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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. Detection of Ultracold Ground-State Molecules by One- and Two-Color Resonance-Enhanced Two-Photon Ionization

    NASA Astrophysics Data System (ADS)

    Li, Zhonghao; Ji, Zhonghua; Zhang, Xiang; Yuan, Jinpeng; Zhao, Yanting; Xiao, Liantuan; Jia, Suotang

    2016-08-01

    One- and two-color resonance-enhanced two-photon ionization (RETPI) is used to detect ultracold ground-state RbCs molecules which are formed via short-range photoassociation from laser-cooled atoms. The transition from the X1Σ+(v = 0) state to the 21Π(v = 10) state of ultracold RbCs molecules shows the consistence of one- and two-color RETPI. A multi-photon photoionization rate model is introduced to interpret the dependence of molecular ion intensity on photoionized laser energy, and can be used to verify the photoionization scheme. This photoionization rate model can be expanded to multi-color photoionization for all kinds of atoms and molecules, which is a powerful method of determining the photoionization scheme.

  3. 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.

  4. Competition of Resonant and Nonresonant Paths in Resonance-Enhanced Two-Photon Single Ionization of He by an Ultrashort Extreme-Ultraviolet Pulse

    NASA Astrophysics Data System (ADS)

    Ishikawa, Kenichi L.; Ueda, Kiyoshi

    2012-01-01

    We theoretically study the pulse-width dependence of the photoelectron angular distribution (PAD) from the resonance-enhanced two-photon single ionization of He by femtosecond (≲20fs) extreme-ultraviolet pulses, based on the time-dependent perturbation theory and simulations with the full time-dependent Schrödinger equation. In particular, we focus on the competition between resonant and nonresonant ionization paths, which leads to the relative phase δ between the S and D wave packets distinct from the corresponding scattering phase shift difference. When the spectrally broadened pulse is resonant with an excited level, the competition varies with pulse width, and, therefore, δ and the PAD also change with it. On the other hand, when the Rydberg manifold is excited, δ and the PAD do not much vary with the pulse width, except for the very short-pulse regime.

  5. Resonance-enhanced two-photon ionization of helium using an Ar{sup +} mode-locked laser synchronized with VUV synchrotron radiation pulses

    SciTech Connect

    Lacoursiere, Jean; Meyer, Michael; Nahon, Laurent; Morin, Paul; Larzilliere, Michel

    1995-04-01

    We report a new experimental set-up consisting in the synchronization of 74.9094 MHz pulses from a mode-locked Ar{sup +} laser with 8.32 MHz pulses of vacuum ultraviolet (VUV) synchrotron radiation from the Super-ACO storage ring of the Laboratorie pour l'Utilisation du Rayonnement Electromagnetique (LURE). The capabilities of the set-up are demonstrated in a time-resolved pump-probe (VUV+visible) experiment in which free helium atoms are resonantly ionized via the short-lived 1s3p ({sup 1}P) state. This experiment allowed us to show the relevance of this technique for the investigation of nanosecond dynamics on gas phase species.

  6. Resonance-enhanced two-photon ionization of helium using an Ar+ mode-locked laser synchronized with VUV synchrotron radiation pulses

    NASA Astrophysics Data System (ADS)

    Lacoursière, Jean; Meyer, Michael; Nahon, Laurent; Morin, Paul; Larzillière, Michel

    1995-04-01

    We report a new experimental set-up consisting in the synchronization of 74.9094 MHz pulses from a mode-locked Ar+ laser with 8.32 MHz pulses of vacuum ultraviolet (VUV) synchrotron radiation from the Super-ACO storage ring of the Laboratorie pour l'Utilisation du Rayonnement Electromagnetique (LURE). The capabilities of the set-up are demonstrated in a time-resolved pump-probe (VUV+visible) experiment in which free helium atoms are resonantly ionized via the short-lived 1s3p (1P) state. This experiment allowed us to show the relevance of this technique for the investigation of nanosecond dynamics on gas phase species.

  7. Two-photon double ionization of helium

    NASA Astrophysics Data System (ADS)

    van der Hart, Hugo W.; Feng, Liang; McKenna, Claire

    2003-12-01

    The combination of B-spline basis sets with R-matrix theory has provided a powerful tool for the description of double ionization processes. We demonstrate this first by investigating electron-impact ionization of Li2+. By applying the Floquet Ansatz, the same techniques can be employed to describe multiphoton double ionization processes through the R-matrix Floquet approach. Results for two-photon double ionization of He confirm the lower values of time-dependent close-coupling calculations compared to perturbation theory. The approach can be extended to quasi-two-electron systems through the use of model potentials. This is demonstrated by calculating photoionization cross sections near threshold for the m = 0 level of the 4s4p 1Po state of calcium.

  8. Two-Photon Ionization of Metastable Helium

    NASA Astrophysics Data System (ADS)

    Czechanski, James Poremba

    There have been relatively few investigations of multiphoton ionization from metastable helium. Of particular interest has been the work of Haberland et al. 1987 and Haberland and Oschwald 1988. In both the 1987 and 1988 papers they have described the two photon ionization of metastable helium. In each of these studies they have reported the occurrence of unexplained structure along the wings of their resonance profiles. Upon the performance of similar measurements by this study, the unexplained structure is not seen and the agreement of the experiment's measurements with the theoretical shape of the resonance curves has been good. To experimentally verify these resonance effects, we have used a tunable dye laser in conjunction with a time of flight mass spectrometer to create and detect ions from metastable helium by two-photon absorption. The use of a metastable state instead of the ground state is advantageous because of its proximity to the ionization continuum and its extended lifetime. Using a metastable state as a starting point for multiphoton absorption requires fewer photons to reach the ionization threshold. The extended lifetime of the state also makes it easy to access experimentally. For helium the singlet metastable state 2^1 S lies at 20.61 eV above the ground level with a natural lifetime of close to a millisecond. Two photons of 501.7 nm and 504.35 nm are required for the ionization processes in resonance with the 3^1P and the 3^1D states. This thesis is the accounting of the experimental process involved in the measurement of the dipole and quadrupole resonances of two photon ionization from singlet metastable helium. The study includes the description of the laser, electron gun assembly for metastable helium creation, and the time of flight mass spectrometer. A discussion of the theory of multiphoton processes is included along with the discussion of the data, its reduction and analysis, and a comparison with theoretical prediction. This study

  9. 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

  10. 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.

  11. Nonsequential two-photon double ionization of helium

    NASA Astrophysics Data System (ADS)

    Feist, J.; Nagele, S.; Pazourek, R.; Persson, E.; Schneider, B. I.; Collins, L. A.; Burgdörfer, J.

    2008-04-01

    We present accurate time-dependent ab initio calculations on fully differential and total integrated (generalized) cross sections for the nonsequential two-photon double ionization of helium at photon energies from 40 to 54 eV. Our computational method is based on the solution of the time-dependent Schrödinger equation and subsequent projection of the wave function onto Coulomb waves. We compare our results with other recent calculations and discuss the emerging similarities and differences. We investigate the role of electronic correlation in the representation of the two-electron continuum states, which are used to extract the ionization yields from the fully correlated final wave function. In addition, we study the influence of the pulse length and shape on the cross sections in time-dependent calculations and address convergence issues.

  12. 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.

  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. Flame temperature measurements by radar resonance-enhanced multiphoton ionization of molecular oxygen.

    PubMed

    Wu, Yue; Sawyer, Jordan; Zhang, Zhili; Adams, Steven F

    2012-10-01

    Here we report nonintrusive local rotational temperature measurements of molecular oxygen, based on coherent microwave scattering (radar) from resonance-enhanced multiphoton ionization (REMPI) in room air and hydrogen/air flames. Analyses of the rotational line strengths of the two-photon molecular oxygen C(3)Π(v=2)←X(3)Σ(v'=0) transition have been used to determine the hyperfine rotational state distribution of the ground X(3)Σ(v'=0) state. Rotationally resolved 2+1 REMPI spectra of the molecular oxygen C(3)Π(v=2)←X(3)Σ(v'=0) transition at different temperatures were obtained experimentally by radar REMPI. Rotational temperatures have been determined from the resulting Boltzmann plots. The measurements in general had an accuracy of ~±60 K in the hydrogen/air flames at various equivalence ratios. Discussions about the decreased accuracy for the temperature measurement at elevated temperatures have been presented. PMID:23033104

  15. Resonant enhanced multiphoton ionization studies of atomic oxygen

    NASA Technical Reports Server (NTRS)

    Dixit, S. N.; Levin, D.; Mckoy, V.

    1987-01-01

    In resonant enhanced multiphoton ionization (REMPI), an atom absorbs several photons making a transition to a resonant intermediate state and subsequently ionizing out of it. With currently available tunable narrow-band lasers, the extreme sensitivity of REMPI to the specific arrangement of levels can be used to selectively probe minute amounts of a single species (atom) in a host of background material. Determination of the number density of atoms from the observed REMPI signal requires a knowledge of the multiphoton ionization cross sections. The REMPI of atomic oxygen was investigated through various excitation schemes that are feasible with available light sources. Using quantum defect theory (QDT) to estimate the various atomic parameters, the REMPI dynamics in atomic oxygen were studied incorporating the effects of saturation and a.c. Stark shifts. Results are presented for REMPI probabilities for excitation through various 2p(3) (4S sup o) np(3)P and 2p(3) (4S sup o) nf(3)F levels.

  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. Two-photon ionization thresholds of matrix-assisted laser desorption/ionization matrix clusters.

    PubMed

    Lin, Q; Knochenmuss, R

    2001-01-01

    Direct two-photon ionization of the matrix has been considered a likely primary ionization mechanism in matrix-assisted laser desorption/ionization (MALDI) mass spectrometry. This mechanism requires that the vertical ionization threshold of matrix materials be below twice the laser photon energy. Because dimers and larger aggregates may be numerous in the early stages of the MALDI plume expansion, their ionization thresholds are important as well. We have used two-color two-photon ionization to determine the ionization thresholds of jet cooled clusters of an important matrix, 2,5-dihydroxy benzoic acid (DHB), and mixed clusters with the thermal decomposition product of DHB, hydroquinone. The thresholds of the clusters were reduced by only a few tenths of an eV compared to the monomers, to an apparent limit of 7.82 eV for pure DHB clusters. None of the investigated clusters can be directly ionized by two nitrogen laser photons (7.36 eV), and the ionization efficiency at the thresholds is low. PMID:11507754

  18. 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.

  19. Two-photon ionization of atomic hydrogen with elliptically polarized light

    NASA Technical Reports Server (NTRS)

    Kassaee, A.; Rustgi, M. L.; Long, S. A. T.

    1988-01-01

    The theory of two-photon ionization of a hydrogenic state in the nonrelativistic dipole approximation is generalized for elliptically polarized light. An application to the metastable 2S state of atomic hydrogen is made. Significant differences in the angular distribution of the outgoing electrons are found depending upon the polarization of the photons. It is claimed that two-photon ionization employing elliptically polarized photons from lasers may provide an additional test for the theories of multiphoton ionization.

  20. Resonantly enhanced multiphoton ionization of pyrrole, N-methyl pyrrole, and furan

    SciTech Connect

    Cooper, C.D.; Williamson, A.D.; Miller, J.C.; Compton, R.N.

    1980-08-15

    The resonantly enhanced multiphoton ionization (REMPI) spectra of pyrrole (C/sub 4/H/sub 5/N), N-methyl pyrrole (C/sub 5/H/sub 7/N), and furan (C/sub 4/H/sub 4/O) have been measured in the wavelength region from 365 to 680 nm. New and previously observed Rydberg states are reported for pyrrole and furan. Vibrational constants are presented for most of the Rydberg series. Accurate ionization potentials are derived for pyrrole (8.207 +- 0.003 eV) and N-methyl pyrrole (7.94 +- 0.02 eV). A strong two photon allowed transition is observed in N-methyl pyrrole at 41 193 cm/sup -1/ (0,0) and is attributed to an /sup 1/A/sub 2/ state. The corresponding state is not seen in pyrrole; however, it may be obscured by overlapping Rydberg series. Mass spectra following REMPI for benzene, pyrrole, and furan are reported. The degree of ionic fragmentation depends upon laser power density and wavelength.

  1. Distinction between sequential and direct ionization in two-photon double ionization of helium

    NASA Astrophysics Data System (ADS)

    Selstø, Sølve; Raynaud, Xavier; Simonsen, Aleksander Skjerlie; Førre, Morten

    2014-11-01

    This paper aims to shed some light on the role of the direct, or nonsequential, ionization channel in the regime in which the sequential channel is open in two-photon double ionization (TPDI) of helium. In this regime the sequential channel dominates any direct contribution unless the laser pulse is of very short duration, in which case their distinction is hard to draw. Based on both a simple model and full solutions of the time-dependent Schrödinger equation, we aim to provide evidence of direct double ionization by identifying a term proportional to the pulse duration in the double ionization yield. Indeed, such a term is identified in the energy-differential yield. When it comes to the total double ionization probability, however, it turns out that the net first-order contribution is negative. The nature of the negative first-order contribution is discussed, and we argue that it is of correlated origin.

  2. Control of two-photon double ionization of helium with intense chirped attosecond laser pulses

    NASA Astrophysics Data System (ADS)

    Barmaki, S.; Lanteigne, P.; Laulan, S.

    2014-06-01

    We study the two-photon double-ionization process of the helium atom by solving numerically the nonrelativistic, time-dependent Schrödinger equation in its full dimensionality. We investigate with intense chirped attosecond laser pulses of 23.5-nm wavelength the two-photon absorption near and above the sequential threshold. We show how it is possible by adjusting the chirp parameter to control the electronic transitions inside the atom, thereby reinforcing or weakening the ionization process. Attosecond chirped laser pulses offer a promising way to probe and control the two-photon double ionization of helium when compared with attosecond transform-limited pulses.

  3. Nonsequential Two-Photon Double Ionization of Atoms: Identifying the Mechanism

    NASA Astrophysics Data System (ADS)

    Førre, Morten; Selstø, Sølve; Nepstad, Raymond

    2010-10-01

    We develop an approximate model for the process of direct (nonsequential) two-photon double ionization of atoms. Employing the model, we calculate (generalized) total cross sections as well as energy-resolved differential cross sections of helium for photon energies ranging from 39 to 54 eV. A comparison with results of ab initio calculations reveals that the agreement is at a quantitative level. We thus demonstrate that this complex ionization process can be described by the simple model, providing insight into the underlying physical mechanism. Finally, we use the model to calculate generalized cross sections for the two-photon double ionization of neon in the nonsequential regime.

  4. Triple Differential Cross sections and Nuclear Recoil in Two-Photon Double Ionization of Helium

    SciTech Connect

    Horner, Daniel A.; McCurdy, C. William; Rescigno, Thomas N

    2008-04-29

    Triple differential cross sections (TDCS) for two-photon double ionization of helium are calculated using the method of exterior complex scaling both above and below the threshold for sequential ionization (54.4 eV). It is found that sequential ionization produces characteristic behavior in the TDCS that identifies that process when it is in competition with nonsequential ionization. Moreover we see the signature in the TDCS and nuclear recoil cross sections of"virtual sequential ionization" below the threshold for the sequential process.

  5. 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.

  6. Two-photon double ionization of atomic beryllium with ultrashort laser pulses

    NASA Astrophysics Data System (ADS)

    Yip, F. L.; Palacios, A.; Martín, F.; Rescigno, T. N.; McCurdy, C. W.

    2015-11-01

    We investigate the two-photon double ionization of beryllium atom induced by ultrashort pulses. We use a time-dependent formalism to evaluate the ionization amplitudes and generalized cross sections for the ejection of the 2 s2 valence shell electrons in the presence of a fully occupied 1 s2 frozen core shell. The relative contributions of the two-photon direct and sequential process are systematically explored by varying both pulse duration and central frequency. The energy and angular differential ionization yields reveal the signatures of both mechanisms, as well as the role of electron correlation in both the single and double ionization continua. In contrast with previous results on the helium atom, the presence of an electronic core strongly affects the final state leading to back-to-back electron emission even in the a priori less correlated two-photon sequential mechanism. In particular, a dominant pathway via excitation ionization through the Be+(2 p ) determines the profiles and pulse-duration dependencies of the energy and angle differential yields.

  7. Control of the two-Photon Double Ionization of Helium with Intense Chirped Attosecond Laser Pulses

    NASA Astrophysics Data System (ADS)

    Barmaki, Samira; Laulan, Stephane

    2014-05-01

    We study the two-photon double ionization process of the helium atom by solving numerically the nonrelativistic time-dependent Schrödinger equation in its full dimensionality. We investigate with an intense chirped attosecond laser pulse of central carrier frequency that corresponds to the 29th harmonic of a Ti-sapphire laser the direct and sequential processes in helium. We show how it is possible by adjusting the chirp parameter to control the dominance of one process over the other within the atom. Attosecond chirped laser pulses offer a promising way to probe and control the two-photon double ionization of helium when compared with attosecond transform-limited pulses.

  8. Spin dynamics in nonsequential two-photon double ionization of helium in an intense laser field

    SciTech Connect

    Bhattacharyya, S.; Mazumder, Mina; Chakrabarti, J.; Faisal, F. H. M.

    2011-04-15

    Nonsequential two-photon double ionization of a two-electron system (He and He-like ions) in a circularly polarized intense laser field is developed in a relativistic field theoretic way. Antisymmetry is maintained in the correlated wave functions of He in the initial state after modification to include Dirac spinor, and in the Volkov wave functions of the two electrons in the final free state. The present theory endeavors to provide an estimate of the helicity-dependent angular asymmetry in spin-current generation in nonsequential two-photon double ionization. Angular dependence of circular dichroism obtained in this paper, in coplanar and orthogonal geometries, is compared with the only existing nonrelativistic result obtained using lowest-order perturbation theory. Present result for dichroism underestimates the nonrelativistic result. Entanglement in the spins of the ejected electrons is concluded.

  9. 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.

  10. Near-threshold photoelectron spectrum in resonant two-photon ionization of atoms

    SciTech Connect

    Raczyn-acute-accentski, A.; Zaremba, J.

    1987-11-15

    The near-threshold photoelectron spectrum in a resonant two-photon ionization process is investigated using a nonperturbative method. The hydrogen atom is represented by a realistic model including an infinite number of Rydberg states converging at the threshold. When the threshold is crossed a typical two-peak structure of the spectrum is modified by cutting off part of the spectrum which may include one or even two peaks.

  11. 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.

  12. Polarization dependence of the phase of interference between single- and two-photon ionization.

    PubMed

    Baranova, N B; Chudinov, A N; Shulginov, A A; Zel'dovich, B Y

    1991-09-01

    The interference between single-photon and two-photon ionization has been observed for electrons ejected in the direction n from the photomultiplier cathode exposed simultaneously to the picosecond pulse of a Nd laser E(omega) and its second harmonic E(2omega). The change of the phase difference of such interference was measured for the switch of the polarizations from E(omega) ||n, E(2omega) ||n to E(omega) ? n, E(2omega) || n. PMID:19776966

  13. Virtual Sequential Picture for Nonsequential Two-Photon Double Ionization of Helium

    NASA Astrophysics Data System (ADS)

    Jiang, Wei-Chao; Shan, Jun-Yi; Gong, Qihuang; Peng, Liang-You

    2015-10-01

    By using a model based on the second-order time-dependent perturbation theory, we show that the nonsequential two-photon double ionization of He can be understood in a virtual sequential picture: to excite the final double continuum state |k1,k2 ⟩ by absorbing two photons from the ground state |1 s2,1S0 ⟩ , the single continuum states |1 s ,k1 ⟩ and |1 s ,k2 ⟩ serve as the dominant intermediate states. This virtual sequential picture is verified by the perfect agreement of the total ionization cross section, respectively, calculated by this model and by the sophisticated numerical solution to the full-dimensional time-dependent Schrödinger equation. This model, without the consideration of the electron correlation in the final double continuum state, works well for a wide range of laser parameters extending from the nonsequential to the sequential regime. The present Letter demonstrates that the electron correlation in the final double continuum state is not important in evaluating the total cross section, while it is indispensable for an accurate computation of a triply differential cross section. In addition, the virtual sequential picture bridges the sequential and nonsequential two-photon double ionization and reveals connections and distinctions between them.

  14. Virtual Sequential Picture for Nonsequential Two-Photon Double Ionization of Helium.

    PubMed

    Jiang, Wei-Chao; Shan, Jun-Yi; Gong, Qihuang; Peng, Liang-You

    2015-10-01

    By using a model based on the second-order time-dependent perturbation theory, we show that the nonsequential two-photon double ionization of He can be understood in a virtual sequential picture: to excite the final double continuum state |k_{1},k_{2}⟩ by absorbing two photons from the ground state |1s^{2},^{1}S_{0}⟩, the single continuum states |1s,k_{1}⟩ and |1s,k_{2}⟩ serve as the dominant intermediate states. This virtual sequential picture is verified by the perfect agreement of the total ionization cross section, respectively, calculated by this model and by the sophisticated numerical solution to the full-dimensional time-dependent Schrödinger equation. This model, without the consideration of the electron correlation in the final double continuum state, works well for a wide range of laser parameters extending from the nonsequential to the sequential regime. The present Letter demonstrates that the electron correlation in the final double continuum state is not important in evaluating the total cross section, while it is indispensable for an accurate computation of a triply differential cross section. In addition, the virtual sequential picture bridges the sequential and nonsequential two-photon double ionization and reveals connections and distinctions between them. PMID:26550720

  15. 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.

  16. Femtosecond two-photon ionization of fluid NH3 at 9.3 eV

    NASA Astrophysics Data System (ADS)

    Urbanek, Janus; Dahmen, Annika; Torres-Alacan, Joel; Vöhringer, Peter

    2013-03-01

    Liquid and supercritical ammonia (NH3) is photo-ionized at an energy of 9.3 eV with 100-fs duration pulses at a wavelength of 266 nm. The ionization involves two photons and generates fully solvated electrons via the conduction band of the solvent within the time resolution of the experiment. The dynamics of their ensuing geminate recombination is followed in real time with femtosecond near-infrared (IR) probe pulses. The recombination mechanism can be understood as an ion-pair mediated reaction. The electron survival probability is found to be in quantitative agreement with the classical Onsager theory for the initial recombination of ions.

  17. Dynamics of two-photon double ionization of helium in short intense xuv laser pulses

    NASA Astrophysics Data System (ADS)

    Guan, Xiaoxu; Bartschat, K.; Schneider, B. I.

    2008-04-01

    We present an ab initio nonperturbative time-dependent approach to the problem of a helium atom driven by an intense xuv laser pulse. Based on the finite-element discrete-variable-representation, a space discretization is proposed for the radial grid in spherical coordinates. Absolute angle-integrated and triple-differential cross sections for double ionization by absorption of two photons are obtained over a range of photon energies between 39.5 eV (31.4 nm) and 54 eV (23 nm), where the process is dominated by nonsequential ionization mechanisms. We show that the agreement with several other sets of previous predictions is good, as long as the effective interaction time is defined properly. Two-photon double ionization at the photon energy of 57 eV (22 nm), for which both sequential and nonsequential channels are open, is also discussed. For double photoionization in the near-threshold regime, our results do not indicate a preferential mode of energy sharing between the two escaping electrons, while asymmetric energy sharing becomes the dominant mode with increasing excess energy. Overall, the two ionized electrons strongly prefer to escape along the polarization axis of linearly polarized laser fields.

  18. Femtosecond two-photon ionization and solvated electron geminate recombination in liquid-to-supercritical ammonia.

    PubMed

    Urbanek, Janus; Dahmen, Annika; Torres-Alacan, Joel; Königshoven, Peter; Lindner, Jörg; Vöhringer, Peter

    2012-02-23

    The first-ever femtosecond pump-probe study is reported on solvated electrons that were generated by multiphoton ionization of neat fluid ammonia. The initial ultrafast ionization was carried out with 266 nm laser pulses and was found to require two photons. The solvated electron was detected with a femtosecond probe pulse that was resonant with its characteristic near-infrared absorption band around 1.7 μm. Furthermore, the geminate recombination dynamics of the solvated electron were studied over wide ranges of temperature (227 K ≤ T ≤ 489 K) and density (0.17 g cm(-3) ≤ ρ ≤ 0.71 g cm(-3)), thereby covering the liquid and the supercritical phase of the solvent. The electron recombines in a first step with ammonium cations originating from the initial two-photon ionization thereby forming transient ion-pairs (e(am)(-)·NH(4)(+)), which subsequently react in a second step with amidogen radicals to reform neutral ammonia. The escape probability, i.e., the fraction of solvated electrons that can avoid the geminate annihilation, was found to be in quantitative agreement with the classical Onsager theory for the initial recombination of ions. When taking the sequential nature of the ion-pair-mediated recombination mechanism explicitly into account, the Onsager model provides a mean thermalization distance of 6.6 nm for the solvated electron, which strongly suggests that the ionization mechanism involves the conduction band of the fluid. PMID:22272761

  19. Two-photon double ionization of neon using an intense attosecond pulse train

    NASA Astrophysics Data System (ADS)

    Manschwetus, B.; Rading, L.; Campi, F.; Maclot, S.; Coudert-Alteirac, H.; Lahl, J.; Wikmark, H.; Rudawski, P.; Heyl, C. M.; Farkas, B.; Mohamed, T.; L'Huillier, A.; Johnsson, P.

    2016-06-01

    We present a demonstration of two-photon double ionization of neon using an intense extreme ultraviolet (XUV) attosecond pulse train (APT) in a photon energy regime where both direct and sequential mechanisms are allowed. For an APT generated through high-order harmonic generation (HHG) in argon we achieve a total pulse energy close to 1 μ J , a central energy of 35 eV, and a total bandwidth of ˜30 eV. The APT is focused by broadband optics in a neon gas target to an intensity of 3 ×1012W cm-2 . By tuning the photon energy across the threshold for the sequential process the double ionization signal can be turned on and off, indicating that the two-photon double ionization predominantly occurs through a sequential process. The demonstrated performance opens up possibilities for future XUV-XUV pump-probe experiments with attosecond temporal resolution in a photon energy range where it is possible to unravel the dynamics behind direct versus sequential double ionization and the associated electron correlation effects.

  20. 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.

  1. Probing Electron Correlation via Attosecond xuv Pulses in the Two-Photon Double Ionization of Helium

    SciTech Connect

    Feist, J.; Nagele, S.; Pazourek, R.; Persson, E.; Burgdoerfer, J.; Schneider, B. I.; Collins, L. A.

    2009-08-07

    Recent experimental developments of high-intensity, short-pulse extreme ultraviolet light sources are enhancing our ability to study electron-electron correlations. We perform time-dependent calculations to investigate the so-called 'sequential' regime ((Planck constant/2pi)omega>54.4 eV) in the two-photon double ionization of helium. We show that attosecond pulses allow us not only to probe but also to induce angular and energy correlations of the emitted electrons. The final momentum distribution reveals regions dominated by the Wannier ridge breakup scenario and by postcollision interaction.

  2. Attosecond timescale analysis of the dynamics of two-photon double ionization of helium

    NASA Astrophysics Data System (ADS)

    Foumouo, Emmanuel; Antoine, Philippe; Bachau, Henri; Piraux, Bernard

    2008-02-01

    We consider the two-photon double ionization (DI) of helium and analyze electron dynamics on the attosecond timescale. We first re-examine the interaction of helium with an ultrashort XUV pulse and study how the electronic correlations affect the electron angular and energy distributions in the direct, sequential and transient regimes of frequency and time duration. We then consider pump probe processes with the aim of extracting indirect information on the pump pulse. In addition, our calculations show clear evidence for the existence under certain conditions of direct two-color DI processes.

  3. Two-photon excitation/ionization of the 1s-shell of the argon atom

    NASA Astrophysics Data System (ADS)

    Novikov, S. A.; Hopersky, A. N.

    2002-02-01

    The absolute values and the shape of the two-photon excitation/ionization cross section of the 1s-shell of the argon atom are calculated with inclusion of the many-particle effects, i.e., the relaxation of the atomic residue in the field of the vacancies created, and the decay of the vacancies into the channels of Auger and (or) radiative types. The wavefunctions of the one-particle states are calculated in non-relativistic approximation. The calculations are performed for both linear and circular polarization of the laser beam.

  4. 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.

  5. Competition of sequential and direct paths in two-photon ionization of He

    NASA Astrophysics Data System (ADS)

    Ishikawa, Kenichi L.; Ma, Ri; Fukuzawa, H.; Motomura, K.; Yamada, A.; Ueda, K.; Nagaya, K.; Yase, S.; Mizoguchi, Y.; Yao, M.; Rouzee, A.; Hundermark, A.; Vrakking, M.; Johnsson, P.; Nagasono, M.; Togashi, T.; Tono, K.; Senba, Y.; Ohashi, H.; Yabashi, M.; Ishikawa, T.

    2012-11-01

    We study the photoelectron angular distribution (PAD) from the two-photon ionization (TPI) of He by femtosecond EUV pulses. The calculation with the time-dependent Schrödinger equation (TDSE) and the measurement at the SPring-8 EUV-FEL show reasonable agreement. The extracted relative phase δ between the s and d wave packets are distinct from that between the corresponding eigenstates, due to the competition between sequential and direct ionization paths. When the pulse is resonant with an excited level, the sequential and direct TPI compete with each other, and δ and the PAD depend on the pulse width. On the other hand, when the Ry-dberg manifold is coherently excited, δ does not vary with the pulse width.

  6. New electronic states of NH and ND observed by resonance enhanced multiphoton ionization spectroscopy

    NASA Technical Reports Server (NTRS)

    Johnson, Russell D., III; Hudgens, Jeffrey W.

    1990-01-01

    Resonance Enhanced MultiPhoton Ionization (REMPI) spectra of NH and ND, which reveal four new electronic states are presented. Transitions from NH a 1 delta to 3s and 3p Rydberg states in both NH and ND have been observed and rotationally analyzed. The transitions were observed in the wavelength range of 258 to 288 nm. The state assignments are: e 1 pi (3s sigma) at 82857/cm, f 1 pi (3p sigma) at 86378/cm, g 1 delta (3p pi) at 88141/cm and h 1 sigma (3p pi) at 89151/cm.

  7. 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.

  8. Nonsequential double ionization of the hydride ion by two-photon absorption

    NASA Astrophysics Data System (ADS)

    Nepstad, Raymond; Førre, Morten

    2011-08-01

    We apply a recently developed ab initio numerical framework to calculate (generalized) total cross sections for the process of nonsequential (direct) two-photon double ionization of the hydride ion (H-), at photon energies ranging from 7.75 to 10.5 eV. The total cross section is about an order of magnitude larger than the corresponding one obtained for helium, the reason being that the electronic correlation is relatively more important in H-. Furthermore, we examine single- and triple-differential cross sections at the photon energies 7.75 and 9 eV and find that for the lower photon energy the electron energy distribution attains a maximum when both electrons are emitted with equal energies.

  9. Two-photon double ionization of H{sub 2} in intense femtosecond laser pulses

    SciTech Connect

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

    2010-10-15

    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 Schroedinger 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 et al. [J. Phys. B 41, 121002 (2008)] and Morales et al. [J. Phys. B 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.

  10. 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.

  11. 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.

  12. Two-photon double ionization of atomic beryllium by ultrashort laser pulses

    NASA Astrophysics Data System (ADS)

    Yip, Frank L.; Palacios, Alicia; Martin, Fernando; Rescigno, Thomas N.; McCurdy, C. William

    2014-05-01

    A time-dependent formalism for evaluating ionization amplitudes and generalized cross sections for two-electron atoms previously used to study the correlated electron dynamics of helium under ultrashort laser pulses is adapted to study similar processes involving the 2s2 valence shell of atomic beryllium in the presence of a fully-occupied 1s2 core shell. The similar symmetry of the overall process in two-photon double ionization permits a direct comparison between Be and He atoms, revealing details about the nature of electron correlation within these two atoms whose impact is manifest in the continuum electron dynamics. In particular, consequences of the different shell structures of the initial states for He and Be are prominent when considering sequential double ionization processes. Work supported by the US Dept. of Energy, Office of Basic Energy Sciences, Chemical Sciences Contract DE-AC02-05CH11231, by the MICINN Projects No. FIS2010-15127 and ERC Advanced Grant 290853.

  13. 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.

  14. 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.

  15. 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...

  16. Zero kinetic energy (ZEKE) photoelectron spectroscopy of ammonia by nonresonant two-photon ionization from the neutral ground state

    NASA Astrophysics Data System (ADS)

    Reiser, Georg; Habenicht, Wieland; Mueller-Dethlefs, Klaus

    1993-06-01

    Results are presented of nonresonant two-photon zero kinetic energy spectroscopy of ammonia, with resolution down to 0.4/cm. The spectra provide new rotational and vibrational data on the nu(2) vibrational progression of NH3(+). The adiabatic (field corrected) ionization energy is confirmed at 82,159 +/- 1 per cm.

  17. 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.

  18. Rotational temperature analysis of N2 by resonant enhanced multi-photon ionization with fluorescence detection

    NASA Astrophysics Data System (ADS)

    Adams, Steven F.; Williamson, James M.; Fisher, Dustin M.

    2011-10-01

    A non-invasive, optical technique to determine the rotational temperature of molecular nitrogen at atmospheric pressure by direct probing of the N2(X1Σg+,v =0) ground state with subsequent analysis of the rotational state distribution is presented. A tunable probe laser was scanned over resonant-enhanced, multi-photon ionization transitions initiating from various N2(X1Σg+,v =0,J″) states. At atmospheric pressure, the laser photo-ionization also induced N2+ fluorescence bands. Analysis of the relative fluorescence as a function of laser wavelength produced a calculated N2(X1Σg+,v =0,J″) rotational state distribution and determined the rotational temperature. The analysis also resulted in the assignment and tabulation of 11 previously unreported term energies for N2(b1Πu+,v =6) and N2(b1Πu-,v =6) for J' > 22, based on the experimental data. The method resulted in temperature determinations for two experimental trials in atmospheric N2 gas flows at room temperature and 600 K that were in good agreement with thermocouple measurements in the vicinity of the laser probe region.

  19. Two-photon ionization of helium studied with the multiconfigurational time-dependent Hartree-Fock method

    SciTech Connect

    Hochstuhl, David; Bonitz, Michael

    2011-02-28

    The multiconfigurational time-dependent Hartree-Fock method (MCTDHF) is applied for simulations of the two-photon ionization of helium. We present results for the single and double ionizations from the ground state for photon energies in the nonsequential regime and compare them to direct solutions of the Schroedinger equation using the time-dependent (full) configuration interaction (TDCI) method. We find that the single ionization is accurately reproduced by MCTDHF, whereas the double ionization results correctly capture the main trends of TDCI.

  20. Method for calculating multiphoton above-threshold processes in atoms: Two-photon above-threshold ionization

    SciTech Connect

    Manakov, N. L. Marmo, S. I.; Sviridov, S. A.

    2009-04-15

    The two-photon above-threshold ionization of atoms is calculated using numerical algorithms of the Pade approximation in the model-potential method with the Coulomb asymptotics. The total and differential cross sections of the above-threshold ionization of helium and alkali metal atoms by elliptically polarized radiation are presented. The dependence of the angular distribution of photoelectrons on the sign of the ellipticity of radiation (the elliptic dichroism phenomenon) is analyzed in the above-threshold frequency range.

  1. Nuclear Recoil Cross Sections from Time-dependent Studies of Two-Photon Double Ionization of Helium

    SciTech Connect

    Horner, Daniel A.; Rescigno, Thomas N.; McCurdy, C. William

    2009-12-21

    We examine the sensitivity of nuclear recoil cross sections produced by two-photon double ionization of helium to the underlying triple differential cross sections (TDCS) used in their computation. We show that this sensitivity is greatest in the energy region just below the threshold for sequential double ionization. Accurate TDCS, extracted from non-perturbative solutions of the time-dependent Schroedinger equation, are used here in new computations of the nuclear recoil cross section.

  2. Frequency-resolved photoelectron spectra of two-photon ionization of He by an attosecond pulse train

    NASA Astrophysics Data System (ADS)

    Benis, E. P.; Tzallas, P.; Nikolopoulos, L. A. A.; Kovacev, M.; Kalpouzos, C.; Charalambidis, D.; Tsakiris, G. D.

    2006-06-01

    We present measured and calculated energy-resolved photoelectron spectra obtained through two-photon ionization of He induced by a superposition from the 9th to the 15th harmonic of a Ti:Sapph laser forming an attosecond (asec) pulse train. The reported measured spectra are a decisive step towards frequency-resolved two-XUV-photon ionization-based second-order autocorrelation (AC) of asec pulse trains, and thus towards a complete reconstruction of asec pulses.

  3. 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. PMID:23811904

  4. 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.

  5. Application of resonance-enhanced multiphoton ionization time-of-flight mass spectrometry (REMPI-TOFMS) for on-line trace analysis of combustion and pyrolysis products in technical processes

    NASA Astrophysics Data System (ADS)

    Zimmermann, Ralf; Heger, H. J.; Dorfner, R.; Kettrup, A. A.; Boesl, Ulrich

    1997-05-01

    We present first applications of resonance-enhanced multiphoton ionization time-of-flight mass spectrometry (REMPI-TOFMS) for on-line monitoring of technical water incinerator flue gases and coffee roasting process off- gases. The results were obtained with a newly developed, mobile REMPI-TOFMS device. The combination of laser induced resonance-enhanced multiphoton ionization and time-of-flight mass spectrometry represents a highly selective as well as sensitive analytical technique, well suited for species selective real-time on-line monitoring of trace-products in of-gases from thermal processes or technical incinerators. The achievable sensitivities are in the ppb-range or better for aromatic compounds. The high selectivity is due to the combination of mass- and optical selectivity, the high sensitivity is caused by the high cross sections of resonance-enhanced two photon ionization with lasers. On- line monitoring of trace chemicals, formed during combustion- or pyrolysis-processes, is useful e.g. for feed back steering of combustion processes in order to minimize the formation of hazardous byproducts or for optimization of the economic efficiency of thermal production processes.

  6. Theory of coherent polarization anisotropy in time-resolved two-photon ionization of isolated molecules. Effects of Coriolis couplings

    NASA Astrophysics Data System (ADS)

    Sato, S.; Nomura, Y.; Fujimura, Y.

    1987-09-01

    Effects of vibration-rotation (Coriolis) couplings on the coherent polarization anisotropy are theoretically studied in a time-resolved two-photon ionization of a symmetric top molecule. This polarization anisotropy originates from a coherent excitation of the resonant rovibronic molecular eigenstates (rovibronic coherence) whose zeroth order states are mixed through the Coriolis coupling. Expressions for the time-dependent degree of polarization after the coherent excitation of the rovibronic states produced by the Coriolis coupling are derived as a function of the delay time in the pump-probe two-photon ionization. Model calculations of the time-dependent degree of polarization as well as the probabilities of the two-photon ionization are performed to demonstrate the Coriolis coupling effects in the low excess energy regions of the resonant intermediate state. It is shown that oscillatory behaviors in the time-dependent degree of polarization should be observed as a result of the creation of the rovibronic coherence. It is demonstrated that oscillations of the degree of polarization involve both contribution of the purely rotational J-coherence and that of the rovibronic coherence in the resonant manifold when the rotational branches are coherently excited and the characteristic rotation-vibration interaction energy is larger than a typical free rotational energy under jet-cooled condition.

  7. 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.

  8. 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.

  9. 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.

  10. Effects of laser pulse duration and intensity on Coulomb explosion of CO2: Signatures of charge-resonance enhanced ionization

    NASA Astrophysics Data System (ADS)

    Litvinyuk, Igor V.; Bocharova, Irina; Sanderson, Joseph; Kieffer, Jean-Claude; Légaré, François

    2009-11-01

    We studied laser-induced Coulomb explosion of CO2 by full triple-coincidence momentum resolved detection of resulting ion fragments. From the coincidence momentum data we can reconstruct molecular geometry immediately before explosion. We observe the dynamics of Coulomb explosion by comparing reconstructed CO2 geometries for different Ti:Sapphire laser pulse durations (at the same intensity) ranging from few cycles (7 fs) to 200 fs. We conclude that for longer pulse durations (>=100 fs) Coulomb explosion proceeds through the enhanced ionization mechanism taking place at the critical O-O distance of 8 a.u., similarly to well known charge-resonance enhanced ionization (CREI) in H2.

  11. 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.

  12. Pulse-delay effects in the angular distribution of near-threshold EUV + IR two-photon ionization of Ne

    NASA Astrophysics Data System (ADS)

    Mondal, S.; Fukuzawa, H.; Motomura, K.; Tachibana, T.; Nagaya, K.; Sakai, T.; Matsunami, K.; Yase, S.; Yao, M.; Wada, S.; Hayashita, H.; Saito, N.; Callegari, C.; Prince, K. C.; Miron, C.; Nagasono, M.; Togashi, T.; Yabashi, M.; Ishikawa, K. L.; Kazansky, A. K.; Kabachnik, N. M.; Ueda, K.

    2014-01-01

    Photoelectron angular distributions (PADs) from two-photon near-threshold ionization of Ne atoms by the combined action of femtosecond pulses from an extreme ultraviolet (EUV) free-electron laser and infrared (IR) laser have been studied experimentally and theoretically. Solutions of the time-dependent Schrödinger equation indicate that the PADs strongly depend on the time delay between EUV and IR pulses. The experimental results obtained for two extreme cases of completely overlapping and nonoverlapping pulses fully confirm the prediction, illustrating that the measurements of the time-delay dependence of the PAD provide a tool for investigating the fundamental problem of the relative importance of the resonant and nonresonant pathways in the two-color two-photon processes.

  13. Electron angular distributions of noble gases in sequential two-photon double ionization

    NASA Astrophysics Data System (ADS)

    Braune, M.; Hartmann, G.; Ilchen, M.; Knie, A.; Lischke, T.; Reinköster, A.; Meissner, A.; Deinert, S.; Glaser, L.; Al-Dossary, O.; Ehresmann, A.; Kheifets, A. S.; Viefhaus, J.

    2016-02-01

    We present an angle resolved study of photoelectrons emitted from ions of the noble gases neon, argon and krypton by means of time-of-flight spectroscopy. The ionic targets are generated in a sequential two-photon process induced by the free-electron laser FLASH. Values of the anisotropy parameters ? and ? are derived from electron angular distribution measurements in the photon energy range from 38 to 91 eV and compared with recent theoretical calculations.

  14. Polarization effects in two-photon nonresonant ionization of argon with extreme-ultraviolet and infrared femtosecond pulses

    SciTech Connect

    O'Keeffe, P.; Lopez-Martens, R.; Mauritsson, J.; Johansson, A.; L'Huillier, A.; Veniard, V.; Taieeb, R.; Maquet, A.; Meyer, M.

    2004-05-01

    We report the results of experimental and theoretical investigations of the two-color, two-photon ionization of Ar atoms, using femtosecond pulses of infrared laser radiation in combination with its extreme-ultraviolet harmonics. It is shown that the intensities of the photoelectron lines resulting from the absorption of photons from both fields strongly depend both on the respective phases of the fields and on atomic quantities such as the asymmetry parameter. These phases, which are notoriously difficult to measure, can be estimated by changing the polarization state of the laser radiation.

  15. 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.

  16. (2 + 1) resonant enhanced multiphoton ionization of H2 via the E,F 1Sigma(+)g state

    NASA Technical Reports Server (NTRS)

    Rudolph, H.; Lynch, D. L.; Dixit, S. N.; Mckoy, V.; Huo, Winifred M.

    1987-01-01

    In this paper, the results of ab initio calculations of photoelectron angular distributions and vibrational branching ratios for the (2 + 1) resonant enhanced multiphoton ionization (REMPI) of H2 via the E,F 1Sigma(+)g state are reported, and these are compared with the experimental data of Anderson et al. (1984). These results show that the observed non-Franck-Condon behavior is predominantly due to the R dependence of the transition matrix elements, and to a lesser degree to the energy dependence. This work presents the first molecular REMPI study employing a correlated wave function to describe the Rydberg-valence mixing in the resonant intermediate state.

  17. Two-photon double ionization of helium by chirped few-cycle attosecond pulses: From nonsequential to sequential regime

    NASA Astrophysics Data System (ADS)

    Yao, Tong; Wei-Chao, Jiang; Pan, Wu; Liang-You, Peng

    2016-07-01

    The two-photon double ionization (TPDI) dynamics of helium by chirped attosecond pulses are theoretically studied by solving the two-electron time-dependent Schrödinger equation in its full dimensions. We show that both the differential and the total double ionization probability can be significantly controlled by adjusting the chirp. The dependence of the TPDI on the chirp can be quite different for different photon energies, relying on the central photon energy being in the sequential region, nonsequential region, or translation region. The physics which lead to the chirp dependence for different photon energies are addressed. Present findings are well reproduced by a model based on the second-order time-dependent perturbation theory. Project supported by the National Natural Science Foundation of China (Grant Nos. 11322437 and 11574010) and the National Basic Research Project of China (Grant No. 2013CB922402).

  18. Interfering one-photon and two-photon ionization by femtosecond VUV pulses in the region of an intermediate resonance

    NASA Astrophysics Data System (ADS)

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

    2015-06-01

    The electron angular distribution after atomic photoionization by the fundamental frequency and its second harmonic is analyzed for a case when the frequency of the fundamental scans the region of an intermediate atomic state. The angular distribution and its left-right asymmetry, due to the two-pathway interference between nonresonant one-photon and resonant two-photon ionization, sharply change as a function of the photon energy. The phenomenon is exemplified by both solving the time-dependent Schrödinger equation on a numerical space-time grid and by applying perturbation theory for ionization of the hydrogen atom in the region of the 1 s -2 p transition for femtosecond pulses as well as an infinitely long exposure to the radiation. Parametrizations for the asymmetry and the anisotropy coefficients, obtained within perturbation theory, reveal general characteristics of observable quantities as functions of the parameters of the radiation beam.

  19. 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.

  20. Identification of Two Allylbenzene Conformers by One- and Two-Photon Resonant Multiphoton Ionization Spectroscopy in a Supersonic Jet

    NASA Astrophysics Data System (ADS)

    Philis, John G.; Kosmidis, Constantine

    1997-02-01

    Two allylbenzene conformers have been identified using resonance-enhanced multiphoton ionization spectroscopy (REMPI) in a supersonic jet expansion. Their existence has been confirmed by the vibrational analysis of theS1← S0ππ* transition, recorded under (1 + 1) and (2 + 2) REMPI schemes and by the intensity variation of their spectra under various expansion conditions. The conformer with higher excitation energy shows strong dependence on the terminal beam temperature, which is consistent with a shallow potential energy well as predicted by theory. The relative abundance of the two conformers and the frequency values of several vibrational modes in their lower excited singlet electronic stateS1have been determined.

  1. 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.

  2. Suppression of ionization probability due to Rabi oscillations in the resonance two-photon ionization of He by EUV free-electron lasers

    SciTech Connect

    Sako, Tokuei; Adachi, Junichi; Yagishita, Akira; Yabashi, Makina; Tanaka, Takashi; Nagasono, Mitsuru; Ishikawa, Tetsuya

    2011-11-15

    The two-photon resonance ionization probability of atoms in strong extreme-ultraviolet free-electron laser (EUV FEL) pulses has been investigated by the model of time-dependent wave packet propagation of a light-coupled multilevel atom. Under the simulation within the model assuming single-mode FEL pulses, the ionization probability P{sub ion} has shown characteristic dependences on the scaled coupling parameter U{sub gi} between two levels of the ground (g) and intermediate (i) resonance states, namely, P{sub ion}{proportional_to}(U{sub gi}){sup n}, with n being equal to {approx}2, less than 1, and {approx}1 for the small, medium, and large U{sub gi} regimes, respectively. This power dependence of the ionization probability has been interpreted due to Rabi oscillations between g and i states. To compare with recent experimental results on the same condition, the multimode nature of self-amplitude spontaneous emission (SASE) FEL pulses has been managed in the simulation. Then, the recent experimental laser-power dependence of the two-photon resonance ionization of He [Sato et al., J. Phys. B 44, 161001 (2011)] has been well described by that for the large U{sub gi} regime of the simulation, i.e., n{approx} 1. Thus, the observed linear laser-power dependence has been rationalized as being caused by the strong Rabi oscillations between the (2p)-(1s) states.

  3. Angular distribution in two-photon double ionization of helium by intense attosecond soft-x-ray pulses

    NASA Astrophysics Data System (ADS)

    Barna, Imre F.; Wang, Jianyi; Burgdörfer, Joachim

    2006-02-01

    We investigate two-photon double ionization of helium by intense (≈1015W/cm2) ultrashort (≈300as) soft-x-ray pulses (E=91.6eV) . The time-dependent two-electron Schrödinger equation is solved using a coupled channel method. We show that for ultrashort pulses the angular distribution of ejected electrons depends on the pulse duration and provides insight into the role of electron correlations in the two-electron photoemission process. The angular distribution at energies near the “independent-electron” peaks is close to dipolar while it acquires in the “valley” of correlated emission a significant quadrupolar component within a few hundred attoseconds.

  4. 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.

  5. 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.

  6. Excited state spectroscopy of para di-substituted benzenes in a supersonic beam using resonant two photon ionization

    NASA Astrophysics Data System (ADS)

    Tembreull, R.; Dunn, T. M.; Lubman, D. M.

    Excited state vibronic spectra of p-aminophenol, p-cresol, p-fluoroaniline, p-fluorophenol, hydroquinone and p-toluidine have been obtained using resonant two photon ionization supersonic beam mass spectrometry. Despite marked similarities in the spectra, notable differences exist and different para polyatomic substituents in the same molecule show vibronic evidence of their real molecular symmetry of C2ν. Expansion of the ring is also noted upon excitation in all cases. Further, it is now evident that the assignment of some vibronic bands historically interpreted as sequence structure must be reconsidered since molecules like hydroquinone are mixtures of cis and trans and others have a vibronic structure arising from the polyatomic nature of the substituents ( cƒ. CH 3).

  7. Mechanism of Resonance-enhanced X-ray Multiple Ionization of Argon Atom in an XFEL Pulse

    NASA Astrophysics Data System (ADS)

    Young, Linda; Ho, Phay

    2014-05-01

    We present a new Monte Carlo rate equation (MCRE) approach to examine the inner-shell ionization dynamics of atoms in an intense x-ray free-electron laser (XFEL) pulse. In addition to photoionization, Auger decay and fluorescence processes, we include bound-to-bound transitions in the rate equation calculations. This computational tool allows us to account for ``hidden resonances'' unveiled in high charge states of atom in XFEL pulse. Using our MCRE approach, we investigated the ionization dynamics of Argon atom exposed to an 480-eV XFEL pulse. At this photon energy, it is not energetically allowed to produce Ar ions with charge 10 + and higher via direct one-photon L-shell ionization. Rather, we found that the resonance-enhanced x-ray multiple ionization (REXMI) pathways play a dominant role in producing these highly charged ions. Our calculated results agree with the measured Ar ion yield data. More importantly, we account for the pulse-duration dependence of experimental ion yield data and identify the responsible REXMI pathways where excitation of multiple electrons into outer valence and Rydberg orbitals are followed by autoionization. Supported by the Chemical Sciences, Geosciences, and Biosciences Di- vision, Office of Basic Energy Sciences, Office of Science, US Dept of Energy, Contract DE-AC02-06CH11357.

  8. 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).

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

    NASA Astrophysics Data System (ADS)

    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.

  10. 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

  11. 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.

  12. 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.

  13. 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

  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. 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.

  16. 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

  17. Population inversion of molecular nitrogen in an Ar: N2 mixture by selective resonance-enhanced multiphoton ionization

    NASA Astrophysics Data System (ADS)

    Shneider, M. N.; Baltuška, A.; Zheltikov, A. M.

    2011-10-01

    Resonance-enhanced multiphoton ionization (REMPI) is shown to offer an attractive strategy for population inversion of molecular nitrogen in an Ar: N2 gas mixture. We present a detailed analysis of the key processes leading to a population inversion of molecular nitrogen in a REMPI-pumped Ar: N2 gas mixture, including a (3 + 1) REMPI of argon atoms, conversion of the REMPI-generated atomic argon ions into molecular ions, and generation of long-lived metastable excited-state argon atoms through dissociative recombination, populating the C3πu states of molecular nitrogen. Population inversion achieved for the second-positive-band laser transitions of molecular nitrogen enables stimulated emission of ultraviolet radiation at 337 nm. A high selectivity of the REMPI process helps to radically reduce the depletion of the working medium through the ionization of N2, providing a pump mechanism that is ideally suited for the creation of a new type of a highly efficient nitrogen laser.

  18. 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

  19. 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

  20. 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.

  1. 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.

  2. Resonance enhanced multiphoton ionization/secondary neutral mass spectrometry and cesium attachment secondary ion mass spectrometry of bronze : a comparison.

    SciTech Connect

    McCann, M. P.; Calaway, W. F.; Pellin, M. J.; Veryovkin, I. V.; Constantinides, I.; Adriaens, A.; Adams, F.; Materials Science Division; Sam Houston State Univ.; Univ. of Antwerp

    2002-05-01

    Archaeologists have considerable interests in ancient bronzes. They want to know how these alloys were produced and how they corroded with time. Modern bronzes, with compositions very close to that of some ancient bronzes, have been produced and two methods were examined to characterize one of these modern bronzes. Analysis of this modern bronze using resonance enhanced multiphoton ionization/secondary neutral mass spectrometry (REMPI/SNMS) is examined in detail and compared to cesium attachment secondary ion mass spectrometry (CsAMS) results. Both REMPI/SNMS and CsAMS were used to quantify the composition of Fe, Ni and Mn in a modern quaternary bronze designed to serve as a certified reference material for an ancient bronze. Both methods exhibit reduced matrix effects when compared to secondary ion mass spectrometry (SIMS) and thus quantification should be simplified. It was found that when relative sensitivity factors obtained from a standard bronze material are used to calibrate the instruments, the REMPI/SNMS measurements yield results that were more sensitive and more accurate.

  3. 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

  4. 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.

  5. Tracing direct and sequential two-photon double ionization of D{sub 2} in femtosecond extreme-ultraviolet laser pulses

    SciTech Connect

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

    2010-02-15

    Two-photon double ionization (TPDI) of D{sub 2} is studied for 38-eV photons at the Free Electron Laser in Hamburg (FLASH). Based on model calculations, instantaneous and sequential absorption pathways are identified as separated peaks in the measured D{sup +}+D{sup +} fragment kinetic energy release (KER) spectra. The instantaneous process appears at high KER, corresponding to ionization at the molecule's equilibrium distance, in contrast to sequential ionization mainly leading to low-KER contributions. Measured fragment angular distributions are in good agreement with theory.

  6. 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

  7. Comparison of the resonance-enhanced multiphoton ionization spectra of pyrrole and 2,5-dimethylpyrrole: Building toward an understanding of the electronic structure and photochemistry of porphyrins

    NASA Astrophysics Data System (ADS)

    Beames, Joseph M.; Nix, Michael G. D.; Hudson, Andrew J.

    2009-11-01

    The photophysical properties of porphyrins have relevance for their use as light-activated drugs in cancer treatment and sensitizers in solid-state solar cells. However, the appearance of their UV-visible spectra is usually explained inadequately by qualitative molecular-orbital theories. We intend to gain a better insight into the intense absorption bands, and excited-state dynamics, that make porphyrins appropriate for both of these applications by gradually building toward an understanding of the macrocyclic structure, starting with studies of smaller pyrrolic subunits. We have recorded the (1+1) and (2+1) resonance-enhanced multiphoton ionization (REMPI) spectra of pyrrole and 2,5-dimethylpyrrole between 25 600 cm-1 (390 nm) and 48 500 cm-1 (206 nm). We did not observe a (1+1) REMPI signal through the optically bright B12 (ππ ∗) and A11 (ππ ∗) states in pyrrole due to ultrafast deactivation via conical intersections with the dissociative A12 (πσ ∗) and B11 (πσ ∗) states. However, we did observe (2+1) REMPI through Rydberg states with a dominant feature at 27 432 cm-1 (two-photon energy, 54 864 cm-1) assigned to a 3d←π transition. In contrast, 2,5-dimethylpyrrole has a broad and structured (1+1) REMPI spectrum between 36 000 and 42 500 cm-1 as a result of vibronic transitions to the B12 (ππ ∗) state, and it does not show the 3d←π Rydberg transition via (2+1) REMPI. We have complemented the experimental studies by a theoretical treatment of the excited states of both molecules using time-dependent density functional theory (TD-DFT) and accounted for the contrasting features in the spectra. TD-DFT modeled the photochemical activity of both the optically dark π1σ∗ states (dissociative) and optically bright π1π∗ states well, predicting the barrierless deactivation of the B12 (ππ ∗) state of pyrrole and the bound minimum of the B12 (ππ ∗) state in 2,5-dimethylpyrrole. However, the quantitative agreement between vibronic

  8. Efficient three-step, two-color ionization of plutonium using a resonance enhanced 2-photon transition into an autoionizing state

    NASA Astrophysics Data System (ADS)

    Kunz, P.; Huber, G.; Passler, G.; Trautmann, N.

    2004-05-01

    Resonance ionization mass spectrometry (RIMS) has proven to be a powerful method for isotope selective ultra-trace analysis of long-lived radioisotopes. For plutonium detection limits of 106 to 107 atoms have been achieved for various types of samples. So far a three-step, three-color laser excitation scheme was applied for efficient ionization. In this work, a two-photon transition from an excited state into a high-lying autoionizing state, will be presented, yielding a similar overall efficiency as the three-step, three-color ionization scheme. In this way, only two tunable lasers are needed, while the advantages of a three-step, three-color excitation (high selectivity, good efficiency and low non-resonant background) are preserved. The two-photon transition has been characterized with respect to saturation behavior and line width. The three-step, two-color ionization is a possibility for an improved RIMS procedure.

  9. New perspectives in laser analytics: Resonance-enhanced multiphoton ionization in a Paul ion trap combined with a time-of-flight mass spectrometer

    NASA Astrophysics Data System (ADS)

    Bisling, Peter; Heger, Hans Jörg; Michaelis, Walfried; Weitkamp, Claus; Zobel, Harald

    1995-04-01

    A new laser analytical device has been developed that is based on resonance-enhanced multiphoton ionization in the very center of a radio-frequency quadrupole ion trap. Applications in speciation anlaysis of biological and enviromental samples and in materials science will all benefit from laser-optical selectivity in the resonance excitation process, combined with mass-spectropic sensivity which is further enhanced by the ion accumulation and storage capability.

  10. 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.

  11. 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. PMID:23876725

  12. Photoelectron angular distributions in infrared one-photon and two-photon ionization of FEL-pumped Rydberg states of helium

    NASA Astrophysics Data System (ADS)

    Mondal, S.; Fukuzawa, H.; Motomura, K.; Tachibana, T.; Nagaya, K.; Sakai, T.; Matsunami, K.; Yase, S.; Yao, M.; Wada, S.; Hayashita, H.; Saito, N.; Callegari, C.; Prince, K. C.; O'Keeffe, P.; Bolognesi, P.; Avaldi, L.; Miron, C.; Nagasono, M.; Togashi, T.; Yabashi, M.; Ishikawa, K. L.; Sazhina, I. P.; Kazansky, A. K.; Kabachnik, N. M.; Ueda, K.

    2013-10-01

    The photoelectron angular distributions (PADs) have been investigated for infrared (IR) ionization of He atoms excited to Rydberg states by extreme ultraviolet free-electron laser pulses. The experiment was carried out with two pulses which do not overlap in time. Depending on the intensity of the IR pulses, one IR photon ionization or additionally two-photon above-threshold ionization is observed. For low IR intensity, the PAD is well described by a contribution of s and d partial waves in accordance with early experiments. At high IR intensity, the PAD for two IR photon ionization clearly shows the contribution of higher partial waves. The experimental data are compared with the results of theoretical calculations based on solving the time-dependent Schrödinger equation.

  13. Recoil-Ion Momentum Distributions for Two-Photon Double Ionization of He and Ne by 44 eV Free-Electron Laser Radiation

    SciTech Connect

    Rudenko, A.; Moshammer, R.; Ullrich, J.; Foucar, L.; Havermeier, T.; Smolarski, M.; Schoessler, S.; Cole, K.; Schoeffler, M.; Doerner, R.; Kurka, M.; Ergler, Th.; Kuehnel, K. U.; Jiang, Y. H.; Voitkiv, A.; Najjari, B.; Luedemann, S.; Schroeter, C. D.; Kheifets, A.; Duesterer, S.

    2008-08-15

    Recoil-ion momentum distributions for two-photon double ionization of He and Ne (({Dirac_h}/2{pi}){omega}=44 eV) have been recorded with a reaction microscope at FLASH (the free-electron laser at Hamburg) at an intensity of {approx}1x10{sup 14} W/cm{sup 2} exploring the dynamics of the two fundamental two-photon-two-electron reaction pathways, namely, sequential and direct (or nonsequential) absorption of the photons. We find strong differences in the recoil-ion momentum patterns for the two mechanisms pointing to the significantly different two-electron emission dynamics and thus provide serious constraints for theoretical models.

  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. Dynamics of C-Br bond dissociation in methyl 2-bromopropionate at 235 nm: A resonance-enhanced multiphoton ionization study

    NASA Astrophysics Data System (ADS)

    Saha, Ankur; Kumar, Awadhesh; Naik, Prakash D.

    2016-01-01

    The dynamics of the C-Br bond dissociation on UV excitation of methyl 2-bromopropionate mainly to the 1(nσ*) state, repulsive in the C-Br bond, has been investigated, employing resonance-enhanced multiphoton ionization. Both the ground state and spin-orbits excited bromine atoms were detected, with the former being the major channel. Bromine fragments show bimodal translational energy distributions, with slow and fast (major) bromine atoms arising mainly from the ground and excited electronic states, respectively. The measured recoil anisotropy suggests isotropic angular distributions of bromine atoms. Molecular orbital calculations reveal an important role of avoided curve crossing on C-Br bond dissociation dynamics.

  18. 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}.

  19. Vibrations of the S1 state of fluorobenzene-h5 and fluorobenzene-d5 via resonance-enhanced multiphoton ionization (REMPI) spectroscopy.

    PubMed

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

    2014-12-28

    We report resonance-enhanced multiphoton ionization spectra of the isotopologues fluorobenzene-h5 and fluorobenzene-d5. 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-d5 observed bands are provided, aided by previous results on fluorobenzene-h5. PMID:25554159

  20. State interactions and illumination of hidden states through perturbations and observations of new states: High energy resonance enhanced multiphoton ionization of HI.

    PubMed

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

    2015-06-28

    Hydrogen iodide, a Hund's case (c) molecule, serves as a benchmark compound for studying rich molecular state interactions between Rydberg and valence states as well as between Rydberg states at high energies (72,300-74,600 cm(-1)) by mass resolved resonance enhanced multiphoton ionization (REMPI). Perturbations in the spectra appearing as deformations in line-positions, line-intensities, and linewidths are found to be either due to near-degenerate or non-degenerate interactions, both homogeneous and heterogeneous in nature. Perturbation analyses allow indirect observation as well as characterization of "hidden states" to some extent. Furthermore, new observable spectral features are assigned and characterized. PMID:26133433

  1. State interactions and illumination of hidden states through perturbations and observations of new states: High energy resonance enhanced multiphoton ionization of HI

    NASA Astrophysics Data System (ADS)

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

    2015-06-01

    Hydrogen iodide, a Hund's case (c) molecule, serves as a benchmark compound for studying rich molecular state interactions between Rydberg and valence states as well as between Rydberg states at high energies (72 300-74 600 cm-1) by mass resolved resonance enhanced multiphoton ionization (REMPI). Perturbations in the spectra appearing as deformations in line-positions, line-intensities, and linewidths are found to be either due to near-degenerate or non-degenerate interactions, both homogeneous and heterogeneous in nature. Perturbation analyses allow indirect observation as well as characterization of "hidden states" to some extent. Furthermore, new observable spectral features are assigned and characterized.

  2. Two-photon double ionization of helium: Evolution of the joint angular distribution with photon energy and two-electron energy sharing

    SciTech Connect

    Zhang Zheng; Peng Liangyou; Xu Minghui; Gong Qihuang; Starace, Anthony F.; Morishita, Toru

    2011-10-15

    Ab initio calculations of two-photon double ionization of helium with photon energies varying from the nonsequential regime to well above the double-ionization threshold are presented. A systematic study of the joint angular distributions of the two ionized electrons at different energy sharing shows that the role of electron correlations is imprinted in the joint angular distribution. In particular, a rather general pattern is identified in the nonsequential regime that is independent of photon energy, pulse length, and energy sharing between the two electrons. Interestingly, the same distribution pattern is found for the equal-energy-sharing case, even when the photon energy is well above the double-ionization threshold. In the case of an extremely uneven energy sharing, the distribution pattern changes drastically as the photon energy is increased. In particular, when the photon energy is greater than the second-ionization threshold, the dominant emission mode of the two electrons switches gradually from ''back to back'' to ''side by side.'' Finally, the joint angular distribution is found to provide clear evidence of the role of electron correlations in the initial state.

  3. Resonant two-photon ionization of LiNa. Observation and preliminary characterization of five new singlet states

    NASA Astrophysics Data System (ADS)

    Kappes, Manfred M.; Marti, Kurt O.; Radi, Peter; Schär, Martin; Schumacher, Ernst

    1984-05-01

    Supersonic molecular beams containing rotationally and vibrationally cold LiNa were probed by one- and multi-photon ionization. Results include determination of a vertical ionization potential (5.05 ± 0.04 eV) as well as first observation of five new singlet states. Preliminary spectroscopic constants ( Te, we and wexe) and term symbols are reported for these five states (A 1Σ +, C 1 Σ +, D 1Π, E 1 Σ + and F 1 E +).

  4. Ultratrace detection of chemical warfare agent simulants using supersonic-molecular-beam, resonance-enhanced multiphoton-ionization, time-of-flight mass spectroscopy. Final report

    SciTech Connect

    Syage, J.A.; Pollard, J.E.; Cohen, R.B.

    1988-02-15

    An ultratrace detection method that offers exceptional selectivity has been developed based on the technique of supersonic molecular beam, resonance enhanced multiphoton ionization, time-of-flight mass spectroscopy (MB/REMPI/TOFMS). Single ion detection capability has given detection limits as low as 300 ppt (dimethyl sulfide). Single vibronic level REMPI of the supercooled molecules in conjunction with TOFMS provides selectivity of 10,000 against chemically similar compounds. Studies were carried out using moist air expansions for a variety of organophosphonate and sulfide chemical warfare agent (CWA) simulant molecules. The preparation of molecules in single vibronic levels by laser excitation in supersonic molecular beams has enabled us to record high resolution spectra of higher excited electronic states showing fully resolved vibrational structure for diisopropyl methylphosphonate (DIMP) and dimethyl sulfide (DMS). VUV absorption spectra have also been recorded for several CWA molecules at ambient temperature, revealing several new electronic states extending up to the ionization threshold.

  5. 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.

  6. 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.

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

    PubMed

    Germann, Matthias; Willitsch, Stefan

    2016-07-28

    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. PMID:27475369

  8. (1 + 1) resonant enhanced multiphoton ionization via the A2Sigma(+) state of NO - Ionic rotational branching ratios and their intensity dependence

    NASA Technical Reports Server (NTRS)

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

    1988-01-01

    Rotational branching ratios resulting from the (1 + 1) resonant enhanced multiphoton ionization spectroscopy of NO via the 0-0 transition of the A-X band for the four possible branches that can be assigned as R(21.5) are explored using calculation performed in the frozen-core approximation at the Hartree-Fock level. The four different branches, of which three are distinctly different in the perturbative limit, have rather different branching ratios. The mixed R12 + Q22(21.5) branch, which is not intense and has the lowest transition energy, appears to give the best agreement with experimental branching ratio for parallel detection. The agreement is less satisfactory for perpendicular detection. Neither the effect of finite-acceptance angle of the photoelectron detector nor high intensities can explain the discrepancy.

  9. 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. PMID:27276949

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

    NASA Astrophysics Data System (ADS)

    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 H 2+ X 1 Σg + (v″) vibrational levels.

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

    NASA Technical Reports Server (NTRS)

    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.

  12. The Vibronic Spectroscopy of Some P-Alkylphenols and Catechols as Examined by Means of Supersonic Jet Resonant Two-Photon Ionization

    NASA Astrophysics Data System (ADS)

    Grace, Louis Immanuel

    I present a set of ground-state assignments, based on infrared and Raman data, for p-ethylphenol, p-isopropylphenol, tyramine, tyrosine, 4-methylcatechol and 3-methoxytyramine. I present supersonic jet resonant two-photon ionization (R2PI) spectra and the corresponding vibronic assignments for all of these molecules and for catechol. Tyramine and tyrosine require a laser-desorption technique, which is described in detail. The ground-state spectra for the four p-alkylphenols studied are quite similar to each other. Thus, analogy to the p-cresol ground state is quite useful for making the assignments. The ground-state data for 4-methylcatechol and 3-methoxytyramine seem to be interpretable by analogy to the spectra of other tri-substituted benzenes. The R2PI spectra for the p-alkylphenols are also similar to each other, despite the fact that the nature of the substituent chain varies considerably among these molecules. The observed (lowest-energy) origins (v ^{''} = 0 to v^' = 0) are: For tyrosine, p-isopropylphenol, p-ethylphenol and tyramine, respectively, 35620, 35587, 35516 and 35492cm^{-1 }, and for 4-methylcatechol, 4-ethylcatechol, 3-methoxytyramine and catechol, respectively, 34781, 34877(?), 35325 and 35655cm^{-1}. Two bands previously assigned as origins in the fluorescence spectrum of tyramine are absent in the R2PI spectrum. Most of these molecules are stable in several geometries. To aid the ground-state assignments for the p-alkyl-phenols, and to examine the issue of multiple conformers, particularly of the catechols, I performed Hartree-Fock calculations at the 3-21G level via the GAUSSIAN program. Results of these are presented. I also attempted to obtain an R2PI spectrum for dopamine. Despite the fact that I tried many experiments with a variety of entrainment conditions, I was unable to do so. Some of the catechols exhibit unusual behavior in that they yield R2PI spectra only for a certain range of jet stagnation pressures. I present the results of

  13. 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

  14. Application of pyrolysis-mass spectrometry and pyrolysis-gas chromatography-mass spectrometry with electron-ionization or resonance-enhanced-multi-photon ionization for characterization of crude oils.

    PubMed

    Otto, Stefan; Streibel, Thorsten; Erdmann, Sabrina; Sklorz, Martin; Schulz-Bull, Detlef; Zimmermann, Ralf

    2015-01-15

    A novel analytical system for gas-chromatographic investigation of complex samples has been developed, that combines the advantages of several analytical principles to enhance the analytical information. Decomposition of high molecular weight structures is achieved by pyrolysis and a high separation capacity due to the chromatographic step provides both an universal as well as a selective and sensitive substance detection. The latter is achieved by simultaneously applying electron ionization quadrupole mass spectrometry (EI-QMS) for structural elucidation and [1+1]-resonance-enhanced-multi-photon ionization (REMPI) combined with time-of-flight mass spectrometry (ToFMS). The system has been evaluated and tested with polycyclic aromatic hydrocarbon (PAH) standards. It was applied to crude oil samples for the first time. In such highly complex samples several thousands of compounds are present and the identification especially of low concentrated chemical species such as PAH or their polycyclic aromatic sulfur containing heterocyclic (PASH) derivatives is often difficult. Detection of unalkylated and alkylated PAH together with PASH is considerably enhanced by REMPI-ToFMS, at times revealing aromatic structures which are not observable by EI-QMS due to their low abundance. On the other hand, the databased structure proposals of the EI-QMS analysis are needed to confirm structural information and isomers distinction. The technique allows a complex structure analysis as well as selective assessment of aromatic substances in one measurement. Information about the content of sulfur containing compounds plays a significant role for the increase of efficiency in the processing of petroleum. PMID:25542090

  15. 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. PMID:27461406

  16. Direct autocorrelation of soft-x-ray free-electron-laser pulses by time-resolved two-photon double ionization of He

    NASA Astrophysics Data System (ADS)

    Mitzner, R.; Sorokin, A. A.; Siemer, B.; Roling, S.; Rutkowski, M.; Zacharias, H.; Neeb, M.; Noll, T.; Siewert, F.; Eberhardt, W.; Richter, M.; Juranic, P.; Tiedtke, K.; Feldhaus, J.

    2009-08-01

    The pulse duration of soft x-ray free-electron laser (FEL) radiation is directly measured by time-resolved observation of doubly charged helium ions at 51.8 eV. A wave front splitting autocorrelator produces two correlated FEL pulses with a resolution of better than a femtosecond. In the interesting intensity range from 1013 to 1016W/cm2 direct and sequential double ionization contribute to the ion yield which has significant influence on the correlation width, being a general feature at high photon energies. Here, a duration of τL=(29±5)fs is derived for the soft x-ray pulses at FLASH.

  17. Resonantly-enhanced, four-photon ionization of krypton at laser intensities exceeding 10/sup 13/ W/cm/sup 2/

    SciTech Connect

    Perry, M.D.; Landen, O.L.; Campbell, E.M.

    1987-12-01

    The yield of singly- and multiply- charged ions of krypton and xenon is presented as a function of laser intensity and frequency. The measurements were performed using the second harmonic output of a well-characterized, tunable picosecond dye laser in the range 285 to 310 nm at laser intensities from 1 x 10/sup 12/ to 10/sup 14/ W/cm/sup 2/. Enhancement of the Kr/sup +/ yield by two orders of magnitude by three-photon resonant, four-photon ionization is observed in the vicinity of the 4d'(5/2)/sub 3/ and the 4d(3/2)/sub 1/ intermediate states. A model incorporating line shifts and widths scaling linearly with intensity is in good agreement with the experimental results.

  18. Nonresonant two-photon mass analyzed threshold ionization and zero kinetic energy photoelectron investigation of the X˜ 2B1 ground state of CH2CO+ and CD2CO+

    NASA Astrophysics Data System (ADS)

    Wang, Shiliang; Shi, Yujun; Jakubek, Zygmunt J.; Barnett, Michael; Simard, Benoit; Müller-Dethlefs, Klaus; Liu, Ching-Ping; Lee, Yuan-Pern

    2002-10-01

    Rotationally resolved nonresonant two-photon mass analyzed threshold ionization (MATI) and zero kinetic energy (ZEKE) photoelectron spectra of CH2CO+ and CD2CO+ are reported. The spectra are dominated by the origin band and totally symmetric a1 vibrations, ν4 (C=C symmetric stretch) and ν2 (C=O asymmetric stretch) for CH2CO+, and ν1 (C=O asymmetric stretch), ν3 (C=C symmetric stretch), and ν4 (CD2 scissor) for CD2CO+. In addition, several weaker bands are observed in the MATI spectra: ν3 (CH2 scissor) in CH2CO+; b1 vibrations ν5 and ν6 (C=C=O linear bend and CH2 wag) in both isotopomers; b2 vibration ν8 (CD2 rock) for CD2CO+; b2 vibration ν9 (C=C=O linear bend) for CH2CO+; as well as overtones and combination bands. Rotational structure of the origin band is dominated by three very strong ΔKa=±1 bands with 2 orders of magnitude weaker ΔKa=+3 bands. A similar ΔKa=±1 three-band pattern is observed for the a1 vibrational modes. For the b1 modes a single-band pattern resulting from the ΔKa=0 selection rule is present. Fundamental wave numbers for six vibrational modes of CH2CO+ and seven modes of CD2CO+ are determined. Rotational analysis of the partially resolved ZEKE spectra yields the ionization potentials (77539.4±2.0 cm-1 for CH2CO and 77534.3±2.0 cm-1 for CD2CO) and rotational constants for the ground states of both ketene cations.

  19. Resonance enhanced multiphoton ionization and zero electron kinetic energy spectroscopy of the DABCO-N2 van der Waals complex: Divergent energy level spacings as evidence for an offset parallel structure

    NASA Astrophysics Data System (ADS)

    Watkins, Mark J.; Cockett, Martin C. R.

    2003-12-01

    The DABCO-N2 van der Waals complex has been investigated using a combination of (1+1') resonance enhanced multiphoton ionization and zero electron kinetic energy spectroscopy, supported by ab initio molecular orbital calculations. The observation of extended vibrational progressions of low wave number with diverging vibrational spacings supports an assignment to an offset parallel structure analogous to the 45° canted parallel structures proposed for the nitrogen dimer. The active vibrational mode is assigned to a mixed van der Waals stretch/rocking mode in which the nitrogen solvent undergoes a hindered rotational motion against the DABCO framework in the plane containing the C3 axis in DABCO and the intermolecular axis in N2. The results of counterpoise corrected ab initio calculations support this assignment to the extent that they suggest that a parallel structure is the most stable with a cross structure identified as a transition state. No experimental evidence is found for the existence of other stable structures.

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

    PubMed

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

    2015-12-28

    We report vibrationally resolved spectra of the S1←S0 transition of bromobenzene using resonance-enhanced multiphoton ionization spectroscopy. We study bromobenzene-h5 as well as its perdeuterated isotopologue, bromobenzene-d5. The form of the vibrational modes between the isotopologues and also between the S0 and S1 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 S1 spectra are discussed. Additionally, the vibrations in the ground state cation, D0 (+), 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 S0 and D0 (+) 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 S0, S1, and D0 (+) states, gaining insight into vibrational activity and vibrational couplings. PMID:26723684

  1. 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). PMID:26884269

  2. 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.

  3. 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.

  4. Two-photon flow cytometry

    NASA Astrophysics Data System (ADS)

    Zhong, Cheng F.; Ye, Jing Yong; Myc, Andrzej; Thomas, Thommey P.; Bielinska, Anna; Baker, James R., Jr.; Norris, Theodore B.

    2005-03-01

    Flow cytometry is a powerful technique for obtaining quantitative information from fluorescence in cells. Quantization 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 (T3FC) 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.

  5. Two Photon Exchange for Exclusive Pion Electroproduction

    SciTech Connect

    Afanaciev, Andrei V.; Aleksejevs, Aleksandrs G.; Barkanova, Svetlana G.

    2013-09-01

    We perform detailed calculations of two-photon-exchange QED corrections to the cross section of pion electroproduction. The results are obtained with and without the soft-photon approximation; analytic expressions for the radiative corrections are derived. The relative importance of the two-photon correction is analyzed for the kinematics of several experiments at Jefferson Lab. A significant, over 20%, effect due to two-photon exchange is predicted for the backward angles of electron scattering at large transferred momenta.

  6. Two-photon absorption in tetraphenylporphycenes: are porphycenes better candidates than porphyrins for providing optimal optical properties for two-photon photodynamic therapy?

    PubMed

    Arnbjerg, Jacob; Jiménez-Banzo, Ana; Paterson, Martin J; Nonell, Santi; Borrell, José I; Christiansen, Ove; Ogilby, Peter R

    2007-04-25

    Porphycenes are structural isomers of porphyrins that have many unique properties and features. In the present work, the resonant two-photon absorption of 2,7,12,17-tetraphenylporphycene (TPPo) and its palladium(II) complex (PdTPPo) has been investigated. The data obtained are compared to those from the isomeric compound, meso-tetraphenylporphyrin (TPP). Detection of phosphorescence from singlet molecular oxygen, O2(a(1)Delta(g)), produced upon irradiation of these compounds, was used to obtain two-photon excitation spectra and to quantify two-photon absorption cross sections, delta. In the spectral region of 750-850 nm, the two-photon absorption cross sections at the band maxima for both TPPo and PdTPPo, delta = 2280 and 1750 GM, respectively, are significantly larger than that for TPP. This difference is attributed to the phenomenon of so-called resonance enhancement; for the porphycenes, the two-photon transition is nearly resonant with a comparatively intense one-photon Q-band transition. The results of quantum mechanical calculations using density functional quadratic response theory are in excellent agreement with the experimental data and, as such, demonstrate that comparatively high-level quantum chemical methods can be used to interpret and predict nonlinear optical properties from such large molecular systems. One important point realized through these experiments and calculations is that one must exercise caution when using qualitative molecular-symmetry-derived arguments to predict the expected spectral relationship between allowed one- and two-photon transitions. From a practical perspective, this study establishes that, in comparison to porphyrins and other tetrapyrrolic macrocyclic systems, porphycenes exhibit many desirable attributes for use as sensitizers in two-photon initiated photodynamic therapy. PMID:17397157

  7. FAST TRACK COMMUNICATION: Photoelectron spectroscopy of sequential three-photon double ionization of Ar irradiated by EUV free-electron laser pulses

    NASA Astrophysics Data System (ADS)

    Fukuzawa, H.; Gryzlova, E. V.; Motomura, K.; Yamada, A.; Ueda, K.; Grum-Grzhimailo, A. N.; Strakhova, S. I.; Nagaya, K.; Sugishima, A.; Mizoguchi, Y.; Iwayama, H.; Yao, M.; Saito, N.; Piseri, P.; Mazza, T.; Devetta, M.; Coreno, M.; Nagasono, M.; Tono, K.; Yabashi, M.; Ishikawa, T.; Ohashi, H.; Kimura, H.; Togashi, T.; Senba, Y.

    2010-06-01

    We have investigated the ionization of the Ar atom by 51 nm extreme-ultraviolet light pulses at the free-electron laser facility, SPring-8 Compact SASE Source test accelerator, in Japan. The angle-resolved photoelectron spectra contain lines due to sequential three-photon double ionization with the second ionization step proceeding via the resonantly enhanced two-photon absorption. The relative intensities of the corresponding photoelectron peaks and their angular dependence are explained in the framework of a three-step model of the process.

  8. 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.

  9. The 700-1500 cm{sup −1} region of the S{sub 1} (A{sup ~1}B{sub 2}) state of toluene studied with resonance-enhanced multiphoton ionization (REMPI), zero-kinetic-energy (ZEKE) spectroscopy, and time-resolved slow-electron velocity-map imaging (tr-SEVI) spectroscopy

    SciTech Connect

    Gardner, Adrian M.; Green, Alistair M.; Tamé-Reyes, Victor M.; Reid, Katharine L.; Davies, Julia A.; Parkes, Victoria H. K.; Wright, Timothy G.

    2014-03-21

    We report (nanosecond) resonance-enhanced multiphoton ionization (REMPI), (nanosecond) zero-kinetic-energy (ZEKE) and (picosecond) time-resolved slow-electron velocity map imaging (tr-SEVI) spectra of fully hydrogenated toluene (Tol-h{sub 8}) and the deuterated-methyl group isotopologue (α{sub 3}-Tol-d{sub 3}). Vibrational assignments are made making use of the activity observed in the ZEKE and tr-SEVI spectra, together with the results from quantum chemical and previous experimental results. Here, we examine the 700–1500 cm{sup −1} region of the REMPI spectrum, extending our previous work on the region ≤700 cm{sup −1}. We provide assignments for the majority of the S{sub 1} and cation bands observed, and in particular we gain insight regarding a number of regions where vibrations are coupled via Fermi resonance. We also gain insight into intramolecular vibrational redistribution in this molecule.

  10. 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.

  11. The nonresonant two-photon zero kinetic energy photoelectron spectrum from the electronic ground state of H2S

    NASA Astrophysics Data System (ADS)

    Fischer, Ingo; Lochschmidt, Andreas; Strobel, Andreas; Niedner-Schatteburg, Gereon; Mueller-Dethlefs, Klaus; Bondybey, Vladimir E.

    1993-03-01

    Zero kinetic energy photoelectron spectra from the electronic ground state of hydrogen sulfide are obtained via nonresonant two-photon ionization with complete rotational resolution in the ion. The two-photon spectra are compared with those recently obtained via one-photon VUV photoionization. The spectra show a close similarity, but type a transitions in the two-photon spectra are twice as intense.

  12. Two-photon induced polymer nanomovement.

    PubMed

    Ishitobi, Hidekazu; Shoji, Satoru; Hiramatsu, Tsunemi; Sun, Hong-Bo; Sekkat, Zouheir; Kawata, Satoshi

    2008-09-01

    We present the first report of two-photon induced plastic surface deformation in solid polymer films. Exposure of azo polymer films, which absorb in the visible range (lambda(max) = 480 nm), to intense 920 nm irradiation leads to polarization dependent photofluidic polymer nanomovement caused by photoselective two-photon trans <-->cis isomerization. The deformations were induced by a gradient of light intensity; and strongly depend on the wavelength and the polarization direction of the incident laser light and the position of the focused spot with respect to the plane of the polymer film. PMID:18773020

  13. Two-Photon Fluorescence Correlation Spectroscopy

    NASA Technical Reports Server (NTRS)

    Zimmerli, Gregory A.; Fischer, David G.

    2002-01-01

    We will describe a two-photon microscope currently under development at the NASA Glenn Research Center. It is composed of a Coherent Mira 900 tunable, pulsed Titanium:Sapphire laser system, an Olympus Fluoview 300 confocal scanning head, and a Leica DM IRE inverted microscope. It will be used in conjunction with a technique known as fluorescence correlation spectroscopy (FCS) to study intracellular protein dynamics. We will briefly explain the advantages of the two-photon system over a conventional confocal microscope, and provide some preliminary experimental results.

  14. Dynamic behavior, electrochromism, and two-photon absorption of dicyanomethylenated quinacridone.

    PubMed

    Takeda, Takashi; Sugihara, Hiroyuki; Suzuki, Yasutaka; Kawamata, Jun; Akutagawa, Tomoyuki

    2014-10-17

    Molecular structures of dicyanomethylenated quinacridone (1) as a solid and in solution were examined on the basis of single-crystal X-ray structural analysis, temperature-dependent (1)H NMR in CD2Cl2, and theoretical calculations. Crystal 1 had a curved, butterfly-shaped molecular structure. Thermally activated flipping between the curved, butterfly-shaped structure and an armchair structure occurred in solution. Electrochemical reduction triggered a dynamic change from the curved, butterfly-shaped conformation in the neutral state to a planar conformation in the dianion state, which represented electrochromic behavior with electrochemical bistability. A large two-photon absorption cross section of compound 1 was observed in the resonance-enhancement region of 423 GM (1 GM = 1 × 10(-50) cm(4) s photon(-1) molecule(-1)) at 710 nm. Multiple donor-acceptor charge-transfer pathways of molecule 1 enhanced two-photon absorption. PMID:25254634

  15. 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.

  16. Two-photon resonant second harmonic generation in atomic xeon

    SciTech Connect

    Shi, Y. J.; Al-Basheer, W.; Thompson, R. I.

    2009-03-07

    Vacuum ultraviolet (VUV) radiation at 124.8 nm (9.93 eV) was produced from two-photon resonant second harmonic generation (SHG) in a xeon gaseous medium and used to probe molecular samples of acetone, furan, thiophene, ammonia, and methane. The mass spectra recorded from the species with ionization energies below 9.93 eV were dominated by the parent ions. The parent ions were only observed when the incident UV radiation was tuned to resonate with the two-photon transition 5p{sup 5}({sup 2}P{sub 3/2}{sup 0})6p[1/2]{sub 0}(leftarrow)5p{sup 6} {sup 1}S{sub 0} of Xe at 80 119.474 cm{sup -1}. The pressure dependence and the resonant nature of the parent ions observed support the mechanism for SHG as the ionization-initiated electric field induced SHG via the third-order nonlinear susceptibility {chi}{sup (3)}, which is enhanced by the coupling between the 5p{sup 5}({sup 2}P{sub 3/2}{sup 0})6p[1/2]{sub 0} and the nearby 5p{sup 5}({sup 2}P{sub 3/2}{sup 0})5d[1/2]{sub 1} states of Xe atoms.

  17. Scattering of entangled two-photon states.

    PubMed

    Schotland, John C; Cazé, A; Norris, Theodore B

    2016-02-01

    We consider the scattering of entangled two-photon states from collections of small particles. We also study the related Mie problem of scattering from a sphere. In both cases, we calculate the entropy of entanglement and investigate the influence of the entanglement of the incident field on the entanglement of the scattered field. PMID:26907393

  18. Two-photon production of ω pairs

    NASA Astrophysics Data System (ADS)

    Albrecht, H.; Hamacher, T.; Hofmann, R. P.; Kirchhoff, T.; Mankel, R.; Nau, A.; Nowak, S.; Reßing, D.; Schröder, H.; Schulz, H. D.; Walter, M.; Wurth, R.; Hast, C.; Kapitza, H.; Kolanoski, H.; Kosche, A.; Lange, A.; Lindner, A.; Schieber, M.; Siegmund, T.; Spaan, B.; Thurn, H.; Töpfer, D.; Wegener, D.; Eckstein, P.; Frankl, C.; Graf, J.; Schmidtler, M.; Schramm, M.; Schubert, K. R.; Schwierz, R.; Waldi, R.; Reim, K.; Wegener, H.; Eckmann, R.; Kuipers, H.; Mai, O.; Mundt, R.; Oest, T.; Reiner, R.; Schmidt-Parzefall, W.; Stiewe, J.; Werner, S.; Ehret, K.; Hofmann, W.; Hüpper, A.; Knöpfle, K. T.; Spengler, J.; Krieger, P.; Macfarlane, D. B.; Prentice, J. D.; Saull, P. R. B.; Tzamariudaki, K.; van de Water, R. G.; Yoon, T.-S.; Schneider, M.; Weseler, S.; Kernel, G.; Križan, P.; Križnič, E.; Podobnik, T.; Živko, T.; Balagura, V.; Barsuk, S.; Belyaev, I.; Chistov, R.; Danilov, M.; Eiges, V.; Gershtein, L.; Gershtein, Yu.; Golutvin, A.; Igonkina, O.; Korolko, I.; Kostina, G.; Litvintsev, D.; Pakhlov, P.; Semenov, S.; Snizhko, A.; Tichomirov, I.; Zaitsev, Yu.; Argus Collaboration

    1996-02-01

    A maximum likelihood analysis of ARGUS data on two-photon production of π+π+π0π0π-π- is presented. A small fraction of events is due to the production of omega pairs. The γγ → ωω cross section has its maximum value close to threshold.

  19. Third-order nonlinearities in molecular hydrogen - Two-photon resonance enhanced third-harmonic generation and Raman scattering

    NASA Technical Reports Server (NTRS)

    Pan, C.-L.; She, C.-Y.; Fairbank, W. M., Jr.; Billman, K. W.

    1977-01-01

    Effects of quantum mechanical interferences on third-order susceptibilities in molecules are studied. First principle calculations for molecular hydrogen are presented and shown to agree with results derived from experimental stimulated Raman gain and spontaneous Raman cross-section data. 10 percent third-harmonic conversion efficiency in H2 at 1 atm without phase matching should require a 150 MW per sq cm at 4.81 microns. As little as 5.9-MW power is sufficient when the beam is properly focused. Resonance Raman scattering (RRS) is proposed for experimentally investigating the interference effects, which tend to reduce the strength of third-order nonlinear susceptibilities.

  20. Magnetic two-photon scattering and two-photon emission - Cross sections and redistribution functions

    NASA Technical Reports Server (NTRS)

    Alexander, S. G.; Meszaros, P.

    1991-01-01

    The magnetic two-photon scattering cross section is discussed within the framework of QED, and the corresponding scattering redistribution function for this process and its inverse, as well as the scattering source function are calculated explicitly. In a similar way, the magnetic two-photon emission process which follows the radiative excitation of Landau levels above ground is calculated. The two-photon scattering and two-photon emission are of the same order as the single-photon magnetic scattering. All three of these processes, and in optically thick cases also their inverses, are included in radiative transport calculations modeling accreting pulsars and gamma-ray bursters. These processes play a prominent role in determining the relative strength of the first two cyclotron harmonics, and their effects extend also to the higher harmonics.

  1. 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.

  2. Denoising Two-Photon Calcium Imaging Data

    PubMed Central

    Malik, Wasim Q.; Schummers, James; Sur, Mriganka; Brown, Emery N.

    2011-01-01

    Two-photon calcium imaging is now an important tool for in vivo imaging of biological systems. By enabling neuronal population imaging with subcellular resolution, this modality offers an approach for gaining a fundamental understanding of brain anatomy and physiology. Proper analysis of calcium imaging data requires denoising, that is separating the signal from complex physiological noise. To analyze two-photon brain imaging data, we present a signal plus colored noise model in which the signal is represented as harmonic regression and the correlated noise is represented as an order autoregressive process. We provide an efficient cyclic descent algorithm to compute approximate maximum likelihood parameter estimates by combing a weighted least-squares procedure with the Burg algorithm. We use Akaike information criterion to guide selection of the harmonic regression and the autoregressive model orders. Our flexible yet parsimonious modeling approach reliably separates stimulus-evoked fluorescence response from background activity and noise, assesses goodness of fit, and estimates confidence intervals and signal-to-noise ratio. This refined separation leads to appreciably enhanced image contrast for individual cells including clear delineation of subcellular details and network activity. The application of our approach to in vivo imaging data recorded in the ferret primary visual cortex demonstrates that our method yields substantially denoised signal estimates. We also provide a general Volterra series framework for deriving this and other signal plus correlated noise models for imaging. This approach to analyzing two-photon calcium imaging data may be readily adapted to other computational biology problems which apply correlated noise models. PMID:21687727

  3. 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

  4. 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.

  5. Dicyanostilbene-derived two-photon fluorescence dyes with large two-photon absorption cross sections

    NASA Astrophysics Data System (ADS)

    Huang, Chibao; Lin, Changhua; Ren, Anxiang; Yang, Nianfa

    2011-12-01

    Four dicyanostilbene-derived two-photon fluorescence (TPF) dyes were synthesized as the model compounds to systematically study the effect of the dicyano and the terminal substituent on the two-photon absorption (TPA). These four compounds ( DSO, DCY, DTO and DPH) exhibit very large two-photon absorption cross sections ( δ). DCY (A- π-A) with the terminal cyano group has especially high fluorescence quantum yield (0.71) and relatively large δ (1480 GM), while DPH (D- π-A) with the substitutedamino group at its terminus possesses the largest δ (2800 GM) and the longest emission wavelength (620 nm). The idealest terminal substituent should not be the alkoxy group but the substitutedamino group. This class of dicyanostilbene dyes possess small molecule size, large δ (830-2800 GM), long-wavelength emission (459-620 nm) and large Stokes shift (80-206 nm), and are ideal chromophores for TPF labels and probes.

  6. Encoded multisite two-photon microscopy

    PubMed Central

    Ducros, Mathieu; Houssen, Yannick Goulam; Bradley, Jonathan; de Sars, Vincent; Charpak, Serge

    2013-01-01

    The advent of scanning two-photon microscopy (2PM) has created a fertile new avenue for noninvasive investigation of brain activity in depth. One principal weakness of this method, however, lies with the limit of scanning speed, which makes optical interrogation of action potential-like activity in a neuronal network problematic. Encoded multisite two-photon microscopy (eMS2PM), a scanless method that allows simultaneous imaging of multiple targets in depth with high temporal resolution, addresses this drawback. eMS2PM uses a liquid crystal spatial light modulator to split a high-power femto-laser beam into multiple subbeams. To distinguish them, a digital micromirror device encodes each subbeam with a specific binary amplitude modulation sequence. Fluorescence signals from all independently targeted sites are then collected simultaneously onto a single photodetector and site-specifically decoded. We demonstrate that eMS2PM can be used to image spike-like voltage transients in cultured cells and fluorescence transients (calcium signals in neurons and red blood cells in capillaries from the cortex) in depth in vivo. These results establish eMS2PM as a unique method for simultaneous acquisition of neuronal network activity. PMID:23798397

  7. 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

  8. 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.

  9. 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.

  10. 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.

  11. Photorejuvenation observation based on two photon microscopy

    NASA Astrophysics Data System (ADS)

    Wu, Shu-lian; Li, Hui; Xiao, Zheng-ying; Xie, Shu-sen

    2008-12-01

    With low risk of complications and little down-time, the non-ablative photo-rejuvenation is playing an increasing role in the therapy of the photo-damaged skin, but the appraisal standard is different. This paper mainly observed the effect of the mouse skin irradiated by intense pulse light source through two photo microscopy in sub-micrometer. The spectrum and morphological imaging between pre- and post-irradiated by Intense Pulse Light (IPL) were obtained from two photon microscopy respectively. The outcome showed that non-ablative IPL irradiated the aging mouse skin got the better effect, and then have gained the changes of spectrum intensity and corresponding photon numbers in a rectangular area, these probable achieve the mechanism of light irradiated skin. The intention of this was offer the theory basis in clinic.

  12. 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.

  13. The CLAS Two Photon Exchange Experiment

    NASA Astrophysics Data System (ADS)

    Adikaram, Dasuni; Bennett, Robert; Weinstein, Larry; Rimal, Dipak; Khetarpal, Puneet; Raue, Brian

    2013-04-01

    There is a large discrepancy between the proton electron form factor (GE^p(Q^2)) measured using the Rosenbluth separation and polarization transfer methods. The most likely explanation of this discrepancy is the inclusion of two-photon exchange (TPE) amplitude contributions to the elastic electron-proton cross section. The TPE contribution can be extracted in a model-independent way from the measured ratio of the cross sections of positron-proton and electron-proton elastic scattering. This ratio was measured in Hall B at Jefferson Lab using a simultaneous mixed tertiary beam of electrons and positrons incident on a liquid hydrogen target in the center of the CLAS detector in 2010-2011. In this talk, the experimental techniques to produce e^+/e^- beam, the analysis techniques to identify the elastic scattering events, and some preliminary results will be presented.

  14. The CLAS Two Photon Exchange Experiment

    NASA Astrophysics Data System (ADS)

    Adikaram, Dasuni; CLAS Collaboration

    2013-10-01

    There is a large discrepancy between the proton electron form factor (GEp(Q2)) measured using the Rosenbluth separation and polarization transfer methods. The most likely explanation of this discrepancy is the inclusion of two-photon exchange (TPE) amplitude contributions to the elastic electron-proton cross section. The TPE contribution can be extracted in a model-independent way from the measured ratio of the cross sections of positron-proton and electron-proton elastic scattering. This ratio was measured in Hall B at Jefferson Lab using a simultaneous mixed tertiary beam of electrons and positrons incident on a liquid hydrogen target in the center of the CLAS detector in 2010-2011. This talk will present the analysis techniques used to identify the elastic scattering events, and some preliminary results at Q2 = 1.4 (GeV/c)2.

  15. 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.

  16. Resonantly-enhanced axion-photon regeneration

    SciTech Connect

    Mueller, Guido; Sikivie, Pierre; Tanner, David B.; Bibber, Karl van

    2010-08-30

    A resonantly-enhanced photon-regeneration experiment to search for the axion or axion-like particles is discussed. Photons enter a strong magnetic field and some are converted to axions; the axions can pass through an opaque wall and some may convert back to photons in a second high-field region. The photon regeneration is enhanced by employing matched Fabry-Perot optical cavities, with one cavity within the axion generation magnet and the second within the photon regeneration magnet. The optics for this experiment are discussed, with emphasis on the alignment of the two cavities.

  17. 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.

  18. Two-photon decay of K-shell vacancies in silver atoms

    SciTech Connect

    Mokler, P.H.; Schaeffer, H.W.; Dunford, R. W.

    2004-09-01

    The spectral distributions for the two-photon decay modes of singly K-shell ionized silver atoms are determined by x-ray-x-ray coincidence measurements. Ag K-shell vacancies were induced by nuclear electron capture decay of radioactive cadmium isotopes {sup 109}Cd and two-photon coincidences were taken back to back (180 deg.) and at a 90 deg. opening angle for the emission. Each of the two-photon transitions from the 2s, 3s, and 3d states exhibits unique angular and spectral distributions. The measurements agree nicely with relativistic self-consistent field calculations of Tong et al. Our results also confirm and extend the earlier experimental data of Ilakovac and co-workers with improved accuracy.

  19. Two-photon decay of K -shell vacancies in silver atoms

    NASA Astrophysics Data System (ADS)

    Mokler, P. H.; Schäffer, H. W.; Dunford, R. W.

    2004-09-01

    The spectral distributions for the two-photon decay modes of singly K -shell ionized silver atoms are determined by x-ray-x-ray coincidence measurements. AgK -shell vacancies were induced by nuclear electron capture decay of radioactive cadmium isotopes Cd109 and two-photon coincidences were taken back to back (180°) and at a 90° opening angle for the emission. Each of the two-photon transitions from the 2s , 3s , and 3d states exhibits unique angular and spectral distributions. The measurements agree nicely with relativistic self-consistent field calculations of Tong Our results also confirm and extend the earlier experimental data of Ilakovac and co-workers with improved accuracy.

  20. Highly selective population of two excited states in nonresonant two-photon absorption

    NASA Astrophysics Data System (ADS)

    Zhang, Hui; Zhang, Shi-An; Sun, Zhen-Rong

    2011-08-01

    A nonresonant two-photon absorption process can be manipulated by tailoring the ultra-short laser pulse. In this paper, we theoretically demonstrate a highly selective population of two excited states in the nonresonant two-photon absorption process by rationally designing a spectral phase distribution. Our results show that one excited state is maximally populated while the other state population is widely tunable from zero to the maximum value. We believe that the theoretical results may play an important role in the selective population of a more complex nonlinear process comprising nonresonant two-photon absorption, such as resonance-mediated (2+1)-three-photon absorption and (2+1)-resonant multiphoton ionization.

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

    NASA Astrophysics Data System (ADS)

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

    2013-05-01

    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.

  2. Ordering of azobenzenes by two-photon isomerization.

    PubMed

    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. PMID:17092131

  3. Two-photon absorption in Hg 2Cl 2 crystals

    NASA Astrophysics Data System (ADS)

    Pelant, I.; Ambrož, M.; Hála, J.; Kohlová, V.; Barta, Č.

    1985-01-01

    Violet luminescence (396 nm) of Hg 2Cl 2 single crystals was observed under excitation of green light (∼ 500 nm) of a pulsed dye laser at liquid helium temperature. The effect is interpreted as due to the two-photon absorption process. The two-photon excitation spectrum of the luminescence was measured in the wavelength range 475-530 nm. Possible mechanisms of the two-photon transition are outlined.

  4. 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.

  5. Resonance production in two-photon interactions

    SciTech Connect

    Roe, N.A.

    1989-02-01

    Resonance production in two-photon interactions is studied using data collected with the ASP detector at the PEP e/sup +/e/sup /minus// storage ring located at the Stanford Linear Accelerator Center. The ASP detector is a non-magnetic lead-glass calorimeter constructed from 632 lead-glass bars. It covers 94% of 4..pi.. in solid angle, extending to within 20/degree/ of the beamline. Lead-scintillator calorimeters extend the coverage to within 21 mr of the beamline on both sides. Energy resolution of ..sqrt..E/10%, where E is the energy is GeV, is achieved for electrons and photons in the lead-glass calorimeter, and particle trajectories are reconstructed with high efficiency. A total luminosity of 108 pb/sup /minus/1/ was collected with the ASP detector at a center-of-mass energy of 29 GeV. The observed process is e/sup +/e/sup /minus// ..-->.. e/sup +/e/sup /minus//..gamma..*..gamma..* ..-->.. e/sup +/e/sup /minus//X, is a pseudoscalar resonance (J/sup PC/ = 0/sup /minus/+/) and ..gamma..* is a virtual (mass /ne/ 0) photon. The outgoing electrons scatter down the beampipe and are not detected. The observed resonances are the /eta/ and /eta/' mesons, with masses of 549 and 958 MeV, respectively. They are detected in the ..gamma gamma.. decay mode; a total of 2380 +- 49 /eta/ ..-->.. ..gamma gamma.. and 568 +- 26 /eta/' ..-->.. ..gamma gamma.. events are observed. From the number of events, the detection efficiency, and the calculated production cross sections the radiative widths, GAMMA/sub ..gamma gamma../, of the /eta/ and /eta/' were measured and found to be: GAMMA/sub ..gamma gamma../(/eta/) = .481 +- .010 +- .047keV and GAMMA/sub ..gamma gamma../(/eta/') = 4.71 +- .22 +- .70keV. These results are in good agreement with the world average values. 67 refs., 42 figs., 20 tabs.

  6. Two-photon interference with true thermal light

    SciTech Connect

    Zhai Yanhua; Zhang Da; Wu Lingan; Chen Xihao

    2005-10-15

    Two-photon interference and 'ghost' imaging with entangled light have attracted much attention since the last century because of features such as nonlocality and subwavelength effects. Recently, it has been found that pseudothermal light can mimic certain effects of entangled light. We report here the first observation of two-photon interference with true thermal light.

  7. Two-photon fluorescence excitation spectroscopy of biological molecules

    NASA Astrophysics Data System (ADS)

    Meshalkin, Yuri P.; Alfimov, E. E.; Groshev, D. E.; Makukha, V. K.

    1996-06-01

    The UV fluorescence spectra of aromatic amino-acids and some proteins at two photon excitation by second harmonic of Nd:YAG laser are received. Two-photon absorption cross sections of tryptophan, tyrosine, phenylalanine and proteins: bovine serum albumin, lysozyme, trypsin, (alpha) - chymotrypsinogen and pepsin at wavelength 532 nm were measured by means of the two-quantum standard method.

  8. Quantum information processing with narrow band two-photon state

    NASA Astrophysics Data System (ADS)

    Lu, Yajun

    Application of quantum sources in communication and information processing are believed to bring a new revolution to the on-going information age. The generation of applicable quantum sources such as single photon state and two-photon state, appears to be one of the most difficult in experimental quantum optics. Spontaneous Parametric Down-Conversion (PDC) is known to generate two-photon state, but bandwidth problem makes it less applicable in quantum information processing. The aim of this work is to generate a narrow band two-photon state and apply it to quantum information processing. We start by developing a cavity enhanced PDC device to narrow the bandwidth of the two-photon state. Direct measurement of the bandwidth of the generated state has been made and the quantum theory of such a device has been investigated. An application of this narrow band two-photon state is to generate anti-bunched photons for quantum cryptography, based on the quantum interference between the two-photon state and a coherent state. The feasibility of this scheme for pulsed pump is also investigated. When applying the concept of mode locking in lasers to a two-photon state, we have mode-locked two-photon state which exhibits a comb-like correlation function and may be used for engineering of quantum states in time domain. Other applications such as demonstration of single photon nonlocality, nonlinear sign gate in quantum computation, and direct measurement of quantum beating, will also be addressed.

  9. 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.

  10. Two-photon finite-pulse model for resonant transitions in attosecond experiments

    NASA Astrophysics Data System (ADS)

    Jiménez-Galán, Álvaro; Martín, Fernando; Argenti, Luca

    2016-02-01

    We present an analytical model capable of describing two-photon ionization of atoms with attosecond pulses in the presence of intermediate and final isolated autoionizing states. The model is based on the finite-pulse formulation of second-order time-dependent perturbation theory. It approximates the intermediate and final states with Fano's theory for resonant continua, and it depends on a small set of atomic parameters that can either be obtained from separate ab initio calculations or be extracted from a few selected experiments. We use the model to compute the two-photon resonant photoelectron spectrum of helium below the N =2 threshold for the RABITT (reconstruction of attosecond beating by interference of two-photon transitions) pump-probe scheme, in which an XUV attosecond pulse train is used in association with a weak IR probe, obtaining results in quantitative agreement with those from accurate ab initio simulations. In particular, we show that (i) the use of finite pulses results in a homogeneous redshift of the RABITT beating frequency, as well as a resonant modulation of the beating frequency in proximity to intermediate autoionizing states; (ii) the phase of resonant two-photon amplitudes generally experiences a continuous excursion as a function of the intermediate detuning, with either zero or 2 π overall variation.

  11. 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

  12. Characterization of one- and two-photon photochemical uncaging efficiency.

    PubMed

    Specht, Alexandre; Bolze, Frederic; Nicoud, Jean Francois; Goeldner, Maurice

    2013-01-01

    The idea of using light to unleash biologically active compounds from inert precursors (uncaging) was introduced over 30 years ago. Recent efforts prompted the development of photoremovable protecting groups that have increased photochemical efficiencies for one- and two-photon excitation to allow more sophisticated applications. This requires characterization of one- and two-photon photochemical efficiencies of the uncaging processes.The present chapter focuses on the characterization of one-photon quantum yields and two-photon cross-sections. PMID:23494373

  13. Random access three-dimensional two-photon microscopy.

    PubMed

    Rózsa, Balázs; Katona, Gergely; Vizi, E Sylvester; Várallyay, Zoltán; Sághy, Attila; Valenta, Lásló; Maák, Pál; Fekete, Júlia; Bányász, Akos; Szipocs, Róbert

    2007-04-01

    We propose a two-photon microscope scheme capable of real-time, three-dimensional investigation of the electric activity pattern of neural networks or signal summation rules of individual neurons in a 0.6 mm x 0.6 mm x 0.2 mm volume of the sample. The points of measurement are chosen according to a conventional scanning two-photon image, and they are addressed by separately adjustable optical fibers. This allows scanning at kilohertz repetition rates of as many as 100 data points. Submicrometer spatial resolution is maintained during the measurement similarly to conventional two-photon microscopy. PMID:17356631

  14. Investigating femtosecond-laser-induced two-photon photoacoustic generation

    PubMed Central

    Urban, Ben E.; Yi, Ji; Yakovlev, Vladislav; Zhang, Hao F.

    2014-01-01

    Abstract. We investigated two-photon absorption-based photoacoustic generation and compared it with corresponding photoluminescence emission. Experimental results revealed expected quadratic dependences on the incident optical fluence in both photoacoustic and photoluminescence processes. We also investigated the influence of optical scattering on the generation of two-photon photoacoustic and photoluminescence signals and found that photoacoustic signals attenuated more slowly than photoluminescence signals when the optical scattering coefficient was increased, which was attributed to a weaker ultrasonic attenuation than that the optical attenuation in the scattering medium. Finally, we showed three-dimensional two-photon photoacoustic imaging. PMID:25084119

  15. Two-photon-induced x-ray emission in neon atoms

    SciTech Connect

    Sun Yuping; Wang Chuankui; Rinkevicius, Zilvinas; Gel'mukhanov, Faris; Carniato, Stephane; Simon, Marc; Taieeb, Richard

    2010-10-15

    We investigated the resonant x-ray emission from a neon atom induced by the two-photon population of a double-core-hole excited state. Two qualitatively different schemes of this process are studied: The first one involves an off-resonant intermediate single-core-hole state; the second scheme passes through a resonant core-ionized intermediate state. The numerical simulations of the resonant x-ray emission performed for different peak intensities and pulse durations show significant population of the double-core-hole final states. Therefore, rather strong two-photon absorption-induced x-ray emission is predicted for both studied schemes. Thus, high counting rates in experimental measurements are expected.

  16. 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.

  17. Pulse-shaping based two-photon FRET stoichiometry

    PubMed Central

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

    2015-01-01

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

  18. 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.

  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. Two photon processes in ZnO quantum dots

    NASA Astrophysics Data System (ADS)

    Maikhuri, Deepti; Purohit, S. P.; Mathur, K. C.

    2016-01-01

    The two-photon bound-bound (TPBB) and the two-photon bound-free (TPBF) processes are studied for the electron in the initial 1S state in the conduction band of the ZnO quantum dot (QD) embedded in the HfO2 and the AlN matrices. The energy and the wave functions of the QD are obtained by using the effective mass approximation with a finite barrier height at the dot-matrix interface. Using the second order perturbation theory results are obtained for the two-photon absorption coefficient and the photoelectric cross section. The photoelectric cross section ratio for the circularly to the linearly polarized photons is also obtained. It is observed that the two-photon processes depend significantly on the polarization of the incident beam, the dot size, and the surrounding matrix. It is found that the electric quadrupole interaction enhance the TPBF photoelectric cross section.

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

    DOE PAGESBeta

    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.

  3. Two-photon transitions to excited states in atomic hydrogen

    SciTech Connect

    Quattropani, A.; Bassani, F.; Carillo, S.

    1982-06-01

    Resonant two-photon transition rates from the ground state of atomic hydrogen to ns excited states have been computed as a function of photon frequencies in the length and velocity gauges in order to test the accuracy of the calculation and to discuss the rate of convergence over the intermediate states. The dramatic structure of the transition rates produced by intermediate-state resonances is exhibited. A two-photon transparency is found in correspondence to each resonance.

  4. 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.

  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. 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

  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. PMID:26466255

  8. 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.

  9. 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.

  10. Primordial helium recombination. II. Two-photon processes

    SciTech Connect

    Hirata, Christopher M.; Switzer, Eric R.

    2008-04-15

    Interpretation of precision measurements of the cosmic microwave background (CMB) will require a detailed understanding of the recombination era, which determines such quantities as the acoustic oscillation scale and the Silk damping scale. This paper is the second in a series devoted to the subject of helium recombination, with a focus on two-photon processes in He i. The standard treatment of these processes includes only the spontaneous two-photon decay from the 2{sup 1}S level. We extend this treatment by including five additional effects, some of which have been suggested in recent papers but whose impact on He i recombination has not been fully quantified. These are: (i) stimulated two-photon decays; (ii) two-photon absorption of redshifted He i line radiation; (iii) two-photon decays from highly excited levels in He i (n{sup 1}S and n{sup 1}D, with n{>=}3); (iv) Raman scattering; and (v) the finite width of the 2{sup 1}P{sup o} resonance. We find that effect (iii) is highly suppressed when one takes into account destructive interference between different intermediate states contributing to the two-photon decay amplitude. Overall, these effects are found to be insignificant: they modify the recombination history at the level of several parts in 10{sup 4}.

  11. 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

  12. 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.

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

    SciTech Connect

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

    1998-12-16

    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.

  14. Two-Photon Absorption of Metal-Assisted Chromophores.

    PubMed

    Li, Xin; Rinkevicius, Zilvinas; Ågren, Hans

    2014-12-01

    Aiming to understand the effect of a metal surface on nonlinear optical properties and the combined effects of surface and solvent environments on such properties, we present a multiscale response theory study, integrated with dynamics of the two-photon absorption of 4-nitro-4'-amino-trans-stilbene physisorbed on noble metal surfaces, considering two such surfaces, Ag(111) and Au(111), and two solvents, cyclohexane and water, as cases for demonstration. A few conclusions of general character could be drawn: While the geometrical change of the chromophore induced by the environment was found to notably alter (diminish) the two-photon absorption cross section in the polar medium, the effects of the metal surface and solvent on the electronic structure of the chromophore surpasses the geometrical effects and leads to a considerably enhanced two-photon absorption cross section in the polar solvent. This enhancement of two-photon absorption arises essentially from the metal charge image induced enlargement of the difference between the dipole moment of the excited state and the ground state. The orientation-dependence of the two-photon absorption is found to connect with the lateral rotation of the chromophore, where the two-photon absorption reaches its maximum when the polarization of the incident light coincides with the long-axis of the chromophore. Our results demonstrate a distinct enhancement of the two-photon absorption by a metal surface and a polar medium and envisage the employment of metal-chromophore composite materials for future development of nonlinear optical materials with desirable properties. PMID:26583246

  15. 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.

  16. 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.

  17. Ionization Energy Measurements and Spectroscopy of HfO and HfO^+

    NASA Astrophysics Data System (ADS)

    Merritt, J. M.; Bondybey, V. E.; Heaven, M. C.

    2009-06-01

    Rotationally resolved spectra of the HfO^+ cation have been recorded using the pulsed field ionization zero electron kinetic energy (PFI-ZEKE) technique. The F(0^+)← X^1Σ_g band system in HfO was resonantly excited to provide vibrational and rotational state selectivity in the two photon ionization process. Using the PFI-ZEKE technique a value of 7.91687(10) eV was determined for the ionization energy (IE) of HfO, 0.37 eV higher than the values reported previously using electron impact ionization measurements. Underestimation of the IE in the previous studies is attributed to ionization of thermally excited states. A progression in the HfO^+ stretching vibration up to ν^+ = 4 was observed in the PFI-ZEKE spectrum, allowing for determination of the ground electronic state vibrational frequency of ν_e = 1017.7(10) cm^{-1} and anharmonicity of ω_ex_e = 3.2(2) cm^{-1}. The rotational constant of HfO^+ was determined to be 0.403(5) cm^{-1}. Benchmark theoretical ab initio calculations were carried out in order to explore the effects of electron correlation on the predicted molecular properties. Survey scans utilizing laser induced fluorescence and resonance enhanced multiphoton ionization detection revealed many previously unassigned bands in the region of the F-X and G-X bands of HfO, which we attribute to nominally forbidden singlet - triplet transitions of HfO.

  18. Mechanism of two-photon excited hemoglobin fluorescence emission

    NASA Astrophysics Data System (ADS)

    Sun, Qiqi; Zheng, Wei; Wang, Jiannong; Luo, Yi; Qu, Jianan Y.

    2015-10-01

    Hemoglobin, one of the most important proteins in the human body, is composed of "heme" groups (iron-containing rings) and "globins" (proteins). We investigate the two-photon excited fluorescence of hemoglobin and its subunit components (heme and globin). We measure the hemoglobin fluorescence lifetime by using a streak camera of ps resolution and confirm that its lifetime is in femtosecond scale. In the study of the fluorescence properties of heme and globin, the experimental results reveal that heme is the sole fluorophore of hemoglobin. Hemoglobin fluorescence can be effectively excited only via two-photon process, because heme has a centrosymmetric molecular structure and two-photon allowed transition is forbidden for single-photon process and vice versa due to the Laporte parity selection rule.

  19. Mechanism of two-photon excited hemoglobin fluorescence emission.

    PubMed

    Sun, Qiqi; Zheng, Wei; Wang, Jiannong; Luo, Yi; Qu, Jianan Y

    2015-10-01

    Hemoglobin, one of the most important proteins in the human body, is composed of “heme” groups (iron-containing rings) and “globins” (proteins). We investigate the two-photon excited fluorescence of hemoglobin and its subunit components (heme and globin). We measure the hemoglobin fluorescence lifetime by using a streak camera of ps resolution and confirm that its lifetime is in femtosecond scale. In the study of the fluorescence properties of heme and globin, the experimental results reveal that heme is the sole fluorophore of hemoglobin. Hemoglobin fluorescence can be effectively excited only via two-photon process, because heme has a centrosymmetric molecular structure and two-photon allowed transition is forbidden for single-photon process and vice versa due to the Laporte parity selection rule. PMID:26506468

  20. Two-photon absorption of few-electron heavy ions

    SciTech Connect

    Surzhykov, A.; Indelicato, P.; Santos, J. P.; Amaro, P.; Fritzsche, S.

    2011-08-15

    The two-photon absorption of few-electron ions has been studied by using second-order perturbation theory and Dirac's relativistic equation. Within this framework, the general expressions for the excitation cross sections and rates are derived including a full account of the higher-order multipole terms in the expansion of the electron-photon interaction. While these expressions can be applied to any ion, independent of its particular shell structure, detailed computations are carried out for the two-photon absorption of hydrogen-, helium-, and berylliumlike ions and are compared with the available theoretical and experimental data. The importance of relativistic and nondipole effects in the analysis and computation of induced two-photon transitions is pointed out. Moreover, we discuss the potential of these transitions for atomic parity-violation studies in the high-Z domain.

  1. 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.

  2. Two-photon imaging of the immune system.

    PubMed

    Dzhagalov, Ivan L; Melichar, Heather J; Ross, Jenny O; Herzmark, Paul; Robey, Ellen A

    2012-04-01

    Two-photon microscopy is a powerful method for visualizing biological processes as they occur in their native environment in real time. The immune system uniquely benefits from this technology as most of its constituent cells are highly motile and interact extensively with each other and with the environment. Two-photon microscopy has provided many novel insights into the dynamics of the development and function of the immune system that could not have been deduced by other methods and has become an indispensible tool in the arsenal of immunologists. In this unit, we provide several protocols for preparation of various organs for imaging by two-photon microscopy that are intended to introduce the new user to some basic aspects of this method. PMID:22470153

  3. Adaptive optics two-photon scanning laser fluorescence microscopy

    NASA Astrophysics Data System (ADS)

    Zhou, Yaopeng; Bifano, Thomas; Lin, Charles

    2011-03-01

    Two-photon fluorescence microscopy provides a powerful tool for deep tissue imaging. However, optical aberrations from illumination beam path limit imaging depth and resolution. Adaptive Optics (AO) is found to be useful to compensate for optical aberrations and improve image resolution and contrast from two-photon excitation. We have developed an AO system relying on a MEMS Deformable Mirror (DM) to compensate the optical aberrations in a two-photon scanning laser fluorescence microscope. The AO system utilized a Zernike polynomial based stochastic parallel gradient descent (SPGD) algorithm to optimize the DM shape for wavefront correction. The developed microscope is applied for subsurface imaging of mouse bone marrow. It was demonstrated that AO allows 80% increase in fluorescence signal intensity from bone cavities 145um below the surface. The AO-enhanced microscope provides cellular level images of mouse bone marrow at depths exceeding those achievable without AO.

  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. Cell assay using a two-photon-excited europium chelate

    PubMed Central

    Xiao, Xudong; Haushalter, Jeanne P.; Kotz, Kenneth T.; Faris, Gregory W.

    2011-01-01

    We report application of two-photon excitation of europium chelates to immunolabeling of epidermal growth factor receptor (EGFR) cell surface proteins on A431 cancer cells. The europium chelates are excited with two photons of infrared light and emit in the visible. Europium chelates are conjugated to antibodies for EGFR. A431 (human epidermoid carcinoma) cells are labeled with this conjugate and imaged using a multiphoton microscope. To minimize signal loss due to the relatively long-lived Eu3+ emission, the multiphoton microscope is used with scanning laser two-photon excitation and non-scanning detection with a CCD. The chelate labels show very little photobleaching (less than 1% during continuous illumination in the microscope for 20 minutes) and low levels of autofluorescence (less than 1% of the signal from labeled cells). The detection limit of the europium label in the cell assay is better than 100 zeptomoles. PMID:21833362

  6. 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

  7. Modulation of Attosecond Beating by Resonant Two-Photon Transition

    NASA Astrophysics Data System (ADS)

    Jiménez Galán, Álvaro; Argenti, Luca; Martín, Fernando

    2015-09-01

    We present an analytical model that characterizes two-photon transitions in the presence of autoionising states. We applied this model to interpret resonant RABITT spectra, and show that, as a harmonic traverses a resonance, the phase of the sideband beating significantly varies with photon energy. This phase variation is generally very different from the π jump observed in previous works, in which the direct path contribution was negligible. We illustrate the possible phase profiles arising in resonant two-photon transitions with an intuitive geometrical representation.

  8. 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.

  9. A fluorescent benzothiazole probe with efficient two-photon absorption

    NASA Astrophysics Data System (ADS)

    Echevarria, Lorenzo; Moreno, Iván; Camacho, José; Salazar, Mary Carmen; Hernández, Antonio

    2012-11-01

    In this work, we report the two-photon absorption of 2-[4-(dimethylamino)phenyl]-1,3-benzothiazole-6-carbonitrile (DBC) in DMSO solution pumping at 779 nm with a 10 ns pulse laser-Nd:YAG system. The obtained two-photon absorption cross-section in DBC (407 ± 18 GM) is considerably high. Because DBC is a novel compound and have high values of fluorescence quantum yield, this result is expected to have an impact in biomolecules detection, diagnosis and treatment of cancer. Similar structures have previously been reported to show remarkable antitumour effects.

  10. Projection two-photon polymerization using a spatial light modulator

    NASA Astrophysics Data System (ADS)

    Yang, Liang; Li, Jiawen; Hu, Yanlei; Zhang, Chenchu; Lao, Zhaoxin; Huang, Wenhao; Chu, Jiaru

    2014-11-01

    The development of a high-efficiency projection two-photon polymerization (P2PP) process by using a liquid crystal spatial light modulator (SLM) is presented. Rapid fabrication of 2D patterned microstructures with P2PP is demonstrated, and the effect of laser pattern and exposure dose on the surface roughness of the fabricated microstructures is investigated. It is found that the distribution of laser intensity at the focal plane of objective has a significant effect on the profiles of microstructures. This unique technology has a promising approach to increase the efficiency of two-photon polymerization (2PP) and a parallel fabrication of complex 2D and 3D microstructures.

  11. Two-photon in vivo imaging of retinal microstructures

    NASA Astrophysics Data System (ADS)

    Schejter, Adi; Farah, Nairouz; Shoham, Shy

    2014-02-01

    Non-invasive fluorescence retinal imaging in small animals is an important requirement in an array of translational vision applications. Two-photon imaging has the potential for long-term investigation of healthy and diseased retinal function and structure in vivo. Here, we demonstrate that two-photon microscopy through a mouse's pupil can yield high-quality optically sectioned fundus images. By remotely scanning using an electronically tunable lens we acquire highly-resolved 3D fluorescein angiograms. These results provide an important step towards various applications that will benefit from the use of infrared light, including functional imaging of retinal responses to light stimulation.

  12. 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.

  13. 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.

  14. 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.

  15. 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.

  16. 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.

  17. Two-Photon-Pumped Perovskite Semiconductor Nanocrystal Lasers.

    PubMed

    Xu, Yanqing; Chen, Qi; Zhang, Chunfeng; Wang, Rui; Wu, Hua; Zhang, Xiaoyu; Xing, Guichuan; Yu, William W; Wang, Xiaoyong; Zhang, Yu; Xiao, Min

    2016-03-23

    Two-photon-pumped lasers have been regarded as a promising strategy to achieve frequency up-conversion for situations where the condition of phase matching required by conventional approaches cannot be fulfilled. However, their practical applications have been hindered by the lack of materials holding both efficient two-photon absorption and ease of achieving population inversion. Here, we show that this challenge can be tackled by employing colloidal nanocrystals of perovskite semiconductors. We observe highly efficient two-photon absorption (with a cross section of 2.7 × 10(6) GM) in toluene solutions of CsPbBr3 nanocrystals that can excite large optical gain (>500 cm(-1)) in thin films. We have succeeded in demonstrating stable two-photon-pumped lasing at a remarkable low threshold by coupling CsPbBr3 nanocrystals with microtubule resonators. Our findings suggest perovskite nanocrystals can be used as excellent gain medium for high-performance frequency-up-conversion lasers toward practical applications. PMID:26938656

  18. 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.

  19. Two-photon excitation endoscopy through a multimode optical fiber

    NASA Astrophysics Data System (ADS)

    Morales Delgado, Edgar E.; Psaltis, Demetri; Moser, Christophe

    2016-03-01

    The vast number of propagating solutions to the wave equation in multimode optical fibers represents a larger information capacity than provided by fiber bundles of the same diameter. Therefore, in the field of imaging, multimode fibers potentially allow the transmission of images with higher resolution. However, image transmission through multimode fibers is not direct as in the fiber bundle case, in which each of the fiber cores can relay a portion of the distal image. In multimode fiber transmission, a distribution of intensity is scrambled in time and space by the propagating modes, leading to a speckle-like pattern that does not resemble the initial distribution. Here, we demonstrate two-photon excitation imaging of fluorescent beads through a multimode optical fiber. We show that our method maintains the advantages of two-photon excitation microscopy compared to single-photon excitation such as reduced photo-bleaching, deeper penetration depth and sectioning capability. Our method is based on time-gated digital phase conjugation, which allows the generation of focused pulses on the other side of a multimode fiber. To acquire an image, the focused femtosecond pulse is scanned in a three-dimensional mesh, producing two-photon excitation on each spatial location of the sample. By collecting the fluorescence through the fiber, a 3D two-photon image is reconstructed.

  20. 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.

  1. 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.

  2. 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.

  3. 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).

  4. Three-dimensional micronanofabrication via two-photon-excited photoisomerization

    NASA Astrophysics Data System (ADS)

    Xia, Hong; Zhang, Wen-Yi; Wang, Fang-Fang; Wu, Dong; Liu, Xiang-Wei; Chen, Lei; Chen, Qi-Dai; Ma, Yu-Guang; Sun, Hong-Bo

    2009-08-01

    In this letter, laser micronanofabrication via two-photon absorption initiated isomerization was proposed and explored. Experimentally a cis-form rich poly[2,5-dihexyloxy-1,4-phenylene] vinylene)-alt-(2,5-diphenyl-1,4-phenylene vinylene)] (DPO-PPV) was used as the precursory material, which underwent pinpoint molecular conformational change upon the near-infrared femtosecond laser irradiation. Due to pronouncedly reduced solubility of trans-configuration molecules, the precipitate at the tiny volumes was implemented as voxels to construct two- and three-dimensional micronanostructures. This mechanism may provide an alternative enabling tool other than two-photon absorption initiated polymerization of resins for designable micronanofabrication of photonic or optoelectronic devices including organic electroluminescent devices, particularly those based on PPV and its derivatives.

  5. A [111]-Cut Si Hemisphere Two-Photon Response Photodetector

    NASA Astrophysics Data System (ADS)

    Liu, Xiu-Huan; Chen, Zhan-Guo; Jia, Gang; Wang, Hai-Yan; Gao, Yan-Jun; Li, Yi

    2011-11-01

    Properties of two-photon response in a [111]-cut nearly-intrinsic Si hemisphere photodetector are studied. The measured photocurrent of the photodetector responding to the 1.32μm continuous wave laser shows a quadratic dependence on the coupled optical power and is saturated with the bias voltage. Also, the photocurrent is independent of polarization. Such properties are in good agreement with the theory of two-photon absorption. The isotropic photocurrent generated from the [111]-cut Si hemisphere is compared to the anisotropic one induced in the [110]-cut Si sample and the ratio of χxxxx/χxxyy for silicon performing at 1.32 μm is calculated to be 2.4 via the fitted function of the anisotropic photocurrent from the [110]-cut sample.

  6. Extended cavity laser enhanced two-photon flow cytometry

    PubMed Central

    Tkaczyk, Eric R.; Tkaczyk, Alan H.; Katnik, Steve; Ye, Jing Yong; Luker, Kathryn E.; Luker, Gary D.; Myc, Andrzej; Baker, James R.; Norris, Theodore B.

    2015-01-01

    We demonstrate enhanced sensitivity in two-photon flow cytometry with an extended cavity laser excitation source. At low power, the home-built 20-MHz oscillator was able to detect a significantly larger fraction, in either phosphate buffered saline (PBS) or whole blood, of green fluorescent protein (GFP) –expressing MCA-207 cells cross-labeled with the membrane-binding lipophilic dye DiD. A geometrical model is used to explain unique features of the signals resulting from the different spatial distribution of DiD and GFP. These unique features include sub-square law scaling of unsaturated two-photon signal, a sigmoidal sensitivity curve for detection under varying powers for cell detection thresholds as low as a single photon, and uncorrelated signal strengths in two detection channels. PMID:19021327

  7. 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.

  8. Thermal light two-photon imaging: magic mirrors

    NASA Astrophysics Data System (ADS)

    Scarcelli, Giuliano; Berardi, Vincenzo; Shih, Yanhua

    2005-08-01

    We show an experimental study of two-photon imaging using thermal light sources. It is interesting to see that the thermal source behaves like a mirror producing an equal size reproduction of a chosen object. We refer to such mirror as "magic" because the ghost image produced by the mirror is real in the sense that it lies in the real space and can be further imaged by a camera or an equivalent optical system. We also show that it is possible to overcome the main limitation towards the actual implementation of thermal light two-photon imaging, i.e. the poor contrast of the imaging pattern, by designing an appropriate correlation measurement scheme that is insensitive to the uncorrelated background noise.

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

    PubMed Central

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

    2014-01-01

    Abstract. 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. PMID:24589986

  10. 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. PMID:27446680