiber exhibiting substantial absorption mediated by a single photon is identified.

  12. Programmable two-photon quantum interference in 103 channels in opaque scattering media

    NASA Astrophysics Data System (ADS)

    Wolterink, Tom A. W.; Uppu, Ravitej; Ctistis, Georgios; Vos, Willem L.; Boller, Klaus-J.; Pinkse, Pepijn W. H.

    2016-05-01

    We investigate two-photon quantum interference in an opaque scattering medium that intrinsically supports a large number of transmission channels. By adaptive spatial phase modulation of the incident wave fronts, the photons are directed at targeted speckle spots or output channels. From 103 experimentally available coupled channels, we select two channels and enhance their transmission to realize the equivalent of a fully programmable 2 ×2 beam splitter. By sending pairs of single photons from a parametric down-conversion source through the opaque scattering medium, we observe two-photon quantum interference. The programed beam splitter need not fulfill energy conservation over the two selected output channels and hence could be nonunitary. Consequently, we have the freedom to tune the quantum interference from bunching (Hong-Ou-Mandel-like) to antibunching. Our results establish opaque scattering media as a platform for high-dimensional quantum interference that is notably relevant for boson sampling and physical-key-based authentication.

  13. In Vivo Monitoring of Multiple Circulating Cell Populations Using Two-photon Flow Cytometry

    PubMed Central

    Tkaczyk, Eric R.; Zhong, Cheng Frank; Ye, Jing Yong; Myc, Andrzej; Thomas, Thommey; Cao, Zhengyi; Duran-Struuck, Raimon; Luker, Kathryn E.; Luker, Gary D.; Norris, Theodore B.; Baker, James R.

    2008-01-01

    To detect and quantify multiple distinct populations of cells circulating simultaneously in the blood of living animals, we developed a novel optical system for two-channel, two-photon flow cytometry in vivo. We used this system to investigate the circulation dynamics in live animals of breast cancer cells with low (MCF-7) and high (MDA-MB-435) metastatic potential, showing for the first time that two different populations of circulating cells can be quantified simultaneously in the vasculature of a single live mouse. We also non-invasively monitored a population of labeled, circulating red blood cells for more than two weeks, demonstrating that this technique can also quantify the dynamics of abundant cells in the vascular system for prolonged periods of time. These data are the first in vivo application of multichannel flow cytometry utilizing two-photon excitation, which will greatly enhance our capability to study circulating cells in cancer and other disease processes. PMID:19221581

  14. In Vivo Monitoring of Multiple Circulating Cell Populations Using Two-photon Flow Cytometry.

    PubMed

    Tkaczyk, Eric R; Zhong, Cheng Frank; Ye, Jing Yong; Myc, Andrzej; Thomas, Thommey; Cao, Zhengyi; Duran-Struuck, Raimon; Luker, Kathryn E; Luker, Gary D; Norris, Theodore B; Baker, James R

    2008-02-15

    To detect and quantify multiple distinct populations of cells circulating simultaneously in the blood of living animals, we developed a novel optical system for two-channel, two-photon flow cytometry in vivo. We used this system to investigate the circulation dynamics in live animals of breast cancer cells with low (MCF-7) and high (MDA-MB-435) metastatic potential, showing for the first time that two different populations of circulating cells can be quantified simultaneously in the vasculature of a single live mouse. We also non-invasively monitored a population of labeled, circulating red blood cells for more than two weeks, demonstrating that this technique can also quantify the dynamics of abundant cells in the vascular system for prolonged periods of time. These data are the first in vivo application of multichannel flow cytometry utilizing two-photon excitation, which will greatly enhance our capability to study circulating cells in cancer and other disease processes.

  15. Performance comparison of acrylic and thiol-acrylic resins in two-photon polymerization.

    PubMed

    Jiang, Lijia; Xiong, Wei; Zhou, Yushen; Liu, Ying; Huang, Xi; Li, Dawei; Baldacchini, Tommaso; Jiang, Lan; Lu, Yongfeng

    2016-06-13

    Microfabrication by two-photon polymerization is investigated using resins based on thiol-ene chemistry. In particular, resins containing different amounts of a tetrafunctional acrylic monomer and a tetrafunctional thiol molecule are used to create complex microstructures. We observe the enhancement of several characteristics of two-photon polymerization when using thiol-acrylic resins. Specifically, microfabrication is carried out using higher writing velocities and it produces stronger polymeric microstructures. Furthermore, the amount of shrinkage typically observed in the production of three-dimensional microstructures is reduced also. By means of microspectrometry, we confirm that the thiol-acrylate mixture in TPP resins promote monomer conversion inducing a higher degree of cross-linked network formation.

  16. Terahertz-visible two-photon rotational spectroscopy of cold OD-

    NASA Astrophysics Data System (ADS)

    Lee, Seunghyun; Hauser, Daniel; Lakhmanskaya, Olga; Spieler, Steffen; Endres, Eric S.; Geistlinger, Katharina; Kumar, Sunil S.; Wester, Roland

    2016-03-01

    We present a method to measure rotational transitions of molecular anions in the terahertz domain by sequential two-photon absorption. Ion excitation by bound-bound terahertz absorption is probed by absorption in the visible on a bound-free transition. The visible frequency is tuned to a state-selective photodetachment transition of the excited anions. This provides a terahertz action spectrum for just a few hundred molecular ions. To demonstrate this we measure the two lowest rotational transitions, J =1 ←0 and J =2 ←1 of OD- anions in a cryogenic 22-pole trap. We obtain rotational transition frequencies of 598 596.08(19) MHz for J =1 ←0 and 1 196 791.57(27) MHz for J =2 ←1 of OD-, in good agreement with their only previous measurement. This two-photon scheme opens up terahertz rovibrational spectroscopy for a range of molecular anions, in particular for polyatomic and cluster anions.

  17. Two-Photon Exchange Corrections to Precise Measurements of Proton Electroweak Form Factors

    NASA Astrophysics Data System (ADS)

    Afanasev, Andrei

    2004-10-01

    Higher-order QED effects play an important role for extracting information on proton form factors from electron scattering data. For the electric form factor of the proton, a previously neglected two-photon-exchange correction reconciles an observed discrepancy between Rosenbluth and polarization techniques [1]. We use a similar approach based on General Parton Distributions to compute additional radiative corrections to parity-violating electron scattering. [1] Y.C. Chen, A. Afanasev, S.J. Brodsky, C.E. Carlson and M. Vanderhaeghen, ``Partonic calculation of the two-photon exchange contribution to elastic electron proton scattering at large momentum transfer,`` arXiv:hep-ph/0403058, to appear in Phys.Rev.Lett.

  18. Performance comparison of acrylic and thiol-acrylic resins in two-photon polymerization.

    PubMed

    Jiang, Lijia; Xiong, Wei; Zhou, Yushen; Liu, Ying; Huang, Xi; Li, Dawei; Baldacchini, Tommaso; Jiang, Lan; Lu, Yongfeng

    2016-06-13

    Microfabrication by two-photon polymerization is investigated using resins based on thiol-ene chemistry. In particular, resins containing different amounts of a tetrafunctional acrylic monomer and a tetrafunctional thiol molecule are used to create complex microstructures. We observe the enhancement of several characteristics of two-photon polymerization when using thiol-acrylic resins. Specifically, microfabrication is carried out using higher writing velocities and it produces stronger polymeric microstructures. Furthermore, the amount of shrinkage typically observed in the production of three-dimensional microstructures is reduced also. By means of microspectrometry, we confirm that the thiol-acrylate mixture in TPP resins promote monomer conversion inducing a higher degree of cross-linked network formation. PMID:27410383

  19. Long-term two-photon fluorescence imaging of mammalian embryos without compromising viability

    PubMed Central

    Squirrell, Jayne M.; Wokosin, David L.; White, John G.; Bavister, Barry D.

    2016-01-01

    A major challenge for fluorescence imaging of living mammalian cells is maintaining viability following prolonged exposure to excitation illumination. We have monitored the dynamics of mitochondrial distribution in hamster embryos at frequent intervals over 24 h using two-photon microscopy (1,047 nm) while maintaining blastocyst, and even fetal, developmental competence. In contrast, confocal imaging for only 8 h inhibits development, even without fluorophore excitation. Photo-induced production of H2O2 may account, in part, for this inhibition. Thus, two-photon microscopy, but not confocal microscopy, has permitted long-term fluorescence observations of the dynamics of three-dimensional cytoarchitecture in highly photosensitive specimens such as mammalian embryos. PMID:10429240

  20. 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.

  1. Two-photon exchange in elastic ep scattering and the status of the OLYMPUS experiment

    NASA Astrophysics Data System (ADS)

    Hasell, Douglas; Olympus Collaboration

    2014-09-01

    Two-photon exchange in elastic ep scattering is believed to explain the observed discrepancy in the proton electric to magnetic form factor ratio, μpGEp /GMp , measured by Rosenbluth separation and by polarization transfer methods. To quantitatively determine the contribution of two-photon exchange to elastic scattering the OLYMPUS experiment was proposed and operated at the DESY laboratory in Hamburg, Germany to measure the ratio in the elastic scattering cross sections, σe+ p /σe- p . The OLYMPUS experiment used the positron and electron beams of the DORIS storage ring at a beam energy of 2.01 GeV incident on a windowless, internal, hydrogen gas target. A left/right symmetric detector measured the rates for elastic scattering over a broad kinematic range together with a redundant set of luminosity monitors. Approximately 4.45 fb-1 of integrated luminosity was collected. The current status of the OLYMPUS analysis will be presented.

  2. Two-photon imaging of a magneto-fluorescent indicator for 3D optical magnetometry.

    PubMed

    Lee, Hohjai; Brinks, Daan; Cohen, Adam E

    2015-10-19

    We developed an optical method to visualize the three-dimensional distribution of magnetic field strength around magnetic microstructures. We show that the two-photon-excited fluorescence of a chained donor-bridge-acceptor compound, phenanthrene-(CH2)12-O-(CH2)2-N,N-dimethylaniline, is sensitive to ambient magnetic field strength. A test structure is immersed in a solution of the magneto-fluorescent indicator and a custom two-photon microscope maps the fluorescence of this compound. The decay kinetics of the electronic excited state provide a measure of magnetic field that is insensitive to photobleaching, indicator concentration, or local variations in optical excitation or collection efficiency. PMID:26480460

  3. Two-photon or higher-order absorbing optical materials for generation of reactive species

    NASA Technical Reports Server (NTRS)

    Cumpston, Brian (Inventor); Lipson, Matthew (Inventor); Marder, Seth R (Inventor); Perry, Joseph W (Inventor)

    2007-01-01

    Disclosed are highly efficient multiphoton absorbing compounds and methods of their use. The compounds generally include a bridge of pi-conjugated bonds connecting electron donating groups or electron accepting groups. The bridge may be substituted with a variety of substituents as well. Solubility, lipophilicity, absorption maxima and other characteristics of the compounds may be tailored by changing the electron donating groups or electron accepting groups, the substituents attached to or the length of the pi-conjugated bridge. Numerous photophysical and photochemical methods are enabled by converting these compounds to electronically excited states upon simultaneous absorption of at least two photons of radiation. The compounds have large two-photon or higher-order absorptivities such that upon absorption, one or more Lewis acidic species, Lewis basic species, radical species or ionic species are formed.

  4. [Frontiers in Live Bone Imaging Researches. Two-Photon Excitation Microscopy, principles and technologies].

    PubMed

    Oikawa, Yoshiro

    2015-06-01

    The "two photon absorption" phenomenon had been predicted by the American Physicist, Maria Ghöppert-Mayer in 1931. Denk and Webb group had proved it in 1990 and the first product had been launched in the market in 1996. But ever since the product became available, the number of users are not increased. Moreover, the system had been too difficult to use and the system sometimes stay not working in labs. But recently, the new easier-to-use products are released and the ultra short pulse IR laser became stable. And its applications are extending from neuro-science to oncology or immunology fields. Due to these reasons, the shipment of multi-photon microscope in Japan in 2013 is approximately 40 units which is 3 times bigger than in 2010. In this paper, I would like to discuss the principles of two-photon microscopy and some of the new technologies for the higher signal capture efficiency. PMID:26017864

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

    PubMed Central

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

    2016-01-01

    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. PMID:26864567

  6. Adaptive wavefront correction in two-photon microscopy using coherence-gated wavefront sensing

    PubMed Central

    Rueckel, Markus; Mack-Bucher, Julia A.; Denk, Winfried

    2006-01-01

    The image quality of a two-photon microscope is often degraded by wavefront aberrations induced by the specimen. We demonstrate here that resolution and signal size in two-photon microcopy can be substantially improved, even in living biological specimens, by adaptive wavefront correction based on sensing the wavefront of coherence-gated backscattered light (coherence-gated wavefront sensing, CGWS) and wavefront control by a deformable mirror. A nearly diffraction-limited focus can be restored even for strong aberrations. CGWS-based wavefront correction should be applicable to samples with a wide range of scattering properties and it should be possible to perform real-time pixel-by-pixel correction even at fast scan speeds. PMID:17088565

  7. Rapid imaging of surgical breast excisions using direct temporal sampling two photon fluorescent lifetime imaging

    PubMed Central

    Giacomelli, Michael G.; Sheikine, Yuri; Vardeh, Hilde; Connolly, James L.; Fujimoto, James G.

    2015-01-01

    Two photon fluorescent lifetime imaging is a modality that enables depth-sectioned, molecularly-specific imaging of cells and tissue using intrinsic contrast. However, clinical applications have not been well explored due to low imaging speed and limited field of view, which make evaluating large pathology samples extremely challenging. To address these limitations, we have developed direct temporal sampling two photon fluorescent lifetime imaging (DTS-FLIM), a method which enables a several order of magnitude increase in imaging speed by capturing an entire lifetime decay in a single fluorescent excitation. We use this greatly increased speed to perform a preliminary study using gigapixel-scale imaging of human breast pathology surgical specimens. PMID:26600997

  8. Electronic-resonance-enhanced coherent anti-Stokes Raman scattering of nitric oxide: Saturation and Stark effects

    NASA Astrophysics Data System (ADS)

    Chai, Ning; Lucht, Robert P.; Kulatilaka, Waruna D.; Roy, Sukesh; Gord, James R.

    2010-08-01

    A theoretical analysis of electronic-resonance-enhanced (ERE) coherent anti-Stokes Raman scattering (CARS) of NO is described. The time-dependent density-matrix equations for the nonlinear ERE-CARS process are derived and manipulated into a form suitable for direct numerical integration. In the ERE-CARS configuration considered in this paper, the pump and Stokes beams are far from electronic-resonance. The visible 532 and 591 nm laser beams are used to excite Q-branch Raman resonances in the vibrational bands of the X Π2 electronic state of NO. An ultraviolet probe beam at 236 nm is used to excite P-, Q-, or R-branch transitions in the (v '=0, v″=1) band of the A Σ2+-X Π2 electronic system of NO molecule. Experimental spectra are obtained either by scanning the ultraviolet probe beam while keeping the Stokes frequency fixed (probe scans) or by scanning the Stokes frequency while keeping the probe frequency fixed (Stokes scans). The calculated NO ERE-CARS spectra are compared with experimental spectra, and good agreement is observed between theory and experiment in terms of spectral peak locations and relative intensities. The effects of saturation of the two-photon Raman-resonant Q-branch transitions, the saturation of a one-photon electronic-resonant P-, Q-, or R-branch transitions in the A Σ2+-X Π2 electronic system, and the coupling of these saturation processes are investigated. The coupling of the saturation processes for the probe and Raman transitions is complex and exhibits behavior similar to that observed in the electromagnetic induced transparency process. The probe scan spectra are significantly affected by Stark broadening due to the interaction of the pump and Stokes radiation with single-photon resonances between the upper vibration-rotation probe level in the A Σ2+ electronic levels and vibration-rotation levels in higher lying electronic levels. The ERE-CARS signal intensity is found to be much less sensitive to variations in the

  9. Endogenous Fluorophores Enable Two-Photon Imaging of the Primate Eye

    PubMed Central

    Palczewska, Grazyna; Golczak, Marcin; Williams, David R.; Hunter, Jennifer J.; Palczewski, Krzysztof

    2014-01-01

    Purpose. Noninvasive two-photon imaging of a living mammalian eye can reveal details of molecular processes in the retina and RPE. Retinyl esters and all-trans-retinal condensation products are two types of retinoid fluorophores present in these tissues. We measured the content of these two types of retinoids in monkey and human eyes to validate the potential of two-photon imaging for monitoring retinoid changes in human eyes. Methods. Two-photon microscopy (TPM) was used to visualize excised retina from monkey eyes. Retinoid composition and content in human and monkey eyes were quantified by HPLC and mass spectrometry (MS). Results. Clear images of inner and outer segments of rods and cones were obtained in primate eyes at different eccentricities. Fluorescence spectra from outer segments revealed a maximum emission at 480 nm indicative of retinols and their esters. In cynomolgus monkey and human retinal extracts, retinyl esters existed predominantly in the 11-cis configuration along with notable levels of 11-cis-retinol, a characteristic of cone-enriched retinas. Average amounts of di-retinoid-pyridinium-ethanolamine (A2E) in primate and human eyes were 160 and 225 pmol/eye, respectively. Conclusions. These data show that human retina contains sufficient amounts of retinoids for two-photon excitation imaging. Greater amounts of 11-cis-retinyl esters relative to rodent retinas contribute to the fluorescence signal from both monkey and human eyes. These observations indicate that TPM imaging found effective in mice could detect early age- and disease-related changes in human retina. PMID:24970255

  10. All-versus-nothing violation of local realism by two-photon, four-dimensional entanglement.

    PubMed

    Yang, Tao; Zhang, Qiang; Zhang, Jun; Yin, Juan; Zhao, Zhi; Zukowski, Marek; Chen, Zeng-Bing; Pan, Jian-Wei

    2005-12-01

    We develop and exploit a source of two-photon, four-dimensional entanglement to report the first two-particle all-versus-nothing test of local realism with a linear optics setup, but without resorting to a noncontextuality assumption. Our experimental results are in good agreement with quantum mechanics while in extreme contradiction to local realism. Potential applications of our experiment are briefly discussed.

  11. High volume confinement in two-photon fluorescence correlation spectroscopy with radially polarized light

    NASA Astrophysics Data System (ADS)

    Ivanov, D.; Shcheslavskiy, V.; Märki, I.; Leutenegger, M.; Lasser, T.

    2009-02-01

    We present the results on two-photon total-internal-reflection fluorescence correlation spectroscopy. The combination of liquid crystal spatial light modulator, providing radial polarization, with ultrafast laser (picosecond Nd:GdVO4 laser) allowed us to take the advantage of nonlinear optical contrast mechanisms to suppress the side-lobe energy specific for radial polarization and reduce the effective excited volume twice compared to one-photon evanescent wave excitation in fluorescence correlation spectroscopy.

  12. High volume confinement in two-photon total-internal-reflection fluorescence correlation spectroscopy

    NASA Astrophysics Data System (ADS)

    Ivanov, D.; Shcheslavskiy, V.; Märki, I.; Leutenegger, M.; Lasser, T.

    2009-02-01

    We report results on two-photon total-internal-reflection fluorescence correlation spectroscopy with radially polarized light. The combination of liquid crystal spatial light modulator, providing radial polarization with ultrafast laser (picosecond Nd:GdVO4 laser), allowed us to take the advantage of nonlinear optical contrast mechanisms to suppress the side-lobe energy specific for radial polarization and reduce the effective excited volume twice compared to one-photon evanescent wave excitation in fluorescence correlation spectroscopy.

  13. Two-photon photoemission and the dynamics of electrons at interfaces

    SciTech Connect

    Padowitz, D.F.; Harris, C.B.; Jordan, R.E.; Lingle, R.L. Jr.; McNeill, J.D.; Merry, W.R.

    1994-01-01

    A new instrument for angle-resolved two-photon photoemission with exceptional sensitivity and energy resolution has allowed a detailed examination of the interaction of image-state electrons with adsorbates. In addition to measuring the electrostatic properties of molecular-thickness films, the technique serves as a probe of adsorbate growth modes, and provides new opportunities to explore the dynamics of electrons in well-controlled two-dimensional systems.

  14. Acute two-photon imaging of the neurovascular unit in the cortex of active mice

    PubMed Central

    Tran, Cam Ha T.; Gordon, Grant R.

    2015-01-01

    In vivo two-photon scanning fluorescence imaging is a powerful technique to observe physiological processes from the millimeter to the micron scale in the intact animal. In neuroscience research, a common approach is to install an acute cranial window and head bar to explore neocortical function under anesthesia before inflammation peaks from the surgery. However, there are few detailed acute protocols for head-restrained and fully awake animal imaging of the neurovascular unit during activity. This is because acutely performed awake experiments are typically untenable when the animal is naïve to the imaging apparatus. Here we detail a method that achieves acute, deep-tissue two-photon imaging of neocortical astrocytes and microvasculature in behaving mice. A week prior to experimentation, implantation of the head bar alone allows mice to train for head-immobilization on an easy-to-learn air-supported ball treadmill. Following just two brief familiarization sessions to the treadmill on separate days, an acute cranial window can subsequently be installed for immediate imaging. We demonstrate how running and whisking data can be captured simultaneously with two-photon fluorescence signals with acceptable movement artifacts during active motion. We also show possible applications of this technique by (1) monitoring dynamic changes to microvascular diameter and red blood cells in response to vibrissa sensory stimulation, (2) examining responses of the cerebral microcirculation to the systemic delivery of pharmacological agents using a tail artery cannula during awake imaging, and (3) measuring Ca2+ signals from synthetic and genetically encoded Ca2+ indicators in astrocytes. This method will facilitate acute two-photon fluorescence imaging in awake, active mice and help link cellular events within the neurovascular unit to behavior. PMID:25698926

  15. A Highly Selective Ratiometric Two-Photon Fluorescent Probe for Human Cytochrome P450 1A.

    PubMed

    Dai, Zi-Ru; Ge, Guang-Bo; Feng, Lei; Ning, Jing; Hu, Liang-Hai; Jin, Qiang; Wang, Dan-Dan; Lv, Xia; Dou, Tong-Yi; Cui, Jing-Nan; Yang, Ling

    2015-11-18

    Cytochrome P450 1A (CYP1A), one of the most important phase I drug-metabolizing enzymes in humans, plays a crucial role in the metabolic activation of procarcinogenic compounds to their ultimate carcinogens. Herein, we reported the development of a ratiometric two-photon fluorescent probe NCMN that allowed for selective and sensitive detection of CYP1A for the first time. The probe was designed on the basis of substrate preference of CYP1A and its high capacity for O-dealkylation, while 1,8-naphthalimide was selected as fluorophore because of its two-photon absorption properties. To achieve a highly selective probe for CYP1A, a series of 1,8-naphthalimide derivatives were synthesized and used to explore the potential structure-selectivity relationship, by using a panel of human CYP isoforms for selectivity screening. After screening and optimization, NCMN displayed the best combination of selectivity, sensitivity and ratiometric fluorescence response following CYP1A-catalyzed O-demetylation. Furthermore, the probe can be used to real-time monitor the enzyme activity of CYP1A in complex biological systems, and it has the potential for rapid screening of CYP1A modulators using tissue preparation as enzyme sources. NCMN has also been successfully used for two-photon imaging of intracellular CYP1A in living cells and tissues, and showed high ratiometric imaging resolution and deep-tissue imaging depth. In summary, a two-photon excited ratiometric fluorescent probe NCMN has been developed and well-characterized for sensitive and selective detection of CYP1A, which holds great promise for bioimaging of endogenous CYP1A in living cells and for further investigation on CYP1A associated biological functions in complex biological systems.

  16. Tailored probes for atomic force microscopy fabricated by two-photon polymerization

    NASA Astrophysics Data System (ADS)

    Göring, Gerald; Dietrich, Philipp-Immanuel; Blaicher, Matthias; Sharma, Swati; Korvink, Jan G.; Schimmel, Thomas; Koos, Christian; Hölscher, Hendrik

    2016-08-01

    3D direct laser writing based on two-photon polymerization is considered as a tool to fabricate tailored probes for atomic force microscopy. Tips with radii of 25 nm and arbitrary shape are attached to conventionally shaped micro-machined cantilevers. Long-term scanning measurements reveal low wear rates and demonstrate the reliability of such tips. Furthermore, we show that the resonance spectrum of the probe can be tuned for multi-frequency applications by adding rebar structures to the cantilever.

  17. Highly-efficient entangled two-photon absorption with the assistance of plasmon nanoantenna

    NASA Astrophysics Data System (ADS)

    Oka, Hisaki

    2015-06-01

    We propose an efficient reaction field for entangled photons utilizing a localized-surface-plasmon (LSP) nanoantenna system. The LSP nanoantenna system consists of two nanometals embedded in a microcavity. For two-photon absorption in a molecule as an example, we show that the excitation population is considerably enhanced by properly choosing the LSP-microcavity parameters. This huge enhancement is attributed to the synergistic effects of the LSP antenna effect and the enhancement effect by entangled photons.

  18. Simultaneous imaging of multiple focal planes using a two-photon scanning microscope

    NASA Astrophysics Data System (ADS)

    Amir, W.; Carriles, R.; Hoover, E. E.; Planchon, T. A.; Durfee, C. G.; Squier, J. A.

    2007-06-01

    Despite all the advances in nonlinear microscopy, all existing instruments are constrained to obtain images of one focal plane at a time. In this Letter we demonstrate a two-photon absorption fluorescence scanning microscope capable of imaging two focal planes simultaneously. This is accomplished by temporally demultiplexing the signal coming from two focal volumes at different sample depths. The scheme can be extended to three or more focal planes.

  19. Development and design of advanced two-photon microscope used in neuroscience

    NASA Astrophysics Data System (ADS)

    Doronin, M. S.; Popov, A. V.

    2016-08-01

    This work represents the real steps to development and design advanced two-photon microscope by efforts of laboratory staff. Self-developed microscopy system provides possibility to service it and modify the structure of microscope depending on highly specialized experimental design and scientific goals. We are presenting here module-based microscopy system which provides an opportunity to looking for new applications of this setup depending on laboratories needs using with galvo and resonant scanners.

  20. Two-photon excitation STED microscopy in two colors in acute brain slices.

    PubMed

    Bethge, Philipp; Chéreau, Ronan; Avignone, Elena; Marsicano, Giovanni; Nägerl, U Valentin

    2013-02-19

    Many cellular structures and organelles are too small to be properly resolved by conventional light microscopy. This is particularly true for dendritic spines and glial processes, which are very small, dynamic, and embedded in dense tissue, making it difficult to image them under realistic experimental conditions. Two-photon microscopy is currently the method of choice for imaging in thick living tissue preparations, both in acute brain slices and in vivo. However, the spatial resolution of a two-photon microscope, which is limited to ~350 nm by the diffraction of light, is not sufficient for resolving many important details of neural morphology, such as the width of spine necks or thin glial processes. Recently developed superresolution approaches, such as stimulated emission depletion microscopy, have set new standards of optical resolution in imaging living tissue. However, the important goal of superresolution imaging with significant subdiffraction resolution has not yet been accomplished in acute brain slices. To overcome this limitation, we have developed a new microscope based on two-photon excitation and pulsed stimulated emission depletion microscopy, which provides unprecedented spatial resolution and excellent experimental access in acute brain slices using a long-working distance objective. The new microscope improves on the spatial resolution of a regular two-photon microscope by a factor of four to six, and it is compatible with time-lapse and simultaneous two-color superresolution imaging in living cells. We demonstrate the potential of this nanoscopy approach for brain slice physiology by imaging the morphology of dendritic spines and microglial cells well below the surface of acute brain slices.

  1. Enhanced weak-signal sensitivity in two-photon microscopy by adaptive illumination.

    PubMed

    Chu, Kengyeh K; Lim, Daryl; Mertz, Jerome

    2007-10-01

    We describe a technique to enhance both the weak-signal relative sensitivity and the dynamic range of a laser scanning optical microscope. The technique is based on maintaining a fixed detection power by fast feedback control of the illumination power, thereby transferring high measurement resolution to weak signals while virtually eliminating the possibility of image saturation. We analyze and demonstrate the benefits of adaptive illumination in two-photon fluorescence microscopy.

  2. Quantum teleportation of a generic two-photon state with weak cross-Kerr nonlinearities

    NASA Astrophysics Data System (ADS)

    Wang, Meiyu; Yan, Fengli

    2016-08-01

    We present a scheme for teleporting a generic two-photon polarization state by using two EPR states as quantum channel based on weak cross-Kerr nonlinearities. As the core component of the present framework, the quantum nondemolition detector based on the weak cross-Kerr nonlinearity acts as an EPR entangler as well as the Bell-state analyzer. This makes the teleportation protocol be achieved near deterministically and be feasible in the current experimental technology.

  3. Two-photon fluorescent probes of biological Zn(II) derived from 7-hydroxyquinoline.

    PubMed

    Chen, Xiao-Yun; Shi, Jing; Li, Yi-Ming; Wang, Feng-Liang; Wu, Xu; Guo, Qing-Xiang; Liu, Lei

    2009-10-01

    A new fluorescent probe for monitoring Zn(2+) was synthesized based on the structure of 7-hydroxyquinoline. Compared with 8-substituted quinolines, the new probe exhibited higher selectivity for Zn(2+) over Cd(2+). Its fluorescence enhancement (14-fold) and nanomolar range sensitivity (K(d) = 0.117 nM) were favorable toward biological applications. Experiments also showed that a cell-permeable derivative of the new probe was potentially useful for two-photon imaging in living cells.

  4. Tunable pattern transitions in a liquid-crystal-monomer mixture using two-photon polymerization.

    PubMed

    Jisha, Chandroth P; Hsu, Kuei-Chu; Lin, Yuanyao; Lin, Ja-Hon; Jeng, Chien-Chung; Lee, Ray-Kuang

    2012-12-01

    Through two-photon lithographic processes, we report experimentally and numerically a series of photoinduced tunable polymerization patterns in shapes from straight channel, serpentine curve, to periodic grating when an ultrashort femtosecond laser pulse directly writes in a liquid-crystal-monomer mixture along a line for different scanning speeds. Laser beams with polarization perpendicular to the direction of writing and the alignment of liquid crystals, produce snake-shaped patterns at an intermediate scan rate. PMID:23202094

  5. Measurement of optical trapping forces by use of the two-photon-excited fluorescence of microspheres.

    PubMed

    Kachynski, A V; Kuzmin, A N; Pudavar, H E; Kaputa, D S; Cartwright, A N; Prasad, P N

    2003-12-01

    A novel technique for the calibration of laser trapping systems that utilizes two-photon-excited fluorescence of commercial dye-stained microspheres has been demonstrated. The trapping forces as well as the trapping efficiency have been measured for various liquid environments and trapping depths. The trapping efficiency in water was found to decrease with an increase of trapping depths because of the enlargement of the trapping beam waist caused by aberrations of the optical system.

  6. Intravital two-photon imaging: a versatile tool for dissecting the immune system.

    PubMed

    Ishii, Taeko; Ishii, Masaru

    2011-03-01

    During the past decade, multi-photon or 'two-photon' excitation microscopy has launched a new era in the field of biological imaging. The near-infrared excitation laser for two-photon microscopy can penetrate thicker specimens, enabling the visualisation of living cell behaviour deep within tissues and organs without thin sectioning. The minimised photobleaching and toxicity enables the visualisation of live and intact specimens for extended periods. In this brief review, recent findings in intravital two-photon imaging for the physiology and pathology of the immune system are discussed. The immune system configures highly dynamic networks, where many cell types actively travel throughout the body and interact with each other in specific areas. Hence, real-time intravital imaging may be a powerful tool for dissecting the mechanisms of this dynamic system. The most unique characteristic of the immune system is its highly dynamic nature. A variety of cell types, such as lymphocytes, macrophages and dendritic cells (DCs), are continuously circulating throughout the body, migrating through the peripheral tissues and interacting with each other in their respective niches. Conventional methodologies in immunology, such as flow cytometry, cell or tissue culture, biochemistry and histology, have brought tremendous achievement within this field, although the dynamics of immune cells in an entire animal remain less clear. Technological progress of fluorescence microscopy has enabled us to visualise the intact biological phenomenon that has been uninvestigated. Among the advancements, the recent emergence and prevalence of two-photon, excitation-based, laser microscopy has revolutionised the research field, such that the dynamic behaviour of cells deep inside living organs can be visualised and analysed.

  7. Reversible two-photon fluorescent probe for imaging of hypochlorous acid in live cells and in vivo.

    PubMed

    Zhang, Wei; Liu, Wei; Li, Ping; kang, Junqing; Wang, Jiaoyang; Wang, Hui; Tang, Bo

    2015-06-25

    Herein, we have developed a novel reversible two-photon fluorescent probe that is well suited for monitoring HOCl levels selectively and instantaneously. Results showed the reversible and instantaneous responses of the probe towards intracellular HOCl. Moreover, the probe was successfully applied to the imaging of the HOCl levels in zebrafish and mice via two-photon imaging.

  8. Determination of Two-Photon Absorption Cross-Section of Noble Gases for Calibration of Laser Spectroscopic Techniques

    SciTech Connect

    Rosa, M. I. de la; Perez, C.; Gruetzmacher, K.; Fuentes, L. M.

    2008-10-22

    The objective of our work is to apply two-photon polarization spectroscopy as a new calibration method for the determination of two-photon excitation cross-sections of noble gases, like Xe and Kr, which are commonly used for calibrations of MP-LIF techniques in other laboratories.

  9. 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.

  10. 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. PMID:26962676

  11. Polarization and spectral characteristics of the two-photon luminescence from colloidal gold nanoparticles excited by tunable laser radiation

    SciTech Connect

    Yashunin, D. A. Korytin, A. I.; Stepanov, A. N.

    2015-12-15

    We have experimentally studied two-photon luminescence from a colloidal solution of spherical gold nanoparticles by tuning the wavelength of the exciting radiation. The measured polarization and spectral characteristics of the two-photon luminescence signal show that the observed nonlinear optical response is determined by the dimers present in the solution with a concentration of a few percent of total nanoparticle number.

  12. Spectroscopy of α,ω-dithienyl polyenes: evidence for two-photon absorption states from fluorescence studies

    NASA Astrophysics Data System (ADS)

    Natarajan, Lalgudi V.; Kirkpatrick, Sean M.; Sutherland, Richard L.; Sowards, Laura A.; Spangler, Charles W.; Fleitz, Paul A.; Cooper, Thomas M.

    1998-10-01

    The photophysics of a series (alpha) ,(omega) -dithienyl polyenes was studied. Both one photon excited fluorescence and fluorescence originating from two photon absorption states were investigated. There is strong evidence of two photon absorption from fluorescence studies in agreement with our earlier studies involving nonlinear absorption.

  13. Two-photon fluorescence and fluorescence imaging of two styryl heterocyclic dyes combined with DNA

    NASA Astrophysics Data System (ADS)

    Gao, Chao; Liu, Shu-yao; Zhang, Xian; Liu, Ying-kai; Qiao, Cong-de; Liu, Zhao-e.

    2016-03-01

    Two new styryl heterocyclic two-photon (TP) materials, 4-[4-(N-methyl)styrene]-imidazo [4,5-f][1,10] phenanthroline-benzene iodated salt (probe-1) and 4,4- [4-(N-methyl)styrene] -benzene iodated salt (probe-2) were successfully synthesized and studied as potential fluorescent probes of DNA detection. The linear and nonlinear photophysical properties of two compounds in different solvents were investigated. The absorption, one- and two-photon fluorescent spectra of the free dye and dye-DNA complex were also examined to evaluate their photophysical properties. The binding constants of dye-DNA were obtained according to Scatchard equation with good values. The results showed that two probes could be used as fluorescent DNA probes by two-photon excitation, and TP fluorescent properties of probe-1 are superior to that of probe-2. The fluorescent method date indicated that the mechanisms of dye-DNA complex interaction may be groove binding for probe-1 and electrostatic interaction for probe-2, respectively. The MTT assay experiments showed two probes are low toxicity. Moreover, the TP fluorescence imaging of DNA detection in living cells at 800 nm indicated that the ability to locate in cell nuclei of probe-1 is better than that of probe-2.

  14. A Series of Imidazole Derivatives: Synthesis, Two-Photon Absorption, and Application for Bioimaging.

    PubMed

    Zhu, Yingzhong; Xiao, Lufei; Zhao, Meng; Zhou, Jiazheng; Zhang, Qiong; Wang, Hui; Li, Shengli; Zhou, Hongping; Wu, Jieying; Tian, Yupeng

    2015-01-01

    A new series of D-π-A type imidazole derivatives have been synthesized and characterized. Two corresponding imidazolium salts (iodine and hexafluorophosphate) were prepared from the imidazole compound. Their electron-withdrawing ability can be largely tunable by salt formation reaction or ion exchange. UV-vis absorption and single-photon fluorescence spectra have been systematically investigated in different solvents. The two-photon cross sections (δ 2PA) of the imidazole derivatives are measured by two-photon excited fluorescence (2PEF) method. Compared with those of T-1 (107 GM) and T-3 (96 GM), T-2 (imidazolium iodine salt) has a large two-photon absorption (2PA) cross section value of 276 GM. Furthermore, the cytotoxicity and applications in bioimaging for the imidazole derivatives were carried out. The results showed that T-1 can be used as a lysosomal tracker with high stability and water solubility within pHs of 4-6, while T-2 and T-3 can be used as probes for cell cytoplasm. PMID:26579544

  15. Enhanced two-photon emission in coupled metal nanoparticles induced by conjugated polymers.

    PubMed

    Guan, Zhenping; Polavarapu, Lakshminarayana; Xu, Qing-Hua

    2010-12-01

    Interactions between noble metal (Ag and Au) nanoparticles and conjugated polymers as well as their one- and two-photon emission have been investigated. Ag and Au nanoparticles exhibited extraordinary quenching effects on the fluorescence of cationic poly(fluorinephenylene). The quenching efficiency by 37-nm Ag nanoparticles is ∼19 times more efficient than that by 13-nm Au nanoparticles, and 9-10 orders of magnitude more efficient than typical small molecule dye-quencher pairs. On the other hand, the cationic conjugated polymers induce the aggregate formation and plasmonic coupling of the metal nanoparticles, as evidenced by transmission electron microscopy images and appearance of a new longitudinal plasmon band in the near-infrared region. The two-photon emissions of Ag and Au nanoparticles were found to be significantly enhanced upon addition of conjugated polymers, by a factor of 51-times and 9-times compared to the isolated nanoparticles for Ag and Au, respectively. These studies could be further extended to the applications of two-photon imaging and sensing of the analytes that can induce formation of metal nanoparticle aggregates, which have many advantages over the conventional one-photon counterparts.

  16. Two-photon absorption in gapped bilayer graphene with a tunable chemical potential.

    PubMed

    Brinkley, M K; Abergel, D S L; Clader, B D

    2016-09-14

    Despite the now vast body of two-dimensional materials under study, bilayer graphene remains unique in two ways: it hosts a simultaneously tunable band gap and electron density; and stems from simple fabrication methods. These two advantages underscore why bilayer graphene is critical as a material for optoelectronic applications. In the work that follows, we calculate the one- and two-photon absorption coefficients for degenerate interband absorption in a graphene bilayer hosting an asymmetry gap and adjustable chemical potential-all at finite temperature. Our analysis is comprehensive, characterizing one- and two-photon absorptive behavior over wide ranges of photon energy, gap, chemical potential, and thermal broadening. The two-photon absorption coefficient for bilayer graphene displays a rich structure as a function of photon energy and band gap due to the existence of multiple absorption pathways and the nontrivial dispersion of the low energy bands. This systematic work will prove integral to the design of bilayer-graphene-based nonlinear optical devices.

  17. Two-photon photoemission from image-potential states of epitaxial graphene

    NASA Astrophysics Data System (ADS)

    Gugel, Dieter; Niesner, Daniel; Eickhoff, Christian; Wagner, Stefanie; Weinelt, Martin; Fauster, Thomas

    2015-12-01

    Using angle- and time-resolved two-photon photoelectron spectroscopy we observe a single series of image-potential states of graphene on monolayer (MLG) and bilayer graphene (BLG) on SiC(0001). The first image-potential state on MLG (BLG) has a binding energy of 0.93 eV (0.84 eV). Lifetimes of the first three image-potential states of MLG are 9, 44 and 110 fs. On hydrogen-intercalated, quasi-freestanding graphene no unoccupied states are observed. We attribute this to the absence of occupied initial states for direct transitions into image-potential states at photon energies below the work function used in two-photon photoemission. The work function varies between 4.14 and 4.79 eV, but the vacuum level stays ∼4.5 eV above the Dirac point for all surfaces studied. This finding suggests that direct excitation of image-potential states cannot be achieved by doping and the electron dynamics for free-standing graphene is not accessible by two-photon photoemission using photon energies below the work function.

  18. Two-photon absorption in gapped bilayer graphene with a tunable chemical potential

    NASA Astrophysics Data System (ADS)

    Brinkley, M. K.; Abergel, D. S. L.; Clader, B. D.

    2016-09-01

    Despite the now vast body of two-dimensional materials under study, bilayer graphene remains unique in two ways: it hosts a simultaneously tunable band gap and electron density; and stems from simple fabrication methods. These two advantages underscore why bilayer graphene is critical as a material for optoelectronic applications. In the work that follows, we calculate the one- and two-photon absorption coefficients for degenerate interband absorption in a graphene bilayer hosting an asymmetry gap and adjustable chemical potential—all at finite temperature. Our analysis is comprehensive, characterizing one- and two-photon absorptive behavior over wide ranges of photon energy, gap, chemical potential, and thermal broadening. The two-photon absorption coefficient for bilayer graphene displays a rich structure as a function of photon energy and band gap due to the existence of multiple absorption pathways and the nontrivial dispersion of the low energy bands. This systematic work will prove integral to the design of bilayer-graphene-based nonlinear optical devices.

  19. Depth and resolution characterization of two-photon photoacoustic spectroscopy for noninvasive subsurface chemical diagnostics

    NASA Astrophysics Data System (ADS)

    Dahal, Sudhir; Kiser, John B.; Cullum, Brian M.

    2011-05-01

    Photoacoustic spectroscopy is a powerful optical biopsy technique that enables rapid tumor diagnosis in situ. It has also been reported that photoacoustic spectroscopy can be used to diagnose pre-malignant tissue based on the chemical differences between healthy and pre-malignant tissues. Since the acoustic signals obtained from tissues in these analyses suffer from minimum damping, photoacoustic spectroscopy can be highly sensitive. This paper focuses on the characterization of a novel multiphoton excited photoacoustic methodology for margining of malignant and pre-malignant tissues. The two-photon excitation process in tissues using nanosecond laser pulses produces ultrasonic signals that transmit through tissue with minimal attenuation. Additionally, the two-photon excitation process is highly localized since only ballistic photons contribute to the excitation process; thereby eliminating potential absorption events in tissue not of interest (i.e., along the beam path) and increasing the spatial resolution of the diagnostic technique to that achievable via optics. This work characterizes the two-photon excitation process for photoacoustic signal measurements on a model dye. Using gelatin phantoms to mimic real tissues, tissue penetration studies were performed, revealing chemical species as deep as 1.3 cm in the tissue can easily be detected using this methodology. Furthermore, the resolution of this multiphoton excitation process was determined to be as great as 50 μm (near cellular level resolution).

  20. New two-photon fluorescent probe for multiphoton microscopy in biological media

    NASA Astrophysics Data System (ADS)

    Gvishi, Raz; Berkovic, Garry; Kotler, Zvi; Krief, P.; Becker, J. Y.; Sigalov, M.; Shapiro, Lev; Khodorkovsky, Vladimir

    2003-07-01

    An important ingredient in improving Multi Photon Laser Scanning Microscopy, MPLSM, is the development of efficient two-photon fluorescent (TPF) probes. We previously reported on a new class of TPF probes, specifically designed in order to maximize their efficiency in potential MPLSM applications. The fluorophores are based on a tetraketo derivative (TK) with a symmetric structure Donor-Acceptor-Donor (D-A-D). Those fluorophores have the following properties: a) Very large two-photon absorption coefficients (δ ~ 1000GM); b) Two-photon excitation (TPE) peak wavelength strongly shifted to the red (λ ~ 1μm) c) High fluorescence quantum efficiency; d) Large Stokes shifts of the fluorescence bands. We extended our work to a new fluorophore from this class that is more suitable for biological settings. This new fluorophore has a structure of crown-TK-crown that incorporates the ability to trap metal ions such as calcium. The TPE wavelength dependence of the TK-crown derivative is very similar to its analogous linear derivative with enhancement in the value of the cross-section, due to the stronger donor moieties. The TPE cross-section for the TK-crown derivative was about δ = 950 GM at λmax = 980 nm.