Laser-induced breakup of helium 3S 1s2s with intermediate doubly excited states

NASA Astrophysics Data System (ADS)

Simonsen, A. S.; Bachau, H.; Førre, M.

2014-02-01

Solving the time-dependent Schrödinger equation in full dimensionality for two electrons, it is found that in the XUV regime the two-photon double ionization dynamics of He(1s2s) is predominantly dictated by the process of resonance enhanced multiphoton ionization via doubly excited states (DESs). We have studied a pump-probe scenario where the full laser-driven breakup of the 3S 1s2s metastable state is dominated by intermediate quasiresonant excitation to doubly excited (autoionizing) states in the 3Po series. Clear evidence of multipath interference effects is revealed in the resulting angular distributions of the ejected electrons in cases where more than one intermediate DES is populated in the process.

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.

Correlated electron and nuclear dynamics in strong field photoionization of H(2)(+).

PubMed

Silva, R E F; Catoire, F; Rivière, P; Bachau, H; Martín, F

2013-03-15

We present a theoretical study of H(2)(+) ionization under strong IR femtosecond pulses by using a method designed to extract correlated (2D) photoelectron and proton kinetic energy spectra. The results show two distinct ionization mechanisms-tunnel and multiphoton ionization-in which electrons and nuclei do not share the energy from the field in the same way. Electrons produced in multiphoton ionization share part of their energy with the nuclei, an effect that shows up in the 2D spectra in the form of energy-conservation fringes similar to those observed in weak-field ionization of diatomic molecules. In contrast, tunneling electrons lead to fringes whose position does not depend on the proton kinetic energy. At high intensity, the two processes coexist and the 2D plots show a very rich behavior, suggesting that the correlation between electron and nuclear dynamics in strong field ionization is more complex than one would have anticipated.

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.

Observation of novel photochemistry in the multiphoton ionization of Mo(CO) sub 6 van der Waals clusters

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

Peifer, W.R.; Garvey, J.F.

1989-07-27

van der Waals clusters of Mo(CO){sub 6} generated in the free-jet expansion of a pulsed beam of seeded helium are subjected to multiphoton ionization and the product ions analyzed by quadrupole mass spectrometry. Oxomolybdenum and dioxomolybdenum ions are observed to be produced with high efficiency. This behavior is in striking contrast to that of metal carbonyl monomers and covalently bound cluster carbonyls, which under complete ligand loss prior to ionization. The observed photochemistry is ascribed to reactions between a photoproduced molybdenum atom and the ligands of neighboring Mo(CO){sub 6} solvent molecules within the van der Waals cluster.

Multi-photon ionization of atoms in intense short-wavelength radiation fields

NASA Astrophysics Data System (ADS)

Meyer, Michael

2015-05-01

The unprecedented characteristics of XUV and X-ray Free Electron Lasers (FELs) have stimulated numerous investigations focusing on the detailed understanding of fundamental photon-matter interactions in atoms and molecules. In particular, the high intensities (up to 106 W/cm2) giving rise to non-linear phenomena in the short wavelength regime. The basic phenomenology involves the production of highly charged ions via electron emission to which both sequential and direct multi-photon absorption processes contribute. The detailed investigation of the role and relative weight of these processes under different conditions (wavelength, pulse duration, intensity) is the key element for a comprehensive understanding of the ionization dynamics. Here the results of recent investigations are presented, performed at the FELs in Hamburg (FLASH) and Trieste (FERMI) on atomic systems with electronic structures of increasing complexity (Ar, Ne and Xe). Mainly, electron spectroscopy is used to obtain quantitative information about the relevance of various multi-photon ionization processes. For the case of Ar, a variety of processes including above threshold ionization (ATI) from 3p and 3s valence shells, direct 2p two-photon ionization and resonant 2p-4p two-photon excitations were observed and their role was quantitatively determined comparing the experimental ionization yields to ab-initio calculations of the cross sections for the multi-photon processes. Using Ar as a benchmark to prove the reliability of the combined experimental and theoretical approach, the more complex and intriguing case of Xe was studied. Especially, the analysis of the two-photon ATI from the Xe 4d shell reveals new insight into the character of the 4d giant resonance, which was unresolved in the linear one-photon regime. Finally, the influence of intense XUV radiation to the relaxation dynamics of the Ne 2s-3p resonance was investigated by angle-resolved electron spectroscopy, especially be observing the intensity dependent variation of the angular distribution patterns for the sequential ionization process.

Impact of Coulomb potential on peak structures arising in momentum and low-energy photoelectron spectra produced in strong-field ionization of laser-irradiated atoms

NASA Astrophysics Data System (ADS)

Pyak, P. E.; Usachenko, V. I.

2018-03-01

The phenomenon of pronounced peak structure(s) of longitudinal momentum distributions as well as a spike-like structure of low-energy spectra of photoelectrons emitted from laser-irradiated Ar and Ne atoms in a single ionization process is theoretically studied in the tunneling and multiphoton regimes of ionization. The problem is addressed assuming only the direct above-threshold ionization (ATI) as a physical mechanism underlying the phenomenon under consideration (viz. solely contributing to observed photoelectron momentum distributions (PMD)) and using the Coulomb-Volkov (CV) ansatz within the frame of conventional strong-field approximation (SFA) applied in the length-gauge formulation. The developed CV-SFA approach also incorporates the density functional theory essentially exploited for numerical composition of initial (laser-free) atomic state(s) constructed from atomic orbitals of Gaussian type. Our presented CV-SFA based (and laser focal-volume averaged) calculation results proved to be well reproducing both the pronounced double-peak and/or ATI-like multi-peak structure(s) experimentally observed in longitudinal PMD under conditions of tunneling and/or multiphoton regime, respectively. In addition, our CV-SFA results presented for tunneling regime also suggest and remarkably reproduce a pronounced structure observed in relevant experiments as a ‘spike-like’ enhanced maximum arising in low-energy region (around the value of about 1 eV) of photoelectron spectra. The latter consistency allows to identify and interpret these results as the so-called low-energy structure (LES) since the phenomenon proved to appear as the most prominent if the influence of Coulomb potential on photoelectron continuum states is maximally taken into account under calculations (viz. if the parameter Z in CV’s functions is put equal to 1). Moreover, the calculated LES proved to correspond (viz., established as closely related) to the mentioned double-peak structure arising in the low-momentum region ({p}| | ≤slant | 0.2| a.u.) of longitudinal PMDs calculated under condition of the tunneling regime. Thus, the phenomena under consideration can be well understood and adequately interpreted beyond the terms and/or concepts of various different alternative strong-field approaches and models (such as e.g., extensively invoked and exploited nowadays though, more sophisticated SFA-based ‘rescattering’ mechanism) compared to which, the currently applied CV-SFA model (through the same underlying physical mechanism of solely direct ATI suggested) is additionally able to provide and reveal an intimate and transparent interrelation between the phenomena of LES and double-peak structure arising in PMDs observed in the tunneling regime.

Disentangling formation of multiple-core holes in aminophenol molecules exposed to bright X-FEL radiation

NASA Astrophysics Data System (ADS)

Zhaunerchyk, V.; Kamińska, M.; Mucke, M.; Squibb, R. J.; Eland, J. H. D.; Piancastelli, M. N.; Frasinski, L. J.; Grilj, J.; Koch, M.; McFarland, B. K.; Sistrunk, E.; Gühr, M.; Coffee, R. N.; Bostedt, C.; Bozek, J. D.; Salén, P.; Meulen, P. v. d.; Linusson, P.; Thomas, R. D.; Larsson, M.; Foucar, L.; Ullrich, J.; Motomura, K.; Mondal, S.; Ueda, K.; Richter, R.; Prince, K. C.; Takahashi, O.; Osipov, T.; Fang, L.; Murphy, B. F.; Berrah, N.; Feifel, R.

2015-12-01

Competing multi-photon ionization processes, some leading to the formation of double core hole states, have been examined in 4-aminophenol. The experiments used the linac coherent light source (LCLS) x-ray free electron laser, in combination with a time-of-flight magnetic bottle electron spectrometer and the correlation analysis method of covariance mapping. The results imply that 4-aminophenol molecules exposed to the focused x-ray pulses of the LCLS sequentially absorb more than two x-ray photons, resulting in the formation of multiple core holes as well as in the sequential removal of photoelectrons and Auger electrons (so-called PAPA sequences).

Disentangling formation of multiple-core holes in aminophenol molecules exposed to bright X-FEL radiation

DOE PAGES

Zhaunerchyk, V.; Kaminska, M.; Mucke, M.; ...

2015-10-28

Competing multi-photon ionization processes, some leading to the formation of double core hole states, have been examined in 4-aminophenol. The experiments used the linac coherent light source (LCLS) x-ray free electron laser, in combination with a time-of-flight magnetic bottle electron spectrometer and the correlation analysis method of covariance mapping. Furthermore, the results imply that 4-aminophenol molecules exposed to the focused x-ray pulses of the LCLS sequentially absorb more than two x-ray photons, resulting in the formation of multiple core holes as well as in the sequential removal of photoelectrons and Auger electrons (so-called PAPA sequences).

Strong field control of the interatomic Coulombic decay process in quantum dots

NASA Astrophysics Data System (ADS)

Haller, Anika; Chiang, Ying-Chih; Menger, Maximilian; Aziz, Emad F.; Bande, Annika

2017-01-01

In recent years the laser-induced interatomic Coulombic decay (ICD) process in paired quantum dots has been predicted (Bande, 2013). In this work we target the enhancement of ICD by scanning over a range of strong-field laser intensities. The GaAs quantum dots are modeled by a one-dimensional double-well potential in which simulations are done with the space-resolved multi-configuration time-dependent Hartree method including antisymmetrization to account for the fermions. As a novelty a complementary state-resolved ansatz is developed to consolidate the interpretation of transient state populations, widths obtained for the ICD and the competing direct ionization channel, and Fano peak profiles in the photoelectron spectra. The major results are that multi-photon processes are unimportant even for the strongest fields. Further, below- π to π pulses display the highest ICD efficiency while the direct ionization becomes less dominant.

Ultrafast Electron Plasma Index: An Ionization Perspective

DTIC Science & Technology

2014-05-29

picture in mind, the derivation of the index was a combination of the principle of least action and Fermat’s principle. In the current textbook ...multiphoton ionization. Phys Rev Lett 71: 1994-1997. 27. Ivanov MY, Spanner M, Smirnova O (2005) Anatomy of strong field ionization. J. Mod.Phys 52

Detection limits of organic compounds achievable with intense, short-pulse lasers.

PubMed

Miles, Jordan; De Camillis, Simone; Alexander, Grace; Hamilton, Kathryn; Kelly, Thomas J; Costello, John T; Zepf, Matthew; Williams, Ian D; Greenwood, Jason B

2015-06-21

Many organic molecules have strong absorption bands which can be accessed by ultraviolet short pulse lasers to produce efficient ionization. This resonant multiphoton ionization scheme has already been exploited as an ionization source in time-of-flight mass spectrometers used for environmental trace analysis. In the present work we quantify the ultimate potential of this technique by measuring absolute ion yields produced from the interaction of 267 nm femtosecond laser pulses with the organic molecules indole and toluene, and gases Xe, N2 and O2. Using multiphoton ionization cross sections extracted from these results, we show that the laser pulse parameters required for real-time detection of aromatic molecules at concentrations of one part per trillion in air and a limit of detection of a few attomoles are achievable with presently available commercial laser systems. The potential applications for the analysis of human breath, blood and tissue samples are discussed.

Detection of polychlorinated biphenyls in transformer oils in Vietnam by multiphoton ionization mass spectrometry using a far-ultraviolet femtosecond laser as an ionization source.

PubMed

Duong, Vu Thi Thuy; Duong, Vu; Lien, Nghiem Thi Ha; Imasaka, Tomoko; Tang, Yuanyuan; Shibuta, Shinpei; Hamachi, Akifumi; Hoa, Do Quang; Imasaka, Totaro

2016-03-01

Polychlorinated biphenyls (PCBs) in transformer and food oils were measured using gas chromatography combined with multiphoton ionization mass spectroscopy. An ultrashort laser pulse emitting in the far-ultraviolet region was utilized for efficient ionization of the analytes. Numerous signal peaks were clearly observed for a standard sample mixture of PCBs when the third and fourth harmonic emissions (267 and 200nm) of a femtosecond Ti:sapphire laser (800nm) were employed. The signal intensities were found to be greater when measured at 200nm compared with those measured at 267nm, providing lower detection limits especially for highly chlorinated PCBs at shorter wavelengths. After simple pretreatment using disposable columns, PCB congeners were measured and found to be present in the transformer oils used in Vietnam. Copyright © 2015 Elsevier B.V. All rights reserved.

Ultrafast multiphoton ionization dynamics and control of NaK molecules

NASA Astrophysics Data System (ADS)

Davidsson, Jan; Hansson, Tony; Mukhtar, Emad

1998-12-01

The multiphoton ionization dynamics of NaK molecules is investigated experimentally using one-color pump-probe femtosecond spectroscopy at 795 nm and intermediate laser field strengths (about 10 GW/cm2). Both NaK+ and Na+ ions are detected as a function of pulse separation time, pulse intensities, and strong pulse-weak pulse order. To aid in the analysis, the potential energy curves of the two lowest electronic states of NaK+ and the electronic transition dipole moment between them are calculated by the GAUSSIAN94 UCIS method. Different ionization pathways are identified by Franck-Condon analysis, and vibrational dynamics in the A 1Σ+ and 3 1Π states, as well as in the ground state, is observed. Further, the existence of a highly excited (above the adiabatic ionization limit) neutral state of NaK is proposed. By changing the strong pulse-weak pulse order of the pulses, the ionization pathways for production of both ions can be varied and thus controlled.

Analysis of plasma-mediated ablation in aqueous tissue

NASA Astrophysics Data System (ADS)

Jiao, Jian; Guo, Zhixiong

2012-06-01

Plasma-mediated ablation using ultrafast lasers in transparent media such as aqueous tissues is studied. It is postulated that a critical seed free electron density exists due to the multiphoton ionization in order to trigger the avalanche ionization which causes ablation and during the avalanche ionization process the contribution of laser-induced photon ionization is negligible. Based on this assumption, the ablation process can be treated as two separate processes - the multiphoton and avalanche ionizations - at different time stages; so that an analytical solution to the evolution of plasma formation is obtained for the first time. The analysis is applied to plasma-mediated ablation in corneal epithelium and validated via comparison with experimental data available in the literature. The critical seed free-electron density and the time to initiate the avalanche ionization for sub-picosecond laser pulses are analyzed. It is found that the critical seed free-electron density decreases as the pulse width increases, obeying a tp-5.65 rule. This model is further extended to the estimation of crater size in the ablation of tissue-mimic polydimethylsiloxane (PDMS). The results match well with the available experimental measurements.

Revisiting photon-statistics effects on multiphoton ionization

NASA Astrophysics Data System (ADS)

Mouloudakis, G.; Lambropoulos, P.

2018-05-01

We present a detailed analysis of the effects of photon statistics on multiphoton ionization. Through a detailed study of the role of intermediate states, we evaluate the conditions under which the premise of nonresonant processes is valid. The limitations of its validity are manifested in the dependence of the process on the stochastic properties of the radiation and found to be quite sensitive to the intensity. The results are quantified through detailed calculations for coherent, chaotic, and squeezed vacuum radiation. Their significance in the context of recent developments in radiation sources such as the short-wavelength free-electron laser and squeezed vacuum radiation is also discussed.

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

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

Hróðmarsson, Helgi Rafn; Wang, Huasheng; Kvaran, Ágúst, E-mail: agust@hi.is

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.

Miniature fiber-optic multiphoton microscopy system using frequency-doubled femtosecond Er-doped fiber laser

PubMed Central

Huang, Lin; Mills, Arthur K.; Zhao, Yuan; Jones, David J.; Tang, Shuo

2016-01-01

We report on a miniature fiber-optic multiphoton microscopy (MPM) system based on a frequency-doubled femtosecond Er-doped fiber laser. The femtosecond pulses from the laser source are delivered to the miniature fiber-optic probe at 1.58 µm wavelength, where a standard single mode fiber is used for delivery without the need of free-space dispersion compensation components. The beam is frequency-doubled inside the probe by a periodically poled MgO:LiNbO3 crystal. Frequency-doubled pulses at 786 nm with a maximum power of 80 mW and a pulsewidth of 150 fs are obtained and applied to excite intrinsic signals from tissues. A MEMS scanner, a miniature objective, and a multimode collection fiber are further used to make the probe compact. The miniature fiber-optic MPM system is highly portable and robust. Ex vivo multiphoton imaging of mammalian skins demonstrates the capability of the system in imaging biological tissues. The results show that the miniature fiber-optic MPM system using frequency-doubled femtosecond fiber laser can potentially bring the MPM imaging for clinical applications. PMID:27231633

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

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

Germann, Matthias; Willitsch, Stefan, E-mail: stefan.willitsch@unibas.ch

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 structuremore » 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.« less

Wavelength dependent photoelectron circular dichroism of limonene studied by femtosecond multiphoton laser ionization and electron-ion coincidence imaging

NASA Astrophysics Data System (ADS)

Rafiee Fanood, Mohammad M.; Janssen, Maurice H. M.; Powis, Ivan

2016-09-01

Enantiomers of the monoterpene limonene have been investigated by (2 + 1) resonance enhanced multiphoton ionization and photoelectron circular dichroism employing tuneable, circularly polarized femtosecond laser pulses. Electron imaging detection provides 3D momentum measurement while electron-ion coincidence detection can be used to mass-tag individual electrons. Additional filtering, by accepting only parent ion tagged electrons, can be then used to provide discrimination against higher energy dissociative ionization mechanisms where more than three photons are absorbed to better delineate the two photon resonant, one photon ionization pathway. The promotion of different vibrational levels and, tentatively, different electronic ion core configurations in the intermediate Rydberg states can be achieved with different laser excitation wavelengths (420 nm, 412 nm, and 392 nm), in turn producing different state distributions in the resulting cations. Strong chiral asymmetries in the lab frame photoelectron angular distributions are quantified, and a comparison made with a single photon (synchrotron radiation) measurement at an equivalent photon energy.

Laser Pulse Width Dependence and Ionization Mechanism of Matrix-Assisted Laser Desorption/Ionization

NASA Astrophysics Data System (ADS)

Liang, Sheng-Ping; Lu, I.-Chung; Tsai, Shang-Ting; Chen, Jien-Lian; Lee, Yuan Tseh; Ni, Chi-Kung

2017-10-01

Ultraviolet laser pulses at 355 nm with variable pulse widths in the region from 170 ps to 1.5 ns were used to investigate the ionization mechanism of matrix-assisted laser desorption/ionization (MALDI) for matrices 2,5-dihydroxybenzoic acid (DHB), α-cyano-4-hydroxycinnamic acid (CHCA), and sinapinic acid (SA). The mass spectra of desorbed ions and the intensity and velocity distribution of desorbed neutrals were measured simultaneously for each laser shot. These quantities were found to be independent of the laser pulse width. A comparison of the experimental measurements and numerical simulations according to the multiphoton ionization, coupled photophysical and chemical dynamics (CPCD), and thermally induced proton transfer models showed that the predictions of thermally induced proton transfer model were in agreement with the experimental data, but those of the multiphoton ionization model were not. Moreover, the predictions of the CPCD model based on singlet-singlet energy pooling were inconsistent with the experimental data of CHCA and SA, but were consistent with the experimental data of DHB only when some parameters used in the model were adjusted to extreme values. [Figure not available: see fulltext.

Multiphoton ionization of many-electron atoms and highly-charged ions in intense laser fields: a relativistic time-dependent density functional theory approach

NASA Astrophysics Data System (ADS)

Tumakov, Dmitry A.; Telnov, Dmitry A.; Maltsev, Ilia A.; Plunien, Günter; Shabaev, Vladimir M.

2017-10-01

We develop an efficient numerical implementation of the relativistic time-dependent density functional theory (RTDDFT) to study multielectron highly-charged ions subject to intense linearly-polarized laser fields. The interaction with the electromagnetic field is described within the electric dipole approximation. The resulting time-dependent relativistic Kohn-Sham (RKS) equations possess an axial symmetry and are solved accurately and efficiently with the help of the time-dependent generalized pseudospectral method. As a case study, we calculate multiphoton ionization probabilities of the neutral argon atom and argon-like xenon ion. Relativistic effects are assessed by comparison of our present results with existing non-relativistic data.

(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.

Alignment, orientation, and Coulomb explosion of difluoroiodobenzene studied with the pixel imaging mass spectrometry (PImMS) camera.

PubMed

Amini, Kasra; Boll, Rebecca; Lauer, Alexandra; Burt, Michael; Lee, Jason W L; Christensen, Lauge; Brauβe, Felix; Mullins, Terence; Savelyev, Evgeny; Ablikim, Utuq; Berrah, Nora; Bomme, Cédric; Düsterer, Stefan; Erk, Benjamin; Höppner, Hauke; Johnsson, Per; Kierspel, Thomas; Krecinic, Faruk; Küpper, Jochen; Müller, Maria; Müller, Erland; Redlin, Harald; Rouzée, Arnaud; Schirmel, Nora; Thøgersen, Jan; Techert, Simone; Toleikis, Sven; Treusch, Rolf; Trippel, Sebastian; Ulmer, Anatoli; Wiese, Joss; Vallance, Claire; Rudenko, Artem; Stapelfeldt, Henrik; Brouard, Mark; Rolles, Daniel

2017-07-07

Laser-induced adiabatic alignment and mixed-field orientation of 2,6-difluoroiodobenzene (C 6 H 3 F 2 I) molecules are probed by Coulomb explosion imaging following either near-infrared strong-field ionization or extreme-ultraviolet multi-photon inner-shell ionization using free-electron laser pulses. The resulting photoelectrons and fragment ions are captured by a double-sided velocity map imaging spectrometer and projected onto two position-sensitive detectors. The ion side of the spectrometer is equipped with a pixel imaging mass spectrometry camera, a time-stamping pixelated detector that can record the hit positions and arrival times of up to four ions per pixel per acquisition cycle. Thus, the time-of-flight trace and ion momentum distributions for all fragments can be recorded simultaneously. We show that we can obtain a high degree of one-and three-dimensional alignment and mixed-field orientation and compare the Coulomb explosion process induced at both wavelengths.

Carrier-envelope-phase control of asymmetries in the multiphoton ionization of xenon atoms by ultrashort bichromatic fields

NASA Astrophysics Data System (ADS)

Kerbstadt, S.; Pengel, D.; Englert, L.; Bayer, T.; Wollenhaupt, M.

2018-06-01

We report on bichromatic multiphoton ionization of xenon atoms (Xe) to demonstrate carrier-envelope-phase (CEP) control of lateral asymmetries in the photoelectron momentum distribution. In the experiments, we employ a 4 f polarization pulse shaper to sculpture bichromatic fields with commensurable center frequencies ω1:ω2=7 :8 from an over-octave-spanning CEP-stable white light supercontinuum by spectral amplitude and phase modulation. The bichromatic fields are spectrally tailored to induce controlled interferences of 7- vs 8-photon quantum pathways in the 5 P3 /2 ionization continuum of Xe. The CEP sensitivity of the asymmetric final-state wave function arises from coherent superposition of continuum states with opposite parity. Our results demonstrate that shaper-generated bichromatic fields with tailored center frequency ratio are a suitable tool to localize CEP-sensitive asymmetries in a specific photoelectron kinetic-energy window.

Spectroscopic Constants of the Known Electronic States of Lead Monofluoride

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

McRaven, C.P.; Sivakumar, P.; Shafer-Ray, N.E.

2010-08-01

Based on measurements made by mass-resolved 1 + 1{prime} + 1{double_prime} resonance-enhanced multiphoton ionization spectroscopy, we have determined new molecular constants describing the rotational and fine structure levels of the B, D, E, and F states of the most abundant isotopic variant {sup 208}Pb{sup 19}F, and we summarize the spectroscopic constants for all the know electronic states of the radical. Many spectroscopic constants for the isotopologues {sup 206}Pb{sup 19}F and {sup 207}Pb{sup 19}F have also been determined. The symmetry of the D-state is found to be {sup 2}{pi}{sub 1/2}, and the F-state is found to be an {Omega} = 3/2more » state.« less

Imaging photoelectron circular dichroism of chiral molecules by femtosecond multiphoton coincidence detection.

PubMed

Lehmann, C Stefan; Ram, N Bhargava; Powis, Ivan; Janssen, Maurice H M

2013-12-21

Here, we provide a detailed account of novel experiments employing electron-ion coincidence imaging to discriminate chiral molecules. The full three-dimensional angular scattering distribution of electrons is measured after photoexcitation with either left or right circular polarized light. The experiment is performed using a simplified photoelectron-photoion coincidence imaging setup employing only a single particle imaging detector. Results are reported applying this technique to enantiomers of the chiral molecule camphor after three-photon ionization by circularly polarized femtosecond laser pulses at 400 nm and 380 nm. The electron-ion coincidence imaging provides the photoelectron spectrum of mass-selected ions that are observed in the time-of-flight mass spectra. The coincident photoelectron spectra of the parent camphor ion and the various fragment ions are the same, so it can be concluded that fragmentation of camphor happens after ionization. We discuss the forward-backward asymmetry in the photoelectron angular distribution which is expressed in Legendre polynomials with moments up to order six. Furthermore, we present a method, similar to one-photon electron circular dichroism, to quantify the strength of the chiral electron asymmetry in a single parameter. The circular dichroism in the photoelectron angular distribution of camphor is measured to be 8% at 400 nm. The electron circular dichroism using femtosecond multiphoton excitation is of opposite sign and about 60% larger than the electron dichroism observed before in near-threshold one-photon ionization with synchrotron excitation. We interpret our multiphoton ionization as being resonant at the two-photon level with the 3s and 3p Rydberg states of camphor. Theoretical calculations are presented that model the photoelectron angular distribution from a prealigned camphor molecule using density functional theory and continuum multiple scattering X alpha photoelectron scattering calculations. Qualitative agreement is observed between the experimental results and the theoretical calculations of the Legendre moments representing the angular distribution for the two enantiomers. The electron-ion coincidence technique using multiphoton ionization opens new directions in table-top analytical mass-spectrometric applications of mixtures of chiral molecules.

Imaging photoelectron circular dichroism of chiral molecules by femtosecond multiphoton coincidence detection

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

Lehmann, C. Stefan; Ram, N. Bhargava; Janssen, Maurice H. M., E-mail: m.h.m.janssen@vu.nl

2013-12-21

Here, we provide a detailed account of novel experiments employing electron-ion coincidence imaging to discriminate chiral molecules. The full three-dimensional angular scattering distribution of electrons is measured after photoexcitation with either left or right circular polarized light. The experiment is performed using a simplified photoelectron-photoion coincidence imaging setup employing only a single particle imaging detector. Results are reported applying this technique to enantiomers of the chiral molecule camphor after three-photon ionization by circularly polarized femtosecond laser pulses at 400 nm and 380 nm. The electron-ion coincidence imaging provides the photoelectron spectrum of mass-selected ions that are observed in the time-of-flightmore » mass spectra. The coincident photoelectron spectra of the parent camphor ion and the various fragment ions are the same, so it can be concluded that fragmentation of camphor happens after ionization. We discuss the forward-backward asymmetry in the photoelectron angular distribution which is expressed in Legendre polynomials with moments up to order six. Furthermore, we present a method, similar to one-photon electron circular dichroism, to quantify the strength of the chiral electron asymmetry in a single parameter. The circular dichroism in the photoelectron angular distribution of camphor is measured to be 8% at 400 nm. The electron circular dichroism using femtosecond multiphoton excitation is of opposite sign and about 60% larger than the electron dichroism observed before in near-threshold one-photon ionization with synchrotron excitation. We interpret our multiphoton ionization as being resonant at the two-photon level with the 3s and 3p Rydberg states of camphor. Theoretical calculations are presented that model the photoelectron angular distribution from a prealigned camphor molecule using density functional theory and continuum multiple scattering X alpha photoelectron scattering calculations. Qualitative agreement is observed between the experimental results and the theoretical calculations of the Legendre moments representing the angular distribution for the two enantiomers. The electron-ion coincidence technique using multiphoton ionization opens new directions in table-top analytical mass-spectrometric applications of mixtures of chiral molecules.« less

Multiphoton Ionization Mass and Photoelectron Spectroscopy.

DTIC Science & Technology

1984-07-01

tracted information about ion vibrational energy levels. Molecules studted include benzene, toluene, aniline, paradifluorobenzene, nitric oxide ...molecules or subgroups and not to others. Ion specific electrodes play an analogous role in electro - chemistry. The prospect of selectively ionizing a... acetaldehyde and butyraldehyde have been studied at the KrF and ArF laser wavelengths. Their ionization potentials are 10.2 and 9.8 eV, respectively

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

Ghosh Deb, S.; Sinha, C.; Chattopadhyay, A.

The modification in the dynamics of the electron-impact ionization process of a Li{sup +} ion due to an intense linearly polarized monochromatic laser field (n{gamma}e,2e) is studied theoretically using coplanar geometry. Significant laser modifications are noted due to multiphoton effects both in the shape and magnitude of the triple-differential cross sections (TDCSs) with respect to the field-free (FF) situation. The net effect of the laser field is to suppress the FF cross sections in the zeroth-order approximation [Coulomb-Volkov (CV)] of the ejected electron wave function, while in the first order [modified Coulomb-Volkov (MCV)], the TDCSs are found to be enhancedmore » or suppressed depending on the kinematics of the process. The strong FF recoil dominance for the (e,2e) process of an ionic target at low incident energy is destroyed in the presence of the laser field. The FF binary-to-recoil ratio changes remarkably in the presence of the laser field, particularly at low incident energies. The difference between the multiphoton CV and the FF results indicates that for the ionic target, the Kroll-Watson sum rule does not hold well at the present energy range in contrast to the neutral atom (He) case. The TDCSs are found to be quite sensitive with respect to the initial phase of the laser field, particularly at higher incident energies. A significant qualitative difference is noted in the multiphoton ejected energy distribution (double-differential cross sections) between the CV and the MCV models. Variation of the TDCSs with respect to the laser phase is also studied.« less

Relaxation channels of multi-photon excited xenon clusters

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

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

2015-09-21

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

Laser-induced radiation microbeam technology and simultaneous real-time fluorescence imaging in live cells.

PubMed

Botchway, Stanley W; Reynolds, Pamela; Parker, Anthony W; O'Neill, Peter

2012-01-01

The use of nano- and microbeam techniques to induce and identify subcellular localized energy deposition within a region of a living cell provides a means to investigate the effects of low radiation doses. Particularly within the nucleus where the propagation and processing of deoxyribonucleic acid (DNA) damage (and repair) in both targeted and nontargeted cells, the latter being able to study cell-cell (bystander) effects. We have pioneered a near infrared (NIR) femtosecond laser microbeam to mimic ionizing radiation through multiphoton absorption within a 3D femtoliter volume of a highly focused Gaussian laser beam. The novel optical microbeam mimics both complex ionizing and UV-radiation-type cell damage including double strand breaks (DSBs). Using the microbeam technology, we have been able to investigate the formation of DNA DSB and subsequent recruitment of repair proteins to the submicrometer size site of damage introduced in viable cells. The use of a phosphorylated H2AX (γ-H2AX a marker for DSBs, visualized by immunofluorescent staining) and real-time imaging of fluorescently labeling proteins, the dynamics of recruitment of repair proteins in viable mammalian cells can be observed. Here we show the recruitment of ATM, p53 binding protein 1 (53BP1), and RAD51, an integral protein of the homologous recombination process in the DNA repair pathway and Ku-80-GFP involved in the nonhomologous end joining (NHEJ) pathway as exemplar repair process to show differences in the repair kinetics of DNA DSBs. The laser NIR multiphoton microbeam technology shows persistent DSBs at later times post laser irradiation which are indicative of DSBs arising at replication presumably from UV photoproducts or clustered damage containing single strand breaks (SSBs) that are also observed. Effects of the cell cycle may also be investigated in real time. Postirradiation and fixed cells studies show that in G1 cells a fraction of multiphoton laser-induced DSBs is persistent for >6h in addition to those induced at replication demonstrating the broad range of timescales taken to repair DNA damage. Copyright © 2012 Elsevier Inc. All rights reserved.

Quantitative measurement of electron number in nanosecond and picosecond laser-induced air breakdown

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

Wu, Yue; Sawyer, Jordan C.; Su, Liu

2016-05-07

Here we present quantitative measurements of total electron numbers in laser-induced air breakdown at pressures ranging from atmospheric to 40 bar{sub g} by 10 ns and 100 ps laser pulses. A quantifiable definition for the laser-induced breakdown threshold is identified by a sharp increase in the measurable total electron numbers via dielectric-calibrated coherent microwave scattering. For the 10 ns laser pulse, the threshold of laser-induced breakdown in atmospheric air is defined as the total electron number of ∼10{sup 6}. This breakdown threshold decreases with an increase of pressure and laser photon energy (shorter wavelength), which is consistent with the theory of initialmore » multiphoton ionization and subsequent avalanche processes. For the 100 ps laser pulse cases, a clear threshold is not present and only marginal pressure effects can be observed, which is due to the short pulse duration leading to stronger multiphoton ionization and minimal collisional avalanche ionization.« less

Quantum description of the high-order harmonic generation in multiphoton and tunneling regimes

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

Perez-Hernandez, J. A.; Plaja, L.

2007-08-15

We employ a recently developed S-matrix approach [L. Plaja and J. A. Perez-Hernandez, Opt. Express 15, 3629 (2007)] to investigate the process of harmonic generation in tunnel and multiphoton ionization regimes. In contrast with most of the previous approaches, this model is developed without the stationary phase approximation and including the relevant continuum-continuum transitions. Therefore, it provides a full quantum description of the harmonic generation process in these two ionization regimes, with a good quantitative accuracy with the exact results of the time-dependent Schroedinger equation. We show how this model can be used to investigate the contribution of the electronicmore » population ionized at different times, thus giving a time-resolved description that, up to now, was reserved only to semiclassical models. In addition, we will show some aspects of harmonic generation beyond the semiclassical predictions as, for instance, the emission of radiation while the electron is leaving the parent ion and the generation of harmonics in semiclassically forbidden situations.« less

L. V. Keldysh’s “Ionization in the Field of a Strong Electromagnetic Wave” and modern physics of atomic interaction with a strong laser field

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

Fedorov, M. V., E-mail: fedorov@gmail.com

2016-03-15

Basic premises, approximations, and results of L.V. Keldysh’s 1964 work on multiphoton ionization of atoms are discussed, as well as its influence on the modern science of the interaction of atomic–molecular systems with a strong laser field.

Investigating multiphoton phenomena using nonlinear dynamics

NASA Astrophysics Data System (ADS)

Huang, Shu

Many seemingly simple systems can display extraordinarily complex dynamics which has been studied and uncovered through nonlinear dynamical theory. The leitmotif of this thesis is changing phase-space structures and their (linear or non-linear) stabilities by adding control functions (which act on the system as external perturbations) to the relevant Hamiltonians. These phase-space structures may be periodic orbits, invariant tori or their stable and unstable manifolds. One-electron systems and diatomic molecules are fundamental and important staging ground for new discoveries in nonlinear dynamics. In past years, increasing emphasis and effort has been put on the control or manipulation of these systems. Recent developments of nonlinear dynamical tools can provide efficient ways of doing so. In the first subtopic of the thesis, we are adding a control function to restore tori at prescribed locations in phase space. In the remainder of the thesis, a control function with parameters is used to change the linear stability of the periodic orbits which govern the processes in question. In this thesis, we report our theoretical analyses on multiphoton ionization of Rydberg atoms exposed to strong microwave fields and the dissociation of diatomic molecules exposed to bichromatic lasers using nonlinear dynamical tools. This thesis is composed of three subtopics. In the first subtopic, we employ local control theory to reduce the stochastic ionization of hydrogen atom in a strong microwave field by adding a relatively small control term to the original Hamiltonian. In the second subtopic, we perform periodic orbit analysis to investigate multiphoton ionization driven by a bichromatic microwave field. Our results show quantitative and qualitative agreement with previous studies, and hence identify the mechanism through which short periodic orbits organize the dynamics in multiphoton ionization. In addition, we achieve substantial time savings with this approach. In the third subtopic we extend our periodic orbit analysis to the dissociation of diatomic molecules driven by a bichromatic laser. In this problem, our results based on periodic orbit analysis again show good agreement with previous work, and hence promise more potential applications of this approach in molecular physics.

Laser-induced periodic surface structures on 6H-SiC single crystals using temporally delayed femtosecond laser double-pulse trains

NASA Astrophysics Data System (ADS)

Song, Juan; Tao, Wenjun; Song, Hui; Gong, Min; Ma, Guohong; Dai, Ye; Zhao, Quanzhong; Qiu, Jianrong

2016-04-01

In this paper, a time-delay-adjustable double-pulse train with 800-nm wavelength, 200-fs pulse duration and a repetition rate of 1 kHz, produced by a collinear two-beam optical system like a Mach-Zehnder interferometer, was employed for irradiation of 6H-SiC crystal. The dependence of the induced structures on time delay of double-pulse train for parallel-polarization configuration was studied. The results show that as the time delay of collinear parallel-polarization dual-pulse train increased, the induced near-subwavelength ripples (NSWRs) turn from irregular rippled pattern to regularly periodic pattern and have their grooves much deepened. The characteristics timescale for this transition is about 6.24 ps. Besides, the areas of NSWR were found to decay exponentially for time delay from 0 to 1.24 ps and then slowly increase for time delay from 1.24 to 14.24 ps. Analysis shows that multiphoton ionization effect, grating-assisted surface plasmon coupling effect, and timely intervene of second pulse in a certain physical stage experienced by 6H-SiC excited upon first pulse irradiation may contribute to the transition of morphology details.

A velocity-map imaging study of methyl non-resonant multiphoton ionization from the photodissociation of CH3I in the A-band

PubMed Central

Poullain, Sonia Marggi; Chicharro, David V.; Rubio-Lago, Luis; García-Vela, Alberto

2017-01-01

Chemical reaction dynamics and, particularly, photodissociation in the gas phase are generally studied using pump–probe schemes where a first laser pulse induces the process under study and a second one detects the produced fragments. Providing an efficient detection of ro-vibrationally state-selected photofragments, the resonance enhanced multiphoton ionization (REMPI) technique is, without question, the most popular approach used for the probe step, while non-resonant multiphoton ionization (NRMPI) detection of the products is scarce. The main goal of this work is to test the sensitivity of the NRMPI technique to fragment vibrational distributions arising from molecular photodissociation processes. We revisit the well-known process of methyl iodide photodissociation in the A-band at around 280 nm, using the velocity-map imaging technique in conjunction with NRMPI of the methyl fragment. The detection wavelength, carefully selected to avoid any REMPI transition, was scanned between 325 and 335 nm seeking correlations between the different observables—the product vibrational, translational and angular distributions—and the excitation wavelength of the probe laser pulse. The experimental results have been discussed on the base of quantum dynamics calculations of photofragment vibrational populations carried out on available ab initio potential-energy surfaces using a four-dimensional model. This article is part of the themed issue ‘Theoretical and computational studies of non-equilibrium and non-statistical dynamics in the gas phase, in the condensed phase and at interfaces’. PMID:28320907

Early stages of styrene-isoprene copolymerization in gas phase clusters probed by resonance enhanced multiphoton ionization.

PubMed

Mahmoud, Hatem; Germanenko, Igor N; El-Shall, M Samy

2006-04-06

We present direct evidence for the formation of the covalent bonded styrene (isoprene)(2) oligomer and the isoprene dimer ions following resonance ionization of the gas phase styrene-isoprene binary clusters. The application of resonance ionization to study polymerization reactions in clusters provides new information on the structure and mechanism of formation of the early stages of polymerization and holds considerable promise for the discovery of new initiation mechanisms and for the development of novel materials with unique properties.

An Automated System for the Control of, and Data Acquisition from Multiphoton Ionization and Fluorescence Lifetime Measurements.

DTIC Science & Technology

1986-09-01

Quanta- Ray company , which also supplied the laser used for the multiphoton work. The, burner was mounted on a translator stage from Velmex, Inc...and no longer exists as a process in the system. When the user analysis program has completed, the lifetime program is again automatically re-started...KCHAR) RETURN 100 FORMAT(I3) 101 FORMAT(F7.2) END SUBROUTINE LAB4 FODA SE"oteD C This routine puts the label "INTEGRAL FROM DATA SET" on the MDP C screen

Wavelength dependence of nanosecond infrared laser-induced breakdown in water: Evidence for multiphoton initiation via an intermediate state

NASA Astrophysics Data System (ADS)

Linz, Norbert; Freidank, Sebastian; Liang, Xiao-Xuan; Vogelmann, Hannes; Trickl, Thomas; Vogel, Alfred

2015-04-01

Investigation of the wavelength dependence (725-1025 nm) of the threshold for nanosecond optical breakdown in water revealed steps consistent with breakdown initiation by multiphoton ionization, with an initiation energy of about 6.6 eV. This value is considerably smaller than the autoionization threshold of about 9.5 eV, which can be regarded as band gap relevant for avalanche ionization. Breakdown initiation is likely to occur via excitation of a valence band electron into a solvated state, followed by rapid excitation into the conduction band. Theoretical analysis based on these assumptions suggests that the seed electron density required for initiating avalanche ionization amounts to 2.5 ×1015c m-3 at 725 nm and drops to 1.1 ×1012c m-3 at 1025 nm. These results demand changes of future breakdown modeling for water, including the use of a larger band gap than previously employed, the introduction of an intermediate energy level for initiation, and consideration of the wavelength dependence of seed electron density.

Internal standards for use in the comprehensive analysis of polychlorinated aromatic hydrocarbons using gas chromatography combined with multiphoton ionization mass spectrometry.

PubMed

Li, Adan; Imasaka, Totaro

2016-10-28

To decrease health-risks to humans, non-toxic compounds were evaluated for use as internal standards for calibrating data obtained by gas chromatography/multiphoton ionization mass spectrometry (GC-MPI-MS) using an ultraviolet femtosecond laser as the ionization source. The retention time in the mass chromatogram was calibrated using a retention index, in which a series of n-alkanes was employed as internal standards for evaluating the retention times for polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs), and polychlorinated biphenyls (PCBs). To compensate for changes in signal intensity in MPI-MS, the dependence of signal intensity on the laser pulse energy was investigated for the dioxin-like compounds, in addition to five non-toxic aromatic hydrocarbons, that were used as internal standards. Based on their similar behavior,the non-toxic PCDD/PCDF, its 13 C-isotope, and pentachlorobenzene behave similarly, we conclude that they can be used for calibrating the signal intensities in MPI-MS. Copyright © 2016 Elsevier B.V. All rights reserved.

Tabletop imaging of structural evolutions in chemical reactions demonstrated for the acetylene cation

NASA Astrophysics Data System (ADS)

Ibrahim, Heide; Wales, Benji; Beaulieu, Samuel; Schmidt, Bruno E.; Thiré, Nicolas; Fowe, Emmanuel P.; Bisson, Éric; Hebeisen, Christoph T.; Wanie, Vincent; Giguére, Mathieu; Kieffer, Jean-Claude; Spanner, Michael; Bandrauk, André D.; Sanderson, Joseph; Schuurman, Michael S.; Légaré, François

2014-07-01

The introduction of femto-chemistry has made it a primary goal to follow the nuclear and electronic evolution of a molecule in time and space as it undergoes a chemical reaction. Using Coulomb Explosion Imaging, we have shot the first high-resolution molecular movie of a to and fro isomerization process in the acetylene cation. So far, this kind of phenomenon could only be observed using vacuum ultraviolet light from a free-electron laser. Here we show that 266 nm ultrashort laser pulses are capable of initiating rich dynamics through multiphoton ionization. With our generally applicable tabletop approach that can be used for other small organic molecules, we have investigated two basic chemical reactions simultaneously: proton migration and C=C bond breaking, triggered by multiphoton ionization. The experimental results are in excellent agreement with the timescales and relaxation pathways predicted by new and quantitative ab initio trajectory simulations.

(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.

Multiphoton near-infrared femtosecond laser pulse-induced DNA damage with and without the photosensitizer proflavine.

PubMed

Shafirovich, V; Dourandin, A; Luneva, N P; Singh, C; Kirigin, F; Geacintov, N E

1999-03-01

The excitation of pBr322 supercoiled plasmid DNA with intense near-IR 810 nm fs laser pulses by a simultaneous multiphoton absorption mechanism results in single-strand breaks after treatment of the irradiated samples with Micrococcus luteus UV endonuclease. This enzyme cleaves DNA strands at sites of cyclobutane dimers that are formed by the simultaneous absorption of three (or more) 810 nm IR photons (pulse width approximately 140 fs, 76 MHz pulse repetition, average power output focused through 10x microscope objective is approximately 1.2 MW/cm2). Direct single-strand breaks (without treatment with M. luteus) were not observed under these conditions. However, in the presence of 6 microM of the intercalator proflavine (PF), both direct single- and double-strand breaks are observed under conditions where substantial fractions of undamaged supercoiled DNA molecules are still present. The fraction of direct double-strand breaks is 30 +/- 5% of all measurable strand cleavage events, is independent of dosage (up to 6.4 GJ/cm2) and is proportional to In, where I is the average power/area of the 810 nm fs laser pulses, and n = 3 +/- 1. The nicking of two DNA strands in the immediate vicinity of the excited PF molecules gives rise to this double-strand cleavage. In contrast, excitation of the same samples under low-power, single-photon absorption conditions (approximately 400-500 nm) gives rise predominantly to single-strand breaks, but some double-strand breaks are observed at the higher dosages. Thus, single-photon excitation with 400-500 nm light and multiphoton activation of PF by near-IR fs laser pulses produces different distributions of single- and double-strand breaks. These results suggest that DNA strand cleavage originates from unrelaxed, higher excited states when PF is excited by simultaneous IR multiphoton absorption processes.

Comparison of the Detection Characteristics of Trace Species Using Laser-Induced Breakdown Spectroscopy and Laser Breakdown Time-of-Flight Mass Spectrometry

PubMed Central

Wang, Zhenzhen; Deguchi, Yoshihiro; Yan, Junjie; Liu, Jiping

2015-01-01

The rapid and precise element measurement of trace species, such as mercury, iodine, strontium, cesium, etc. is imperative for various applications, especially for industrial needs. The elements mercury and iodine were measured by two detection methods for comparison of the corresponding detection features. A laser beam was focused to induce plasma. Emission and ion signals were detected using laser-induced breakdown spectroscopy (LIBS) and laser breakdown time-of-flight mass spectrometry (LB-TOFMS). Multi-photon ionization and electron impact ionization in the plasma generation process can be controlled by the pressure and pulse width. The effect of electron impact ionization on continuum emission, coexisting molecular and atomic emissions became weakened in low pressure condition. When the pressure was less than 1 Pa, the plasma was induced by laser dissociation and multi-photon ionization in LB-TOFMS. According to the experimental results, the detection limits of mercury and iodine in N2 were 3.5 ppb and 60 ppb using low pressure LIBS. The mercury and iodine detection limits using LB-TOFMS were 1.2 ppb and 9.0 ppb, which were enhanced due to different detection features. The detection systems of LIBS and LB-TOFMS can be selected depending on the condition of each application. PMID:25769051

Tabletop Imaging of Structural Evolutions in Chemical Reactions

NASA Astrophysics Data System (ADS)

Ibrahim, Heide; Wales, Benji; Beaulieu, Samuel; Schmidt, Bruno E.; Thiré, Nicolas; Fowe, Emmanuel P.; Bisson, Éric; Hebeisen, Christoph T.; Wanie, Vincent; Giguére, Mathieu; Kieffer, Jean-Claude; Spanner, Michael; Bandrauk, André D.; Sanderson, Joseph; Schuurman, Michael S.; Légaré, François

The first high-resolution molecular movie of proton migration in the acetylene cation is obtained using a tabletop multiphoton pump-probe approach—an alternative to demanding free-electron-lasers and other VUV light sources when ionizing from the HOMO-1.

THE APPLICATION OF JET REMPI/TOFMS TO REAL-TIME MONITORING OF DIOXINS

EPA Science Inventory

An advanced rapid monitoring technology, Jet Resonance Enhanced Multi-Photon Ionization, (Jet REMPI) is being applied to the measurement of air toxics, including chlorinated dibenzodioxins and dibenzofurans (CDD/CDF), for mechanistic understanding, process monitoring, and regulat...

Torsional, Vibrational and Vibration-Torsional Levels in the S_{1} and Ground Cationic D_{0}^{+} States of Para-Xylene

NASA Astrophysics Data System (ADS)

Gardner, Adrian M.; Tuttle, William Duncan; Groner, Peter; Wright, Timothy G.

2017-06-01

Insight gained from examining the "pure" torsional, vibrational and vibration-torsional (vibtor) levels of the single rotor molecules: toluene (methylbenzene) and para-fluorotoluene (pFT), is applied to the double rotor para-xylene (p-dimethylbenzene) molecule . Resonance-enhanced multiphoton ionization (REMPI) spectroscopy and zero-kinetic-energy (ZEKE) spectroscopy are employed in order to investigate the S_{1} and ground cationic states of para-xylene. Observed transitions are assigned in the full molecular symmetry group (G_{72}) for the first time. J. R. Gascooke, E. A. Virgo, and W. D. Lawrance, J. Chem. Phys., 143, 044313 (2015). A. M. Gardner, W. D. Tuttle, L. Whalley, A. Claydon, J. H. Carter and T. G. Wright, J. Chem. Phys., 145, 124307 (2016). A. M. Gardner, W. D. Tuttle, P. Groner and T. G. Wright, J. Chem. Phys., (2017, in press).

Spectroscopy of Isolated Prebiotic Nucleobases

NASA Technical Reports Server (NTRS)

Svadlenak, Nathan; Callahan, Michael P.; Ligare, Marshall; Gulian, Lisa; Gengeliczki, Zsolt; Nachtigallova, Dana; Hobza, Pavel; deVries, Mattanjah

2011-01-01

We use multiphoton ionization and double resonance spectroscopy to study the excited state dynamics of biologically relevant molecules as well as prebiotic nucleobases, isolated in the gas phase. Molecules that are biologically relevant to life today tend to exhibit short excited state lifetimes compared to similar but non-biologically relevant analogs. The mechanism is internal conversion, which may help protect the biologically active molecules from UV damage. This process is governed by conical intersections that depend very strongly on molecular structure. Therefore we have studied purines and pyrimidines with systematic variations of structure, including substitutions, tautomeric forms, and cluster structures that represent different base pair binding motifs. These structural variations also include possible alternate base pairs that may shed light on prebiotic chemistry. With this in mind we have begun to probe the ultrafast dynamics of molecules that exhibit very short excited states and search for evidence of internal conversions.

Experimental observation of multiphoton Thomson scattering

NASA Astrophysics Data System (ADS)

Yan, Wenchao; Golovin, Grigory; Fruhling, Colton; Haden, Daniel; Zhang, Ping; Zhang, Jun; Zhao, Baozhen; Liu, Cheng; Chen, Shouyuan; Banerjee, Sudeep; Umstadter, Donald

2016-10-01

With the advent of high-power lasers, several multiphoton processes have been reported involving electrons in strong fields. For electrons that were initially bound to atoms, both multiphoton ionization and scattering have been reported. However, for free electrons, only low-order harmonic generation has been observed until now. This limitation stems from past difficulty in achieving the required ultra-high-field strengths in scattering experiments. Highly relativistic laser intensities are required to reach the multiphoton regime of Thomson scattering, and generate high harmonics from free electrons. The scaling parameter is the normalized vector potential (a0). Previous experiments have observed phenomena in the weakly relativistic case (a0 >> 1). In ultra-intense fields (a0 >>1), the anomalous electron trajectory is predicted to produce a spectrum characterized by the merging of multiple high-order harmonic generation into a continuum. This may be viewed as the multiphoton Thomson scattering regime analogous to the wiggler of a synchrotron. Thus, the light produced reflects the electrons behavior in an ultra-intense lase field. We discuss the first experiments in the highly relativistic case (a0 15). This material is based upon work supported by NSF No. PHY-153700; US DOE, Office of Science, BES, # DE-FG02-05ER15663; AFOSR # FA9550-11-1-0157; and DHS DNDO # HSHQDC-13-C-B0036.

Measurements of trap dynamics of cold OH molecules using resonance-enhanced multiphoton ionization

NASA Astrophysics Data System (ADS)

Gray, John M.; Bossert, Jason A.; Shyur, Yomay; Lewandowski, H. J.

2017-08-01

Trapping cold, chemically important molecules with electromagnetic fields is a useful technique to study small molecules and their interactions. Traps provide long interaction times, which are needed to precisely examine these low-density molecular samples. However, the trapping fields lead to nonuniform molecular density distributions in these systems. Therefore, it is important to be able to experimentally characterize the spatial density distribution in the trap. Ionizing molecules at different locations in the trap using resonance-enhanced multiphoton ionization (REMPI) and detecting the resulting ions can be used to probe the density distribution even at the low density present in these experiments because of the extremely high efficiency of detection. Until recently, one of the most chemically important molecules, OH, did not have a convenient REMPI scheme identified. Here, we use a newly developed 1 +1' REMPI scheme to detect trapped cold OH molecules. We use this capability to measure the trap dynamics of the central density of the cloud and the density distribution. These types of measurements can be used to optimize loading of molecules into traps, as well as to help characterize the energy distribution, which is critical knowledge for interpreting molecular collision experiments.

Exploration of laser-driven electron-multirescattering dynamics in high-order harmonic generation

DOE PAGES

Li, Peng -Cheng; Sheu, Yae -Lin; Jooya, Hossein Z.; ...

2016-09-06

Multiple rescattering processes play an important role in high-order harmonic generation (HHG) in an intense laser field. However, the underlying multi-rescattering dynamics are still largely unexplored. Here we investigate the dynamical origin of multiple rescattering processes in HHG associated with the odd and even number of returning times of the electron to the parent ion. We perform fully ab initio quantum calculations and extend the empirical mode decomposition method to extract the individual multiple scattering contributions in HHG. We find that the tunneling ionization regime is responsible for the odd number times of rescattering and the corresponding short trajectories aremore » dominant. On the other hand, the multiphoton ionization regime is responsible for the even number times of rescattering and the corresponding long trajectories are dominant. Moreover, we discover that the multiphoton- and tunneling-ionization regimes in multiple rescattering processes occur alternatively. Our results uncover the dynamical origin of multiple rescattering processes in HHG for the first time. As a result, it also provides new insight regarding the control of the multiple rescattering processes for the optimal generation of ultrabroad band supercontinuum spectra and the production of single ultrashort attosecond laser pulse.« less

Exploration of laser-driven electron-multirescattering dynamics in high-order harmonic generation

PubMed Central

Li, Peng-Cheng; Sheu, Yae-Lin; Jooya, Hossein Z.; Zhou, Xiao-Xin; Chu, Shih-I

2016-01-01

Multiple rescattering processes play an important role in high-order harmonic generation (HHG) in an intense laser field. However, the underlying multi-rescattering dynamics are still largely unexplored. Here we investigate the dynamical origin of multiple rescattering processes in HHG associated with the odd and even number of returning times of the electron to the parent ion. We perform fully ab initio quantum calculations and extend the empirical mode decomposition method to extract the individual multiple scattering contributions in HHG. We find that the tunneling ionization regime is responsible for the odd number times of rescattering and the corresponding short trajectories are dominant. On the other hand, the multiphoton ionization regime is responsible for the even number times of rescattering and the corresponding long trajectories are dominant. Moreover, we discover that the multiphoton- and tunneling-ionization regimes in multiple rescattering processes occur alternatively. Our results uncover the dynamical origin of multiple rescattering processes in HHG for the first time. It also provides new insight regarding the control of the multiple rescattering processes for the optimal generation of ultrabroad band supercontinuum spectra and the production of single ultrashort attosecond laser pulse. PMID:27596056

Exploration of laser-driven electron-multirescattering dynamics in high-order harmonic generation.

PubMed

Li, Peng-Cheng; Sheu, Yae-Lin; Jooya, Hossein Z; Zhou, Xiao-Xin; Chu, Shih-I

2016-09-06

Multiple rescattering processes play an important role in high-order harmonic generation (HHG) in an intense laser field. However, the underlying multi-rescattering dynamics are still largely unexplored. Here we investigate the dynamical origin of multiple rescattering processes in HHG associated with the odd and even number of returning times of the electron to the parent ion. We perform fully ab initio quantum calculations and extend the empirical mode decomposition method to extract the individual multiple scattering contributions in HHG. We find that the tunneling ionization regime is responsible for the odd number times of rescattering and the corresponding short trajectories are dominant. On the other hand, the multiphoton ionization regime is responsible for the even number times of rescattering and the corresponding long trajectories are dominant. Moreover, we discover that the multiphoton- and tunneling-ionization regimes in multiple rescattering processes occur alternatively. Our results uncover the dynamical origin of multiple rescattering processes in HHG for the first time. It also provides new insight regarding the control of the multiple rescattering processes for the optimal generation of ultrabroad band supercontinuum spectra and the production of single ultrashort attosecond laser pulse.

Multiple hydrogen bonds. Mass spectra of hydrogen bonded heterodimers. A comparison of ESI- and REMPI-ReTOF-MS.

PubMed

Taubitz, Jörg; Lüning, Ulrich; Grotemeyer, Jürgen

2004-11-07

Resonance enhanced multi-photon ionization-reflectron time of flight mass spectrometry is the analytical method of choice to observe hydrogen bonded supramolecules in the gas phase when protonation of basic centers competes with cluster formation.

APPLICATION OF JET REMPI AND LIBS TO AIR TOXIC MONITORING

EPA Science Inventory

The paper discusses three advanced, laser-based monitoring techniques that the EPA is assisting in developing for real time measurement of toxic aerosol compounds. One of the three techniques is jet resonance enhanced multiphoton ionization (Jet REMPI) coupled with a time-of-flig...

WAVELENGTH-RESOLVED REMPI MASS SPECTROMETRY FOR THE MONITORING OF TOXIC INCINERATION TRACE GASES

EPA Science Inventory

Structure-selective measurement techniques are needed for the assessment of the toxic loading of incinerator gases. This review article shows that wavelength-resolved, resonance-enhanced, multiphoton- ionization (REMPY) mass spectrometry can be used to this end. In this case, how...

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.

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.

DEVELOPMENT OF A JET-REMPI (RESONANTLY ENHANCED MULTIPHOTON IONIZATION) CONTINUOUS MONITOR FOR ENVIRONMENTAL APPLICATIONS. (R827927)

EPA Science Inventory

The perspectives, information and conclusions conveyed in research project abstracts, progress reports, final reports, journal abstracts and journal publications convey the viewpoints of the principal investigator and may not represent the views and policies of ORD and EPA. Concl...

Monitoring of Hazardous Air Pollutant Surrogates Using Resonance Enhanced Multiphoton Ionization/Time of Flight Mass Spectrometry

EPA Science Inventory

EPA’s preferred approach for regulatory emissions compliance is based upon real-time monitoring of individual hazardous air pollutants (HAPs). Real-time, continuous monitoring not only provides the most comprehensive assurance of emissions compliance, but also can serve as...

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

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

Gardner, Adrian M.; Green, Alistair M.; Tamé-Reyes, Victor M.

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 wemore » 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.« less

Conformational analysis of quinine and its pseudo enantiomer quinidine: a combined jet-cooled spectroscopy and vibrational circular dichroism study.

PubMed

Sen, Ananya; Bouchet, Aude; Lepère, Valeria; Le Barbu-Debus, Katia; Scuderi, D; Piuzzi, F; Zehnacker-Rentien, A

2012-08-16

Laser-desorbed quinine and quinidine have been studied in the gas phase by combining supersonic expansion with laser spectroscopy, namely, laser-induced fluorescence (LIF), resonance-enhanced multiphoton ionization (REMPI), and IR-UV double resonance experiments. Density funtional theory (DFT) calculations have been done in conjunction with the experimental work. The first electronic transition of quinine and quinidine is of π-π* nature, and the studied molecules weakly fluoresce in the gas phase, in contrast to what was observed in solution (Qin, W. W.; et al. J. Phys. Chem. C2009, 113, 11790). The two pseudo enantiomers quinine and quinidine show limited differences in the gas phase; their main conformation is of open type as it is in solution. However, vibrational circular dichroism (VCD) experiments in solution show that additional conformers exist in condensed phase for quinidine, which are not observed for quinine. This difference in behavior between the two pseudo enantiomers is discussed.

Organic chemical analysis on a microscopic scale using two-step laser desorption/laser ionization mass spectrometry

NASA Technical Reports Server (NTRS)

Kovalenko, L. J.; Philippoz, J.-M.; Bucenell, J. R.; Zenobi, R.; Zare, R. N.

1991-01-01

The distribution of PAHs in the Allende meteorite has been measured using two-step laser desorption and laser multiphoton-ionization mass spectrometry. This method enables in situ analysis (with a spatial resolution of 1 mm or better) of selected organic molecules. Results show that PAH concentrations are locally high compared to the average concentration found by analysis of pulverized samples, and are found primarily in the fine-grained matrix; no PAHs were detected in the interiors of individual chondrules at the detection limit (about 0.05 ppm).

Experimental investigation of strong-field-ionization theories for laser fields from visible to midinfrared frequencies

NASA Astrophysics Data System (ADS)

Lai, Yu Hang; Xu, Junliang; Szafruga, Urszula B.; Talbert, Bradford K.; Gong, Xiaowei; Zhang, Kaikai; Fuest, Harald; Kling, Matthias F.; Blaga, Cosmin I.; Agostini, Pierre; DiMauro, Louis F.

2017-12-01

Strong-field-ionization yield versus intensity is investigated for various atomic targets (Ne, Ar, Kr, Xe, Na, K, Zn, and Mg) and light polarization from visible to mid-infrared (0.4-4 μ m ), from multiphoton to tunneling regimes. The experimental findings (normalized yield vs intensity, ratio of circular to linear polarization and saturation intensities) are compared to the theoretical models of Perelomov-Popov-Terent'ev (PPT) and Ammosov-Delone-Krainov (ADK). While PPT is generally satisfactory, ADK validity is found, as expected, to be much more limited.

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.

Resonant- and avalanche-ionization amplification of laser-induced plasma in air

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

Wu, Yue; Zhang, Zhili, E-mail: zzhang24@utk.edu; Jiang, Naibo

2014-10-14

Amplification of laser-induced plasma in air is demonstrated utilizing resonant laser ionization and avalanche ionization. Molecular oxygen in air is ionized by a low-energy laser pulse employing (2 + 1) resonance-enhanced multi-photon ionization (REMPI) to generate seed electrons. Subsequent avalanche ionization of molecular oxygen and nitrogen significantly amplifies the laser-induced plasma. In this plasma-amplification effect, three-body attachments to molecular oxygen dominate the electron-generation and -loss processes, while either nitrogen or argon acts as the third body with low electron affinity. Contour maps of the electron density within the plasma obtained in O₂/N₂ and O₂/Ar gas mixtures are provided to showmore » relative degrees of plasma amplification with respect to gas pressure and to verify that the seed electrons generated by O₂ 2 + 1 REMPI are selectively amplified by avalanche ionization of molecular nitrogen in a relatively low-pressure condition (≤100 Torr). Such plasma amplification occurring in air could be useful in aerospace applications at high altitude.« less

Field enhancement of multiphoton induced luminescence processes in ZnO nanorods

NASA Astrophysics Data System (ADS)

Hyyti, Janne; Perestjuk, Marko; Mahler, Felix; Grunwald, Rüdiger; Güell, Frank; Gray, Ciarán; McGlynn, Enda; Steinmeyer, Günter

2018-03-01

The near-ultraviolet photoluminescence of ZnO nanorods induced by multiphoton absorption of unamplified Ti:sapphire pulses is investigated. Power dependence measurements have been conducted with an adaptation of the ultrashort pulse characterization method of interferometric frequency-resolved optical gating. These measurements enable the separation of second harmonic and photoluminescence bands due to their distinct coherence properties. A detailed analysis yields fractional power dependence exponents in the range of 3-4, indicating the presence of multiple nonlinear processes. The range in measured exponents is attributed to differences in local field enhancement, which is supported by independent photoluminescence and structural measurements. Simulations based on Keldysh theory suggest contributions by three- and four-photon absorption as well as avalanche ionization in agreement with experimental findings.

Total angular momenta of high-lying odd levels of U I at ∼ 4 eV using resonance ionization laser polarization spectroscopy

NASA Astrophysics Data System (ADS)

Rath, Asawari D.; Kundu, S.; Ray, A. K.

2018-02-01

Laser induced photoionization of atoms shows significant dependence on the choice of polarizations of lasers. In multi-step, multi-photon excitation and subsequent ionization of atoms different polarization combinations of the exciting lasers lead to distinctly different ion yields. This fact is exploited in this work to determine total angular momenta of odd-parity energy levels of U I lying at ∼ 4 eV from its ground level using resonance ionization laser polarization spectroscopy in time of flight mass spectrometer. These levels are populated by two-step resonant excitation using two pulsed dye lasers with preset polarizations of choice followed by nonresonant ionization by third laser. The dependence of ionization yield on specific polarizations of the first two lasers is studied experimentally for each level under consideration. This dependence when compared to simulations makes possible unambiguous assignment of J angular momenta to these levels.

The laser lightning rod system: thunderstorm domestication.

PubMed

Ball, L M

1974-10-01

An unusual application of the laser, namely protection of life and property from lightning, is described. The device relies on multiphoton ionization in mode-locked beams, rather than on collisional (avalanche) electron production. Feasibility is demonstrated numerically, and relevant principles explained. A method of mobile deployment is mentioned, by which economic (as opposed to scientific) feasibility might be achieved.

REAL-TIME EMISSION CHARACTERIZATION OF ORGANIC AIR TOXIC POLLUTANTS DURING STEADY STATE AND TRANSIENT OPERATION OF A MEDIUM DUTY DIESEL ENGINE

EPA Science Inventory

An on-line monitoring method, jet resonance-enhanced multi-photon ionization (REMPI) with time-of-flight mass spectrometry (TOFMS) was used to measure emissions of organic air toxics from a medium-duty (60 kW)diesel generator during transient and steady state operations. Emission...

Initiation of air ionization by ultrashort laser pulses: evidence for a role of metastable-state air molecules

NASA Astrophysics Data System (ADS)

Bulgakov, A. V.; Mirza, I.; Bulgakova, N. M.; Zhukov, V. P.; Machulka, R.; Haderka, O.; Campbell, E. E. B.; Mocek, T.

2018-06-01

Transmission measurements for femtosecond laser pulses focused in air with spectral analysis of emission from the focal region have been carried out for various pulse energies and air pressures. The air breakdown threshold and pulse attenuation due to plasma absorption are evaluated and compared with calculations based on the multiphoton ionization model. The plasma absorption is found to depend on the pulse repetition rate and is considerably stronger at 1 kHz than at 1–10 Hz. This suggests that accumulation of metastable states of air molecules plays an important role in initiation of air breakdown, enhancing the ionization efficiency at high repetition rates. Possible channels of metastable-state-assisted air ionization and the role of the observed accumulation effect in laser material processing are discussed.

Adaptive multiphoton endomicroscopy through a dynamically deformed multicore optical fiber using proximal detection.

PubMed

Warren, Sean C; Kim, Youngchan; Stone, James M; Mitchell, Claire; Knight, Jonathan C; Neil, Mark A A; Paterson, Carl; French, Paul M W; Dunsby, Chris

2016-09-19

This paper demonstrates multiphoton excited fluorescence imaging through a polarisation maintaining multicore fiber (PM-MCF) while the fiber is dynamically deformed using all-proximal detection. Single-shot proximal measurement of the relative optical path lengths of all the cores of the PM-MCF in double pass is achieved using a Mach-Zehnder interferometer read out by a scientific CMOS camera operating at 416 Hz. A non-linear least squares fitting procedure is then employed to determine the deformation-induced lateral shift of the excitation spot at the distal tip of the PM-MCF. An experimental validation of this approach is presented that compares the proximally measured deformation-induced lateral shift in focal spot position to an independent distally measured ground truth. The proximal measurement of deformation-induced shift in focal spot position is applied to correct for deformation-induced shifts in focal spot position during raster-scanning multiphoton excited fluorescence imaging.

UV and VUV spectroscopy and photochemistry of small molecules in a supersonic jet

NASA Technical Reports Server (NTRS)

Ruehl, E.; Vaida, V.

1990-01-01

UV and VUV absorption and emission spectroscopy is used to probe jet cooled molecules, free radicals, and clusters in the gas phase. Due to efficient cooling inhomogeneous effects on spectral line widths are eliminated. Therefore from these spectra, both structural and dynamical information is obtained. The photoproducts of these reactions are probed by resonance enhanced multiphoton ionization.

Study on the decomposition of trace benzene over V2O5-WO3/TiO2-based catalysts in simulated flue gas

EPA Science Inventory

Commercial and laboratory-prepared V2O5–WO3/TiO2-based catalysts with different compositions were tested for catalytic decomposition of chlorobenzene （ClBz） in simulated flue gas. Resonance enhanced multiphoton ionization-time of flight mass spectrometry (REMPI-TOFMS) was employe...

Dynamics of focused femtosecond laser pulse during photodisruption of crystalline lens

NASA Astrophysics Data System (ADS)

Gupta, Pradeep Kumar; Singh, Ram Kishor; Sharma, R. P.

2018-04-01

Propagation of laser pulses of femtosecond time duration (focused through a focusing lens inside the crystalline lens) has been investigated in this paper. Transverse beam diffraction, group velocity dispersion, graded refractive index structure of the crystalline lens, self-focusing, and photodisruption in which plasma is formed due to the high intensity of laser pulses through multiphoton ionization have been taken into account. The model equations are the modified nonlinear Schrödinger equation along with a rate equation that takes care of plasma generation. A close analysis of model equations suggests that the femtosecond laser pulse duration is critical to the breakdown in the lens. Our numerical simulations reveal that the combined effect of self-focusing and multiphoton ionization provides the breakdown threshold. During the focusing of femtosecond laser pulses, additional spatial pulse splitting arises along with temporal splitting. This splitting of laser pulses arises on account of self-focusing, laser induced breakdown, and group velocity distribution, which modifies the shape of laser pulses. The importance of the present study in cavitation bubble generation to improve the elasticity of the eye lens has also been discussed in this paper.

Collective Autoionization in Multiply-Excited Systems: A novel ionization process observed in Helium Nanodroplets

PubMed Central

LaForge, A. C.; Drabbels, M.; Brauer, N. B.; Coreno, M.; Devetta, M.; Di Fraia, M.; Finetti, P.; Grazioli, C.; Katzy, R.; Lyamayev, V.; Mazza, T.; Mudrich, M.; O'Keeffe, P.; Ovcharenko, Y.; Piseri, P.; Plekan, O.; Prince, K. C.; Richter, R.; Stranges, S.; Callegari, C.; Möller, T.; Stienkemeier, F.

2014-01-01

Free electron lasers (FELs) offer the unprecedented capability to study reaction dynamics and image the structure of complex systems. When multiple photons are absorbed in complex systems, a plasma-like state is formed where many atoms are ionized on a femtosecond timescale. If multiphoton absorption is resonantly-enhanced, the system becomes electronically-excited prior to plasma formation, with subsequent decay paths which have been scarcely investigated to date. Here, we show using helium nanodroplets as an example that these systems can decay by a new type of process, named collective autoionization. In addition, we show that this process is surprisingly efficient, leading to ion abundances much greater than that of direct single-photon ionization. This novel collective ionization process is expected to be important in many other complex systems, e.g. macromolecules and nanoparticles, exposed to high intensity radiation fields. PMID:24406316

Wavelength Dependence of Nanosecond IR Laser-Induced Breakdown in Water: Evidence for Multiphoton Initiation via an Intermediate State

DTIC Science & Technology

2015-04-29

bubble generation and shock wave emission in water for femtosecond to nanosecond laser pulses . ...breakdown threshold in water for nanosecond (ns) IR laser pulses . Avalanche ionization (AI) is the most powerful mechanism driving IR ns laser-induced...acknowledged that femtosecond (fs) and picosecond (ps) IR breakdown is initiated by photoionization because ultrashort pulses are sufficiently

Analysis of Parent/Nitrated Polycyclic Aromatic Hydrocarbons in Particulate Matter 2.5 Based on Femtosecond Ionization Mass Spectrometry.

PubMed

Itouyama, Noboru; Matsui, Taiki; Yamamoto, Shigekazu; Imasaka, Tomoko; Imasaka, Totaro

2016-02-01

Particulate matter 2.5 (PM2.5), collected from ambient air in Fukuoka City, was analyzed by gas chromatography combined with multiphoton ionization mass spectrometry using an ultraviolet femtosecond laser (267 nm) as the ionization source. Numerous parent polycyclic aromatic hydrocarbons (PPAHs) were observed in a sample extracted from PM2.5, and their concentrations were determined to be in the range from 30 to 190 pg/m(3) for heavy PPAHs. Standard samples of nitrated polycyclic aromatic hydrocarbons (NPAHs) were examined, and the limits of detection were determined to be in the picogram range. The concentration of NPAH adsorbed on PM2.5 in the air was less than 900-1300 pg/m(3). Graphical Abstract ᅟ.

Platinum Acetylide Two-Photon Chromophores (Preprint)

DTIC Science & Technology

2007-04-01

nonlinear photonics,6-s microfabrication,9,10 fluorescence imaging, II and photodynamic therapy.12Instantaneous absorption of two lower energy photons...results in initiation of the same photophysical processes as one-photon absorption (lP A) of one high- energy photon. This is advantageous for two...reasons. The first is that because of the use of a lower energy photon a material will be guarded from ionization effects from multiphoton absorption in

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.

Optimal control of multiphoton ionization dynamics of small alkali aggregates

NASA Astrophysics Data System (ADS)

Lindinger, A.; Bartelt, A.; Lupulescu, C.; Vajda, S.; Woste, Ludger

2003-11-01

We have performed transient multi-photon ionization experiments on small alkali clusters of different size in order to probe their wave packet dynamics, structural reorientations, charge transfers and dissociative events in different vibrationally excited electronic states including their ground state. The observed processes were highly dependent on the irradiated pulse parameters like wavelength range or its phase and amplitude; an emphasis to employ a feedback control system for generating the optimum pulse shapes. Their spectral and temporal behavior reflects interesting properties about the investigated system and the irradiated photo-chemical process. First, we present the vibrational dynamics of bound electronically excited states of alkali dimers and trimers. The scheme for observing the wave packet dynamics in the electronic ground state using stimulated Raman-pumping is shown. Since the employed pulse parameters significantly influence the efficiency of the irradiated dynamic pathways photo-induced ioniziation experiments were carried out. The controllability of 3-photon ionization pathways is investigated on the model-like systems NaK and K2. A closed learning loop for adaptive feedback control is used to find the optimal fs pulse shape. Sinusoidal parameterizations of the spectral phase modulation are investigated in regard to the obtained optimal field. By reducing the number of parameters and thereby the complexity of the phase moduation, optimal pulse shapes can be generated that carry fingerprints of the molecule's dynamical properties. This enables to find "understandable" optimal pulse forms and offers the possiblity to gain insight into the photo-induced control process. Characteristic motions of the involved wave packets are proposed to explain the optimized dynamic dissociation pathways.

Ratios of double to single ionization of He and Ne by strong 400-nm laser pulses using the quantitative rescattering theory

NASA Astrophysics Data System (ADS)

Chen, Zhangjin; Li, Xiaojin; Zatsarinny, Oleg; Bartschat, Klaus; Lin, C. D.

2018-01-01

We present numerical simulations of the ratio between double and single ionization of He and Ne by intense laser pulses at wavelengths of 390 and 400 nm, respectively. The yields of doubly charged ions due to nonsequential double ionization (NSDI) are obtained by employing the quantitative rescattering (QRS) model. In this model, the NSDI ionization probability is expressed as a product of the returning electron wave packet (RWP) and the total scattering cross sections for laser-free electron impact excitation and electron impact ionization of the parent ion. According to the QRS theory, the same RWP is also responsible for the emission of high-energy above-threshold ionization photoelectrons. To obtain absolute double-ionization yields, the RWP is generated by solving the time-dependent Schrödinger equation (TDSE) within a one-electron model. The same TDSE results can also be taken to obtain single-ionization yields. By using the TDSE results to calibrate single ionization and the RWP obtained from the strong-field approximation, we further simplify the calculation such that the nonuniform laser intensity distribution in the focused laser beam can be accounted for. In addition, laser-free electron impact excitation and ionization cross sections are calculated using the state-of-the-art many-electron R -matrix theory. The simulation results for double-to-single-ionization ratios are found to compare well with experimental data and support the validity of the nonsequential double-ionization mechanism for the covered intensity region.

New Technique for Barium Daughter Ion Identification in a Liquid Xe-136 Double Beta Decay Experiment

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

Fairbank, William

2016-06-08

This work addresses long-standing issues of fundamental interest in elementary particle physics. The most important outcome of this work is a new limit on neutrinoless double beta decay. This is an extremely rare and long-sought-after type of radioactive decay. If discovered, it would require changes in the standard model of the elementary constituents of matter, and would prove that neutrinos and antineutrinos are the same, a revolutionary concept in particle physics. Neutrinos are major components of the matter in the universe that are so small and so weakly interacting with other matter that their masses have not yet been discovered.more » A discovery of neutrinoless double beta decay could help determine the neutrino masses. An important outcome of the work on this project was the Colorado State University role in operating the EXO-200 neutrinoless double beta decay experiment and in analysis of the data from this experiment. One type of double beta decay of the isotope 136Xe, the two-neutrino variety, was discovered in this work. Although the other type of double beta decay, the neutrinoless variety, was not yet discovered in this work, a world’s best sensitivity of 1.9x10 25 year half-life was obtained. This result rules out a previous claim of a positive result in a different isotope. This work also establishes that the masses of the neutrinos are less than one millionth of that of electrons. A unique EXO-200 analysis, in which the CSU group had a leading role, has established for the first time ever in a liquid noble gas the fraction of daughter atoms from alpha and beta decay that are ionized. This result has important impact on other pending studies, including nucleon decay and barium tagging. Novel additional discoveries include multiphoton ionization of liquid xenon with UV pulsed lasers, which may find application in calibration of future noble liquid detectors, and studies of association and dissociation reactions of Ba + ions in gaseous xenon. Through this project, we are substantially closer to demonstrating “barium tagging”, i.e., detection of single daughter 136Ba atoms from 136Xe double beta decay. Milestones achieved include obtaining spectra of small numbers of Ba atoms and cryoprobe advances toward trapping single 136Ba atoms in solid xenon and probe extraction for detection. One of the other benefits to society is the training of six Ph.D. students in a variety of state-of-the-art technologies, half under primary support of this grant and half with partial support, with four finishing their Ph.D. degrees and two well on their way.« less

Interatomic Coulombic decay cascades in multiply excited neon clusters

PubMed Central

Nagaya, K.; Iablonskyi, D.; Golubev, N. V.; Matsunami, K.; Fukuzawa, H.; Motomura, K.; Nishiyama, T.; Sakai, T.; Tachibana, T.; Mondal, S.; Wada, S.; Prince, K. C.; Callegari, C.; Miron, C.; Saito, N.; Yabashi, M.; Demekhin, Ph. V.; Cederbaum, L. S.; Kuleff, A. I.; Yao, M.; Ueda, K.

2016-01-01

In high-intensity laser light, matter can be ionized by direct multiphoton absorption even at photon energies below the ionization threshold. However on tuning the laser to the lowest resonant transition, the system becomes multiply excited, and more efficient, indirect ionization pathways become operative. These mechanisms are known as interatomic Coulombic decay (ICD), where one of the species de-excites to its ground state, transferring its energy to ionize another excited species. Here we show that on tuning to a higher resonant transition, a previously unknown type of interatomic Coulombic decay, intra-Rydberg ICD occurs. In it, de-excitation of an atom to a close-lying Rydberg state leads to electron emission from another neighbouring Rydberg atom. Moreover, systems multiply excited to higher Rydberg states will decay by a cascade of such processes, producing even more ions. The intra-Rydberg ICD and cascades are expected to be ubiquitous in weakly-bound systems exposed to high-intensity resonant radiation. PMID:27917867

Electron and fluorescence spectra of a water molecule irradiated by an x-ray free-electron laser pulse

NASA Astrophysics Data System (ADS)

Schäfer, Julia M.; Inhester, Ludger; Son, Sang-Kil; Fink, Reinhold F.; Santra, Robin

2018-05-01

With the highly intense x-ray light generated by x-ray free-electron lasers (XFELs), molecular samples can be ionized many times in a single pulse. Here we report on a computational study of molecular spectroscopy at the high x-ray intensity provided by XFELs. Calculated photoelectron, Auger electron, and x-ray fluorescence spectra are presented for a single water molecule that reaches many electronic hole configurations through repeated ionization steps. The rich details shown in the spectra depend on the x-ray pulse parameters in a nonintuitive way. We discuss how the observed trends can be explained by the competition of microscopic electronic transition processes. A detailed comparison between spectra calculated within the independent-atom model and within the molecular-orbital framework highlights the chemical sensitivity of the spectral lines of multiple-hole configurations. Our results demonstrate how x-ray multiphoton ionization-related effects such as charge-rearrangement-enhanced x-ray ionization of molecules and frustrated absorption manifest themselves in the electron and fluorescence spectra.

Real-time detection of hazardous materials in air

NASA Astrophysics Data System (ADS)

Schechter, Israel; Schroeder, Hartmut; Kompa, Karl L.

1994-03-01

A new detection system has been developed for real-time analysis of organic compounds in ambient air. It is based on multiphoton ionization by an unfocused laser beam in a single parallel-plate device. Thus, the ionization volume can be relatively large. The amount of laser created ions is determined quantitatively from the induced total voltage drop between the biased plates (Q equals (Delta) V(DOT)C). Mass information is obtained from computer analysis of the time-dependent signal. When a KrF laser (5 ev) is used, most of the organic compounds can be ionized in a two-photon process, but none of the standard components of atmospheric air are ionized by this process. Therefore, this instrument may be developed as a `sniffer' for organic materials. The method has been applied for benzene analysis in air. The detection limit is about 10 ppb. With a simple preconcentration technique the detection limit can be decreased to the sub-ppb range. Simple binary mixtures are also resolved.

Photoionization pathways and thresholds in generation of Lyman-α radiation by resonant four-wave mixing in Kr-Ar mixture

NASA Astrophysics Data System (ADS)

Louchev, Oleg A.; Saito, Norihito; Oishi, Yu; Miyazaki, Koji; Okamura, Kotaro; Nakamura, Jumpei; Iwasaki, Masahiko; Wada, Satoshi

2016-09-01

We develop a set of analytical approximations for the estimation of the combined effect of various photoionization processes involved in the resonant four-wave mixing generation of ns pulsed Lyman-α (L-α ) radiation by using 212.556 nm and 820-845 nm laser radiation pulses in Kr-Ar mixture: (i) multi-photon ionization, (ii) step-wise (2+1)-photon ionization via the resonant 2-photon excitation of Kr followed by 1-photon ionization and (iii) laser-induced avalanche ionization produced by generated free electrons. Developed expressions validated by order of magnitude estimations and available experimental data allow us to identify the area for the operation under high input laser intensities avoiding the onset of full-scale discharge, loss of efficiency and inhibition of generated L-α radiation. Calculations made reveal an opportunity for scaling up the output energy of the experimentally generated pulsed L-α radiation without significant enhancement of photoionization.

Measurement of plasma decay processes in mixture of sodium and argon by coherent microwave scattering

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

Zhang Zhili; Shneider, Mikhail N.

2010-03-15

This paper presents the experimental measurement and computational model of sodium plasma decay processes in mixture of sodium and argon by using radar resonance-enhanced multiphoton ionization (REMPI), coherent microwave Rayleigh scattering of REMPI. A single laser beam resonantly ionizes the sodium atoms by means of 2+1 REMPI process. The laser beam can only generate the ionization of the sodium atoms and have negligible ionization of argon. Coherent microwave scattering in situ measures the total electron number in the laser-induced plasma. Since the sodium ions decay by recombination with electrons, microwave scattering directly measures the plasma decay processes of the sodiummore » ions. A theoretical plasma dynamic model, including REMPI of the sodium and electron avalanche ionization (EAI) of sodium and argon in the gas mixture, has been developed. It confirms that the EAI of argon is several orders of magnitude lower than the REMPI of sodium. The theoretical prediction made for the plasma decay process of sodium plasma in the mixture matches the experimental measurement.« less

Density-Functional Theory with Optimized Effective Potential and Self-Interaction Correction for the Double Ionization of He and Be Atoms

NASA Astrophysics Data System (ADS)

Heslar, John; Telnov, Dmitry; Chu, Shih-I.

2012-06-01

We present a self-interaction-free (SIC) time-dependent density-functional theory (TDDFT) for the treatment of double ionization processes of many-electron systems. The method is based on the Krieger-Li-Iafrate (KLI) treatment of the optimized effective potential (OEP) theory and the incorporation of an explicit self-interaction correction (SIC) term. In the framework of the time-dependent density functional theory, we have performed 3D calculations of double ionization of He and Be atoms by strong near-infrared laser fields. We make use of the exchange-correlation potential with the integer discontinuity which improves the description of the double ionization process. We found that proper description of the double ionization requires the TDDFT exchange-correlation potential with the discontinuity with respect to the variation of the spin particle numbers (SPN) only. The results for the intensity-dependent probabilities of single and double ionization are presented and reproduce the famous ``knee'' structure.

Coulomb-repulsion-assisted double ionization from doubly excited states of argon

NASA Astrophysics Data System (ADS)

Liao, Qing; Winney, Alexander H.; Lee, Suk Kyoung; Lin, Yun Fei; Adhikari, Pradip; Li, Wen

2017-08-01

We report a combined experimental and theoretical study to elucidate nonsequential double-ionization dynamics of argon atoms at laser intensities near and below the recollision-induced ionization threshold. Three-dimensional momentum measurements of two electrons arising from strong-field nonsequential double ionization are achieved with a custom-built electron-electron-ion coincidence apparatus, showing laser intensity-dependent Coulomb repulsion effect between the two outgoing electrons. Furthermore, a previously predicted feature of double ionization from doubly excited states is confirmed in the distributions of sum of two-electron momenta. A classical ensemble simulation suggests that Coulomb-repulsion-assisted double ionization from doubly excited states is at play at low laser intensity. This mechanism can explain the dependence of Coulomb repulsion effect on the laser intensity, as well as the transition from side-by-side to back-to-back dominant emission along the laser polarization direction.

Two-color above-threshold and two-photon sequential double ionization beyond the dipole approximation

NASA Astrophysics Data System (ADS)

Grum-Grzhimailo, A. N.; Gryzlova, E. V.; Kuzmina, E. I.; Chetverkina, A. S.; Strakhova, S. I.

2015-04-01

Two nonlinear atomic photoprocesses are theoretically considered with the emphasis on the photoelectron angular distributions and their modifications due to violation of the dipole approximation: sequential two-photon double ionization and two-color above threshold ionization. These reactions are now accessible with X-ray free electron lasers. Both processes are exemplified by the ionization of krypton: from the 4p shell in the sequential two-photon double ionization and from the 2s shell in the two-color above-threshold ionization, which are compared to the Ar(3p) and Ne(1s) ionization, respectively. Noticeable nondipole effects are predicted.

Recollision induced excitation-ionization with counter-rotating two-color circularly polarized laser field

NASA Astrophysics Data System (ADS)

Ben, Shuai; Guo, Pei-Ying; Pan, Xue-Fei; Xu, Tong-Tong; Song, Kai-Li; Liu, Xue-Shen

2017-07-01

Nonsequential double ionization of Ar by a counter-rotating two-color circularly polarized laser field is theoretically investigated. At the combined intensity in the "knee" structure range, the double ionization occurs mainly through recollision induced excitation followed by subsequent ionization of Ar+∗ . By tracing the history of the recollision trajectories, we explain how the relative intensity ratio of the two colors controls the correlated electron dynamics and optimizes the ionization yields. The major channels contributing to enhancing the double ionization are through the elliptical trajectories with smaller travel time but not through the triangle shape or the other long cycle trajectories. Furthermore, the correlated electron dynamics could be limited to the attosecond time scale by adjusting the relative intensity ratio. Finally, the double ionization from doubly excited complex at low laser intensity is qualitatively discussed.

Double ionization in R -matrix theory using a two-electron outer region

NASA Astrophysics Data System (ADS)

Wragg, Jack; Parker, J. S.; van der Hart, H. W.

2015-08-01

We have developed a two-electron outer region for use within R -matrix theory to describe double ionization processes. The capability of this method is demonstrated for single-photon double ionization of He in the photon energy region between 80 and 180 eV. The cross sections are in agreement with established data. The extended R -matrix with time dependence method also provides information on higher-order processes, as demonstrated by the identification of signatures for sequential double ionization processes involving an intermediate He+ state with n =2 .

Photoelectron spectroscopy of aqueous solutions: Streaming potentials of NaX (X = Cl, Br, and I) solutions and electron binding energies of liquid water and X{sup −}

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

Kurahashi, Naoya; Horio, Takuya; Suzuki, Toshinori, E-mail: suzuki@kuchem.kyoto-u.ac.jp

2014-05-07

The streaming potentials of liquid beams of aqueous NaCl, NaBr, and NaI solutions are measured using soft X-ray, He(I), and laser multiphoton ionization photoelectron spectroscopy. Gaseous molecules are ionized in the vicinity of liquid beams and the photoelectron energy shifts are measured as a function of the distance between the ionization point and the liquid beam. The streaming potentials change their polarity with concentration of electrolytes, from which the singular points of concentration eliminating the streaming potentials are determined. The streaming currents measured in air also vanish at these concentrations. The electron binding energies of liquid water and I{sup −},more » Br{sup −}, and Cl{sup −} anions are revisited and determined more accurately than in previous studies.« less

Ion-Pair States in Triplet Molecular Hydrogen

NASA Astrophysics Data System (ADS)

Setzer, W.; Baker, B. C.; Ashman, S.; Morgan, T. J.

2016-05-01

An experimental search is underway to observe the long range triplet ionic states H+ H- of molecular hydrogen. Resonantly enhanced multi-photon ionization of the metastable c 3∏u- 2 pπ state is used access to the R(1)nd1 n = 21 Rydberg state that serves as an intermediate stepping stone state to probe the energy region above the ionization limit with a second tunable laser photon. The metastable state is prepared by electron capture of 6 keV H2+ions in potassium in a molecular beam. Formation of the H+ H- triplet configuration involves triplet excited states of the H- ion, especially the 2p23Pe state, the second bound state of H- predicted to exist with a lifetime long compared to typical auto ionization lifetimes but not yet observed experimentally. Details of the experiment and preliminary results to date will be presented at the conference.

Chemical analyses of provided samples

NASA Technical Reports Server (NTRS)

Becker, Christopher H.

1993-01-01

Two batches of samples were received and chemical analysis was performed of the surface and near surface regions of the samples by the surface analysis by laser ionization (SALI) method. The samples included four one-inch optics and several paint samples. The analyses emphasized surface contamination or modification. In these studies, pulsed sputtering by 7 keV Ar+ and primarily single-photon ionization (SPI) by coherent 118 nm radiation (at approximately 5 x 10(exp 5) W/cm(sup 2) were used. For two of the samples, also multiphoton ionization (MPI) at 266 nm (approximately 5 x 10(exp 11) W/cm(sup 2) was used. Most notable among the results was the silicone contamination on Mg2 mirror 28-92, and that the Long Duration Exposure Facility (LDEF) paint sample had been enriched in K and Na and depleted in Zn, Si, B, and organic compounds relative to the control paint.

An alternative mechanism for spin-forbidden photo-ionization of diatomic molecules and its rotation-electronic selection rules

NASA Astrophysics Data System (ADS)

Chiu, Ying-Nan; Chiu, Lue-Yung Chow

1990-02-01

The spin-forbidden photo-ionization of diatomic molecules is proposed. Spin orbit interaction is invoked, resulting in the correction and mixing of the wave functions of different multiplicities. The rotation-electronic selection rules given by Dixit and McKoy (1986) for Hund's case a based on the conventional mechanism of electric dipole transition are rederived and expressed in a different format. This new format permits the generalization of the selection rules to other photoionization transitions caused by the magnetic dipole, the electric quadrupole, and the two- and three-photon operators. These selection rules, which are for transitions from one specific rotational level of a given Kronig reflection symmetry to another, will help understand rotational branching and the dynamics of interaction in the excited state. They will also help in the selective preparation of well-defined rovibronic states in resonant-enhanced multi-photon ionization processes.

Ionization-induced solvent migration in acetanilide-methanol clusters inferred from isomer-selective infrared spectroscopy.

PubMed

Weiler, Martin; Nakamura, Takashi; Sekiya, Hiroshi; Dopfer, Otto; Miyazaki, Mitsuhiko; Fujii, Masaaki

2012-12-07

We present the resonance-enhanced multiphoton ionization, infrared-ultraviolet hole burning (IR-UV HB), and IR dip spectra of the trans-acetanilide-methanol (AA-MeOH) cluster in the S(0), S(1), and cationic ground state (D(0)) in a supersonic jet. The IR-UV HB spectra demonstrate the co-existence of two isomers in S(0,1), in which MeOH binds either to the NH or the CO site of the peptide linkage in AA, denoted as AA(NH)-MeOH and AA(CO)-MeOH. When AA(CO)-MeOH is selectively ionized, its IR spectrum in D(0) is the same as that measured for AA(+) (NH)-MeOH. Thus, photoionization of AA(CO)-MeOH induces migration of MeOH from the CO to the NH site with 100% yield. Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Far-Infrared Magneto-Optical Studies in Germanium and Indium-Antimonide at High Intensities

NASA Astrophysics Data System (ADS)

Leung, Michael

Observations of nonlinear magneto-optical phenomena occurring in p-type Germanium and n-type Indium Antimonide are reported. These include multi-photon ionization of impurity states, and a new observation, the magneto-photon ionization of impurity states, and a new observation, the magneto-photon drag effect. A novel source of far-infrared radiation has been used. This source uses a pulsed CO(,2) LASER to optically pump a super-radiant cell, generating light with intensities up to 100 KW/cm('2) and wavelengths from 66 (mu)m to 496 (mu)m in a pulse of 150 nanoseconds duration. The Germanium samples were doped with Gallium, which is a shallow acceptor with an ionization potential of 11 meV. At liquid Helium temperature virtually all charge carriers are bound to acceptor sites. However, the high intensity radiation unexpectedly ionizes the acceptors. This is demonstrated through measurements of photoconductivity, transmission and the photo-Hall Effect. This observation is unexpected because the photon energy is one-fourth the ionization potential. Rate equations describing sequential multiphoton excitations are in agreement with the experimental results. The intermediate states are postulated to be acceptor exciton band states. Studies of the photoexcited mobility at 496 (mu)m suggest that at non-saturating levels of photoexcitation, the primary scattering mechanism of hot holes in Germanium is by neutral impurities. A new magneto-optical effect, the magneto-photon drag effect, has been studied in both Germanium and Indium Antimonide. This is simply the absorption of momentum by free carriers, from an incident photon field. It has been found that the mechanism for this effect is different in the two materials. In Germanium, the effect occurs when carriers make optical transitions from the heavy hole band to the light hole band. Thus, the magneto-optical behavior depends heavily upon the band structure. On the other hand, a modified Drude model (independent electron) has been found to be reasonably successful in describing the effect in InSb. The inclusion of non-parabolicity and hot electron effects gives a consistent description of the experimental observations.

Design and implementation of fiber-based multiphoton endoscopy with microelectromechanical systems scanning

PubMed Central

Tang, Shuo; Jung, Woonggyu; McCormick, Daniel; Xie, Tuqiang; Su, Jiangping; Ahn, Yeh-Chan; Tromberg, Bruce J.; Chen, Zhongping

2010-01-01

A multiphoton endoscopy system has been developed using a two-axis microelectromechanical systems (MEMS) mirror and double-cladding photonic crystal fiber (DCPCF). The MEMS mirror has a 2-mm-diam, 20-deg optical scanning angle, and 1.26-kHz and 780-Hz resonance frequencies on the x and y axes. The maximum number of resolvable focal spots of the MEMS scanner is 720×720 on the x and y axes, which indicates that the MEMS scanner can potentially support high-resolution multiphoton imaging. The DCPCF is compared with standard single-mode fiber and hollow-core photonic bandgap fiber on the basis of dispersion, attenuation, and coupling efficiency properties. The DCPCF has high collection efficiency, and its dispersion can be compensated by grating pairs. Three configurations of probe design are investigated, and their imaging quality and field of view are compared. A two-lens configuration with a collimation and a focusing lens provides the optimum imaging performance and packaging flexibility. The endoscope is applied to image fluorescent microspheres and bovine knee joint cartilage. PMID:19566298

Fundamental mechanisms of laser damage of dielectric crystals by ultrashort pulse: ionization dynamics for the Keldysh model

NASA Astrophysics Data System (ADS)

Gruzdev, Vitaly

2014-12-01

Laser-induced ionization is a major process that initiates and drives the initial stages of laser-induced damage (LID) of high-quality transparent solids. The ionization and its contribution to LID are characterized in terms of the time-dependent ionization rate and conduction-band electron density. Considering femtosecond pulses of various durations (from 35 to 706 fs) and variable peak irradiances (from 0.01 to 60 TW/cm2), we use a single-rate equation to simulate time variations of conduction-band electron density and rates of the photoionization and impact ionization. The photoionization rate is evaluated with the Keldysh equation. At low irradiance, the electron density and total ionization rate demonstrate power scaling characteristic of multiphoton ionization. With the increase of irradiance, there is observed a saturation of the photoionization rate due to photoionization suppression by the Keldysh-type singularity during the increase in the number of simultaneously absorbed photons by 1. A striking result is that the saturation is followed by a stepwise transition from the ionization regime which is completely dominated by the photoionization to a regime totally dominated by the impact ionization. The transition results in the increase of the electron density by a few orders of magnitude induced by a variation of peak laser irradiance by about 15% to 20%. The physical effects that are involved are discussed.

Differentiation and Distributions of DNA/Cisplatin Crosslinks by Liquid Chromatography-Electrospray Ionization-Infrared Multiphoton Dissociation Mass Spectrometry

PubMed Central

Xu, Zhe; Brodbelt, Jennifer S.

2013-01-01

Liquid chromatography-electrospray ionization-infrared multiphoton dissociation (IRMPD) mass spectrometry was developed to investigate the distributions of intrastrand crosslinks formed between cisplatin and two oligodeoxynucleotides (ODNs), d(A1T2G3G4G5T6A7C8C9C10A11T12) (G3-D) and its analog d(A1T2G3G4G5T6T7C8C9C10A11T12) (G3-H), that have been reported to adopt different secondary structures in solution. Based on the formation of site-specific fragment ions upon IRMPD, two isobaric crosslink products were differentiated for each ODN. The preferential formation of G3G4 and G4G5 crosslinks was determined as a function of reaction conditions, including incubation temperature and presence of metal ions. G3-D consistently exhibited a greater preference for formation of the G4G5 crosslink compared to the G3-H ODN. The ratio of G3G4:G4G5 crosslinks increased for both G3-D and G3-H at higher incubation temperatures or when metal salts were added. Comparison of the IRMPD fragmentation patterns of the unmodified ODNs and the intramolecular platinated crosslinks indicated that backbone cleavage was significantly suppressed near the crosslink. PMID:24135806

Correlated electron-nuclear dynamics in above-threshold multiphoton ionization of asymmetric molecule.

PubMed

Wang, Zhuo; Li, Min; Zhou, Yueming; Lan, Pengfei; Lu, Peixiang

2017-02-20

The partition of the photon energy into the subsystems of molecules determines many photon-induced chemical and physical dynamics in laser-molecule interactions. The electron-nuclear energy sharing from multiphoton ionization of molecules has been used to uncover the correlated dynamics of the electron and fragments. However, most previous studies focus on symmetric molecules. Here we study the electron-nuclear energy sharing in strong-field photoionization of HeH 2+ by solving the one-dimensional time-dependent Schrödinger equation (TDSE). Compared with symmetric molecules, the joint electron-nuclear energy spectrum (JES) of HeH 2+ reveals an anomalous energy shift at certain nuclear energies, while it disappears at higher and lower nuclear energies. Through tracing the time evolution of the wavepacket of bound states, we identify that this energy shift originates from the joint effect of the Stark shift, associated with the permanent dipole, and the Autler-Townes effect due to the coupling of the 2pσ and 2sσ states in strong fields. The energy shift in the JES appears at certain nuclear distances only when both Stark effect and Autler-Townes effect play important roles. We further demonstrate that the electron-nuclei energy sharing can be controlled by varying laser intensity for asymmetric molecules, providing alternative approaches to manipulate photochemical reactions for more complex molecules.

Time-dependent density-functional theory with optimized effective potential and self-interaction correction and derivative discontinuity for the treatment of double ionization of He and Be atoms in intense laser fields

NASA Astrophysics Data System (ADS)

Heslar, John; Telnov, Dmitry A.; Chu, Shih-I.

2013-05-01

We present a self-interaction-free time-dependent density-functional theory (TDDFT) for the treatment of double-ionization processes of many-electron systems. The method is based on the extension of the Krieger-Li-Iafrate (KLI) treatment of the optimized effective potential (OEP) theory and the incorporation of an explicit self-interaction correction (SIC) term. In the framework of the time-dependent density functional theory, we have performed three-dimensional (3D) calculations of double ionization of He and Be atoms by intense near-infrared laser fields. We make use of the exchange-correlation potential with the integer discontinuity which improves the description of the double-ionization process. We found that a proper description of the double ionization requires the TDDFT exchange-correlation potential with the discontinuity with respect to the variation of the total particle number (TPN). The results for the intensity-dependent rates of double ionization of He and Be atoms are presented.

Factorization of laser-pulse ionization probabilities in the multiphotonic regime

NASA Astrophysics Data System (ADS)

Della Picca, R.; Fiol, J.; Fainstein, P. D.

2013-09-01

We present a detailed study of the ionization probability of H and H_{2}^{+} induced by a short intense laser pulse. Starting from a Coulomb-Volkov description of the process we derive a multipole-like expansion where each term is factored into two contributions: one that accounts for the effect of the electromagnetic field on the free-electron final state and a second factor that depends only on the target structure. Such a separation may be valuable to solve complex atomic or molecular systems as well as to interpret the dynamics of the process in simpler terms. We show that the series expansion converges rapidly, and thus the inclusion of the first few terms is sufficient to produce accurate results.

Jet-resolved vibronic structure in the higher excited states of N2O - Ultraviolet three-photon absorption spectroscopy from 80,000 to 90,000/cm

NASA Technical Reports Server (NTRS)

Patsilinakou, E.; Wiedmann, R. T.; Fotakis, C.; Grant, E. R.

1989-01-01

Ionization-detected UV multiphoton absorption spectroscopy of the excited states of N2O is presented, showing Rydberg structure within 20,000/cm of the first ionization threshold. Despite evidence for strong Rydberg-continuum coupling in the form of broadened bands and Fano line-shapes, the Rydberg structure persists, with atomic-like quantum defects and vibration structure well-matched with that of the ion. In the most clearly resolved spectrum, corresponding to the 3p(delta)1Pi state, Renner-Teller and Herzberg-Teller coupling of electronic and vibrational angular momentum are revealed. It is suggested that these mixings are properties of the N2O(+)Pi ion core.

Giant plasmon excitation in single and double ionization of C60 by fast highly charged Si and O ions

NASA Astrophysics Data System (ADS)

Kelkar, A. H.; Kadhane, U.; Misra, D.; Tribedi, L. C.

2007-09-01

Se have investigated single and double ionization of C60 molecule in collisions with 2.33 MeV/u Siq+ (q=6-14) and 3.125 MeV/u Oq+ (q=5-8) projectiles. The projectile charge state dependence of the single and double ionization yields of C60 are then compared to those for an ion-atom collision system using Ne gas as a target. A large difference between the gas and the cluster target behaviour was partially explained in terms of a model based on collective excitation namely the giant dipole plasmon resonance (GDPR). The qualitative agreement between the data and GDPR model prediction for single and double ionization signifies the importance of single and double plasmon excitations in the ionization process. A large deviation of the GDPR model for triple and quadruple ionization from the experimental data imply the importance of the other low impact parameter processes such as evaporation, fragmentation and a possible solid-like dynamical screening.

Effect of multiple plasmon excitation on single, double and multiple ionizations of C60 in collisions with fast highly charged Si ions

NASA Astrophysics Data System (ADS)

Kelkar, A. H.; Kadhane, U.; Misra, D.; Kumar, A.; Tribedi, L. C.

2007-06-01

We have investigated the single and multiple ionizations of the C60 molecule in collisions with fast Siq+ projectiles for various projectile charge states (q) between q = 6 and 14. The q-dependence of the ionization cross sections and their ratios is compared with the giant dipole plasmon resonance (GDPR) model. The excellent qualitative agreement with the model in case of single and double ionizations and also a reasonable agreement with the triple (and to some extent with quadruple) ionization (without evaporation) yields signify dominant contributions of the single-, double- and triple-plasmon excitations on the single- and multiple-ionization process.

Visualizing and Steering Dissociative Frustrated Double Ionization of Hydrogen Molecules

NASA Astrophysics Data System (ADS)

Zhang, Wenbin; Yu, Zuqing; Gong, Xiaochun; Wang, Junping; Lu, Peifen; Li, Hui; Song, Qiying; Ji, Qinying; Lin, Kang; Ma, Junyang; Li, Hanxiao; Sun, Fenghao; Qiang, Junjie; Zeng, Heping; He, Feng; Wu, Jian

2017-12-01

We experimentally visualize the dissociative frustrated double ionization of hydrogen molecules by using few-cycle laser pulses in a pump-probe scheme, in which process the tunneling ionized electron is recaptured by one of the outgoing nuclei of the breaking molecule. Three internuclear distances are recognized to enhance the dissociative frustrated double ionization of molecules at different instants after the first ionization step. The recapture of the electron can be further steered to one of the outgoing nuclei as desired by using phase-controlled two-color laser pulses. Both the experimental measurements and numerical simulations suggest that the Rydberg atom is favored to emit to the direction of the maximum of the asymmetric optical field. Our results on the one hand intuitively visualize the dissociative frustrated double ionization of molecules, and on the other hand open the possibility to selectively excite the heavy fragment ejected from a molecule.

Mass Spectroscopy of Neutral Metal Oxide Clusters Using a Desk-Top Soft X-Ray Laser

NASA Astrophysics Data System (ADS)

Dong, F.; Heinbuch, S.; Bernstein, E. R.; Rocca, J. J.

We report the use of a compact 46.9 nm capillary discharge soft x-ray laser in the study of metal-oxide nanoclusters using mass spectroscopy. Transition metal oxides are widely used as heterogeneous catalysts and catalytic supports in industrial processes. There are numerous applications for transition metal oxide catalysts, and although they are widely used, there is a lack of fundamental understanding of the complicated processes that occur on the metal oxide surface during catalysis. Conventional nanocluster spectroscopy techniques have used 193 nm radiation from an ArF excimer laser corresponding to a photon energy of 6.4 eV in order to photoionize a sample. Typical metal oxide nanocluster ionization energies fall into the range of 7-12 eV while some have even higher energies. Therefore a single 6.4 eV photon can not ionize the cluster making multiphoton processes the dominant ionization method. A major problem associated with mass spectroscopy can become evident during the multiphoton ionization of clusters. Specifically, the clusters may fragment during the ionization process and the identification of the neutral parent cluster can become difficult. In the present experiment neutral vanadium, niobium and tantalum oxide clusters are studied by single photon ionization with the 26.5 eV photons produced by a capillary discharge soft x-ray laser.1 During ionization, the metal oxide clusters are observed to be almost free of serious fragmentation. The most stable neutral cluster of vanadium, niobium, and tantalum oxide growth in a saturated oxygen condition are identified as MO2, M2O4/M2O5, M3O7, M4O10, M5O12, M6O15, M7O17, M8O20, and M9O22, which can be represented as a form (MO2)0,1(M2O5)y. M2O5 is identified as a basic unit to build-up the three kinds of metal oxide clusters. In the case of niobium and tantalum oxide clusters, the oxygen-deficient clusters with a structure of (MO2)2(M2O5)y are detected for groups that contain an even number of metal atoms. For vanadium oxide clusters, the oxygen-deficient clusters are detected for every family, indicating a stable structure of (VO2)x(V2O5)y. The stoichiometry of oxygen-rich clusters can be expressed as (MO2)0,1(M2O5)yO1-3 and their structures are consistent with chemically bonded species.

Supramolecular clusters between carbohydrates and concave pyridines. Detection in the gas phase by resonance-enhanced multi-photon ionization reflectron time-of-flight mass spectrometer.

PubMed

Liebig, Timo; Lüning, Ulrich; Grotemeyer, Jürgen

2006-01-01

For the first time the formation of supramolecular clusters between concave pyridines and different carbohydrates could be observed in the gas phase. The different clusters have been investigated by means of laser desorption into a supersonic beam followed by resonant multi photon excitation yielding mass spectra with high intensity of the different cluster. These preliminary results open a way for the investigations of the hydrogen bonds in these compounds.

Disentangling Intracycle Interferences in Photoelectron Momentum Distributions Using Orthogonal Two-Color Laser Fields

NASA Astrophysics Data System (ADS)

Xie, Xinhua; Wang, Tian; Yu, ShaoGang; Lai, XuanYang; Roither, Stefan; Kartashov, Daniil; Baltuška, Andrius; Liu, XiaoJun; Staudte, André; Kitzler, Markus

2017-12-01

We use orthogonally polarized two-color (OTC) laser pulses to separate quantum paths in the multiphoton ionization of Ar atoms. Our OTC pulses consist of 400 and 800 nm light at a relative intensity ratio of 10 ∶1 . We find a hitherto unobserved interference in the photoelectron momentum distribution, which exhibits a strong dependence on the relative phase of the OTC pulse. Analysis of model calculations reveals that the interference is caused by quantum pathways from nonadjacent quarter cycles.

Carrier-envelope phase-dependent atomic coherence and quantum beats

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

Wu Ying; State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, Wuhan Institute of Physics and Mathematics, Chinese Academy of Sciences, Wuhan 430071; Yang Xiaoxue

2007-07-15

It is shown that the carrier-envelope phase (CEP) of few-cycle laser pulses has profound effects on the bound-state atomic coherence even in the weak-field regime where both tunneling and multiphoton ionization hardly take place. The atomic coherence thus produced is shown to be able to be mapped onto the CEP-dependent signal of quantum beats (and other quantum-interference phenomena) and hence might be used to extract information about and ultimately to measure the carrier-envelope phase.

Charge transfer and charge localization in extended radical cations: Investigation of model molecules for peptides

NASA Astrophysics Data System (ADS)

Weinkauf, Rainer; Lehrer, Florian

1998-12-01

Molecules consisting of a flexible tail and an aromatic chromophore are used as model systems to understand the situation of a single chromophore in a small peptide. Their S0-S1 resonant multiphoton ionization (REMPI) spectra show, that in neutral molecules the tail-chromophore interaction is weak and electronic excitation is localized at the chromophore. For molecules, where the ionization energy of the tail is considerable higher than that of the chromophore, by high resolution REMPI photoelectron spectroscopy we find the charge to be localized on the aromatic chromophore. This scheme also in suitable peptides allows local ionization at the aromatic chromophore. An estimate for various charge positions in peptide chains, however, shows, that for most of the amino acids electron hole positions in the nitrogen and oxygen "lone pair" orbitals of the peptide bond are nearly degenerate. REMPI photoelectron spectra of phenylethylamine, which as a model system contains such two degenerate charge positions, show small energetic shift of the ionization energy but strong geometry changes upon electron removal. This result is interpreted as direct ionization into a mixed charge delocalized state. Consequences for the charge transfer mechanism in peptides are discussed.

Quasistatic limit of the strong-field approximation describing atoms in intense laser fields: Circular polarization

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

Bauer, Jaroslaw H.

2011-03-15

In the recent work of Vanne and Saenz [Phys. Rev. A 75, 063403 (2007)] the quasistatic limit of the velocity gauge strong-field approximation describing the ionization rate of atomic or molecular systems exposed to linearly polarized laser fields was derived. It was shown that in the low-frequency limit the ionization rate is proportional to the laser frequency {omega} (for a constant intensity of the laser field). In the present work I show that for circularly polarized laser fields the ionization rate is proportional to {omega}{sup 4} for H(1s) and H(2s) atoms, to {omega}{sup 6} for H(2p{sub x}) and H(2p{sub y})more » atoms, and to {omega}{sup 8} for H(2p{sub z}) atoms. The analytical expressions for asymptotic ionization rates (which become nearly accurate in the limit {omega}{yields}0) contain no summations over multiphoton contributions. For very low laser frequencies (optical or infrared) these expressions usually remain with an order-of-magnitude agreement with the velocity gauge strong-field approximation.« less

High-order above-threshold dissociation of molecules

NASA Astrophysics Data System (ADS)

Lu, Peifen; Wang, Junping; Li, Hui; Lin, Kang; Gong, Xiaochun; Song, Qiying; Ji, Qinying; Zhang, Wenbin; Ma, Junyang; Li, Hanxiao; Zeng, Heping; He, Feng; Wu, Jian

2018-03-01

Electrons bound to atoms or molecules can simultaneously absorb multiple photons via the above-threshold ionization featured with discrete peaks in the photoelectron spectrum on account of the quantized nature of the light energy. Analogously, the above-threshold dissociation of molecules has been proposed to address the multiple-photon energy deposition in the nuclei of molecules. In this case, nuclear energy spectra consisting of photon-energy spaced peaks exceeding the binding energy of the molecular bond are predicted. Although the observation of such phenomena is difficult, this scenario is nevertheless logical and is based on the fundamental laws. Here, we report conclusive experimental observation of high-order above-threshold dissociation of H2 in strong laser fields where the tunneling-ionized electron transfers the absorbed multiphoton energy, which is above the ionization threshold to the nuclei via the field-driven inelastic rescattering. Our results provide an unambiguous evidence that the electron and nuclei of a molecule as a whole absorb multiple photons, and thus above-threshold ionization and above-threshold dissociation must appear simultaneously, which is the cornerstone of the nowadays strong-field molecular physics.

Multiphoton Rydberg and valence dynamics of CH3Br probed by mass spectrometry and slice imaging.

PubMed

Hafliðason, Arnar; Glodic, Pavle; Koumarianou, Greta; Samartzis, Peter C; Kvaran, Ágúst

2018-06-18

The multiphoton dynamics of CH3Br were probed by Mass Resolved MultiPhoton Ionization (MR-MPI), Slice Imaging and Photoelectron Imaging in the two-photon excitation region of 66 000 to 80 000 cm-1. Slice images of the CH3+ and Br+ photoproducts of ten two-photon resonant transitions to np and nd Rydberg states of the parent molecule were recorded. CH3+ ions dominate the mass spectra. Kinetic energy release spectra (KERs) were derived from slice and photoelectron images and anisotropy parameters were extracted from the angular distributions of the ions to identify the processes and the dynamics involved. At all wavelengths we observe three-photon excitations, via the two-photon resonant transitions to molecular Rydberg states, forming metastable, superexcited (CH3Br#) states which dissociate to form CH3 Rydberg states (CH3**) along with Br/Br*. A correlation between the parent Rydberg states excited and CH3** formed is evident. For the three highest excitation energies used, the CH3Br# metastable states also generate high kinetic energy fragments of CH3(X) and Br/Br*. In addition for two out of these three wavelengths we also measure one-photon photolysis of CH3Br in the A band forming CH3(X) in various vibrational modes and bromine atoms in the ground (Br) and spin-orbit excited (Br*) states.

Origin of double-line structure in nonsequential double ionization by few-cycle laser pulses

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

Huang, Cheng, E-mail: huangcheng@swu.edu.cn; Zhong, Mingmin; Wu, Zhengmao

2016-07-28

We investigate nonsequential double ionization (NSDI) of molecules by few-cycle laser pulses at the laser intensity of 1.2–1.5 × 10{sup 14} W/cm{sup 2} using the classical ensemble model. The same double-line structure as the lower intensity (1.0 × 10{sup 14} W/cm{sup 2}) is also observed in the correlated electron momentum spectra for 1.2–1.4 × 10{sup 14} W/cm{sup 2}. However, in contrast to the lower intensity where NSDI proceeds only through the recollision-induced double excitation with subsequent ionization (RDESI) mechanism, here, the recollision-induced excitation with subsequent ionization (RESI) mechanism has a more significant contribution to NSDI. This indicates that RDESI ismore » not necessary for the formation of the double-line structure and RESI can give rise to the same type of structure independently. Furthermore, we explore the ultrafast dynamics underlying the formation of the double-line structure in RESI.« less

Open-Ended Recursive Approach for the Calculation of Multiphoton Absorption Matrix Elements

PubMed Central

2015-01-01

We present an implementation of single residues for response functions to arbitrary order using a recursive approach. Explicit expressions in terms of density-matrix-based response theory for the single residues of the linear, quadratic, cubic, and quartic response functions are also presented. These residues correspond to one-, two-, three- and four-photon transition matrix elements. The newly developed code is used to calculate the one-, two-, three- and four-photon absorption cross sections of para-nitroaniline and para-nitroaminostilbene, making this the first treatment of four-photon absorption in the framework of response theory. We find that the calculated multiphoton absorption cross sections are not very sensitive to the size of the basis set as long as a reasonably large basis set with diffuse functions is used. The choice of exchange–correlation functional, however, significantly affects the calculated cross sections of both charge-transfer transitions and other transitions, in particular, for the larger para-nitroaminostilbene molecule. We therefore recommend the use of a range-separated exchange–correlation functional in combination with the augmented correlation-consistent double-ζ basis set aug-cc-pVDZ for the calculation of multiphoton absorption properties. PMID:25821415

High-precision two-dimensional atom localization from four-wave mixing in a double-Λ four-level atomic system

NASA Astrophysics Data System (ADS)

Shui, Tao; Yang, Wen-Xing; Chen, Ai-Xi; Liu, Shaopeng; Li, Ling; Zhu, Zhonghu

2018-03-01

We propose a scheme for high-precision two-dimensional (2D) atom localization via the four-wave mixing (FWM) in a four-level double-Λ atomic system. Due to the position-dependent atom-field interaction, the 2D position information of the atoms can be directly determined by the measurement of the normalized light intensity of output FWM-generated field. We further show that, when the position-dependent generated FWM field has become sufficiently intense, efficient back-coupling to the FWM generating state becomes important. This back-coupling pathway leads to competitive multiphoton destructive interference of the FWM generating state by three supplied and one internally generated fields. We find that the precision of 2D atom localization can be improved significantly by the multiphoton destructive interference and depends sensitively on the frequency detunings and the pump field intensity. Interestingly enough, we show that adjusting the frequency detunings and the pump field intensity can modify significantly the FWM efficiency, and consequently lead to a redistribution of the atoms. As a result, the atom can be localized in one of four quadrants with holding the precision of atom localization.

Molecular symmetry group analysis of the low-wavenumber torsions and vibration-torsions in the S1 state and ground state cation of p-xylene: An investigation using resonance-enhanced multiphoton ionization (REMPI) and zero-kinetic-energy (ZEKE) spectroscopy

NASA Astrophysics Data System (ADS)

Gardner, Adrian M.; Tuttle, William D.; Groner, Peter; Wright, Timothy G.

2017-03-01

For the first time, a molecular symmetry group (MSG) analysis has been undertaken in the investigation of the electronic spectroscopy of p-xylene (p-dimethylbenzene). Torsional and vibration-torsional (vibtor) levels in the S1 state and ground state of the cation of p-xylene are investigated using resonance-enhanced multiphoton ionization (REMPI) and zero-kinetic-energy (ZEKE) spectroscopy. In the present work, we concentrate on the 0-350 cm-1 region, where there are a number of torsional and vibtor bands and we discuss the assignment of this region. In Paper II [W. D. Tuttle et al., J. Chem. Phys. 146, 124309 (2017)], we examine the 350-600 cm-1 region where vibtor levels are observed as part of a Fermi resonance. The similarity of much of the observed spectral activity to that in the related substituted benzenes, toluene and para-fluorotoluene, is striking, despite the different symmetries. The discussion necessitates a consideration of the MSG of p-xylene, which has been designated G72, but we shall also designate [{3,3}]D2h and we include the symmetry operations, character table, and direct product table for this. We also discuss the symmetries of the internal rotor (torsional) levels and the selection rules for the particular electronic transition of p-xylene investigated here.

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

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

Andrejeva, Anna; Tuttle, William D.; Harris, Joe P.

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, themore » 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.« less

Increased upstream ionization due to formation of a double layer.

PubMed

Thakur, S Chakraborty; Harvey, Z; Biloiu, I A; Hansen, A; Hardin, R A; Przybysz, W S; Scime, E E

2009-01-23

We report observations that confirm a theoretical prediction that formation of a current-free double layer in a plasma expanding into a chamber of larger diameter is accompanied by an increase in ionization upstream of the double layer. The theoretical model argues that the increased ionization is needed to balance the difference in diffusive losses upstream and downstream of the expansion region. In our expanding helicon source experiments, we find that the upstream plasma density increases sharply at the same antenna frequency at which the double layer appears.

Circular dichroism in photoelectron images from aligned nitric oxide molecules

DOE PAGES

Sen, Ananya; Pratt, S. T.; Reid, K. L.

2017-05-03

We have used velocity map photoelectron imaging to study circular dichroism of the photoelectron angular distributions (PADs) of nitric oxide following two-color resonanceenhanced two-photon ionization via selected rotational levels of the A 2Σ +, v' = 0 state. By using a circularly polarized pump beam and a counter-propagating, circularly polarized probe beam, cylindrical symmetry is preserved in the ionization process, and the images can be reconstructed using standard algorithms. The VMI set up enables individual ion rotational states to be resolved with excellent collection efficiency, rendering the measurements considerably simpler to perform than previous measurements conducted with a conventional photoelectronmore » spectrometer. The results demonstrate that circular dichroism is observed even when cylindrical symmetry is maintained, and serve as a reminder that dichroism is a general feature of the multiphoton ionization of atoms and molecules. Furthermore, the observed PADs are in good agreement with calculations based on parameters extracted from previous experimental results obtained by using a time-offlight electron spectrometer.« less

Circular dichroism in photoelectron images from aligned nitric oxide molecules

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

Sen, Ananya; Pratt, S. T.; Reid, K. L.

We have used velocity map photoelectron imaging to study circular dichroism of the photoelectron angular distributions (PADs) of nitric oxide following two-color resonanceenhanced two-photon ionization via selected rotational levels of the A 2Σ +, v' = 0 state. By using a circularly polarized pump beam and a counter-propagating, circularly polarized probe beam, cylindrical symmetry is preserved in the ionization process, and the images can be reconstructed using standard algorithms. The VMI set up enables individual ion rotational states to be resolved with excellent collection efficiency, rendering the measurements considerably simpler to perform than previous measurements conducted with a conventional photoelectronmore » spectrometer. The results demonstrate that circular dichroism is observed even when cylindrical symmetry is maintained, and serve as a reminder that dichroism is a general feature of the multiphoton ionization of atoms and molecules. Furthermore, the observed PADs are in good agreement with calculations based on parameters extracted from previous experimental results obtained by using a time-offlight electron spectrometer.« less

Multiple ionization of C 60 in collisions with 2.33 MeV/u O-ions and giant plasmon excitation

NASA Astrophysics Data System (ADS)

Kelkar, A. H.; Kadhane, U.; Misra, D.; Kumar, Ajay; Tribedi, L. C.

2007-03-01

Single and multiple ionization of C60 in collisions with fast (v = 9.7 a.u.) Oq+ ions have been studied. Relative cross sections for production of C 601+ to C 604+ have been measured. The intensity ratios of double-to-single ionization agree very well with a model based on giant dipole plasmon resonance (GDPR). Almost linear increasing trend of the yields of single and double ionizations with projectile charge state is well reproduced by the single and double plasmon excitation mechanisms. The observed charge state independence of triple and quadruple ionization is in sharp contrast to the GDPR model.

Double-frequency microwave ionization of Na

NASA Astrophysics Data System (ADS)

Ruff, G. A.; Dietrick, K. M.; Gallagher, T. F.

1990-11-01

We report the ionization of Na atoms by the simultaneous application of microwave fields of two different frequencies. We conclude that the salient features of double-frequency ionization can be readily understood. Both the hydrogenlike ||m||=2 states and the nonhydrogenic ||m||=0 and 1 states ionize when the sum of the field amplitudes, the peak field, reaches the field required for ionization by a single microwave frequency, E=1/9n4 and E=1/3n5, respectively.

Bond-rearrangement and ionization mechanisms in the photo-double-ionization of simple hydrocarbons (C 2H 4, C 2H 3F, and 1,1-C 2H 2F 2) near and above threshold

DOE PAGES

Gaire, B.; Gatton, A. S.; Wiegandt, F.; ...

2016-09-14

We have investigated bond-rearrangement driven by photo-double-ionization (PDI) near and above the double ionization threshold in a sequence of carbon-carbon double bonded hydrocarbon molecules: ethylene, fluoroethylene, and 1,1-difluoroethylene. We employ the kinematically complete cold target recoil ion momentum spectroscopy (COLTRIMS) method to resolve all photo-double-ionization events leading to two-ionic fragments. We observe changes in the branching ratios of different dissociative ionization channels depending on the presence of none, one, or two fluorine atoms. The role of the fluorine atom in the bond-rearrangement channels is intriguing as evident by the re-ordering of the threshold energies of the PDI in the fluorinatedmore » molecules. These effects offer a compelling argument that the electronegativity of the fluorine (or the polarity of the molecule) strongly influences the potential energy surfaces of the molcules and drives bond-rearrangement during the dissociation process. The energy sharing and the relative angle between the 3D-momentum vectors of the two electrons provide clear evidence of direct and indirect PDI processes.« less

Electron-helium S-wave model benchmark calculations. II. Double ionization, single ionization with excitation, and double excitation

NASA Astrophysics Data System (ADS)

Bartlett, Philip L.; Stelbovics, Andris T.

2010-02-01

The propagating exterior complex scaling (PECS) method is extended to all four-body processes in electron impact on helium in an S-wave model. Total and energy-differential cross sections are presented with benchmark accuracy for double ionization, single ionization with excitation, and double excitation (to autoionizing states) for incident-electron energies from threshold to 500 eV. While the PECS three-body cross sections for this model given in the preceding article [Phys. Rev. A 81, 022715 (2010)] are in good agreement with other methods, there are considerable discrepancies for these four-body processes. With this model we demonstrate the suitability of the PECS method for the complete solution of the electron-helium system.

Probing cis-trans isomerization in the S{sub 1} state of C{sub 2}H{sub 2} via H-atom action and hot band-pumped IR-UV double resonance spectroscopies

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

Changala, P. Bryan; Baraban, Joshua H.; Field, Robert W., E-mail: rwfield@mit.edu

2015-08-28

We report novel experimental strategies that should prove instrumental in extending the vibrational and rotational assignments of the S{sub 1} state of acetylene, C{sub 2}H{sub 2}, in the region of the cis-trans isomerization barrier. At present, the assignments are essentially complete up to ∼500 cm{sup −1} below the barrier. Two difficulties arise when the assignments are continued to higher energies. One is that predissociation into C{sub 2}H + H sets in roughly 1100 cm{sup −1} below the barrier; the resulting quenching of laser-induced fluorescence (LIF) reduces its value for recording spectra in this region. The other difficulty is that tunnelingmore » through the barrier causes a staggering in the K-rotational structure of isomerizing vibrational levels. The assignment of these levels requires data for K values up to at least 3. Given the rotational selection rule K′ − ℓ{sup ′′} = ± 1, such data must be obtained via excited vibrational levels of the ground state with ℓ{sup ′′} > 0. In this paper, high resolution H-atom resonance-enhanced multiphoton ionization spectra are demonstrated to contain predissociated bands which are almost invisible in LIF spectra, while preliminary data using a hyperthermal pulsed nozzle show that ℓ{sup ′′} = 2 states can be selectively populated in a jet, giving access to K′ = 3 states in IR-UV double resonance.« less

Nonsequential double ionization channels control of Ar with few-cycle elliptically polarized laser pulse by carrier-envelope-phase.

PubMed

Ben, Shuai; Wang, Tian; Xu, Tongtong; Guo, Jing; Liu, Xueshen

2016-04-04

The carrier-envelop-phase (CEP) dependence of nonsequential double ionization (NSDI) of atomic Ar with few-cycle elliptically polarized laser pulse is investigated using 2D classical ensemble method. We distinguish two particular recollision channels in NSDI, which are recollision-impact ionization (RII) and recollision-induced excitation with subsequent ionization (RESI). We separate the RII and RESI channels according to the delay time between recollision and final double ionization. By tracing the history of the trajectories, we find the electron correlation spectra as well as the competition between the two channels are sensitively dependent on the laser field CEP. Finally, control can be achieved between the two channels by varying the CEP.

OSA (Optical Society of America) Proceedings on Short Wavelength Coherent Radiation: Generation and Applications Held in North Falmouth, Massachusetts on 26-29 September 1988. Volume 2

DTIC Science & Technology

1988-09-01

obtained using CVI 6d-2p line 142 Axial as a reference line[5]. The maximum en- hancement factor of 4.2 and corresponding cv1 gain length product of...C. Solem, and C. K. Rhodes ..... .............. 220 Multiphoton Ionization for the Production of X-Ray Laser Plasmas by P. B. Corkum and N. H...Diffraction Using Synchrotron Radiation by Rudolf Ruffer ......... ............................... 400 The Production of Long Coherence-Length Hard X

Free Radical-Surface Interactions Using Multiphoton Ionization of Free Radicals

DTIC Science & Technology

1989-01-01

Atoms, Rgf4PI 9 t Free Radl!cals)aj" i Atoms, Cross Section -’r RE)* I of Free Radicals arid Atonn. 𔄃 43S’RACT (Conti n reverse if necessary Ind identi...these surfaces. The basic philosophy of our CF 3I -+- nhv-CF, - t - I . program consists of generating a particular neutral species at A low pressures...constant for the escape of radicals out of the " reactor is shown in Eq. (6): .= k =, 4 .4,., I /V, (6) L !J 7 where t ,,, is the thermal molecular

Selectivity of Electronic Coherence and Attosecond Ionization Delays in Strong-Field Double Ionization

NASA Astrophysics Data System (ADS)

Kobayashi, Yuki; Reduzzi, Maurizio; Chang, Kristina F.; Timmers, Henry; Neumark, Daniel M.; Leone, Stephen R.

2018-06-01

Experiments are presented on real-time probing of coherent electron dynamics in xenon initiated by strong-field double ionization. Attosecond transient absorption measurements allow for characterization of electronic coherences as well as relative ionization timings in multiple electronic states of Xe+ and Xe2 + . A high degree of coherence g =0.4 is observed between P3 2 0-P3 0 0 of Xe2 + , whereas for other possible pairs of states the coherences are below the detection limits of the experiments. A comparison of the experimental results with numerical simulations based on an uncorrelated electron-emission model shows that the coherences produced by strong-field double ionization are more selective than predicted. Surprisingly short ionization time delays, 0.85 fs, 0.64 fs, and 0.75 fs relative to Xe+ formation, are also measured for the P2 3 , P0 3 , and P1 3 states of Xe2 + , respectively. Both the unpredicted selectivity in the formation of coherence and the subfemtosecond time delays of specific states provide new insight into correlated electron dynamics in strong-field double ionization.

Observation of two-center interference effects for electron impact ionization of N2

NASA Astrophysics Data System (ADS)

Chaluvadi, Hari; Nur Ozer, Zehra; Dogan, Mevlut; Ning, Chuangang; Colgan, James; Madison, Don

2015-08-01

In 1966, Cohen and Fano (1966 Phys. Rev. 150 30) suggested that one should be able to observe the equivalent of Young’s double slit interference if the double slits were replaced by a diatomic molecule. This suggestion inspired many experimental and theoretical studies searching for double slit interference effects both for photon and particle ionization of diatomic molecules. These effects turned out to be so small for particle ionization that this work proceeded slowly and evidence for interference effects were only found by looking at cross section ratios. Most of the early particle work concentrated on double differential cross sections for heavy particle scattering and the first evidence for two-center interference for electron-impact triple differential cross section (TDCS) did not appear until 2006 for ionization of H2. Subsequent work has now firmly established that two-center interference effects can be seen in the TDCS for electron-impact ionization of H2. However, in spite of several experimental and theoretical studies, similar effects have not been found for electron-impact ionization of N2. Here we report the first evidence for two-center interference for electron-impact ionization of N2.

Nuclear-Recoil Differential Cross Sections for the Two Photon Double Ionization of Helium

NASA Astrophysics Data System (ADS)

Abdel Naby, Shahin; Ciappina, M. F.; Lee, T. G.; Pindzola, M. S.; Colgan, J.

2013-05-01

In support of the reaction microscope measurements at the free-electron laser facility at Hamburg (FLASH), we use the time-dependent close-coupling method (TDCC) to calculate fully differential nuclear-recoil cross sections for the two-photon double ionization of He at photon energy of 44 eV. The total cross section for the double ionization is in good agreement with previous calculations. The nuclear-recoil distribution is in good agreement with the experimental measurements. In contrast to the single-photon double ionization, maximum nuclear recoil triple differential cross section is obtained at small nuclear momenta. This work was supported in part by grants from NSF and US DoE. Computational work was carried out at NERSC in Oakland, California and the National Institute for Computational Sciences in Knoxville, Tennessee.

Probing Long-Range Configurations of Molecular Hydrogen

NASA Astrophysics Data System (ADS)

McCormack, Elizabeth

2011-05-01

Very long-range molecular configurations are of interest in a variety of contexts, for example, in the astro-chemistry of cold molecular clouds and in planetary atmospheres, including our own. Such states can be more than 10 times the size of the ground state and often possess energies above multiple ionization potentials and dissociation limits resulting in diverse and complex decay dynamics. Many of these configurations possess a double-well character arising from the interaction of molecular Rydberg states, repulsive doubly-excited states, and ionic states. The ion pair in hydrogen, an unusual molecular configuration consisting of one proton shrouded in a cloud of two electrons separated very far from the other proton, is notoriously difficult to create and study. We report results from on our investigation of such states using resonantly enhanced multi-photon ionization via the E,F v = 6, J = 0, 1, and 2 states to probe the H(n = 1) + H(n = 3) dissociation threshold energy region. Both molecular and atomic ion production were detected as a function of wavelength by using a time-of-flight mass spectrometer. Below threshold a series of highly excited vibrational levels of several long range states are observed. Above threshold broad resonances are observed with energies that agree well with the predictions of a mass-scaled Rydberg formula for bound states of the H+ H- ion pair. Measured linewidths, quantum defects, and rotational dependences are reported for ion pair principal quantum numbers in the range of n = 130 to 206. Our new results can be compared to recent experimental work using a different excitation scheme, which was the first spectroscopic observation of heavy Rydberg states in hydrogen, and new ab initio theoretical work. Supported by the National Science Foundation.

Attosecond Spectroscopy Probing Electron Correlation Dynamics

NASA Astrophysics Data System (ADS)

Winney, Alexander H.

Electrons are the driving force behind every chemical reaction. The exchange, ionization, or even relaxation of electrons is behind every bond broken or formed. According to the Bohr model of the atom, it takes an electron 150 as to orbit a proton[6]. With this as a unit time scale for an electron, it is clear that a pulse duration of several femtoseconds will not be sufficient to understanding electron dynamics. Our work demonstrates both technical and scientific achievements that push the boundaries of attosecond dynamics. TDSE studies show that amplification the yield of high harmonic generation (HHG) may be possible with transverse confinement of the electron. XUV-pump-XUV-probe shows that the yield of APT train can be sufficient for 2-photon double ionization studies. A zero dead-time detection system allows for the measurement of state-resolved double ionization for the first time. Exploiting attosecond angular streaking[7] probes sequential and non-sequential double ionization via electron-electron correlations with attosecond time resolution. Finally, using recoil frame momentum correlation, the fast dissociation of CH 3I reveals important orbital ionization dynamics of non-dissociative & dissociative, single & double ionization.

Single-shot measurements of laser-induced avalanche breakdown demonstrating spatial and temporal control by an external source

NASA Astrophysics Data System (ADS)

Woodbury, Daniel; Wahlstrand, Jared; Goers, Andy; Feder, Linus; Miao, Bo; Hine, George; Salehi, Fatholah; Milchberg, Howard

2016-10-01

We report on the use of single-shot supercontinuum spectral interferometry (SSSI) to make temporally and spatially resolved measurements of laser-induced avalanche breakdown in ambient air by a 200 ps pulse. By seeding the breakdown using an external 100 fs pulse, we demonstrate control over the timing and spatial characteristics of the avalanche. In addition, we calculate the collisional ionization rates at various laser intensities and demonstrate seeding of the avalanche breakdown both by multiphoton ionization and by photodetaching ions produced from a radioactive source. These observations provide proof-of-concept support for recent proposals to remotely measure radioactivity using laser-induced avalanche breakdown. This work supported by a DTRA, C-WMD Basic Research Program, and by the DOE NNSA Stewardship Science Graduate Fellowship, provided under Grant Number DE-NA0002135.

REMPI detection of singlet oxygen 1O2 arising from UV-photodissociation of van der Waals complex isoprene-oxygen C5H8-O2

NASA Astrophysics Data System (ADS)

Bogomolov, Alexandr S.; Dozmorov, Nikolay V.; Kochubei, Sergei A.; Baklanov, Alexey V.

2018-01-01

The one-laser two-color resonance enhanced multiphoton ionization REMPI [(1 + 1‧) + 1] and velocity map imaging have been applied to investigate formation of molecular oxygen in excited singlet O2(a1Δg) and ground O2(X3Σg-) states in the photodissociation of van der Waals complex isoprene-oxygen C5H8-O2. These molecules were found to appear in the different rotational states with translational energy varied from a value as low as ∼1 meV to a distribution with temperature of about 940 K. The observed traces of electron recoil in the images of photoions reveal participation of several ionization pathways of the resonantly excited intermediate states of O2.

Timing Recollision in Nonsequential Double Ionization by Intense Elliptically Polarized Laser Pulses.

PubMed

Kang, H; Henrichs, K; Kunitski, M; Wang, Y; Hao, X; Fehre, K; Czasch, A; Eckart, S; Schmidt, L Ph H; Schöffler, M; Jahnke, T; Liu, X; Dörner, R

2018-06-01

We examine correlated electron and doubly charged ion momentum spectra from strong field double ionization of neon employing intense elliptically polarized laser pulses. An ellipticity-dependent asymmetry of correlated electron and ion momentum distributions has been observed. Using a 3D semiclassical model, we demonstrate that our observations reflect the subcycle dynamics of the recollision process. Our Letter reveals a general physical picture for recollision impact double ionization with elliptical polarization and demonstrates the possibility of ultrafast control of the recollision dynamics.

Timing Recollision in Nonsequential Double Ionization by Intense Elliptically Polarized Laser Pulses

NASA Astrophysics Data System (ADS)

Kang, H.; Henrichs, K.; Kunitski, M.; Wang, Y.; Hao, X.; Fehre, K.; Czasch, A.; Eckart, S.; Schmidt, L. Ph. H.; Schöffler, M.; Jahnke, T.; Liu, X.; Dörner, R.

2018-06-01

We examine correlated electron and doubly charged ion momentum spectra from strong field double ionization of neon employing intense elliptically polarized laser pulses. An ellipticity-dependent asymmetry of correlated electron and ion momentum distributions has been observed. Using a 3D semiclassical model, we demonstrate that our observations reflect the subcycle dynamics of the recollision process. Our Letter reveals a general physical picture for recollision impact double ionization with elliptical polarization and demonstrates the possibility of ultrafast control of the recollision dynamics.

High-order above-threshold dissociation of molecules.

PubMed

Lu, Peifen; Wang, Junping; Li, Hui; Lin, Kang; Gong, Xiaochun; Song, Qiying; Ji, Qinying; Zhang, Wenbin; Ma, Junyang; Li, Hanxiao; Zeng, Heping; He, Feng; Wu, Jian

2018-02-27

Electrons bound to atoms or molecules can simultaneously absorb multiple photons via the above-threshold ionization featured with discrete peaks in the photoelectron spectrum on account of the quantized nature of the light energy. Analogously, the above-threshold dissociation of molecules has been proposed to address the multiple-photon energy deposition in the nuclei of molecules. In this case, nuclear energy spectra consisting of photon-energy spaced peaks exceeding the binding energy of the molecular bond are predicted. Although the observation of such phenomena is difficult, this scenario is nevertheless logical and is based on the fundamental laws. Here, we report conclusive experimental observation of high-order above-threshold dissociation of H 2 in strong laser fields where the tunneling-ionized electron transfers the absorbed multiphoton energy, which is above the ionization threshold to the nuclei via the field-driven inelastic rescattering. Our results provide an unambiguous evidence that the electron and nuclei of a molecule as a whole absorb multiple photons, and thus above-threshold ionization and above-threshold dissociation must appear simultaneously, which is the cornerstone of the nowadays strong-field molecular physics. Copyright © 2018 the Author(s). Published by PNAS.

SFC-APLI-(TOF)MS: Hyphenation of Supercritical Fluid Chromatography to Atmospheric Pressure Laser Ionization Mass Spectrometry.

PubMed

Klink, Dennis; Schmitz, Oliver Johannes

2016-01-05

Atmospheric-pressure laser ionization mass spectrometry (APLI-MS) is a powerful method for the analysis of polycyclic aromatic hydrocarbon (PAH) molecules, which are ionized in a selective and highly sensitive way via resonance-enhanced multiphoton ionization. APLI was presented in 2005 and has been hyphenated successfully to chromatographic separation techniques like high performance liquid chromatography (HPLC) and gas chromatography (GC). In order to expand the portfolio of chromatographic couplings to APLI, a new hyphenation setup of APLI and supercritical-fluid chromatography (SFC) was constructed and aim of this work. Here, we demonstrate the first hyphenation of SFC and APLI in a simple designed way with respect to different optimization steps to ensure a sensitive analysis. The new setup permits qualitative and quantitative determination of native and also more polar PAH molecules. As a result of the altered ambient characteristics within the source enclosure, the quantification of 1-hydroxypyrene (1-HP) in human urine is possible without prior derivatization. The limit of detection for 1-HP by SFC-APLI-TOF(MS) was found to be 0.5 μg L(-1), which is lower than the 1-HP concentrations found in exposed persons.

A practical theoretical formalism for atomic multielectron processes: direct multiple ionization by a single auger decay or by impact of a single electron or photon

NASA Astrophysics Data System (ADS)

Liu, Pengfei; Zeng, Jiaolong; Yuan, Jianmin

2018-04-01

Multiple electron processes occur widely in atoms, molecules, clusters, and condensed matters when they are interacting with energetic particles or intense laser fields. Direct multielectron processes (DMEP) are the most complicated among the general multiple electron processes and are the most difficult to describe theoretically. In this work, a unified and accurate theoretical formalism is proposed on the DMEP of atoms including the multiple auger decay and multiple ionization by an impact of a single electron or a single photon based on the atomic collision theory described by a correlated many-body Green's function. Such a practical treatment is made possible by taking consideration of the different coherence features of the atoms (matter waves) in the initial and final states. We first explain how the coherence characteristics of the ejected continuum electrons is largely destructed, by taking the electron impact direct double ionization process as an example. The direct double ionization process is completely different from the single ionization where the complete interference can be maintained. The detailed expressions are obtained for the energy correlations among the continuum electrons and energy resolved differential and integral cross sections according to the separation of knock-out (KO) and shake-off (SO) mechanisms for the electron impact direct double ionization, direct double and triple auger decay, and double and triple photoionization (TPI) processes. Extension to higher order DMEP than triple ionization is straight forward by adding contributions of the following KO and SO processes. The approach is applied to investigate the electron impact double ionization processes of C+, N+, and O+, the direct double and triple auger decay of the K-shell excited states of C+ 1s2{s}22{p}2{}2D and {}2P, and the double and TPI of lithium. Comparisons with the experimental and other theoretical investigations wherever available in the literature show that our theoretical formalism is accurate and effective in treating the atomic multielectron processes.

How the laser-induced ionization of transparent solids can be suppressed

NASA Astrophysics Data System (ADS)

Gruzdev, Vitaly

2013-12-01

A capability to suppress laser-induced ionization of dielectric crystals in controlled and predictable way can potentially result in substantial improvement of laser damage threshold of optical materials. The traditional models that employ the Keldysh formula do not predict any suppression of the ionization because of the oversimplified description of electronic energy bands underlying the Keldysh formula. To fix this gap, we performed numerical simulations of time evolution of conduction-band electron density for a realistic cosine model of electronic bands characteristic of wide-band-gap cubic crystals. The simulations include contributions from the photo-ionization (evaluated by the Keldysh formula and by the formula for the cosine band of volume-centered cubic crystals) and from the avalanche ionization (evaluated by the Drude model). Maximum conduction-band electron density is evaluated from a single rate equation as a function of peak intensity of femtosecond laser pulses for alkali halide crystals. Results obtained for high-intensity femtosecond laser pulses demonstrate that the ionization can be suppressed by proper choice of laser parameters. In case of the Keldysh formula, the peak electron density exhibits saturation followed by gradual increase. For the cosine band, the electron density increases with irradiance within the low-intensity multiphoton regime and switches to decrease with intensity approaching threshold of the strong singularity of the ionization rate characteristic of the cosine band. Those trends are explained with specific modifications of band structure by electric field of laser pulses.

Multiphoton microscopy system with a compact fiber-based femtosecond-pulse laser and handheld probe

PubMed Central

Liu, Gangjun; Kieu, Khanh; Wise, Frank W.; Chen, Zhongping

2012-01-01

We report on the development of a compact multiphoton microscopy (MPM) system that integrates a compact and robust fiber laser with a miniature probe. The all normal dispersion fiber femtosecond laser has a central wavelength of 1.06 μm, pulse width of 125 fs and average power of more than 1 W. A double cladding photonic crystal fiber was used to deliver the excitation beam and to collect the two-photon signal. The hand-held probe included galvanometer-based mirror scanners, relay lenses and a focusing lens. The packaged probe had a diameter of 16 mm. Second harmonic generation (SHG) images and two-photon excited fluorescence (TPEF) images of biological tissues were demonstrated using the system. MPM images of different biological tissues acquired by the compact system which integrates an FBFP laser, an DCPCF and a miniature handheld probe. PMID:20635426

Dissociation of heme from gaseous myoglobin ions studied by infrared multiphoton dissociation spectroscopy and Fourier-transform ion cyclotron resonance mass spectrometry

NASA Astrophysics Data System (ADS)

Wang, Yi-Sheng; Sabu, Sahadevan; Wei, Shih-Chia; Josh Kao, C.-M.; Kong, Xianglei; Liau, Shing-Chih; Han, Chau-Chung; Chang, Huan-Cheng; Tu, Shih-Yu; Kung, A. H.; Zhang, John Z. H.

2006-10-01

Detachment of heme prosthetic groups from gaseous myoglobin ions has been studied by collision-induced dissociation and infrared multiphoton dissociation in combination with Fourier-transform ion cyclotron resonance mass spectrometry. Multiply charged holomyoglobin ions (hMbn +) were generated by electrospray ionization and transferred to an ion cyclotron resonance cell, where the ions of interest were isolated and fragmented by either collision with Ar atoms or irradiation with 3μm photons, producing apomyoglobin ions (aMbn +). Both charged heme loss (with [Fe(III)-heme]+ and aMb(n-1)+ as the products) and neutral heme loss (with [Fe(II)-heme] and aMbn + as the products) were detected concurrently for hMbn + produced from a myoglobin solution pretreated with reducing reagents. By reference to Ea=0.9eV determined by blackbody infrared radiative dissociation for charged heme loss of ferric hMbn +, an activation energy of 1.1eV was deduced for neutral heme loss of ferrous hMbn + with n =9 and 10.

Mechanisms of H{sub 2}O desorption from amorphous solid water by 157-nm irradiation: An experimental and theoretical study

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

DeSimone, Alice J.; Crowell, Vernon D.; Sherrill, C. David

2013-10-28

The photodesorption of water molecules from amorphous solid water (ASW) by 157-nm irradiation has been examined using resonance-enhanced multiphoton ionization. The rotational temperature has been determined, by comparison with simulations, to be 425 ± 75 K. The time-of-flight spectrum of H{sub 2}O (v= 0) has been fit with a Maxwell-Boltzmann distribution with a translational temperature of 700 ± 200 K (0.12 ± 0.03 eV). H{sup +} and OH{sup +} fragment ions have been detected with non-resonant multiphoton ionization, indicating vibrationally excited parent water molecules with translational energies of 0.24 ± 0.08 eV. The cross section for water removal from ASWmore » by 7.9-eV photons near 100 K is (6.9 ± 1.8) × 10{sup −20} cm{sup 2} for >10 L H{sub 2}O exposure. Electronic structure computations have also probed the excited states of water and the mechanisms of desorption. Calculated electron attachment and detachment densities show that exciton delocalization leads to a dipole reversal state in the first singlet excited state of a model system of hexagonal water ice. Ab Initio Molecular Dynamics simulations show possible desorption of a photo-excited water molecule from this cluster, though the non-hydrogen bonded OH bond is stretched significantly before desorption. Potential energy curves of this OH stretch in the electronic excited state show a barrier to dissociation, lending credence to the dipole reversal mechanism.« less

Sequential Double lonization: The Timing of Release

NASA Astrophysics Data System (ADS)

Pfeiffer, A.

2011-05-01

The timing of electron release in strong field double ionization poses great challenges both for conceptual definition and for conducting experimental measurement. Here we present coincidence momentum measurements of the doubly charged ion and of the two electrons arising from double ionization of Argon using elliptically (close to circularly) polarized laser pulses. Based on a semi-classical model, the ionization times are calculated from the measured electron momenta across a large intensity range. Exploiting the attoclock technique we have direct access to timings on a coarse and on a fine scale, similar to the hour and the minute hand of a clock. In our attoclock, the magnitude of the electron momenta follows the envelope of the laser pulse and gives a coarse timing for the electron releases (the hour hand), while the fine timing (the minute hand) is provided by the emission angle of the electrons. The first of our findings is that due to depletion the averaged ionization time moves towards the beginning of the pulse with increasing intensity, confirming the results of Maharjan et al., and that the ion momentum distribution projected onto the minor polarization axis shows a bifurcation from a 3-peak to a 4-peak structure. This effect can be fully understood by modeling the process semi-classically in the independent electron approximation following the simple man's model. The ionization time measurement performed with the attoclock shows that the release time of the first electron is in good agreement with the semi-classical simulation performed on the basis of Sequential Double lonization (SDI), whereas the ionization of the second electron occurs significantly earlier than predicted. This observation suggests that electron correlation and other Non-Sequential Double lonization (NSDI) mechanisms may play an important role also in the case of strong field double ionization by close-to-circularly polarized laser pulses. The timing of electron release in strong field double ionization poses great challenges both for conceptual definition and for conducting experimental measurement. Here we present coincidence momentum measurements of the doubly charged ion and of the two electrons arising from double ionization of Argon using elliptically (close to circularly) polarized laser pulses. Based on a semi-classical model, the ionization times are calculated from the measured electron momenta across a large intensity range. Exploiting the attoclock technique we have direct access to timings on a coarse and on a fine scale, similar to the hour and the minute hand of a clock. In our attoclock, the magnitude of the electron momenta follows the envelope of the laser pulse and gives a coarse timing for the electron releases (the hour hand), while the fine timing (the minute hand) is provided by the emission angle of the electrons. The first of our findings is that due to depletion the averaged ionization time moves towards the beginning of the pulse with increasing intensity, confirming the results of Maharjan et al., and that the ion momentum distribution projected onto the minor polarization axis shows a bifurcation from a 3-peak to a 4-peak structure. This effect can be fully understood by modeling the process semi-classically in the independent electron approximation following the simple man's model. The ionization time measurement performed with the attoclock shows that the release time of the first electron is in good agreement with the semi-classical simulation performed on the basis of Sequential Double lonization (SDI), whereas the ionization of the second electron occurs significantly earlier than predicted. This observation suggests that electron correlation and other Non-Sequential Double lonization (NSDI) mechanisms may play an important role also in the case of strong field double ionization by close-to-circularly polarized laser pulses. In collaboration with C. Cirelli and M. Smolarski, Physics Department, ETH Zurich, 8093 Zurich, Switzerland; R. Doerner, Institut fiir Kernphysik, Johann Wolfgang Goethe Universitat, 60438 Frankfurt am Main, Germany; and U. Keller, ETH Zurich.

Investigation of the 6 p 2(3 P 0) n p Rydberg series of bismuth by multiphoton excitation

NASA Astrophysics Data System (ADS)

Bühler, B.; Cremer, C.; Gerber, G.

1985-03-01

Rydberg states of the odd-parity series 6 p 2(3 p 0) n p of BiI are excited by a three-photon process. A two-photon dissociation of Bi2 into excited atomic states followed by a one-photon absorption leads to highly excited atomic Rydberg states up to n = 32. States of the even-parity Rydberg series 6 p 2(3 p 0) nsJ=1/2, ndJ=3/2 and ndJ=5/2 are also observed. In order to avoid the background caused by ionization of the bismuth molecules we performed a two-color excitation with pulsed dye lasers. With this experiment the 6 p 2(3 p 0) npJ=3/2 Rydberg series could be resolved up to n=75. The increasing quantum defect of this series is due to a perturbing state close to the first ionization limit. By a MQDT analysis we obtain the energy of the perturbing state and a value of 58,761.68±0.1 cm-1 for the first ionization limit of atomic bismuth.

Revisiting the relaxation dynamics of isolated pyrrole

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

Montero, Raúl; Ovejas, Virginia; Fernández-Fernández, Marta

Herein, the interpretation of the femtosecond-scale temporal evolution of the pyrrole ion signal, after excitation in the 267–217 nm interval, recently published by our group [R. Montero, A. Peralta Conde, V. Ovejas, M. Fernández-Fernández, F. Castaño, J. R. Vázquez de Aldana, and A. Longarte, J. Chem. Phys.137, 064317 (2012)] is re-visited. The observation of a shift in the pyrrole{sup +} transient respect to zero delay reference, initially attributed to ultrafast dynamics on the πσ{sup *} type state (3s a{sub 1} ← π 1a{sub 2}), is demonstrated to be caused by the existence of pump + probe populated states, along themore » ionization process. The influence of these resonances in pump-prone ionization experiments, when multi-photon probes are used, and the significance of a proper zero-time reference, is discussed. The possibility of preparing the πσ{sup *} state by direct excitation is investigated by collecting 1 + 1 photoelectron spectra, at excitation wavelengths ranging from 255 to 219 nm. No conclusive evidences of ionization through this state are found.« less

Multiphoton laser ionization for energy conversion in barium vapor

NASA Astrophysics Data System (ADS)

Makdisi, Y.; Kokaj, J.; Afrousheh, K.; Mathew, J.; Nair, R.; Pichler, G.

2013-03-01

We have studied the ion detection of barium atoms in special heated ovens with a tungsten rod in the middle of the stainless steel tube. The tungsten rod was heated indirectly by the oven body heaters. A bias voltage between the cell body and the tungsten rod of 9 V was used to collect electrons, after the barium ions had been created. However, we could collect the electrons even without the bias voltage, although with ten times less efficiency. We studied the conditions for the successful bias-less thermionic signal detection using excimer/dye laser two-photon excitation of Rydberg states below and above the first ionization limit (two-photon wavelength at 475.79 nm). We employed a hot-pipe oven and heat-pipe oven (with inserted mesh) in order to generate different barium vapor distributions inside the oven. The thermionic signal increased by a factor of two under heat-pipe oven conditions.

Unified Time and Frequency Picture of Ultrafast Atomic Excitation in Strong Laser Fields

NASA Astrophysics Data System (ADS)

Zimmermann, H.; Patchkovskii, S.; Ivanov, M.; Eichmann, U.

2017-01-01

Excitation and ionization in strong laser fields lies at the heart of such diverse research directions as high-harmonic generation and spectroscopy, laser-induced diffraction imaging, emission of femtosecond electron bunches from nanotips, self-guiding, filamentation and mirrorless lasing during propagation of light in atmospheres. While extensive quantum mechanical and semiclassical calculations on strong-field ionization are well backed by sophisticated experiments, the existing scattered theoretical work aiming at a full quantitative understanding of strong-field excitation lacks experimental confirmation. Here we present experiments on strong-field excitation in both the tunneling and multiphoton regimes and their rigorous interpretation by time dependent Schrödinger equation calculations, which finally consolidates the seemingly opposing strong-field regimes with their complementary pictures. Most strikingly, we observe an unprecedented enhancement of excitation yields, which opens new possibilities in ultrafast strong-field control of Rydberg wave packet excitation and laser intensity characterization.

Second generation measurement of the electric dipole moment of the electron using trapped ThF+ ions

NASA Astrophysics Data System (ADS)

Ng, Kia Boon; Zhou, Yan; Gresh, Daniel; Cairncross, William; Grau, Matthew; Ni, Yiqi; Ye, Jun; Cornell, Eric

2016-05-01

ThF+ has been chosen as the candidate for a second generation measurement of the electric dipole moment of the electron (eEDM). Compared to the current HfF+ eEDM experiment, ThF+ has several advantages: (i) the eEDM-sensitive state (3Δ1) is the ground state, which facilitates a long coherence time; (ii) its effective electric field (38 GV/cm) is 50% larger than that of HfF+, which promises a direct increase of the eEDM sensitivity; and (iii) the ionization energy of neutral ThF is lower than its dissociation energy, which introduces greater flexibility in rotational state-selective photoionization via core-nonpenetrating Rydberg states. Here, we present progress of our experimental setup, preliminary spectroscopic data of multi-photon ionization, and discussions of new features in ion trapping, state preparation and population readout.

A Double Decarboxylation in Superfolder Green Fluorescent Protein Leads to High Contrast Photoactivation.

PubMed

Slocum, Joshua D; Webb, Lauren J

2017-07-06

A photoactivatable variant of superfolder green fluorescent protein (GFP) was created by replacing the threonine at position 203 with aspartic acid. Photoactivation by exposure of this mutant to UV light resulted in conversion of the fluorophore from the neutral to the negatively charged form, accompanied by a ∼95-fold increase in fluorescence under 488 nm excitation. Mass spectrometry before and after exposure to UV light revealed a change in mass of 88 Da, attributed to the double decarboxylation of Glu 222 and Asp 203. Kinetics studies and nonlinear power-dependence of the initial rate of photoconversion indicated that the double decarboxylation occurred via a multiphoton absorption process at 254 nm. In addition to providing a photoactivatable GFP with robust folding properties, a detailed mechanistic understanding of this double decarboxylation in GFP will lead to a better understanding of charge transfer in fluorescent proteins.

Numerical calculation of nonlinear ultrashort laser pulse propagation in transparent Kerr media

NASA Astrophysics Data System (ADS)

Arnold, Cord L.; Heisterkamp, Alexander; Ertmer, Wolfgang; Lubatschowski, Holger

2005-03-01

In the focal region of tightly focused ultrashort laser pulses, sufficient high intensities to initialize nonlinear ionization processes are easily achieved. Due to these nonlinear ionization processes, mainly multiphoton ionization and cascade ionization, free electrons are generated in the focus resulting in optical breakdown. A model including both nonlinear pulse propagation and plasma generation is used to calculate numerically the interaction of ultrashort pulses with their self-induced plasma in the vicinity of the focus. The model is based on a (3+1)-dimensional nonlinear Schroedinger equation describing the pulse propagation coupled to a system of rate equations covering the generation of free electrons. It is applicable to any transparent Kerr medium, whose linear and nonlinear optical parameters are known. Numerical calculations based on this model are used to understand nonlinear side effects, such as streak formation, occurring in addition to optical breakdown during short pulse refractive eye surgeries like fs-LASIK. Since the optical parameters of water are a good first-order approximation to those of corneal tissue, water is used as model substance. The free electron density distribution induced by focused ultrashort pulses as well as the pulses spatio-temporal behavior are studied in the low-power regime around the critical power for self-focusing.

Electron ionization of SiCl4

NASA Astrophysics Data System (ADS)

King, Simon J.; Price, Stephen D.

2011-02-01

Relative partial ionization cross sections (PICS) for the formation of fragment ions following electron ionization of SiCl4, in the electron energy range 30-200 eV, have been determined using time-of-flight mass spectrometry coupled with an ion coincidence technique. By this method, the contributions to the yield of each fragment ion from dissociative single, double, and triple ionization, are distinguished. These yields are quantified in the form of relative precursor-specific PICS, which are reported here for the first time for SiCl4. For the formation of singly charged ionic fragments, the low-energy maxima appearing in the PICS curves are due to contributions from single ionization involving predominantly indirect ionization processes, while contributions to the yields of these ions at higher electron energies are often dominated by dissociative double ionization. Our data, in the reduced form of relative PICS, are shown to be in good agreement with a previous determination of the PICS of SiCl4. Only for the formation of doubly charged fragment ions are the current relative PICS values lower than those measured in a previous study, although both datasets agree within combined error limits. The relative PICS data presented here include the first quantitative measurements of the formation of Cl2+ fragment ions and of the formation of ion pairs via dissociative double ionization. The peaks appearing in the 2D ion coincidence data are analyzed to provide further information concerning the mechanism and energetics of the charge-separating dissociations of SiCl42+. The lowest energy dicationic precursor state, leading to SiCl3+ + Cl+ formation, lies 27.4 ± 0.3 eV above the ground state of SiCl4 and is in close agreement with a calculated value of the adiabatic double ionization energy (27.3 eV).

Electron ionization of SiCl4.

PubMed

King, Simon J; Price, Stephen D

2011-02-21

Relative partial ionization cross sections (PICS) for the formation of fragment ions following electron ionization of SiCl(4), in the electron energy range 30-200 eV, have been determined using time-of-flight mass spectrometry coupled with an ion coincidence technique. By this method, the contributions to the yield of each fragment ion from dissociative single, double, and triple ionization, are distinguished. These yields are quantified in the form of relative precursor-specific PICS, which are reported here for the first time for SiCl(4). For the formation of singly charged ionic fragments, the low-energy maxima appearing in the PICS curves are due to contributions from single ionization involving predominantly indirect ionization processes, while contributions to the yields of these ions at higher electron energies are often dominated by dissociative double ionization. Our data, in the reduced form of relative PICS, are shown to be in good agreement with a previous determination of the PICS of SiCl(4). Only for the formation of doubly charged fragment ions are the current relative PICS values lower than those measured in a previous study, although both datasets agree within combined error limits. The relative PICS data presented here include the first quantitative measurements of the formation of Cl(2) (+) fragment ions and of the formation of ion pairs via dissociative double ionization. The peaks appearing in the 2D ion coincidence data are analyzed to provide further information concerning the mechanism and energetics of the charge-separating dissociations of SiCl(4) (2+). The lowest energy dicationic precursor state, leading to SiCl(3) (+) + Cl(+) formation, lies 27.4 ± 0.3 eV above the ground state of SiCl(4) and is in close agreement with a calculated value of the adiabatic double ionization energy (27.3 eV).

Fast monitoring of motor exhaust components by resonant multi-photon ionisation and time-of-flight mass spectrometry

NASA Astrophysics Data System (ADS)

Franzen, Jochen; Frey, Rüdiger; Nagel, Holger

1995-03-01

A new analytical procedure is provided by the combination of two types of spectroscopy. Resonant ionization of selected compounds by multiphoton ionization is based on results of absorption spectroscopy for the compound molecules of interest and time-of-flight mass spectrometry serves for the unambigious detection of these compounds. An interesting application of this method is the fast exhaust gas analysis. In the development of future combustion engines, the management of dynamic motor processes becomes predominant because by more than 90 % of all the dangerous exhaust pollutions are produced in instationary motor phases such as fast speed or load changes. The investigation of dynamic processes however, requires fast analytical procedures with millisecond time resolution together with the capability to measure individual components in a very complex gas mixture The objectives for a development project of such an instrument were set by the Research Association for Combustion Engines (Forschungsvereinigung Verbrennungskraftmaschinen, FVV, Germany): Up to ten substances should be monitored synchroneously with a time resolution of about 10 milliseconds, with concentration limits of 1 part per million and with a precision better than 10 % relative standard deviation. Such a laser mass spectrometer for fast multi-component automotive exhaust analyses has been developed in a joint research project by Bruker-Franzen Analytik GmbH, Dornier GmbH and the Technical University of Munich. The system has been applied at a motor test facility to investigate the emissions of the aromatic hydrocarbons benzene, toluene and xylene, of nitric oxide and acetaldehyde in stationary and dynamic engine operation. These measurements demonstrate that strong emission of these pollutants takes place at instationary engine operation and in particular that these compounds are emitted at different times, giving new information about the processes in the combustion chamber and in the exhaust pipe.

Double ionization of nitrogen molecules in orthogonal two-color femtosecond laser fields

NASA Astrophysics Data System (ADS)

Song, Qiying; Li, Hui; Wang, Junping; Lu, Peifen; Gong, Xiaochun; Ji, Qinying; Lin, Kang; Zhang, Wenbin; Ma, Junyang; Li, Hanxiao; Zeng, Heping; He, Feng; Wu, Jian

2018-04-01

Double ionization of nitrogen molecules in orthogonally polarized two-color femtosecond laser fields is investigated by varying the relative intensity between the fundamental wave (FW) and its second harmonic (SH) components. The yield ratios of the double ionization channels, i.e., the non-dissociative {{{{N}}}2}2+ and Coulomb exploded (N+, N+), to the singly charged N2 + channel exhibit distinct dependences on the relative strength between the FW and SH fields. As the intensity ratio of SH to FW increases, the yield ratio of (N+, N+)/N2 + gradually increases, while the ratio of {{{{N}}}2}2+/N2 + first descends and then increases constituting a valley shape which is similar to the behavior of Ar2+/Ar+ observed in the same experimental condition. Based on the classical trajectory simulations, we found that the different characteristics of the two doubly ionized channels stem from two mechanisms, i.e., the {{{{N}}}2}2+ is mostly accessed by the (e, 2e) impact ionization while the recollision-induced excitation with subsequent ionization plays an important role in producing the (N+, N+) channel.

Enhanced one-photon double ionization of atoms and molecules in an environment of different species.

PubMed

Stumpf, V; Kryzhevoi, N V; Gokhberg, K; Cederbaum, L S

2014-05-16

The correlated nature of electronic states in atoms and molecules is manifested in the simultaneous emission of two electrons after absorption of a single photon close to the respective threshold. Numerous observations in atoms and small molecules demonstrate that the double ionization efficiency close to threshold is rather small. In this Letter we show that this efficiency can be dramatically enhanced in the environment. To be specific, we concentrate on the case where the species in question has one or several He atoms as neighbors. The enhancement is achieved by an indirect process, where a He atom of the environment absorbs a photon and the resulting He(+) cation is neutralized fast by a process known as electron transfer mediated decay, producing thereby doubly ionized species. The enhancement of the double ionization is demonstrated in detail for the example of the Mg · He cluster. We show that the double ionization cross section of Mg becomes 3 orders of magnitude larger than the respective cross section of the isolated Mg atom. The impact of more neighbors is discussed and the extension to other species and environments is addressed.

Theoretical Studies Relating to the Interaction of Radiation with Matter

DTIC Science & Technology

1989-09-15

and Heisenberg picture calculations of resonance fluorescence in the presence of a strong field. Again, the Schrodinger calculation is quite...discussed in Sec. VIII. numerous effects have been discussed assuming fluctuat- ing radiation fields (resonant fluorescence , double reso- nance, multiphoton...tered at t12 =0. The peak has temporal width It 2 1 = rcl2 and, moreover, for fully correlated pulses (0) = 1) there is FIG. 6. Signal of order n = 1 as a

Structural characterization of arginine-vasopressin and lysine-vasopressin by Fourier- transform ion cyclotron resonance mass spectrometry and infrared multiphoton dissociation.

PubMed

Bianco, Giuliana; Battista, Fabio; Buchicchio, Alessandro; Amarena, Concetta G; Schmitt-Kopplin, Philippe; Guerrieri, Antonio

2015-01-01

Arginine-vasopressin (AVP) and lysine-vasopressin (LVP) were analyzed by reversed-phase liquid chromatography/mass spectrometry (LC-MS) using Fourier-transform ion cyclotron resonance (FT-ICR) mass spectrometry (MS) electrospray ionization (ESI) in the positive ion mode. LVP and AVP exhibited the protonated adduct [M+H](+) as the predominant ion at m/z 1056.43965 and at m/z 1084.44561, respectively. Infrared multiphoton dissociation (IRMPD), using a CO(2) laser source at a wavelength of 10.6 μm, was applied to protonated vasopressin molecules. The IRMPD mass spectra presented abundant mass fragments essential for a complete structural information. Several fragment ions, shared between two target molecules, are discussed in detail. Some previously unpublished fragments were identified unambiguously utilizing the high resolution and accurate mass information provided by the FT-ICR mass spectrometer. The opening of the disulfide loop and the cleavage of the peptide bonds within the ring were observed even under low-energy fragmentation conditions. Coupling the high-performance FT-ICR mass spectrometer with IRMPD as a contemporary fragmentation technique proved to be very promising for the structural characterization of vasopressin.

Electron-Impact Ionization and Dissociative Ionization of Biomolecules

NASA Technical Reports Server (NTRS)

Huo, Winifred M.; Chaban, Galina M.; Dateo, Christopher E.

2006-01-01

It is well recognized that secondary electrons play an important role in radiation damage to humans. Particularly important is the damage of DNA by electrons, potentially leading to mutagenesis. Molecular-level study of electron interaction with DNA provides information on the damage pathways and dominant mechanisms. Our study of electron-impact ionization of DNA fragments uses the improved binary-encounter dipole model and covers DNA bases, sugar phosphate backbone, and nucleotides. An additivity principle is observed. For example, the sum of the ionization cross sections of the separate deoxyribose and phosphate fragments is in close agreement with the C3(sup prime)- and C5 (sup prime)-deoxyribose-phospate cross sections, differing by less than 5%. Investigation of tandem double lesion initiated by electron-impact dissociative ionization of guanine, followed by proton reaction with the cytosine in the Watson-Crick pair, is currently being studied to see if tandem double lesion can be initiated by electron impact. Up to now only OH-induced tandem double lesion has been studied.

Nonsequential double ionization with mid-infrared laser fields

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

Li, Ying -Bin; Wang, Xu; Yu, Ben -Hai

Using a full-dimensional Monte Carlo classical ensemble method, we present a theoretical study of atomic nonsequential double ionization (NSDI) with mid-infrared laser fields, and compare with results from near-infrared laser fields. Unlike single-electron strong-field processes, double ionization shows complex and unexpected interplays between the returning electron and its parent ion core. As a result of these interplays, NSDI for mid-IR fields is dominated by second-returning electron trajectories, instead of first-returning trajectories for near-IR fields. Here, some complex NSDI channels commonly happen with near-IR fields, such as the recollision-excitation-with-subsequent-ionization (RESI) channel, are virtually shut down by mid-IR fields. Besides, the finalmore » energies of the two electrons can be extremely unequal, leading to novel e-e momentum correlation spectra that can be measured experimentally.« less

Nonsequential double ionization with mid-infrared laser fields

DOE PAGES

Li, Ying -Bin; Wang, Xu; Yu, Ben -Hai; ...

2016-11-18

Using a full-dimensional Monte Carlo classical ensemble method, we present a theoretical study of atomic nonsequential double ionization (NSDI) with mid-infrared laser fields, and compare with results from near-infrared laser fields. Unlike single-electron strong-field processes, double ionization shows complex and unexpected interplays between the returning electron and its parent ion core. As a result of these interplays, NSDI for mid-IR fields is dominated by second-returning electron trajectories, instead of first-returning trajectories for near-IR fields. Here, some complex NSDI channels commonly happen with near-IR fields, such as the recollision-excitation-with-subsequent-ionization (RESI) channel, are virtually shut down by mid-IR fields. Besides, the finalmore » energies of the two electrons can be extremely unequal, leading to novel e-e momentum correlation spectra that can be measured experimentally.« less

Fast detection of narcotics by single photon ionization mass spectrometry and laser ion mobility spectrometry

NASA Astrophysics Data System (ADS)

Laudien, Robert; Schultze, Rainer; Wieser, Jochen

2010-10-01

In this contribution two analytical devices for the fast detection of security-relevant substances like narcotics and explosives are presented. One system is based on an ion trap mass spectrometer (ITMS) with single photon ionization (SPI). This soft ionization technique, unlike electron impact ionization (EI), reduces unwanted fragment ions in the mass spectra allowing the clear determination of characteristic (usually molecular) ions. Their enrichment in the ion trap and identification by tandem MS investigations (MS/MS) enables the detection of the target substances in complex matrices at low concentrations without time-consuming sample preparation. For SPI an electron beam pumped excimer light source of own fabrication (E-Lux) is used. The SPI-ITMS system was characterized by the analytical study of different drugs like cannabis, heroin, cocaine, amphetamines, and some precursors. Additionally, it was successfully tested on-site in a closed illegal drug laboratory, where low quantities of MDMA could be directly detected in samples from floors, walls and lab equipments. The second analytical system is based on an ion mobility (IM) spectrometer with resonant multiphoton ionization (REMPI). With the frequency quadrupled Nd:YAG laser (266 nm), used for ionization, a selective and sensitive detection of aromatic compounds is possible. By application of suited aromatic dopants, in addition, also non-aromatic polar compounds are accessible by ion molecule reactions like proton transfer or complex formation. Selected drug precursors could be successfully detected with this device as well, qualifying it to a lower-priced alternative or useful supplement of the SPI-ITMS system for security analysis.

Rotational spectroscopy with an optical centrifuge.

PubMed

Korobenko, Aleksey; Milner, Alexander A; Hepburn, John W; Milner, Valery

2014-03-07

We demonstrate a new spectroscopic method for studying electronic transitions in molecules with extremely broad range of angular momentum. We employ an optical centrifuge to create narrow rotational wave packets in the ground electronic state of (16)O2. Using the technique of resonance-enhanced multi-photon ionization, we record the spectrum of multiple ro-vibrational transitions between X(3)Σg(-) and C(3)Πg electronic manifolds of oxygen. Direct control of rotational excitation, extending to rotational quantum numbers as high as N ≳ 120, enables us to interpret the complex structure of rotational spectra of C(3)Πg beyond thermally accessible levels.

A method of extracting speed-dependent vector correlations from 2 + 1 REMPI ion images.

PubMed

Wei, Wei; Wallace, Colin J; Grubb, Michael P; North, Simon W

2017-07-07

We present analytical expressions for extracting Dixon's bipolar moments in the semi-classical limit from experimental anisotropy parameters of sliced or reconstructed non-sliced images. The current method focuses on images generated by 2 + 1 REMPI (Resonance Enhanced Multi-photon Ionization) and is a necessary extension of our previously published 1 + 1 REMPI equations. Two approaches for applying the new equations, direct inversion and forward convolution, are presented. As demonstration of the new method, bipolar moments were extracted from images of carbonyl sulfide (OCS) photodissociation at 230 nm and NO 2 photodissociation at 355 nm, and the results are consistent with previous publications.

Non-volatile analysis in fruits by laser resonant ionization spectrometry: application to resveratrol (3,5,4'-trihydroxystilbene) in grapes

NASA Astrophysics Data System (ADS)

Montero, C.; Orea, J. M.; Soledad Muñoz, M.; Lobo, R. F. M.; González Ureña, A.

A laser desorption (LD) coupled with resonance-enhanced multiphoton ionisation (REMPI) and time-of-flight mass spectrometry (TOFMS) technique for non-volatile trace analysis compounds is presented. Essential features are: (a) an enhanced desorption yield due to the mixing of metal powder with the analyte in the sample preparation, (b) a high resolution, great sensitivity and low detection limit due to laser resonant ionisation and mass spectrometry detection. Application to resveratrol content in grapes demonstrated the capability of the analytical method with a sensitivity of 0.2 pg per single laser shot and a detection limit of 5 ppb.

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

Fu, H.B.; Hu, Y.J.; Bernstein, E.R.

Small methanol clusters are formed by expanding a mixture of methanol vapor seeded in helium and are detected using vacuum UV (vuv) (118 nm) single-photon ionization/linear time-of-flight mass spectrometer (TOFMS). Protonated cluster ions, (CH{sub 3}OH){sub n-1}H{sup +} (n=2-8), formed through intracluster ion-molecule reactions following ionization, essentially correlate to the neutral clusters, (CH{sub 3}OH){sub n}, in the present study using 118 nm light as the ionization source. Both experimental and Born-Haber calculational results clarify that not enough excess energy is released into protonated cluster ions to initiate further fragmentation in the time scale appropriate for linear TOFMS. Size-specific spectra for (CH{submore » 3}OH){sub n} (n=4 to 8) clusters in the OH stretch fundamental region are recorded by IR+vuv (118 nm) nonresonant ion-dip spectroscopy through the detection chain of IR multiphoton predissociation and subsequent vuv single-photon ionization. The general structures and gross features of these cluster spectra are consistent with previous theoretical calculations. The lowest-energy peak contributed to each cluster spectrum is redshifted with increasing cluster size from n=4 to 8, and limits near {approx}3220 cm{sup -1} in the heptamer and octamer. Moreover, IR+vuv nonresonant ionization detected spectroscopy is employed to study the OH stretch first overtone of the methanol monomer. The rotational temperature of the clusters is estimated to be at least 50 K based on the simulation of the monomer rotational envelope under clustering conditions.« less

Femtosecond laser three-dimensional micro- and nanofabrication

NASA Astrophysics Data System (ADS)

Sugioka, Koji; Cheng, Ya

2014-12-01

The rapid development of the femtosecond laser has revolutionized materials processing due to its unique characteristics of ultrashort pulse width and extremely high peak intensity. The short pulse width suppresses the formation of a heat-affected zone, which is vital for ultrahigh precision fabrication, whereas the high peak intensity allows nonlinear interactions such as multiphoton absorption and tunneling ionization to be induced in transparent materials, which provides versatility in terms of the materials that can be processed. More interestingly, irradiation with tightly focused femtosecond laser pulses inside transparent materials makes three-dimensional (3D) micro- and nanofabrication available due to efficient confinement of the nonlinear interactions within the focal volume. Additive manufacturing (stereolithography) based on multiphoton absorption (two-photon polymerization) enables the fabrication of 3D polymer micro- and nanostructures for photonic devices, micro- and nanomachines, and microfluidic devices, and has applications for biomedical and tissue engineering. Subtractive manufacturing based on internal modification and fabrication can realize the direct fabrication of 3D microfluidics, micromechanics, microelectronics, and photonic microcomponents in glass. These microcomponents can be easily integrated in a single glass microchip by a simple procedure using a femtosecond laser to realize more functional microdevices, such as optofluidics and integrated photonic microdevices. The highly localized multiphoton absorption of a tightly focused femtosecond laser in glass can also induce strong absorption only at the interface of two closely stacked glass substrates. Consequently, glass bonding can be performed based on fusion welding with femtosecond laser irradiation, which provides the potential for applications in electronics, optics, microelectromechanical systems, medical devices, microfluidic devices, and small satellites. This review paper describes the concepts and principles of femtosecond laser 3D micro- and nanofabrication and presents a comprehensive review on the state-of-the-art, applications, and the future prospects of this technology.

Femtosecond laser three-dimensional micro- and nanofabrication

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

Sugioka, Koji, E-mail: ksugioka@riken.jp; Cheng, Ya, E-mail: ya.cheng@siom.ac.cn

2014-12-15

The rapid development of the femtosecond laser has revolutionized materials processing due to its unique characteristics of ultrashort pulse width and extremely high peak intensity. The short pulse width suppresses the formation of a heat-affected zone, which is vital for ultrahigh precision fabrication, whereas the high peak intensity allows nonlinear interactions such as multiphoton absorption and tunneling ionization to be induced in transparent materials, which provides versatility in terms of the materials that can be processed. More interestingly, irradiation with tightly focused femtosecond laser pulses inside transparent materials makes three-dimensional (3D) micro- and nanofabrication available due to efficient confinement ofmore » the nonlinear interactions within the focal volume. Additive manufacturing (stereolithography) based on multiphoton absorption (two-photon polymerization) enables the fabrication of 3D polymer micro- and nanostructures for photonic devices, micro- and nanomachines, and microfluidic devices, and has applications for biomedical and tissue engineering. Subtractive manufacturing based on internal modification and fabrication can realize the direct fabrication of 3D microfluidics, micromechanics, microelectronics, and photonic microcomponents in glass. These microcomponents can be easily integrated in a single glass microchip by a simple procedure using a femtosecond laser to realize more functional microdevices, such as optofluidics and integrated photonic microdevices. The highly localized multiphoton absorption of a tightly focused femtosecond laser in glass can also induce strong absorption only at the interface of two closely stacked glass substrates. Consequently, glass bonding can be performed based on fusion welding with femtosecond laser irradiation, which provides the potential for applications in electronics, optics, microelectromechanical systems, medical devices, microfluidic devices, and small satellites. This review paper describes the concepts and principles of femtosecond laser 3D micro- and nanofabrication and presents a comprehensive review on the state-of-the-art, applications, and the future prospects of this technology.« less

An investigation on 800 nm femtosecond laser ablation of K9 glass in air and vacuum

NASA Astrophysics Data System (ADS)

Xu, Shi-zhen; Yao, Cai-zhen; Dou, Hong-qiang; Liao, Wei; Li, Xiao-yang; Ding, Ren-jie; Zhang, Li-juan; Liu, Hao; Yuan, Xiao-dong; Zu, Xiao-tao

2017-06-01

Ablation rates of K9 glass were studied as a function of femtosecond laser fluences. The central wavelength was 800 nm, and pulse durations of 35 fs and 500 fs in air and vacuum were employed. Ablation thresholds of 0.42 J/cm2 and 2.1 J/cm2 were obtained at 35 fs and 500 fs, respectively, which were independent with the ambient conditions and depend on the incident pulse numbers due to incubation effects. The ablation rate of 35 fs pulse laser increased with the increasing of laser fluence in vacuum, while in air condition, it slowly increased to a plateau at high fluence. The ablation rate of 500 fs pulse laser showed an increase at low fluence and a slow drop of ablation rate was observed at high fluence in air and vacuum, which may due to the strong defocusing effects associated with the non-equilibrium ionization of air, and/or the shielding effects of conduction band electrons (CBEs) produced by multi-photon ionization and impact ionization in K9 glass surface. The typical ablation morphologies, e.g. smooth zone and laser-induced periodic surface structures (LIPSS) were also presented and illustrated.

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

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

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

Calculation of fully differential cross sections for the near threshold double ionization of helium atoms

NASA Astrophysics Data System (ADS)

Singh, Prithvi; Purohit, Ghanshyam; Dorn, Alexander; Ren, Xueguang; Patidar, Vinod

2016-01-01

Fully differential cross sectional (FDCS) results are reported for the electron-impact double ionization of helium atoms at 5 and 27 eV excess energy. The present attempt to calculate the FDCS in the second Born approximation and treating the postcollision interaction is helpful to analyze the measurements of Ren et al (2008 Phys. Rev. Lett. 101 093201) and Durr et al (2007 Phys. Rev. Lett. 98 193201). The second-order processes and postcollision interaction have been found to be significant in describing the trends of the FDCS. More theoretical effort is required to describe the collision dynamics of electron-impact double ionization of helium atoms at near threshold.

Attosecond Electron Correlation Dynamics in Double Ionization of Benzene Probed with Two-Electron Angular Streaking

NASA Astrophysics Data System (ADS)

Winney, Alexander H.; Lee, Suk Kyoung; Lin, Yun Fei; Liao, Qing; Adhikari, Pradip; Basnayake, Gihan; Schlegel, H. Bernhard; Li, Wen

2017-09-01

With a novel three-dimensional electron-electron coincidence imaging technique and two-electron angular streaking method, we show that the emission time delay between two electrons can be measured from tens of attoseconds to more than 1 fs. Surprisingly, in benzene, the double ionization rate decays as the time delay between the first and second electron emission increases during the first 500 as. This is further supported by the decay of the Coulomb repulsion in the direction perpendicular to the laser polarization. This result reveals that laser-induced electron correlation plays a major role in strong field double ionization of benzene driven by a nearly circularly polarized field.

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

Watanabe, N.; Takahashi, M.; Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, Sendai 980-8577

The double processes of He in electron-impact ionization, single ionization with simultaneous excitation and double ionization, have been studied at large momentum transfer using an energy- and momentum-dispersive binary (e,2e) spectrometer. The experiment has been performed at an impact energy of 2080 eV in the symmetric noncoplanar geometry. In this way we have achieved a large momentum transfer of 9 a.u., a value that has never been realized so far for the study on double ionization. The measured (e,2e) and (e,3-1e) cross sections for transitions to the n=2 excited state of He{sup +} and to doubly ionized He{sup 2+} aremore » presented as normalized intensities relative to that to the n=1 ground state of He{sup +}. The results are compared with first-order plane-wave impulse approximation (PWIA) calculations using various He ground-state wave functions. It is shown that shapes of the momentum-dependent (e,2e) and (e,3-1e) cross sections are well reproduced by the PWIA calculations only when highly correlated wave functions are employed. However, noticeable discrepancies between experiment and theory remain in magnitude for both the double processes, suggesting the importance of higher-order effects under the experimental conditions examined as well as of acquiring more complete knowledge of electron correlation in the target.« less

Transition-matrix theory for two-photon ionization of rare-gas atoms and isoelectronic ions with application to argon

NASA Astrophysics Data System (ADS)

Starace, Anthony F.; Jiang, Tsin-Fu

1987-08-01

A transition-matrix theory for two-photon ionization processes in rare-gas atoms or isoelectronic ions is presented. Uncoupled ordinary differential equations are obtained for the radial functions needed to calculate the two-photon transition amplitude. The implications of these equations are discussed in detail. In particular, the role of correlations involving virtually excited electron pairs, which are known to be essential to the description of single-photon processes, is examined for multiphoton ionization processes. Additionally, electron scattering interactions between two electron-hole pairs are introduced into our transition amplitude in the boson approximation since these have been found important in two-photon ionization of xenon by L'Huillier and Wendin [J. Phys. B 20, L37 (1987)]. Application of our theory is made to two-photon ionization of the 3p subshell of argon below the one-photon ionization threshold. Our results are compared to previous calculations of McGuire [Phys. Rev. A 24, 835 (1981)], of Moccia, Rahman, and Rizzo [J. Phys. B 16, 2737 (1983)], and of Pindzola and Kelly [Phys. Rev. A 11, 1543 (1975)]. Results are presented for both circularly and linearly polarized photons. Among our findings are, firstly, that the electron scattering interactions, which have not been included in previous calculations for argon, produce a substantial reduction in the two-photon single-ionization cross section below the one-photon ionization threshold, which is in agreement with findings of L'Huillier and Wendin for xenon. Secondly, we find that de-excitation of virtually excited electron pairs by absorption of a photon is important for describing the interaction of the atom with the photon field, as in the case of single-photon ionization processes, but that further excitation of virtually excited electron pairs by the photon field has completely negligible effects, indicating a major simplification of the theory for higher-order absorption processes.

Far-UV photochemical bond cleavage of n-amyl nitrite: bypassing a repulsive surface.

PubMed

Minitti, Michael P; Zhang, Yao; Rosenberg, Martin; Brogaard, Rasmus Y; Deb, Sanghamitra; Sølling, Theis I; Weber, Peter M

2012-01-19

We have investigated the deep-UV photoinduced, homolytic bond cleavage of amyl nitrite to form NO and pentoxy radicals. One-color multiphoton ionization with ultrashort laser pulses through the S(2) state resonance gives rise to photoelectron spectra that reflect ionization from the S(1) state. Time-resolved pump-probe photoionization measurements show that upon excitation at 207 nm, the generation of NO in the v = 2 state is delayed, with a rise time of 283 (16) fs. The time-resolved mass spectrum shows the NO to be expelled with a kinetic energy of 1.0 eV, which is consistent with dissociation on the S(1) state potential energy surface. Combined, these observations show that the first step of the dissociation reaction involves an internal conversion from the S(2) to the S(1) state, which is followed by the ejection of the NO radical on the predissociative S(1) state potential energy surface.

Facile time-of-flight methods for characterizing pulsed superfluid helium droplet beams

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

He, Yunteng; Zhang, Jie; Li, Yang

2015-08-15

We present two facile time-of-flight (TOF) methods of detecting superfluid helium droplets and droplets with neutral dopants. Without an electron gun and with only a heated filament and pulsed electrodes, the electron impact ionization TOF mass spectrometer can resolve ionized helium clusters such as He{sub 2}{sup +} and He{sub 4}{sup +}, which are signatures of superfluid helium droplets. Without ionizing any helium atoms, multiphoton non-resonant laser ionization of CCl{sub 4} doped in superfluid helium droplets at 266 nm generates complex cluster ions of dopant fragments with helium atoms, including (He){sub n}C{sup +}, (He){sub n}Cl{sup +}, and (He){sub n}CCl{sup +}. Usingmore » both methods, we have characterized our cryogenic pulsed valve—the Even-Lavie valve. We have observed a primary pulse with larger helium droplets traveling at a slower speed and a rebound pulse with smaller droplets at a faster speed. In addition, the pickup efficiency of dopant is higher for the primary pulse when the nozzle temperature is higher than 13 K, and the total time duration of the doped droplet pulse is only on the order of 20 μs. These results stress the importance of fast and easy characterization of the droplet beam for sensitive measurements such as electron diffraction of doped droplets.« less

A new high intensity and short-pulse molecular beam valve

NASA Astrophysics Data System (ADS)

Yan, B.; Claus, P. F. H.; van Oorschot, B. G. M.; Gerritsen, L.; Eppink, A. T. J. B.; van de Meerakker, S. Y. T.; Parker, D. H.

2013-02-01

In this paper, we report on the design and performance of a new home-built pulsed gas valve, which we refer to as the Nijmegen Pulsed Valve (NPV). The main output characteristics include a short pulse width (as short as 20 μs) combined with operating rates up to 30 Hz. The operation principle of the NPV is based on the Lorentz force created by a pulsed current passing through an aluminum strip located within a magnetic field, which opens the nozzle periodically. The amplitude of displacement of the opening mechanism is sufficient to allow the use of nozzles with up to 1.0 mm diameter. To investigate the performance of the valve, several characterizations were performed with different experimental methods. First, a fast ionization gauge was used to measure the beam intensity of the free jet emanating from the NPV. We compare free jets from the NPV with those from several other pulsed valves in current use in our laboratory. Results showed that a high intensity and short pulse-length beam could be generated by the new valve. Second, the NPV was tested in combination with a skimmer, where resonance enhanced multiphoton ionization combined with velocity map imaging was used to show that the NPV was able to produce a pulsed molecular beam with short pulse duration (˜20 μs using 0.1% NO/He at 6 bars) and low rotational temperature (˜1 K using 0.5% NO/Ar at 6 bars). Third, a novel two-point pump-probe method was employed which we label double delay scan. This method allows a full kinematic characterization of the molecular beam, including accurate speed ratios at different temporal positions. It was found that the speed ratio was maximum (S = 50 using 0.1% NO/He at 3 bars) at the peak position of the molecular beam and decreased when it was on the leading or falling edge.

Neutron-Impact Ionization of H and He

NASA Astrophysics Data System (ADS)

Lee, T.-G.; Ciappina, M. F.; Robicheaux, F.; Pindzola, M. S.

2014-05-01

Perturbative distorted-wave and non-perturbative close-coupling methods are used to study neutron-impact ionization of H and He. For single ionization of H, we find excellent agreement between the distorted-wave and close-coupling results at all incident energies. For double ionization of He, we find poor agreement between the distorted-wave and close-coupling results, except at the highest incident energies. We present the ratio of double to single ionization for He as a guide to experimental checks of theory at low energies and experimental confirmation of the rapid rise of the ratio at high energies. This work was supported in part by grants from NSF and US DoE. Computational work was carried out at NERSC in Oakland, California, NICS in Knoxville, Tennessee, and OLCF in Oak Ridge, Tennessee.

Ionizing radiation, ion transports, and radioresistance of cancer cells

PubMed Central

Huber, Stephan M.; Butz, Lena; Stegen, Benjamin; Klumpp, Dominik; Braun, Norbert; Ruth, Peter; Eckert, Franziska

2013-01-01

The standard treatment of many tumor entities comprises fractionated radiation therapy which applies ionizing radiation to the tumor-bearing target volume. Ionizing radiation causes double-strand breaks in the DNA backbone that result in cell death if the number of DNA double-strand breaks exceeds the DNA repair capacity of the tumor cell. Ionizing radiation reportedly does not only act on the DNA in the nucleus but also on the plasma membrane. In particular, ionizing radiation-induced modifications of ion channels and transporters have been reported. Importantly, these altered transports seem to contribute to the survival of the irradiated tumor cells. The present review article summarizes our current knowledge on the underlying mechanisms and introduces strategies to radiosensitize tumor cells by targeting plasma membrane ion transports. PMID:23966948

Upstream ionization instability associated with a current-free double layer.

PubMed

Aanesland, A; Charles, C; Lieberman, M A; Boswell, R W

2006-08-18

A low frequency instability has been observed using various electrostatic probes in a low-pressure expanding helicon plasma. The instability is associated with the presence of a current-free double layer (DL). The frequency of the instability increases linearly with the potential drop of the DL, and simultaneous measurements show their coexistence. A theory for an upstream ionization instability has been developed, which shows that electrons accelerated through the DL increase the ionization upstream and are responsible for the observed instability. The theory is in good agreement with the experimental results.

Propagation of intense short laser pulses in the atmosphere.

PubMed

Sprangle, P; Peñano, J R; Hafizi, B

2002-10-01

The propagation of short, intense laser pulses in the atmosphere is investigated theoretically and numerically. A set of three-dimensional (3D), nonlinear propagation equations is derived, which includes the effects of dispersion, nonlinear self-focusing, stimulated molecular Raman scattering, multiphoton and tunneling ionization, energy depletion due to ionization, relativistic focusing, and ponderomotively excited plasma wakefields. The instantaneous frequency spread along a laser pulse in air, which develops due to various nonlinear effects, is analyzed and discussed. Coupled equations for the power, spot size, and electron density are derived for an intense ionizing laser pulse. From these equations we obtain an equilibrium for a single optical-plasma filament, which involves a balancing between diffraction, nonlinear self-focusing, and plasma defocusing. The equilibrium is shown to require a specific distribution of power along the filament. It is found that in the presence of ionization a self-guided optical filament is not realizable. A method for generating a remote spark in the atmosphere is proposed, which utilizes the dispersive and nonlinear properties of air to cause a low-intensity chirped laser pulse to compress both longitudinally and transversely. For optimally chosen parameters, we find that the transverse and longitudinal focal lengths can be made to coincide, resulting in rapid intensity increase, ionization, and white light generation in a localized region far from the source. Coupled equations for the laser spot size and pulse duration are derived, which can describe the focusing and compression process in the low-intensity regime. More general examples involving beam focusing, compression, ionization, and white light generation near the focal region are studied by numerically solving the full set of 3D, nonlinear propagation equations.

A High Pressure Pulsed Expansion Valve for Gases, Liquids, and Supercritical Fluids

NASA Astrophysics Data System (ADS)

Köster, C.; Grotemeyer, J.; Schlag, E. W.

1990-12-01

A novel design of a pulsed valve for coupling chromatographic techniques with gaseous and liquid mobile phases to a time-of-flight mass spectrometer with multiphoton ionization (MUPI) is presented. The valve can be operated in low pressure regions ( <10 bar) up to temperatures of 350 °C and at higher pressures (300 bar) up to temperatures of 200 °C. Pulse widths lower than 100 μs could be measured. First results demonstrate the ability of interfacing of liquid chromatography to MUPI-mass spectrometry. Additional coupling of CO2-laser desorption to the valve allows the interface to be used for mass spectrometric measurements of nonvolatile biomolecules.

Production of a beam of highly vibrationally excited CO using perturbations.

PubMed

Bartels, Nils; Schäfer, Tim; Hühnert, Jens; Field, Robert W; Wodtke, Alec M

2012-06-07

An intense molecular beam of CO (X(1)Σ(+)) in high vibrational states (v = 17, 18) was produced by a new approach that we call PUMP - PUMP - PERTURB and DUMP. The basic idea is to access high vibrational states of CO e(3)Σ(-) via a two-photon doubly resonant transition that is perturbed by the A(1)Π state. DUMP -ing from this mixed (predominantly triplet) state allows access to high vibrational levels of CO (X(1)Σ(+)). The success of the approach, which avoids the use of vacuum UV radiation in any of the excitation steps, is proven by laser induced fluorescence and resonance enhanced multi-photon ionization spectroscopy.

Production of a beam of highly vibrationally excited CO using perturbations

NASA Astrophysics Data System (ADS)

Bartels, Nils; Schäfer, Tim; Hühnert, Jens; Field, Robert W.; Wodtke, Alec M.

2012-06-01

An intense molecular beam of CO (X1Σ+) in high vibrational states (v = 17, 18) was produced by a new approach that we call PUMP - PUMP - PERTURB and DUMP. The basic idea is to access high vibrational states of CO e3Σ- via a two-photon doubly resonant transition that is perturbed by the A1Π state. DUMP -ing from this mixed (predominantly triplet) state allows access to high vibrational levels of CO (X1Σ+). The success of the approach, which avoids the use of vacuum UV radiation in any of the excitation steps, is proven by laser induced fluorescence and resonance enhanced multi-photon ionization spectroscopy.

Surface Temperature Dependence of Hydrogen Ortho-Para Conversion on Amorphous Solid Water.

PubMed

Ueta, Hirokazu; Watanabe, Naoki; Hama, Tetsuya; Kouchi, Akira

2016-06-24

The surface temperature dependence of the ortho-to-para conversion of H_{2} on amorphous solid water is first reported. A combination of photostimulated desorption and resonance-enhanced multiphoton ionization techniques allowed us to sensitively probe the conversion on the surface of amorphous solid water at temperatures of 9.2-16 K. Within a narrow temperature window of 8 K, the conversion time steeply varied from ∼4.1×10^{3} to ∼6.4×10^{2}  s. The observed temperature dependence is discussed in the context of previously suggested models and the energy dissipation process. The two-phonon process most likely dominates the conversion rate at low temperatures.

Spatially resolved organic analysis of the Allende meteorite

NASA Technical Reports Server (NTRS)

Zenobi, Renato; Philippoz, Jean-Michel; Zare, Richard N.; Buseck, Peter R.

1989-01-01

The distribution of polycyclic aromatic hydrocarbons (PAHs) in the Allende meteorite has been probed with two-step laser desorption/laser multiphoton ionization mass spectrometry. This method allows direct in situ analysis with a spatial resolution of 1 sq mm or better of selected organic molecules. Spectra from freshly fractured interior surfaces of the meteorite show that PAH concentrations are locally high compared to the average concentrations found by wet chemical analysis of pulverized samples. The data suggest that the PAHs are primarily associated with the fine-grained matrix, where the organic polymer occurs. In addition, highly substituted PAH skeletons were observed. Interiors of individual chondrules were devoid of PAHs at the detection limit (about 0.05 ppm).

Observations of the high vibrational levels of the B ' ' B ¯ 1 Σu + state of H2

NASA Astrophysics Data System (ADS)

Chartrand, A. M.; Duan, W.; Ekey, R. C.; McCormack, E. F.

2016-01-01

Double-resonance laser spectroscopy via the E F 1 Σg + , v ' = 6 , J ' = 0 -2 state was used to probe the high vibrational levels of the B ' ' B ¯ 1 Σu + state of molecular hydrogen. Resonantly enhanced multiphoton ionization spectra were recorded by detecting ion production as a function of energy using a time of flight mass spectrometer. New measurements of energies for the v = 51-66 levels for the B ' ' B ¯ state of H2 are reported, which, taken with previous results, span the v = 46-69 vibrational levels. Results for energy levels are compared to theoretical close-coupled calculations [L. Wolniewicz, T. Orlikowski, and G. Staszewska, J. Mol. Spectrosc. 238, 118-126 (2006)]. The average difference between the 84 measured energies and calculated energies is -3.8 cm-1 with a standard deviation of 5.3 cm-1. This level of agreement showcases the success of the theoretical calculations in accounting for the strong rovibronic mixing of the 1 Σu + and 1 Πu + states. Due to the ion-pair character of the outer well, the observed energies of the vibrational levels below the third dissociation limit smoothly connect with previously observed energies of ion-pair states above this limit. The results provide an opportunity for testing a heavy Rydberg multi-channel quantum defect analysis of the high vibrational states below the third dissociation limit.

Sequential two-photon double ionization of noble gases by circularly polarized XUV radiation

NASA Astrophysics Data System (ADS)

Gryzlova, E. V.; Grum-Grzhimailo, A. N.; Kuzmina, E. I.; Strakhova, S. I.

2014-10-01

Photoelectron angular distributions (PADs) and angular correlations between two emitted electrons in sequential two-photon double ionization (2PDI) of atoms by circularly polarized radiation are studied theoretically. In particular, the sequential 2PDI of the valence n{{p}6} shell in noble gas atoms (neon, argon, krypton) is analyzed, accounting for the first-order corrections to the dipole approximation. Due to different selection rules in ionization transitions, the circular polarization of photons causes some new features of the cross sections, PADs and angular correlation functions in comparison with the case of linearly polarized photons.

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

DOE PAGES

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

2017-01-09

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

Modeling of ablation threshold dependence on pulse duration for dielectrics with ultrashort pulsed laser

NASA Astrophysics Data System (ADS)

Sun, Mingying; Zhu, Jianqiang; Lin, Zunqi

2017-01-01

We present a numerical model of plasma formation in ultrafast laser ablation on the dielectrics surface. Ablation threshold dependence on pulse duration is predicted with the model and the numerical results for water agrees well with the experimental data for pulse duration from 140 fs to 10 ps. Influences of parameters and approximations of photo- and avalanche-ionization on the ablation threshold prediction are analyzed in detail for various pulse lengths. The calculated ablation threshold is strongly dependent on electron collision time for all the pulse durations. The complete photoionization model is preferred for pulses shorter than 1 ps rather than the multiphoton ionization approximations. The transition time of inverse bremsstrahlung absorption needs to be considered when pulses are shorter than 5 ps and it can also ensure the avalanche ionization (AI) coefficient consistent with that in multiple rate equations (MREs) for pulses shorter than 300 fs. The threshold electron density for AI is only crucial for longer pulses. It is reasonable to ignore the recombination loss for pulses shorter than 100 fs. In addition to thermal transport and hydrodynamics, neglecting the threshold density for AI and recombination could also contribute to the disagreements between the numerical and the experimental results for longer pulses.

Ophthalmic imaging using multiphoton microscopy

NASA Astrophysics Data System (ADS)

Teng, Shu-Wen; Peng, Ju-Li; Lin, Huei-Hsing; Wu, Hai-Yin; Lo, Wen; Sun, Yen; Lin, Wei-Chou; Lin, Sung-Jan; Jee, Shiou-Hwa; Tan, Hsin-Yuan; Dong, Chen-Yuan

2005-04-01

This purpose of this study is to demonstrate the feasibility of using multiphoton microscopy in ophthalmologic imaging. Without the introduction of extrinsic fluorescence molecules, multiphoton induced autofluorescence and second harmonic generation signals can be used to obtain useful structural information of normal and diseased corneas. Our work can potentially lead to the in vivo application of multiphoton microscopy in investigating corneal physiology and pathologies.

Multiphoton gradient index endoscopy for evaluation of diseased human prostatic tissue ex vivo

NASA Astrophysics Data System (ADS)

Huland, David M.; Jain, Manu; Ouzounov, Dimitre G.; Robinson, Brian D.; Harya, Diana S.; Shevchuk, Maria M.; Singhal, Paras; Xu, Chris; Tewari, Ashutosh K.

2014-11-01

Multiphoton microscopy can instantly visualize cellular details in unstained tissues. Multiphoton probes with clinical potential have been developed. This study evaluates the suitability of multiphoton gradient index (GRIN) endoscopy as a diagnostic tool for prostatic tissue. A portable and compact multiphoton endoscope based on a 1-mm diameter, 8-cm length GRIN lens system probe was used. Fresh ex vivo samples were obtained from 14 radical prostatectomy patients and benign and malignant areas were imaged and correlated with subsequent H&E sections. Multiphoton GRIN endoscopy images of unfixed and unprocessed prostate tissue at a subcellular resolution are presented. We note several differences and identifying features of benign versus low-grade versus high-grade tumors and are able to identify periprostatic tissues such as adipocytes, periprostatic nerves, and blood vessels. Multiphoton GRIN endoscopy can be used to identify both benign and malignant lesions in ex vivo human prostate tissue and may be a valuable diagnostic tool for real-time visualization of suspicious areas of the prostate.

Multiphoton versus confocal high resolution z-sectioning of enhanced green fluorescent microtubules: increased multiphoton photobleaching within the focal plane can be compensated using a Pockels cell and dual widefield detectors.

PubMed

Drummond, D R; Carter, N; Cross, R A

2002-05-01

Multiphoton excitation was originally projected to improve live cell fluorescence imaging by minimizing photobleaching effects outside the focal plane, yet reports suggest that photobleaching within the focal plane is actually worse than with one photon excitation. We confirm that when imaging enhanced green fluorescent protein, photobleaching is indeed more acute within the multiphoton excitation volume, so that whilst fluorescence increases as predicted with the square of the excitation power, photobleaching rates increase with a higher order relationship. Crucially however, multiphoton excitation also affords unique opportunities for substantial improvements to fluorescence detection. By using a Pockels cell to minimize exposure of the specimen together with multiple nondescanned detectors we show quantitatively that for any particular bleach rate multiphoton excitation produces significantly more signal than one photon excitation confocal microscopy in high resolution Z-axis sectioning of thin samples. Both modifications are readily implemented on a commercial multiphoton microscope system.

Performance analysis of junction-less double Gate n-p-n impact ionization MOS transistor (JLDG n-IMOS)

NASA Astrophysics Data System (ADS)

Chauhan, Manvendra Singh; Chauhan, R. K.

2018-04-01

This paper demonstrates a Junction-less Double Gate n-p-n Impact ionization MOS transistor (JLDG n-IMOS) on a very light doped p-type silicon body. Device structure proposed in the paper is based on charge plasma concept. There is no metallurgical junctions in the proposed device and does not need any impurity doping to create the drain and source regions. Due to doping-less nature, the fabrication process is simple for JLDG n-IMOS. The double gate engineering in proposed device leads to reduction in avalanche breakdown via impact ionization, generating large number of carriers in drain-body junction, resulting high ION current, small IOFF current and great improvement in ION/IOFF ratio. The simulation and examination of the proposed device have been performed on ATLAS device simulatorsoftware.

Indirect contributions to electron-impact ionization of Li+ (1 s 2 s S31 ) ions: Role of intermediate double-K -vacancy states

NASA Astrophysics Data System (ADS)

Müller, A.; Borovik, A.; Huber, K.; Schippers, S.; Fursa, D. V.; Bray, I.

2018-02-01

Fine details of the cross section for electron-impact ionization of metastable two-electron Li+(1 s 2 s S31) ions are scrutinized by both experiment and theory. Beyond direct knockoff ionization, indirect ionization mechanisms proceeding via formation of intermediate double-K-vacancy (hollow) states either in a Li+ ion or in a neutral lithium atom and subsequent emission of one or two electrons, respectively, can contribute to the net production of Li2 + ions. The partial cross sections for such contributions are less than 4% of the total single-ionization cross section. The characteristic steps, resonances, and interference phenomena in the indirect ionization contribution are measured with an experimental energy spread of less than 0.9 eV and with a statistical relative uncertainty of the order of 1.7%, requiring a level of statistical uncertainty in the total single-ionization cross section of better than 0.05%. The measurements are accompanied by convergent-close-coupling calculations performed on a fine energy grid. Theory and experiment are in remarkable agreement concerning the fine details of the ionization cross section. Comparison with previous R-matrix results is less favorable.

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.

Critical Assessment of Theoretical Methods for Li3+ Collisions with He at Intermediate and High Impact Energies

NASA Astrophysics Data System (ADS)

Belkić, Dževad; Mančev, Ivan; Milojevićb, Nenad

2013-09-01

The total cross sections for the various processes for Li3+-He collisions at intermediate-to-high impact energies are compared with the corresponding theories. The possible reasons for the discrepancies among various theoretical predictions are thoroughly discussed. Special attention has been paid to single and double electron capture, simultaneous transfer and ionization, as well as to single and double ionization.

Phase-space perspective on the wavelength-dependent electron correlation of strong-field double ionization of Xe

NASA Astrophysics Data System (ADS)

Shao, Yun; Yuan, Zongqiang; Ye, Difa; Fu, Libin; Liu, Ming-Ming; Sun, Xufei; Wu, Chengyin; Liu, Jie; Gong, Qihuang; Liu, Yunquan

2017-12-01

We measure the wavelength-dependent correlated-electron momentum (CEM) spectra of strong-field double ionization of Xe atoms, and observe a significant change from a roughly nonstructured (uncorrelated) pattern at 795 nm to an elongated distribution with V-shaped structure (correlated) at higher wavelengths of 1320 and 1810 nm, pointing to the transition of the ionization dynamics imprinted in the momentum distributions. These observations are well reproduced by a semiclassical model using Green-Sellin-Zachor potential to take into account the screening effect. We show that the momentum distribution of Xe2+ undergoes a bifurcation structure emerging from single-hump to double-hump structure as the laser wavelength increases, which is dramatically different from that of He2+, indicating the complex multi-electron effect. By back analyzing the double ionization trajectories in the phase space (the initial transverse momentum and the laser phase at the tunneling exit) of the first tunneled electrons, we provide deep insight into the physical origin for electron correlation dynamics. We find that a random distribution in phase-space is responsible for a less distinct structured CEM spectrum at shorter wavelength. While increasing the laser wavelength, a topology-invariant pattern in phase-space appears, leading to the clearly visible V-shaped structures.

In vivo multiphoton tomography and fluorescence lifetime imaging of human brain tumor tissue.

PubMed

Kantelhardt, Sven R; Kalasauskas, Darius; König, Karsten; Kim, Ella; Weinigel, Martin; Uchugonova, Aisada; Giese, Alf

2016-05-01

High resolution multiphoton tomography and fluorescence lifetime imaging differentiates glioma from adjacent brain in native tissue samples ex vivo. Presently, multiphoton tomography is applied in clinical dermatology and experimentally. We here present the first application of multiphoton and fluorescence lifetime imaging for in vivo imaging on humans during a neurosurgical procedure. We used a MPTflex™ Multiphoton Laser Tomograph (JenLab, Germany). We examined cultured glioma cells in an orthotopic mouse tumor model and native human tissue samples. Finally the multiphoton tomograph was applied to provide optical biopsies during resection of a clinical case of glioblastoma. All tissues imaged by multiphoton tomography were sampled and processed for conventional histopathology. The multiphoton tomograph allowed fluorescence intensity- and fluorescence lifetime imaging with submicron spatial resolution and 200 picosecond temporal resolution. Morphological fluorescence intensity imaging and fluorescence lifetime imaging of tumor-bearing mouse brains and native human tissue samples clearly differentiated tumor and adjacent brain tissue. Intraoperative imaging was found to be technically feasible. Intraoperative image quality was comparable to ex vivo examinations. To our knowledge we here present the first intraoperative application of high resolution multiphoton tomography and fluorescence lifetime imaging of human brain tumors in situ. It allowed in vivo identification and determination of cell density of tumor tissue on a cellular and subcellular level within seconds. The technology shows the potential of rapid intraoperative identification of native glioma tissue without need for tissue processing or staining.

Three holes bound to a double acceptor - Be(+) in germanium

NASA Technical Reports Server (NTRS)

Haller, E. E.; Mcmurray, R. E., Jr.; Falicov, L. M.; Haegel, N. M.; Hansen, W. L.

1983-01-01

A double acceptor binding three holes has been observed for the first time with photoconductive far-infrared spectroscopy in beryllium-doped germanium single crystals. This new center, Be(+), has a hole binding energy of about 5 meV and is only present when free holes are generated by ionization of either neutral shallow acceptors or neutral Be double acceptors. The Be(+) center thermally ionizes above 4 K. It disappears at a uniaxial stress higher than about a billion dyn/sq cm parallel to (111) as a result of the lifting of the valence-band degeneracy.

Electron-electron correlation in two-photon double ionization of He-like ions [Counterintuitive electron correlation in two-photon double ionization of He-like ions

DOE PAGES

Hu, S. X.

2018-01-18

Electron correlation plays a crucial role in quantum many-body physics ranging from molecular bonding, strong-field–induced multi-electron ionization, to superconducting in materials. Understanding the dynamic electron correlation in the photoionization of relatively simple quantum three-body systems, such as He and He-like ions, is an important step toward manipulating complex systems through photo-induced processes. Here we have performed ab initio investigations of two-photon double ionization (TPDI) of He and He-like ions [Li +, Be 2+, and C 4+] exposed to intense attosecond x-ray pulses. Results from such fully correlated quantum calculations show weaker and weaker electron correlation effects in TPDI spectra asmore » the ionic charge increases, which is counterintuitive to the belief that the strongly correlated ground state and the strong Coulomb field of He-like ions should lead to more equal-energy sharing in photoionization. Lastly, these findings indicate that the final-state electron–electron correlation ultimately determines their energy sharing in TPDI.« less

Electron-electron correlation in two-photon double ionization of He-like ions [Counterintuitive electron correlation in two-photon double ionization of He-like ions

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

Hu, S. X.

Electron correlation plays a crucial role in quantum many-body physics ranging from molecular bonding, strong-field–induced multi-electron ionization, to superconducting in materials. Understanding the dynamic electron correlation in the photoionization of relatively simple quantum three-body systems, such as He and He-like ions, is an important step toward manipulating complex systems through photo-induced processes. Here we have performed ab initio investigations of two-photon double ionization (TPDI) of He and He-like ions [Li +, Be 2+, and C 4+] exposed to intense attosecond x-ray pulses. Results from such fully correlated quantum calculations show weaker and weaker electron correlation effects in TPDI spectra asmore » the ionic charge increases, which is counterintuitive to the belief that the strongly correlated ground state and the strong Coulomb field of He-like ions should lead to more equal-energy sharing in photoionization. Lastly, these findings indicate that the final-state electron–electron correlation ultimately determines their energy sharing in TPDI.« less

High-resolution imaging of basal cell carcinoma: a comparison between multiphoton microscopy with fluorescence lifetime imaging and reflectance confocal microscopy.

PubMed

Manfredini, Marco; Arginelli, Federica; Dunsby, Christopher; French, Paul; Talbot, Clifford; König, Karsten; Pellacani, Giovanni; Ponti, Giovanni; Seidenari, Stefania

2013-02-01

The aim of this study was to compare morphological aspects of basal cell carcinoma (BCC) as assessed by two different imaging methods: in vivo reflectance confocal microscopy (RCM) and multiphoton tomography with fluorescence lifetime imaging implementation (MPT-FLIM). The study comprised 16 BCCs for which a complete set of RCM and MPT-FLIM images were available. The presence of seven MPT-FLIM descriptors was evaluated. The presence of seven RCM equivalent parameters was scored in accordance to their extension. Chi-squared test with Fisher's exact test and Spearman's rank correlation coefficient were determined between MPT-FLIM scores and adjusted-RCM scores. MPT-FLIM and RCM descriptors of BCC were coupled to match the descriptors that define the same pathological structures. The comparison included: Streaming and Aligned elongated cells, Streaming with multiple directions and Double alignment, Palisading (RCM) and Palisading (MPT-FLIM), Typical tumor islands, and Cell islands surrounded by fibers, Dark silhouettes and Phantom islands, Plump bright cells and Melanophages, Vessels (RCM), and Vessels (MPT-FLIM). The parameters that were significantly correlated were Melanophages/Plump Bright Cells, Aligned elongated cells/Streaming, Double alignment/Streaming with multiple directions, and Palisading (MPT-FLIM)/Palisading (RCM). According to our data, both methods are suitable to image BCC's features. The concordance between MPT-FLIM and RCM is high, with some limitations due to the technical differences between the two devices. The hardest difficulty when comparing the images generated by the two imaging modalities is represented by their different field of view. © 2012 John Wiley & Sons A/S.

Electron Capture Dissociation of Divalent Metal-adducted Sulfated N-Glycans Released from Bovine Thyroid Stimulating Hormone

NASA Astrophysics Data System (ADS)

Zhou, Wen; Håkansson, Kristina

2013-11-01

Sulfated N-glycans released from bovine thyroid stimulating hormone (bTSH) were ionized with the divalent metal cations Ca2+, Mg2+, and Co by electrospray ionization (ESI). These metal-adducted species were subjected to infrared multiphoton dissociation (IRMPD) and electron capture dissociation (ECD) and the corresponding fragmentation patterns were compared. IRMPD generated extensive glycosidic and cross-ring cleavages, but most product ions suffered from sulfonate loss. Internal fragments were also observed, which complicated the spectra. ECD provided complementary structural information compared with IRMPD, and all observed product ions retained the sulfonate group, allowing sulfonate localization. To our knowledge, this work represents the first application of ECD towards metal-adducted sulfated N-glycans released from a glycoprotein. Due to the ability of IRMPD and ECD to provide complementary structural information, the combination of the two strategies is a promising and valuable tool for glycan structural characterization. The influence of different metal ions was also examined. Calcium adducts appeared to be the most promising species because of high sensitivity and ability to provide extensive structural information.

A Double-Blind Placebo-Controlled Crossover Trial of Intravenous Magnesium Sulfate for Foscarnet-Induced Ionized Hypocalcemia and Hypomagnesemia in Patients with AIDS and Cytomegalovirus Infection

PubMed Central

Huycke, Mark M.; Naguib, M. Tarek; Stroemmel, Mathias M.; Blick, Kenneth; Monti, Katherine; Martin-Munley, Sarah; Kaufman, Chris

2000-01-01

Foscarnet (trisodium phosphonoformate hexahydrate) is an antiviral agent used to treat cytomegalovirus disease in immunocompromised patients. One common side effect is acute ionized hypocalcemia and hypomagnesemia following intravenous administration. Foscarnet-induced ionized hypomagnesemia might contribute to ionized hypocalcemia by impairing excretion of preformed parathyroid hormone (PTH) or by producing target organ resistance. Prevention of ionized hypomagnesemia following foscarnet administration could blunt the development of ionized hypocalcemia. To determine whether intravenous magnesium ameliorates the decline in ionized calcium and/or magnesium following foscarnet infusions, MgSO4 at doses of 1, 2, and 3 g was administered in a double-blind, placebo-controlled, randomized, crossover trial to 12 patients with AIDS and cytomegalovirus disease. Overall, increasing doses of MgSO4 reduced or eliminated foscarnet-induced acute ionized hypomagnesemia. Supplementation, however, had no discernible effect on foscarnet-induced ionized hypocalcemia despite significant increases in serum PTH levels. No dose-related, clinically significant adverse events were found, suggesting that intravenous supplementation with up to 3 g of MgSO4 was safe in this chronically ill population. Since parenteral MgSO4 did not alter foscarnet-induced ionized hypocalcemia or symptoms associated with foscarnet, routine intravenous supplementation for patients with normal serum magnesium levels is not recommended during treatment with foscarnet. PMID:10898688

Photon-momentum transfer in molecular photoionization

NASA Astrophysics Data System (ADS)

Chelkowski, Szczepan; Bandrauk, André D.

2018-05-01

In most models and theoretical calculations describing multiphoton ionization by infrared light, the dipole approximation is used. This is equivalent to setting the very small photon momentum to zero. Using numerical solutions of the (nondipole) three-dimensional time-dependent Schrödinger equation for one electron in a H2+ molecular ion we investigate the effect the photon-momentum transfer to the photoelectron in an H2+ ion in various regimes. We find that the photon-momentum transfer in a molecule is very different from the transfer in atoms due to two-center interference effects. The photon-momentum transfer is very sensitive to the symmetry of the initial electronic state and is strongly dependent on the internuclear distance and on the ellipticity of the laser.

An ultracold potassium Rydberg source for experiments in quantum optics and many-body physics

NASA Astrophysics Data System (ADS)

Conover, Charles; Dupre, Pamela; Tong, Ai Phuong; Sanon, Carlvin; Clarke, Kevin; Doolittle, Brian; Louria, Stephen; Adamson, Philip

2017-04-01

We report on the development of an apparatus for the study of quantum dynamics of Rydberg atoms of potassium. Samples of Rydberg atoms at 1 mK and varying density are excited in a magneto-optical trap of 107 K-39 atoms. The atoms are excited to Rydberg states in a steps from 4s to 5p and from 5p to ns and nd states using stabilized external-cavity diode lasers at 405 nm and 980 nm. Selective field ionization and detection with microchannel plates provides a platform for spectroscopic measurements in potassium, exploration of multiphoton processes, and experiments on cold atom collisions. This research was supported by the National Science Foundation under Grant PHY-1126599.

STORAGE RING CROSS SECTION MEASUREMENTS FOR ELECTRON IMPACT SINGLE AND DOUBLE IONIZATION OF Fe{sup 13+} AND SINGLE IONIZATION OF Fe{sup 16+} AND Fe{sup 17+}

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

Hahn, M.; Novotny, O.; Savin, D. W.

2013-04-10

We report measurements of electron impact ionization for Fe{sup 13+}, Fe{sup 16+}, and Fe{sup 17+} over collision energies from below threshold to above 3000 eV. The ions were recirculated using an ion storage ring. Data were collected after a sufficiently long time that essentially all the ions had relaxed radiatively to their ground state. For single ionization of Fe{sup 13+}, we find that previous single pass experiments are more than 40% larger than our results. Compared to our work, the theoretical cross section recommended by Arnaud and Raymond is more than 30% larger, while that of Dere is about 20%more » greater. Much of the discrepancy with Dere is due to the theory overestimating the contribution of excitation-autoionization via n = 2 excitations. Double ionization of Fe{sup 13+} is dominated by direct ionization of an inner shell electron accompanied by autoionization of a second electron. Our results for single ionization of Fe{sup 16+} and Fe{sup 17+} agree with theoretical calculations to within the experimental uncertainties.« less

Single and multiple ionization of C60 fullerenes and collective effects in collisions with highly charged C, F, and Si ions with energy 3 MeV/u

NASA Astrophysics Data System (ADS)

Kelkar, A. H.; Kadhane, U.; Misra, D.; Gulyas, L.; Tribedi, L. C.

2010-10-01

We have measured absolute cross sections for single, double, triple, and quadruple ionization of C60 in collisions with 3 MeV/u C, F, and Si projectile ions at various projectile charge states. The experiment was performed using the recoil-ion time-of-flight technique. Projectile charge state dependence of the ionization yields was compared mainly with a model based on the giant dipole plasmon resonance (GDPR). In some cases, the continuum-distorted-wave-eikonal-initial-state (CDW-EIS) model which is normally applied for ion-atom collisions was also used as a reference. An excellent qualitative agreement between the experimental data for single and double ionization and the GDPR model predictions was found for all projectile charge states.

Double ionization of helium by ion impact: second Born order treatment at the fully differential level

NASA Astrophysics Data System (ADS)

López, S. D.; Otranto, S.; Garibotti, C. R.

2015-01-01

In this work, a theoretical study of the double ionization of He by ion impact at the fully differential level is presented. Emphasis is made in the role played by the projectile in the double emission process depending on its charge and the amount of momentum transferred to the target. A Born-CDW model including a second-order term in the projectile charge is introduced and evaluated within an on-shell treatment. We find that emission geometries for which the second-order term dominates lead to asymmetric structures around the momentum transfer direction, a typical characteristic of higher order transitions.

Signature of charge migration in modulations of double ionization

NASA Astrophysics Data System (ADS)

Mauger, François; Abanador, Paul M.; Bruner, Adam; Sissay, Adonay; Gaarde, Mette B.; Lopata, Kenneth; Schafer, Kenneth J.

2018-04-01

We present a theoretical investigation of charge migration following strong-field ionization in a multielectron system. We study a model homonuclear molecule with two electrons, each restricted to one dimension (1 +1 D ), interacting with a strong, static electric field. We show that in this system charge migration results from the interplay between multiple ionization channels that overlap in space, creating a coherent electron-hole wave packet in the cation. We also find that, in our case, charge migration following the first ionization manifests as a modulation of the subsequent double-ionization signal. We derive a parametrized semiclassical model from the full multielectron system and we discuss the importance of the choice of cation electronic-structure basis for the efficacy of the semiclassical representation. We use the ab initio solution of the full 1 +1 D system as a reference for the qualitative and quantitative results of the parametrized semiclassical model. We discuss the extension of our model to long-wavelength time-dependent fields with full-dimension, many-electron targets.

Temporal correlation and correlated momentum distribution in nonsequential double ionization of Mg by circularly polarized laser fields

NASA Astrophysics Data System (ADS)

Xu, Tong-Tong; Ben, Shuai; Guo, Pei-Ying; Song, Kai-Li; Zhang, Jun; Liu, Xue-Shen

2017-07-01

We use the classical ensemble method to investigate the nonsequential double ionization (NSDI) process of Mg atoms in circularly polarized laser fields at a lower laser intensity. We illustrate the temporal correlation of the ‘side-by-side’ and the ‘back-to-back emission’. It indicates that the two electrons are more likely to be emitted at the same time for the ‘side-by-side emission’. We demonstrate the electronic trajectories from recollision-induced ionization (RII) and recollision-induced excitation with subsequent ionization (RESI). The distribution of the angle between the two ionized directions of the two electrons and the ion momentum distribution show that the anticorrelation distribution is dominant in the RESI mechanism and correlation distribution is dominant in the RII mechanism. The momentum distributions of Mg atoms for the slow and the fast electrons present a similar structure to the experimental observation of Ar atoms by Liu et al 2014 (Phys. Rev. Lett. 112 013003).

Optical tweezers and multiphoton microscopies integrated photonic tool for mechanical and biochemical cell processes studies

NASA Astrophysics Data System (ADS)

de Thomaz, A. A.; Faustino, W. M.; Fontes, A.; Fernandes, H. P.; Barjas-Castro, M. d. L.; Metze, K.; Giorgio, S.; Barbosa, L. C.; Cesar, C. L.

2007-09-01

The research in biomedical photonics is clearly evolving in the direction of the understanding of biological processes at the cell level. The spatial resolution to accomplish this task practically requires photonics tools. However, an integration of different photonic tools and a multimodal and functional approach will be necessary to access the mechanical and biochemical cell processes. This way we can observe mechanicaly triggered biochemical events or biochemicaly triggered mechanical events, or even observe simultaneously mechanical and biochemical events triggered by other means, e.g. electricaly. One great advantage of the photonic tools is its easiness for integration. Therefore, we developed such integrated tool by incorporating single and double Optical Tweezers with Confocal Single and Multiphoton Microscopies. This system can perform 2-photon excited fluorescence and Second Harmonic Generation microscopies together with optical manipulations. It also can acquire Fluorescence and SHG spectra of specific spots. Force, elasticity and viscosity measurements of stretched membranes can be followed by real time confocal microscopies. Also opticaly trapped living protozoas, such as leishmania amazonensis. Integration with CARS microscopy is under way. We will show several examples of the use of such integrated instrument and its potential to observe mechanical and biochemical processes at cell level.

Multiphoton dynamics of qutrits in the ultrastrong coupling regime with a quantized photonic field

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

Avetissian, H. K., E-mail: avetissian@ysu.am; Avetissian, A. K.; Mkrtchian, G. F.

2015-12-15

Multiphoton resonant excitation of a three-state quantum system (a qutrit) with a single-mode photonic field is considered in the ultrastrong coupling regime, when the qutrit–photonic field coupling rate is comparable to appreciable fractions of the photon frequency. For ultrastrong couplings, the obtained solutions of the Schrödinger equation that reveal multiphoton Rabi oscillations in qutrits with the interference effects leading to the collapse and revival of atomic excitation probabilities at the direct multiphoton resonant transitions.

High-resolution multimodal clinical multiphoton tomography of skin

NASA Astrophysics Data System (ADS)

König, Karsten

2011-03-01

This review focuses on multimodal multiphoton tomography based on near infrared femtosecond lasers. Clinical multiphoton tomographs for 3D high-resolution in vivo imaging have been placed into the market several years ago. The second generation of this Prism-Award winning High-Tech skin imaging tool (MPTflex) was introduced in 2010. The same year, the world's first clinical CARS studies have been performed with a hybrid multimodal multiphoton tomograph. In particular, non-fluorescent lipids and water as well as mitochondrial fluorescent NAD(P)H, fluorescent elastin, keratin, and melanin as well as SHG-active collagen has been imaged with submicron resolution in patients suffering from psoriasis. Further multimodal approaches include the combination of multiphoton tomographs with low-resolution wide-field systems such as ultrasound, optoacoustical, OCT, and dermoscopy systems. Multiphoton tomographs are currently employed in Australia, Japan, the US, and in several European countries for early diagnosis of skin cancer, optimization of treatment strategies, and cosmetic research including long-term testing of sunscreen nanoparticles as well as anti-aging products.

Application of Negative Curvature Hollow-Core Fiber in an Optical Fiber Sensor Setup for Multiphoton Spectroscopy

PubMed Central

Stawska, Hanna Izabela; Mazur, Leszek Mateusz; Kosolapov, Alexey; Kolyadin, Anton; Bereś-Pawlik, Elżbieta

2017-01-01

In this paper, an application of negative curvature hollow core fiber (NCHCF) in an all-fiber, multiphoton fluorescence sensor setup is presented. The dispersion parameter (D) of this fiber does not exceed the value of 5 ps/nm × km across the optical spectrum of (680–750) nm, making it well suited for the purpose of multiphoton excitation of biological fluorophores. Employing 1.5 m of this fiber in a simple, all-fiber sensor setup allows us to perform multiphoton experiments without any dispersion compensation methods. Multiphoton excitation of nicotinamide adenine dinucleotide (NADH) and flavin adenine dinucleotide (FAD) with this fiber shows a 6- and 9-fold increase, respectively, in the total fluorescence signal collected when compared with the commercial solution in the form of a hollow-core photonic band gap fiber (HCPBF). To the author’s best knowledge, this is the first time an NCHCF was used in an optical-fiber sensor setup for multiphoton fluorescence experiments. PMID:28984838

Application of Negative Curvature Hollow-Core Fiber in an Optical Fiber Sensor Setup for Multiphoton Spectroscopy.

PubMed

Popenda, Maciej Andrzej; Stawska, Hanna Izabela; Mazur, Leszek Mateusz; Jakubowski, Konrad; Kosolapov, Alexey; Kolyadin, Anton; Bereś-Pawlik, Elżbieta

2017-10-06

In this paper, an application of negative curvature hollow core fiber (NCHCF) in an all-fiber, multiphoton fluorescence sensor setup is presented. The dispersion parameter (D) of this fiber does not exceed the value of 5 ps/nm × km across the optical spectrum of (680-750) nm, making it well suited for the purpose of multiphoton excitation of biological fluorophores. Employing 1.5 m of this fiber in a simple, all-fiber sensor setup allows us to perform multiphoton experiments without any dispersion compensation methods. Multiphoton excitation of nicotinamide adenine dinucleotide (NADH) and flavin adenine dinucleotide (FAD) with this fiber shows a 6- and 9-fold increase, respectively, in the total fluorescence signal collected when compared with the commercial solution in the form of a hollow-core photonic band gap fiber (HCPBF). To the author's best knowledge, this is the first time an NCHCF was used in an optical-fiber sensor setup for multiphoton fluorescence experiments.

Strong-Field Control of Laser Filamentation Mechanisms

NASA Astrophysics Data System (ADS)

Levis, Robert; Romanov, Dmitri; Filin, Aleskey; Compton, Ryan

2008-05-01

The propagation of short strong-file laser pulses in gas and solution phases often result in formation of filaments. This phenomenon involves many nonlinear processes including Kerr lensing, group velocity dispersion, multi-photon ionization, plasma defocusing, intensity clamping, and self-steepening. Of these, formation and dynamics of pencil-shape plasma areas plays a crucial role. The fundamental understanding of these laser-induced plasmas requires additional effort, because the process is highly nonlinear and complex. We studied the ultrafast laser-generated plasma dynamics both experimentally and theoretically. Ultrafast plasma dynamics was probed using Coherent Anti-Stokes Raman Scattering. The measurements were made in a room temperature gas maintained at 1 atm in a flowing cell. The time dependent scattering was measured by delaying the CARS probe with respect to the intense laser excitation pulse. A general trend is observed between the spacing of the ground state and the first allowed excited state with the rise time for the noble gas series and the molecular gases. This trend is consistent with our theoretical model, which considers the ultrafast dynamics of the strong field generated plasma as a three-step process; (i) strong-field ionization followed by the electron gaining considerable kinetic energy during the pulse; (ii) immediate post-pulse dynamics: fast thermalization, impact-ionization-driven electron multiplication and cooling; (iii) ensuing relaxation: evolution to electron-ion equilibrium and eventual recombination.

Toward Rotational State-Selective Photoionization of ThF+ Ions

NASA Astrophysics Data System (ADS)

Zhou, Yan; Ng, Kia Boon; Gresh, Dan; Cairncross, William; Grau, Matt; Ni, Yiqi; Cornell, Eric; Ye, Jun

2016-06-01

ThF+ has been chosen to replace HfF+ for a second-generation measurement of the electric dipole moment of the electron (eEDM). Compared to the currently running HfF+ eEDM experiment, ThF+ has several advantages: (i) the eEDM-sensitive state (3Δ1) is the ground state, which facilitates a long coherence time [1]; (ii) its effective electric field (35 GV/cm) is 50% larger than that of HfF+, which promises a direct increase of the eEDM sensitivity [2]; and (iii) the ionization energy of neutral ThF is lower than its dissociation energy, which introduces greater flexibility in rotational state-selective photoionization via core-nonpenetrating Rydberg states [3]. In this talk, we first present our strategy of preparing and utilizing core-nonpenetrating Rydberg states for rotational state-selective ionization. Then, we report spectroscopic data of laser-induced fluorescence of neutral ThF, which provides critical information for multi-photon ionization spectroscopy. [1] D. N. Gresh, K. C. Cossel, Y. Zhou, J. Ye, E. A. Cornell, Journal of Molecular Spectroscopy, 319 (2016), 1-9 [2] M. Denis, M. S. Nørby, H. J. A. Jensen, A. S. P. Gomes, M. K. Nayak, S. Knecht, T. Fleig, New Journal of Physics, 17 (2015) 043005. [3] Z. J. Jakubek, R. W. Field, Journal of Molecular Spectroscopy 205 (2001) 197-220.

Detection of gaseous compounds by needle trap sampling and direct thermal-desorption photoionization mass spectrometry: concept and demonstrative application to breath gas analysis.

PubMed

Kleeblatt, Juliane; Schubert, Jochen K; Zimmermann, Ralf

2015-02-03

A fast detection method to analyze gaseous organic compounds in complex gas mixtures was developed, using a needle trap device (NTD) in conjunction with thermal-desorption photoionization time-of-flight mass spectrometry (TD-PI-TOFMS). The mass spectrometer was coupled via a deactivated fused silica capillary to an injector of a gas chromatograph. In the hot injector, the analytes collected on the NTD were thermally desorbed and directly transferred to the PI-TOFMS ion source. The molecules are softly ionized either by single photon ionization (SPI, 118 nm) or by resonance enhanced multiphoton ionization (REMPI, 266 nm), and the molecular ion signals are detected in the TOF mass analyzer. Analyte desorption and the subsequent PI-TOFMS detection step only lasts ten seconds. The specific selectivity of REMPI (i.e., aromatic compounds) and universal ionization characteristics render PI-MS as a promising detection system. As a first demonstrative application, the alveolar phase breath gas of healthy, nonsmoking subjects was sampled on NTDs. While smaller organic compounds such as acetone, acetaldehyde, isoprene, or cysteamine can be detected in the breath gas with SPI, REMPI depicts the aromatic substances phenol and indole at 266 nm. In the breath gas of a healthy, smoking male subject, several xenobiotic substances such as benzene, toluene, styrene, and ethylbenzene can be found as well. Furthermore, the NTD-REMPI-TOFMS setup was tested for breath gas taken from a mechanically ventilated pig under continuous intravenous propofol (2,6-diisopropylphenol, narcotic drug) infusion.

Compton spectra of atoms at high x-ray intensity

NASA Astrophysics Data System (ADS)

Son, Sang-Kil; Geffert, Otfried; Santra, Robin

2017-03-01

Compton scattering is the nonresonant inelastic scattering of an x-ray photon by an electron and has been used to probe the electron momentum distribution in gas-phase and condensed-matter samples. In the low x-ray intensity regime, Compton scattering from atoms dominantly comes from bound electrons in neutral atoms, neglecting contributions from bound electrons in ions and free (ionized) electrons. In contrast, in the high x-ray intensity regime, the sample experiences severe ionization via x-ray multiphoton multiple ionization dynamics. Thus, it becomes necessary to take into account all the contributions to the Compton scattering signal when atoms are exposed to high-intensity x-ray pulses provided by x-ray free-electron lasers (XFELs). In this paper, we investigate the Compton spectra of atoms at high x-ray intensity, using an extension of the integrated x-ray atomic physics toolkit, xatom. As the x-ray fluence increases, there is a significant contribution from ionized electrons to the Compton spectra, which gives rise to strong deviations from the Compton spectra of neutral atoms. The present study provides not only understanding of the fundamental XFEL-matter interaction but also crucial information for single-particle imaging experiments, where Compton scattering is no longer negligible. , which features invited work from the best early-career researchers working within the scope of J. Phys. B. This project is part of the Journal of Physics series’ 50th anniversary celebrations in 2017. Sang-Kil Son was selected by the Editorial Board of J. Phys. B as an Emerging Leader.

Simulation of double stage hall thruster with double-peaked magnetic field

NASA Astrophysics Data System (ADS)

Ding, Yongjie; Li, Peng; Sun, Hezhi; Wei, Liqiu; Xu, Yu; Peng, Wuji; Su, Hongbo; Li, Hong; Yu, Daren

2017-07-01

This study adopts double permanent magnetic rings and four permanent magnetic rings to form two symmetrical magnetic peaks and two asymmetrical magnetic peaks in the channel of a Hall thruster, and uses a 2D-3V PIC-MCC model to analyze the influence of magnetic strength on the discharge characteristic and performance of Hall thrusters with an intermediate electrode and double-peaked magnetic field. As opposed to the two symmetrical magnetic peaks formed by double permanent magnetic rings, increasing the magnetic peak value deep within the channel can cause propellant ionization to occur; with the increase in the magnetic peak deep in the channel, the propellant utilization, thrust, and anode efficiency of the thruster are significantly improved. Double-peaked magnetic field can realize separate control of ionization and acceleration in a Hall thruster, and provide technical means for further improving thruster performance. Contribution to the Topical Issue "Physics of Ion Beam Sources", edited by Holger Kersten and Horst Neumann.

Renormalization shielding effect on the Wannier-ridge mode for double-electron continua in partially ionized dense hydrogen plasmas

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

Lee, Myoung-Jae; Jung, Young-Dae, E-mail: ydjung@hanyang.ac.kr; Department of Physics, Applied Physics, and Astronomy, Rensselaer Polytechnic Institute, 110 8th Street, Troy, New York 12180-3590

2016-01-15

The influence of renormalization shielding on the Wannier threshold law for the double-electron escapes by the electron-impact ionization is investigated in partially ionized dense plasmas. The renormalized electron charge and Wannier exponent are obtained by considering the equation of motion in the Wannier-ridge including the renormalization shielding effect. It is found that the renormalization shielding effect reduces the magnitude of effective electron charge, especially, within the Bohr radius in partially ionized dense plasmas. The maximum position of the renormalized electron charge approaches to the center of the target atom with an increase of the renormalization parameter. In addition, the Wanniermore » exponent increases with an increase of the renormalization parameter. The variations of the renormalized electron charge and Wannier exponent due to the renormalization shielding effect are also discussed.« less

Single and multiple ionization of C{sub 60} fullerenes and collective effects in collisions with highly charged C, F, and Si ions with energy 3 MeV/u

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

Kelkar, A. H.; Kadhane, U.; Misra, D.

2010-10-15

We have measured absolute cross sections for single, double, triple, and quadruple ionization of C{sub 60} in collisions with 3 MeV/u C, F, and Si projectile ions at various projectile charge states. The experiment was performed using the recoil-ion time-of-flight technique. Projectile charge state dependence of the ionization yields was compared mainly with a model based on the giant dipole plasmon resonance (GDPR). In some cases, the continuum-distorted-wave-eikonal-initial-state (CDW-EIS) model which is normally applied for ion-atom collisions was also used as a reference. An excellent qualitative agreement between the experimental data for single and double ionization and the GDPR modelmore » predictions was found for all projectile charge states.« less

Laser-induced periodic surface structures on zinc oxide crystals upon two-colour femtosecond double-pulse irradiation

NASA Astrophysics Data System (ADS)

Höhm, S.; Rosenfeld, A.; Krüger, J.; Bonse, J.

2017-03-01

In order to study the temporally distributed energy deposition in the formation of laser-induced periodic surface structures (LIPSS) on single-crystalline zinc oxide (ZnO), two-colour double-fs-pulse experiments were performed. Parallel or cross-polarised double-pulse sequences at 400 and 800 nm wavelength were generated by a Mach-Zehnder interferometer, exhibiting inter-pulse delays up to a few picoseconds between the sub-ablation 50-fs-pulses. Twenty two-colour double-pulse sequences were collinearly focused by a spherical mirror to the sample surface. The resulting LIPSS periods and areas were analysed by scanning electron microscopy. The delay-dependence of these LIPSS characteristics shows a dissimilar behaviour when compared to the semiconductor silicon, the dielectric fused silica, or the metal titanium. A wavelength-dependent plasmonic mechanism is proposed to explain the delay-dependence of the LIPSS on ZnO when considering multi-photon excitation processes. Our results support the involvement of nonlinear processes for temporally overlapping pulses. These experiments extend previous two-colour studies on the indirect semiconductor silicon towards the direct wide band-gap semiconductor ZnO and further manifest the relevance of the ultrafast energy deposition for LIPSS formation.

QED theory of multiphoton transitions in atoms and ions

NASA Astrophysics Data System (ADS)

Zalialiutdinov, Timur A.; Solovyev, Dmitry A.; Labzowsky, Leonti N.; Plunien, Günter

2018-03-01

This review surveys the quantum theory of electromagnetic radiation for atomic systems. In particular, a review of current theoretical studies of multiphoton processes in one and two-electron atoms and highly charged ions is provided. Grounded on the quantum electrodynamics description the multiphoton transitions in presence of cascades, spin-statistic behaviour of equivalent photons and influence of external electric fields on multiphoton in atoms and anti-atoms are discussed. Finally, the nonresonant corrections which define the validity of the concept of the excited state energy levels are introduced.

Correlation-driven charge migration following double ionization and attosecond transient absorption spectroscopy

NASA Astrophysics Data System (ADS)

Hollstein, Maximilian; Santra, Robin; Pfannkuche, Daniela

2017-05-01

We theoretically investigate charge migration following prompt double ionization. Thereby, we extend the concept of correlation-driven charge migration, which was introduced by Cederbaum and coworkers for single ionization [Chem. Phys. Lett. 307, 205 (1999), 10.1016/S0009-2614(99)00508-4], to doubly ionized molecules. This allows us to demonstrate that compared to singly ionized molecules, in multiply ionized molecules, electron dynamics originating from electronic relaxation and correlation are particularly prominent. In addition, we also discuss how these correlation-driven electron dynamics might be evidenced and traced experimentally using attosecond transient absorption spectroscopy. For this purpose, we determine the time-resolved absorption cross section and find that the correlated electron dynamics discussed are reflected in it with exceptionally great detail. Strikingly, we find that features in the cross section can be traced back to electron hole populations and time-dependent partial charges and hence, can be interpreted with surprising ease. By taking advantage of element-specific core-to-valence transitions even atomic spatial resolution can be achieved. Thus, with the theoretical considerations presented, not only do we predict particularly diverse and correlated electron dynamics in molecules to follow prompt multiple ionization but we also identify a promising route towards their experimental investigation.

The concept of quasi-tissue-equivalent nanodosimeter based on the glow peak 5a/5 in LiF:Mg,Ti (TLD-100).

PubMed

Oster, L; Horowitz, Y S; Biderman, S; Haddad, J

2003-12-01

We demonstrate the viability of the concept of using existing molecular nanostructures in thermoluminescent solid-state materials as solid-state nanodosimeters. The concept is based on mimicking radiobiology (specifically the ionization density dependence of double strand breaks in DNA) by using the similar ionization density dependence of simultaneous electron-hole capture in spatially correlated trapping and luminescent centres pairs in the thermoluminescence of LiF:Mg,Ti. This simultaneous electron-hole capture has been shown to lead to ionization density dependence in the relative intensity of peak 5a to peak 5 similar to the ratio of double-strand breaks to single-strand breaks for low energy He ions.

Dissociation kinetics of excited ions: PEPICO measurements of Os3(CO)12 - The 7-35 eV single ionization binding energy region.

PubMed

Schalk, Oliver; Josefsson, Ida; Geng, Ting; Richter, Robert; Sa'adeh, Hanan; Thomas, Richard D; Mucke, Melanie

2018-02-28

In this article, we study the photoinduced dissociation pathways of a metallocarbonyl, Os 3 (CO) 12 , in particular the consecutive loss of CO groups. To do so, we performed photoelectron-photoion coincidence (PEPICO) measurements in the single ionization binding energy region from 7 to 35 eV using 45-eV photons. Zero-energy ion appearance energies for the dissociation steps were extracted by modeling the PEPICO data using the statistical adiabatic channel model. Upon ionization to the excited ionic states above 13 eV binding energy, non-statistical behavior was observed and assigned to prompt CO loss. Double ionization was found to be dominated by the knockout process with an onset of 20.9 ± 0.4 eV. The oscillator strength is significantly larger for energies above 26.6 ± 0.4 eV, corresponding to one electron being ejected from the Os 3 center and one from the CO ligands. The cross section for double ionization was found to increase linearly up to 35 eV ionization energy, at which 40% of the generated ions are doubly charged.

Coherent control of photoelectron wavepacket angular interferograms

NASA Astrophysics Data System (ADS)

Hockett, P.; Wollenhaupt, M.; Baumert, T.

2015-11-01

Coherent control over photoelectron wavepackets, via the use of polarization-shaped laser pulses, can be understood as a time and polarization-multiplexed process, where the final (time-integrated) observable coherently samples all instantaneous states of the light-matter interaction. In this work, we investigate this multiplexing via computation of the observable photoelectron angular interferograms resulting from multi-photon atomic ionization with polarization-shaped laser pulses. We consider the polarization sensitivity of both the instantaneous and cumulative continuum wavefunction; the nature of the coherent control over the resultant photoelectron interferogram is thus explored in detail. Based on this understanding, the use of coherent control with polarization-shaped pulses as a methodology for a highly multiplexed coherent quantum metrology is also investigated, and defined in terms of the information content of the observable.

Optimized cell geometry for buffer-gas-cooled molecular-beam sources

NASA Astrophysics Data System (ADS)

Singh, Vijay; Samanta, Amit K.; Roth, Nils; Gusa, Daniel; Ossenbrüggen, Tim; Rubinsky, Igor; Horke, Daniel A.; Küpper, Jochen

2018-03-01

We have designed, constructed, and commissioned a cryogenic helium buffer-gas source for producing a cryogenically cooled molecular beam and evaluated the effect of different cell geometries on the intensity of the produced molecular beam, using ammonia as a test molecule. Planar and conical entrance and exit geometries are tested. We observe a threefold enhancement in the NH3 signal for a cell with planar entrance and conical-exit geometry, compared to that for a typically used "boxlike" geometry with planar entrance and exit. These observations are rationalized by flow field simulations for the different buffer-gas cell geometries. The full thermalization of molecules with the helium buffer gas is confirmed through rotationally resolved resonance-enhanced multiphoton ionization spectra yielding a rotational temperature of 5 K.

Self-channeling of high-power laser pulses through strong atmospheric turbulence

NASA Astrophysics Data System (ADS)

Peñano, J.; Palastro, J. P.; Hafizi, B.; Helle, M. H.; DiComo, G. P.

2017-07-01

We present an unusual example of truly long-range propagation of high-power laser pulses through strong atmospheric turbulence. A form of nonlinear self-channeling is achieved when the laser power is close to the self-focusing power of air and the transverse dimensions of the pulse are smaller than the coherence diameter of turbulence. In this mode, nonlinear self-focusing counteracts diffraction, and turbulence-induced spreading is greatly reduced. Furthermore, the laser intensity is below the ionization threshold so that multiphoton absorption and plasma defocusing are avoided. Simulations show that the pulse can propagate many Rayleigh lengths (several kilometers) while maintaining a high intensity. In the presence of aerosols, or other extinction mechanisms that deplete laser energy, the pulse can be chirped to maintain the channeling.

Ultrafast photodissociation dynamics of 1,4-diiodobenzene

NASA Astrophysics Data System (ADS)

Stankus, Brian; Zotev, Nikola; Rogers, David M.; Gao, Yan; Odate, Asami; Kirrander, Adam; Weber, Peter M.

2018-05-01

The photodissociation dynamics of 1,4-diiodobenzene is investigated using ultrafast time-resolved photoelectron spectroscopy. Following excitation by laser pulses at 271 nm, the excited-state dynamics is probed by resonance-enhanced multiphoton ionization with 405 nm probe pulses. A progression of Rydberg states, which come into resonance sequentially, provide a fingerprint of the dissociation dynamics of the molecule. The initial excitation decays with a lifetime of 33 ± 4 fs, in good agreement with a previous study. The spectrum is interpreted by reference to ab initio calculations at the CASPT2(18,14) level, including spin-orbit coupling. We propose that both the 5B1 and 6B1 states are excited initially, and based on the calculations, we identify diabatic spin-orbit coupled states corresponding to the main dissociation pathways.

Double ionization of He(1[ital s][sup 2]) and He(1[ital s]2[ital s] [sup 3][ital S]) by a single high-energy photon

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

Teng, Z.; Shakeshaft, R.

1994-05-01

We have calculated the energy and angular distributions for double ionization of He(1[ital s][sup 2]) and He(1[ital s]2[ital s] [sup 3][ital S]) by one photon, over a range of photon energies up to a few keV. The calculations were based on using a fairly accurate initial-state wave function, determined so as to exactly satisfy the Kato cusp conditions, and a final-state wave function which is a product of three Coulomb wave functions modified by a short-range correction term. There are at least three different mechanisms for double ionization, and each one leaves a mark on the angular distribution. When themore » energies of the two electrons are equal, the contribution of each mechanism to the angular asymmetry parameter can be estimated on theoretical grounds; we compare these estimates with the calculated results to give a further indication of the roles of the various mechanisms. Concerning the shapes of the energy and angular distributions, we find significant differences between double ionization of singlet and triplet helium; in particular, the probability for one high-energy photon to eject two equal-energy electrons from triplet helium nearly vanishes owing to the Pauli exclusion principle and to interference effects resulting from antisymmetrization. In two appendixes we present some details of the integration involved in the calculations.« less

Current developments in clinical multiphoton tomography

NASA Astrophysics Data System (ADS)

König, Karsten; Weinigel, Martin; Breunig, Hans Georg; Gregory, Axel; Fischer, Peter; Kellner-Höfer, Marcel; Bückle, Rainer

2010-02-01

Two-photon microscopy has been introduced in 1990 [1]. 13 years later, CE-marked clinical multiphoton systems for 3D imaging of human skin with subcellular resolution have been launched by the JenLab company with the tomograph DermaInspectTM. In 2010, the second generation of clinical multiphoton tomographs was introduced. The novel mobile multiphoton tomograph MPTflexTM, equipped with a flexible articulated optical arm, provides an increased flexibility and accessibility especially for clinical and cosmetical examinations. The multiphoton excitation of fluorescent biomolecules like NAD(P)H, flavins, porphyrins, elastin, and melanin as well as the second harmonic generation of collagen is induced by picojoule femtosecond laser pulses from an tunable turn-key near infrared laser system. The ability for rapid highquality image acquisition, the user-friendly operation of the system, and the compact and flexible design qualifies this system to be used for melanoma detection, diagnostics of dermatological disorders, cosmetic research, and skin aging measurements as well as in situ drug monitoring and animal research. So far, more than 1,000 patients and volunteers have been investigated with the multiphoton tomographs in Europe, Asia, and Australia.

Amplitudes for multiphoton quantum processes in linear optics

NASA Astrophysics Data System (ADS)

Urías, Jesús

2011-07-01

The prominent role that linear optical networks have acquired in the engineering of photon states calls for physically intuitive and automatic methods to compute the probability amplitudes for the multiphoton quantum processes occurring in linear optics. A version of Wick's theorem for the expectation value, on any vector state, of products of linear operators, in general, is proved. We use it to extract the combinatorics of any multiphoton quantum processes in linear optics. The result is presented as a concise rule to write down directly explicit formulae for the probability amplitude of any multiphoton process in linear optics. The rule achieves a considerable simplification and provides an intuitive physical insight about quantum multiphoton processes. The methodology is applied to the generation of high-photon-number entangled states by interferometrically mixing coherent light with spontaneously down-converted light.

Invited Review Article: Imaging techniques for harmonic and multiphoton absorption fluorescence microscopy

PubMed Central

Carriles, Ramón; Schafer, Dawn N.; Sheetz, Kraig E.; Field, Jeffrey J.; Cisek, Richard; Barzda, Virginijus; Sylvester, Anne W.; Squier, Jeffrey A.

2009-01-01

We review the current state of multiphoton microscopy. In particular, the requirements and limitations associated with high-speed multiphoton imaging are considered. A description of the different scanning technologies such as line scan, multifoci approaches, multidepth microscopy, and novel detection techniques is given. The main nonlinear optical contrast mechanisms employed in microscopy are reviewed, namely, multiphoton excitation fluorescence, second harmonic generation, and third harmonic generation. Techniques for optimizing these nonlinear mechanisms through a careful measurement of the spatial and temporal characteristics of the focal volume are discussed, and a brief summary of photobleaching effects is provided. Finally, we consider three new applications of multiphoton microscopy: nonlinear imaging in microfluidics as applied to chemical analysis and the use of two-photon absorption and self-phase modulation as contrast mechanisms applied to imaging problems in the medical sciences. PMID:19725639

Rippled area formed by surface plasmon polaritons upon femtosecond laser double-pulse irradiation of silicon.

PubMed

Derrien, Thibault J-Y; Krüger, Jörg; Itina, Tatiana E; Höhm, Sandra; Rosenfeld, Arkadi; Bonse, Jörn

2013-12-02

The formation of near-wavelength laser-induced periodic surface structures (LIPSS) on silicon upon irradiation with sequences of Ti:sapphire femtosecond laser pulse pairs (pulse duration 150 fs, central wavelength 800 nm) is studied theoretically. For this purpose, the nonlinear generation of conduction band electrons in silicon and their relaxation is numerically calculated using a two-temperature model approach including intrapulse changes of optical properties, transport, diffusion and recombination effects. Following the idea that surface plasmon polaritons (SPP) can be excited when the material turns from semiconducting to metallic state, the "SPP active area" is calculated as function of fluence and double-pulse delay up to several picoseconds and compared to the experimentally observed rippled surface areas. Evidence is presented that multi-photon absorption explains the large increase of the rippled area for temporally overlapping pulses. For longer double-pulse delays, relevant relaxation processes are identified. The results demonstrate that femtosecond LIPSS on silicon are caused by the excitation of SPP and can be controlled by temporal pulse shaping.

Multi-photon EIT

NASA Astrophysics Data System (ADS)

Laarits, Toomas; O'Gorman, Bryan; Crescimanno, Michael

2008-03-01

We describe and solve a quantum optics models for multiphoton interrogation of an electromagnetically induced transparency (EIT) resonance. Multiphoton EIT, like its well studied Lambda-system EIT progenitor, is a generalization of the N-resonance process recently studied for atomic time keeping. The solution of these models allows a preliminary determination of this processes utility as the basis of a frequency standard.

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

Avetissian, H. K.; Avchyan, B. R.; Mkrtchian, G. F.

The multiphoton resonant excitation of three-level atoms by the two laser fields of different frequencies is investigated. The time evolution of the system and analytical solutions expressing Rabi oscillations of the probability amplitudes at the two-color multiphoton resonant excitation are found using a nonperturbative resonant approach. The specific examples for experimental implementation of two-color multiphoton resonant excitation of hydrogen atoms are considered.

Ionization Cross Sections and Dissociation Channels of DNA Bases by Electron Collisions

NASA Technical Reports Server (NTRS)

Huo, Winifred M.; Dateo, Christopher E.; Fletcher, Graham D.

2004-01-01

Free secondary electrons are the most abundant secondary species in ionizing radiation. Their role in DNA damage, both direct and indirect, is an active area of research. While indirect damage by free radicals, particularly by the hydroxyl radical generated by electron collision with water. is relatively well studied, damage by direct electron collision with DNA is less well understood. Only recently Boudaiffa et al. demonstrated that electrons at energies well below ionization thresholds can induce substantial yields of single- and double-strand breaks in DNA by a resonant, dissociative attachment process. This study attracted renewed interest in electron collisions with DNA, especially in the low energy region. At higher energies ionization becomes important. While Monte Carlo track simulations of radiation damage always include ionization, the probability of dissociative ionization, i.e., simultaneous ionization and dissociation, is ignored. Just like dissociative attachment, dissociative ionization may be an important contributor to double-strand breaks since the radicals and ions produced by dissociative ionization, located in the vicinity of the DNA coil, can readily interact with other parts of the DNA. Using the improved binary-encounter dipole (iBED) formulation, we calculated the ionization cross sections of the four DNA bases, adenine, cytosine, guanine, and thymine, by electrons at energies from threshold to 1 KeV. The present calculation gives cross sections approximately 20% lower than the results by Bemhardt and Paretzke using the Deutsch-Mark and Binary-Encounter-Bethe (BEB) formalisms. The difference is most likely due to the lack of a shielding term in the dipole potential used in the Deutsch-Mark and BEB formalisms. The dissociation channels of ionization for the bases are currently being studied.

O({sup 3}P{sub J}) formation and desorption by 157-nm photoirradiation of amorphous solid water

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

DeSimone, Alice J.; Orlando, Thomas M., E-mail: thomas.orlando@chemistry.gatech.edu; School of Physics, Georgia Institute of Technology, Atlanta, Georgia 30332–0400

2014-03-07

Photodissociation of amorphous solid water (ASW) deposited on a thinly oxidized copper substrate at 82 K was studied by measuring O({sup 3}P{sub J=2,1,0}) photoproducts detected with resonance-enhanced multiphoton ionization. For each spin-orbit state, the oxygen atom time-of-flight spectrum was measured as a function of H{sub 2}O exposure, which is related to ice thickness, and 157-nm irradiation time. Four Maxwell-Boltzmann distributions with translational temperatures of 10 000 K, 1800 K, 400 K, and 82 K were found to fit the data. The most likely formation mechanisms are molecular elimination following ionization of water and ion-electron recombination, secondary recombination of hydroxyl radicals, andmore » photodissociation of adsorbed hydroxyl radicals. Evidence for O-atom diffusion through bulk ASW was found for H{sub 2}O exposures of at least 5 Langmuir (1 L = 10{sup −6} Torr s). The cross sections for O({sup 3}P{sub 2}) depletion were 1.3 × 10{sup −19} and 6.5 × 10{sup −20} cm{sup 2} for 1 and 5 L, respectively.« less

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

Barc, B.; Ryszka, M.; Spurrell, J.

Multi-photon ionization (MPI) of the RNA base uracil has been studied in the wavelength range 220–270 nm, coinciding with excitation to the S{sub 2}(ππ*) state. A fragment ion at m/z = 84 was produced by 2-photon absorption at wavelengths ≤232 nm and assigned to C{sub 3}H{sub 4}N{sub 2}O{sup +} following CO abstraction. This ion has not been observed in alternative dissociative ionization processes (notably electron impact) and its threshold is close to recent calculations of the minimum activation energy for a ring opening conical intersection to a σ(n-π)π* closed shell state. Moreover, the predicted ring opening transition leaves a COmore » group at one end of the isomer, apparently vulnerable to abstraction. An MPI mass spectrum of uracil-water clusters is presented for the first time and compared with an equivalent dry measurement. Hydration enhances certain fragment ion pathways (particularly C{sub 3}H{sub 3}NO{sup +}) but represses C{sub 3}H{sub 4}N{sub 2}O{sup +} production. This indicates that hydrogen bonding to water stabilizes uracil with respect to neutral excited-state ring opening.« less

New diagnostic methods for laser plasma- and microwave-enhanced combustion

PubMed Central

Miles, Richard B; Michael, James B; Limbach, Christopher M; McGuire, Sean D; Chng, Tat Loon; Edwards, Matthew R; DeLuca, Nicholas J; Shneider, Mikhail N; Dogariu, Arthur

2015-01-01

The study of pulsed laser- and microwave-induced plasma interactions with atmospheric and higher pressure combusting gases requires rapid diagnostic methods that are capable of determining the mechanisms by which these interactions are taking place. New rapid diagnostics are presented here extending the capabilities of Rayleigh and Thomson scattering and resonance-enhanced multi-photon ionization (REMPI) detection and introducing femtosecond laser-induced velocity and temperature profile imaging. Spectrally filtered Rayleigh scattering provides a method for the planar imaging of temperature fields for constant pressure interactions and line imaging of velocity, temperature and density profiles. Depolarization of Rayleigh scattering provides a measure of the dissociation fraction, and multi-wavelength line imaging enables the separation of Thomson scattering from Rayleigh scattering. Radar REMPI takes advantage of high-frequency microwave scattering from the region of laser-selected species ionization to extend REMPI to atmospheric pressures and implement it as a stand-off detection method for atomic and molecular species in combusting environments. Femtosecond laser electronic excitation tagging (FLEET) generates highly excited molecular species and dissociation through the focal zone of the laser. The prompt fluorescence from excited molecular species yields temperature profiles, and the delayed fluorescence from recombining atomic fragments yields velocity profiles. PMID:26170432

Laser machining of explosives

DOEpatents

Perry, Michael D.; Stuart, Brent C.; Banks, Paul S.; Myers, Booth R.; Sefcik, Joseph A.

2000-01-01

The invention consists of a method for machining (cutting, drilling, sculpting) of explosives (e.g., TNT, TATB, PETN, RDX, etc.). By using pulses of a duration in the range of 5 femtoseconds to 50 picoseconds, extremely precise and rapid machining can be achieved with essentially no heat or shock affected zone. In this method, material is removed by a nonthermal mechanism. A combination of multiphoton and collisional ionization creates a critical density plasma in a time scale much shorter than electron kinetic energy is transferred to the lattice. The resulting plasma is far from thermal equilibrium. The material is in essence converted from its initial solid-state directly into a fully ionized plasma on a time scale too short for thermal equilibrium to be established with the lattice. As a result, there is negligible heat conduction beyond the region removed resulting in negligible thermal stress or shock to the material beyond a few microns from the laser machined surface. Hydrodynamic expansion of the plasma eliminates the need for any ancillary techniques to remove material and produces extremely high quality machined surfaces. There is no detonation or deflagration of the explosive in the process and the material which is removed is rendered inert.

Spatial Characterization of Polycyclic Aromatic Hydrocarbons in 2008 TC3 Samples

NASA Astrophysics Data System (ADS)

Sabbah, Hassan; Morrow, A.; Zare, R. N.; Jenniskens, P.

2009-09-01

Hassan Sabbah1, Amy L. Morrow1, Richard N. Zare1 and Petrus Jenniskens2 1Stanford University, Stanford, California 94305, 2 SETI Institute, Carl Sagan Center, 515 North Whisman Road, Mountain View, California 94043, USA. In October 2006 a small asteroid (2-3 meters) was observed in outer space. On October 7, 2008, it entered the Earth's atmosphere creating a fireball over Northern Sudan. Some 280 meteorites were collected by the University of Khartoum. In order to explore the existence of organic materials, specifically polycyclic aromatic hydrocarbons (PAHs), we applied two-step laser desorption laser ionization mass spectrometry (L2MS) to some selected fragments. This technique consists of desorbing with a pulsed infrared laser beam the solid materials into a gaseous phase with no fragmentation followed by resonance enhanced multiphoton ionization to analyze the PAH content. L2MS was already applied to an array of extraterrestrial objects including interplanetary dust particles IDPs, carbonaceous chondrites and comet coma particles. Moreover, spatial resolution of PAHs in 2008 TC3 samples was achieved to explore the heterogeneity within individual fragments. The results of these studies and their contribution to understanding the formation of this asteroid will be discussed.

Overcritical plasma ignition and diagnostics from oncoming interaction of two color low energy tightly focused femtosecond laser pulses inside fused silica

NASA Astrophysics Data System (ADS)

Potemkin, F. V.; Bravy, B. G.; Bezsudnova, Yu I.; Mareev, E. I.; Starostin, V. M.; Platonenko, V. T.; Gordienko, V. M.

2016-04-01

We report overcritical (3.3  ×  1021 cm-3) microplasma produced by low energy colliding IR (infrared) (1.24 μm) and visible (0.62 μm) femtosecond pulses tightly focused (NA  =  0.5) into the bulk of fused silica with on-line monitoring based on third harmonic generated by the IR beam. It was established that the absorbed energy density is the key parameter that determines the micromodification formation threshold and in our experimental conditions it is close to 4.5 kJ cm-3. Non-monotonic behavior of the third harmonic signal as a function of time delay between visible (0.62 μm) and IR (1.24 μm) femtosecond pulses demonstrates the qualitative differences about the two phenomena: one is the seed electrons generation by the visible pulse via multiphoton ionization and second is the avalanche ionization by the IR pulse. We predict that the tandem two-color excitation of wide-bandgap dielectric in comparison with single-color pulse interaction regime allows providing a much higher absorbed energy density and overcritical plasma.

Multiphoton microscopy and image guided light activated therapy using nanomaterials (Conference Presentation)

NASA Astrophysics Data System (ADS)

Prasad, Paras N.

2017-02-01

This talk will focus on design and applications of nanomaterials exhibiting strong multiphoton upconversion for multiphoton microscopy as well as for image-guided and light activated therapy .1-3 Such processes can occur by truly nonlinear optical interactions proceeding through virtual intermediate states or by stepwise coupled linear excitations through real intermediate states. Multiphoton processes in biocompatible multifunctional nanoparticles allow for 3D deep tissue imaging. In addition, they can produce in-situ photon conversion of deep tissue penetrating near IR light into a needed shorter wavelength light for photo-activated therapy at a targeted site, thus overcoming the limited penetration of UV or visible light into biological media. We are using near IR emitters such as silicon quantum dots which also exhibit strong multiphoton excitation for multiphoton microscopy. Another approach involves nonlinear nanocrystals such as ZnO which can produce four wave mixing, sum frequency generation as well as second harmonic generation to convert a deep tissue penetrating Near IR light at the targeted biological site to a desired shorter wavelength light suitable for bio imaging or activation of a therapy. We have utilized this approach to activate a photosensitizer for photodynamic therapy. Yet another type of upconversion materials is rare-earth ion doped optical nanotransformers which transform a Near IR (NIR) light from an external source by sequential single photon absorption, in situ and on demand, to a needed wavelength. Applications of these nanotransformers in multiphoton photoacoustic imaging will also be presented. An exciting direction pursued by us using these multiphoton nanoparticles, is functional imaging of brain. Simultaneously, they can effect optogenetics for regioselective stimulation of neurons for providing an effective intervention/augmentation strategy to enhance the cognitive state and lead to a foundation for futuristic vision of super human capabilities. Challenges and opportunities will be discussed.

Identification of doubly excited states in nonsequential double ionization of Ar in strong laser fields

NASA Astrophysics Data System (ADS)

Chen, Zhangjin; Li, Xiaojin; Sun, Xiaoli; Hao, Xiaolei; Chen, Jing

2017-12-01

We use the semiclassical model to study the intensity dependence of nonsequential double ionization (NSDI) of Ar in short strong laser pulses. The contributions to NSDI through sequential ionization of doubly excited states (SIDE) are identified by tracking the energy trajectories of the two outgoing electrons. The correlated electron momentum distributions are calculated from which the longitudinal momentum distributions of the fast and the slow electrons for the side-by-side and the back-to-back emissions are obtained. The simulated momentum distributions of the fast and the slow electrons for NSDI of Ar by linearly polarized fields with a wavelength of 795 nm at an intensity of 7 × 1013 W cm-2 are in good agreement with the experimental measurements of Liu et al (2014 Phys. Rev. Lett. 112 013003). We demonstrate that the process of double ionization through SIDE dominates NSDI only when the laser intensities are below the recollision threshold; nevertheless, for higher intensities the SIDE process still takes place although the contribution to the NSDI yields decreases rapidly as the intensity increases. It has been found that for SIDE at different intensities, both the correlated electron momentum spectra and the momentum distributions of the fast and the slow electrons remain the same.

Hydrogenic molecular transitions in double concentric quantum donuts by changing geometrical parameters

NASA Astrophysics Data System (ADS)

Ospina-Londoño, D. A.; Fulla, M. R.; Marín, J. H.

2013-03-01

In this work it is considered a versatile model to study two different ionization processes starting from a D20 homonuclear hydrogenic molecule confined in double concentric quantum donuts. Very narrow quantum donut circular cross sections are considered to separate the radial and angular variables in the D20 Hamiltonian by using the well-known adiabatic approximation D20 total energy as a function of the inter donor spacing and the outer donut center line radius is calculated. The salient features of an artificial D20 hydrogenic molecule such as the dissociation energy and the equilibrium length are strongly dependent on the quantum donut geometrical parameters. By increasing systematically the quantum donut outer center line radius, it is possible to understand a first ionization process: D20→D2++e-. A second ionization process D20→D-+D+ can be carried out by fixing the first donor position and gradually moving away the second one. The results obtained in this study are in good agreement with those previously obtained in the limiting cases of very large inter donor separation. The model proposed here is computationally economical and provides a realistic description of both ionization processes and the few-particle system confined in double concentric quantum donuts.

Dissociative-ionization cross sections for 12-keV-electron impact on CO{sub 2}

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

Bhatt, Pragya; Singh, Raj; Yadav, Namita

The dissociative ionization of a CO{sub 2} molecule is studied at an electron energy of 12 keV using the multiple ion coincidence imaging technique. The absolute partial ionization cross sections and the precursor-specific absolute partial ionization cross sections of resulting fragment ions are obtained and reported. It is found that {approx}75% of single ionization, 22% of double ionization, and {approx}2% of triple ionization of the parent molecule contribute to the total fragment ion yield; quadruple ionization of CO{sub 2} is found to make a negligibly small contribution. Furthermore, the absolute partial ionization cross sections for ion-pair and ion-triple formation aremore » measured for nine dissociative ionization channels of up to a quadruply ionized CO{sub 2} molecule. In addition, the branching ratios for single-ion, ion-pair, and ion-triple formation are also determined.« less

In situ optical measurements for characterization of flame species and remote sensing

NASA Astrophysics Data System (ADS)

Cullum, Brian Michael

1998-12-01

The following dissertation describes the use of spectroscopic techniques for both characterization of combustion intermediates and remote chemical sensing. The primary techniques that have been used for these measurements include, laser-induced fluorescence (LIF), time resolved LIF, resonance enhanced multiphoton ionization (REMPI) and Raman spectroscopy. A simple and quantitative means of measuring the efficiency of halogenated flame retardants is described, using laser-induced fluorescence (LIF). Intensity based LIF measurements of OH radical have been used to quantitatively measure the efficacy of halogenated flame retardant/polymer plaques. Temporally resolved LIF has been used to determine the extent to which the chemical kinetic theory of flame retardation applies to the effect of these compounds on combustion. We have shown that LIF of OH radicals is a very sensitive means of measuring the efficiency of these flame retardants as well as the giving information about the nature of flame retardation. In addition, we have developed a technique for the introduction of insoluble polymer plaques into a flame for fluorescence analysis. A high power pulsed Nd:YAG laser is used to ablate the sample into the flame while a second pulse from a dye laser is used to measure the LIF of OH radicals. Spectroscopic techniques are also very useful for trace remote analysis of environmental pollutants via optical fibers. A simple fiber-optic probe suitable for remote analysis using resonance enhanced multiphoton ionization (REMPI) has been developed for this purpose and is used to determine the toluene/gasoline concentration in water samples via a headspace measurement. The limit of detection for toluene in water using this probe is 0.54 ppb (wt/wt) with a sample standard deviation of 0.02 ppb (wt/wt). Another technique that has great potential for optical sensing is fluorescence lifetime imaging. A new method for measuring fluorescence lifetime images of quickly decaying species has been developed. This method employs a high powered pulsed laser that excites the fluorescent species in a dual pulse manner, and a non-gated charge coupled device (CCD) for detection of the fluorescence. Unlike other fluorescence lifetime imaging methods, this technique has the potential of monitoring fluorescent species with picosecond lifetimes.

Photochemical and Spectroscopic Effects Resulting from Excimer Laser Excitation.

NASA Astrophysics Data System (ADS)

Wang, Xuan Xiao

I. Photochemical production of ozone from pure oxygen using excimer lasers. Production of ozone was observed from experiments when oxygen was under a broadband pulsed KrF laser radiation. The production process was found to be autocatalytic. Mechanisms for the ozone formation were proposed. Experimental results over a range of oxygen pressure and laser pulse energy (irradiance) provided evidences in favor of the proposed mechanisms. Experiments were also numerically modeled. Good agreement between the experimental and the numerical results were observed, which provided further evidence to support the proposed mechanisms. Cross sections for some photochemical processes in the mechanisms were estimated. Production of ozone from pure oxygen under a ArF excimer laser radiation (193 nm) was also studied and numerically modeled. Effects of ambient water vapor on ozone production were investigated. Experimental results showed a fast ozone destruction when water vapor was present in the cell. However, numerical results obtained from the well-known OH and HO _2 chain ozone destruction mechanism predicted a slower ozone destruction. Possible reasons for the discrepancy are discussed. II. Resonance-enhanced multiphoton ionization of N_2 at 193 and 248 nm detected by N_sp{2}{+} fluorescence. Using a broadband excimer laser operating at 193 and 248 nm multiphoton ionization at high pressures in air and pure nitrogen has been detected by fluorescence from N_sp{2}{+} in the B-X firstnegative system. Measurements of the fluorescence intensity as a function of beam irradiance indicate resonance in N_2 at the energy of two 193 nm photons (2 + 1 REMPI) and three 248 nm photons (3 + 1 REMPI). Possible intermediate states are discussed. III. Excimer laser-induced fluorescence from some organic solvents. Fluorescence was observed from vapor phase benzene, toluene, p-xylene, benzyl chloride, methyl benzoate, acetic anhydride, ether, methanol, ethyl acetone, acetone, and 2-butanone using a broadband excimer laser operating at 248 nm and 308 nm as the source of excitation. Absolute fluorescence quantum yields for the substances under study were measured at 248 nm using toluene as the fluorescence standard. Fluorescence spectra from species produced from nonlinear photochemical processes were also studied.

Double gate impact ionization MOS transistor: Proposal and investigation

NASA Astrophysics Data System (ADS)

Yang, Zhaonian; Zhang, Yue; Yang, Yuan; Yu, Ningmei

2017-02-01

In this paper, a double gate impact ionization MOS (DG-IMOS) transistor with improved performance is proposed and investigated by TCAD simulation. In the proposed design, a second gate is introduced in a conventional impact ionization MOS (IMOS) transistor that lengthens the equivalent channel length and suppresses the band-to-band tunneling. The OFF-state leakage current is reduced by over four orders of magnitude. At the ON-state, the second gate is negatively biased in order to enhance the electric field in the intrinsic region. As a result, the operating voltage does not increase with the increase in the channel length. The simulation result verifies that the proposed DG-IMOS achieves a better switching characteristic than the conventional is achieved. Lastly, the application of the DG-IMOS is discussed theoretically.

Single-shot carrier-envelope-phase-tagged ion-momentum imaging of nonsequential double ionization of argon in intense 4-fs laser fields

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

Johnson, Nora G.; Herrwerth, O.; Wirth, A.

2011-01-15

Single-shot carrier-envelope-phase (CEP) tagging is combined with a reaction mircoscope (REMI) to investigate CEP-dependent processes in atoms. Excellent experimental stability and data acquisition longevity are achieved. Using this approach, we study the CEP effects for nonsequential double ionization of argon in 4-fs laser fields at 750 nm and an intensity of 1.6x10{sup 14} W/cm{sup 2}. The Ar{sup 2+} ionization yield shows a pronounced CEP dependence which compares well with recent theoretical predictions employing quantitative rescattering theory [S. Micheau et al., Phys. Rev. A 79, 013417 (2009)]. Furthermore, we find strong CEP influences on the Ar{sup 2+} momentum spectra along themore » laser polarization axis.« less

Double proton transfer behavior and one-electron oxidation effect in double H-bonded glycinamide-formic acid complex.

PubMed

Li, Ping; Bu, Yuxiang

2004-11-22

The behavior of double proton transfer occurring in a representative glycinamide-formic acid complex has been investigated at the B3LYP/6-311 + + G( * *) level of theory. Thermodynamic and, especially, kinetic parameters, such as tautomeric energy, equilibrium constant, and barrier heights have been discussed, respectively. The relevant quantities involved in the double proton transfer process, such as geometrical changes, interaction energies, and intrinsic reaction coordinate calculations have also been studied. Computational results show that the participation of a formic acid molecule favors the proceeding of the proton transfer for glycinamide compared with that without mediate-assisted case. The double proton transfer process proceeds with a concerted mechanism rather than a stepwise one since no ion-pair complexes have been located during the proton transfer process. The calculated barrier heights are 11.48 and 0.85 kcal/mol for the forward and reverse directions, respectively. However, both of them have been reduced by 2.95 and 2.61 kcal/mol to 8.53 and -1.76 kcal/mol if further inclusion of zero-point vibrational energy corrections, where the negative barrier height implies that the reverse reaction should proceed with barrierless spontaneously, analogous to that occurring between glycinamide and formamide. Furthermore, solvent effects on the thermodynamic and kinetic processes have also been predicted qualitatively employing the isodensity surface polarized continuum model within the framework of the self-consistent reaction field theory. Additionally, the oxidation process for the double H-bonded glycinamide-formic acid complex has also been investigated. Contrary to that neutral form possessing a pair of two parallel intermolecular H bonds, only a single H bond with a comparable strength has been found in its ionized form. The vertical and adiabatic ionization potentials for the neutral complex have been determined to be about 9.40 and 8.69 eV, respectively, where ionization is mainly localized on the glycinamide fragment. Like that ionized glycinamide-formamide complex, the proton transfer in the ionized complex is characterized by a single-well potential, implying that the proton initially attached to amide N4 in the glycinamide fragment cannot be transferred to carbonyl O13 in the formic acid fragment at the geometry of the optimized complex. Copyright 2004 American Institute of Physics.

Multiphoton excitation and high-harmonics generation in topological insulator.

PubMed

Avetissian, H K; Avetissian, A K; Avchyan, B R; Mkrtchian, G F

2018-05-10

Multiphoton interaction of coherent electromagnetic radiation with 2D metallic carriers confined on the surface of the 3D topological insulator is considered. A microscopic theory describing the nonlinear interaction of a strong wave and metallic carriers with many-body Coulomb interaction is developed. The set of integrodifferential equations for the interband polarization and carrier occupation distribution is solved numerically. Multiphoton excitation of Fermi-Dirac sea of 2D massless carriers is considered for a THz pump wave. It is shown that in the moderately strong pump wave field along with multiphoton interband/intraband transitions the intense radiation of high harmonics takes place.

Multiphoton excitation and high-harmonics generation in topological insulator

NASA Astrophysics Data System (ADS)

Avetissian, H. K.; Avetissian, A. K.; Avchyan, B. R.; Mkrtchian, G. F.

2018-05-01

Multiphoton interaction of coherent electromagnetic radiation with 2D metallic carriers confined on the surface of the 3D topological insulator is considered. A microscopic theory describing the nonlinear interaction of a strong wave and metallic carriers with many-body Coulomb interaction is developed. The set of integrodifferential equations for the interband polarization and carrier occupation distribution is solved numerically. Multiphoton excitation of Fermi–Dirac sea of 2D massless carriers is considered for a THz pump wave. It is shown that in the moderately strong pump wave field along with multiphoton interband/intraband transitions the intense radiation of high harmonics takes place.

Computational code in atomic and nuclear quantum optics: Advanced computing multiphoton resonance parameters for atoms in a strong laser field

NASA Astrophysics Data System (ADS)

Glushkov, A. V.; Gurskaya, M. Yu; Ignatenko, A. V.; Smirnov, A. V.; Serga, I. N.; Svinarenko, A. A.; Ternovsky, E. V.

2017-10-01

The consistent relativistic energy approach to the finite Fermi-systems (atoms and nuclei) in a strong realistic laser field is presented and applied to computing the multiphoton resonances parameters in some atoms and nuclei. The approach is based on the Gell-Mann and Low S-matrix formalism, multiphoton resonance lines moments technique and advanced Ivanov-Ivanova algorithm of calculating the Green’s function of the Dirac equation. The data for multiphoton resonance width and shift for the Cs atom and the 57Fe nucleus in dependence upon the laser intensity are listed.

In vivo multiphoton imaging of human skin: assessment of topical corticosteroid-induced epidermis atrophy and depigmentation

NASA Astrophysics Data System (ADS)

Ait El Madani, Hassan; Tancrède-Bohin, Emmanuelle; Bensussan, Armand; Colonna, Anne; Dupuy, Alain; Bagot, Martine; Pena, Ana-Maria

2012-02-01

Multiphoton microscopy has emerged in the past decade as a promising tool for noninvasive skin imaging. Our aim was to evaluate the potential of multiphoton microscopy to detect topical corticosteroids side effects within the epidermis and to provide new insights into their dynamics. Healthy volunteers were topically treated with clobetasol propionate on a small region of their forearms under overnight occlusion for three weeks. The treated region of each patient was investigated at D0, D7, D15, D22 (end of the treatment), and D60. Our study shows that multiphoton microscopy allows for the detection of corticoid-induced epidermis modifications: thinning of stratum corneum compactum and epidermis, decrease of keratinocytes size, and changes in their morphology from D7 to D22. We also show that multiphoton microscopy enables in vivo three-dimensional (3-D) quantitative assessment of melanin content. We observe that melanin density decreases during treatment and almost completely disappears at D22. Moreover, these alterations are reversible as they are no longer present at D60. Our study demonstrates that multiphoton microscopy is a convenient and powerful tool for noninvasive 3-D dynamical studies of skin integrity and pigmentation.

Footprints of electron correlation in strong-field double ionization of Kr close to the sequential-ionization regime

NASA Astrophysics Data System (ADS)

Li, Xiaokai; Wang, Chuncheng; Yuan, Zongqiang; Ye, Difa; Ma, Pan; Hu, Wenhui; Luo, Sizuo; Fu, Libin; Ding, Dajun

2017-09-01

By combining kinematically complete measurements and a semiclassical Monte Carlo simulation we study the correlated-electron dynamics in the strong-field double ionization of Kr. Interestingly, we find that, as we step into the sequential-ionization regime, there are still signatures of correlation in the two-electron joint momentum spectrum and, more intriguingly, the scaling law of the high-energy tail is completely different from early predictions on the low-Z atom (He). These experimental observations are well reproduced by our generalized semiclassical model adapting a Green-Sellin-Zachor potential. It is revealed that the competition between the screening effect of inner-shell electrons and the Coulomb focusing of nuclei leads to a non-inverse-square central force, which twists the returned electron trajectory at the vicinity of the parent core and thus significantly increases the probability of hard recollisions between two electrons. Our results might have promising applications ranging from accurately retrieving atomic structures to simulating celestial phenomena in the laboratory.

Electron-electron correlation in two-photon double ionization of He-like ions

NASA Astrophysics Data System (ADS)

Hu, S. X.

2018-01-01

Electron correlation plays a crucial role in quantum many-body physics ranging from molecular bonding and strong-field-induced multielectron ionization, to superconducting in materials. Understanding the dynamic electron correlation in the photoionization of relatively simple quantum three-body systems, such as He and He-like ions, is an important step toward manipulating complex systems through photoinduced processes. Here we have performed ab initio investigations of two-photon double ionization (TPDI) of He and He-like ions (L i+,B e2 + , and C4 +) exposed to intense attosecond x-ray pulses. Results from such fully correlated quantum calculations show weaker and weaker electron correlation effects in TPDI spectra as the ionic charge increases, which is opposite to the intuition that the absolute increase of correlation in the ground state should lead to more equal energy sharing in photoionization. These findings indicate that the final-state electron-electron correlation ultimately determines the energy sharing of the two ionized electrons in TPDI.

Light/negative bias stress instabilities in indium gallium zinc oxide thin film transistors explained by creation of a double donor

NASA Astrophysics Data System (ADS)

Migliorato, Piero; Delwar Hossain Chowdhury, Md; Gwang Um, Jae; Seok, Manju; Jang, Jin

2012-09-01

The analysis of current-voltage (I-V) and capacitance-voltage (C-V) characteristics for amorphous indium gallium zinc oxide Thin film transistors as a function of active layer thickness shows that negative bias under illumination stress (NBIS) is quantitatively explained by creation of a bulk double donor, with a shallow singly ionized state ɛ(0/+) > EC-0.073 eV and a deep doubly ionized state ɛ(++/+) < EC-0.3 eV. The gap density of states, extracted from the capacitance-voltage curves, shows a broad peak between EC-E = 0.3 eV and 1.0 eV, which increases in height with NBIS stress time and corresponds to the broadened transition energy between singly and doubly ionized states. We propose that the center responsible is an oxygen vacancy and that the presence of a stable singly ionized state, necessary to explain our experimental results, could be due to the defect environment provided by the amorphous network.

New developments in multimodal clinical multiphoton tomography

NASA Astrophysics Data System (ADS)

König, Karsten

2011-03-01

80 years ago, the PhD student Maria Goeppert predicted in her thesis in Goettingen, Germany, two-photon effects. It took 30 years to prove her theory, and another three decades to realize the first two-photon microscope. With the beginning of this millennium, first clinical multiphoton tomographs started operation in research institutions, hospitals, and in the cosmetic industry. The multiphoton tomograph MPTflexTM with its miniaturized flexible scan head became the Prism-Award 2010 winner in the category Life Sciences. Multiphoton tomographs with its superior submicron spatial resolution can be upgraded to 5D imaging tools by adding spectral time-correlated single photon counting units. Furthermore, multimodal hybrid tomographs provide chemical fingerprinting and fast wide-field imaging. The world's first clinical CARS studies have been performed with a hybrid multimodal multiphoton tomograph in spring 2010. In particular, nonfluorescent lipids and water as well as mitochondrial fluorescent NAD(P)H, fluorescent elastin, keratin, and melanin as well as SHG-active collagen have been imaged in patients with dermatological disorders. Further multimodal approaches include the combination of multiphoton tomographs with low-resolution imaging tools such as ultrasound, optoacoustic, OCT, and dermoscopy systems. Multiphoton tomographs are currently employed in Australia, Japan, the US, and in several European countries for early diagnosis of skin cancer (malignant melanoma), optimization of treatment strategies (wound healing, dermatitis), and cosmetic research including long-term biosafety tests of ZnO sunscreen nanoparticles and the measurement of the stimulated biosynthesis of collagen by anti-ageing products.

Multiphoton entanglement concentration and quantum cryptography.

PubMed

Durkin, Gabriel A; Simon, Christoph; Bouwmeester, Dik

2002-05-06

Multiphoton states from parametric down-conversion can be entangled both in polarization and photon number. Maximal high-dimensional entanglement can be concentrated postselectively from these states via photon counting. This makes them natural candidates for quantum key distribution, where the presence of more than one photon per detection interval has up to now been considered undesirable. We propose a simple multiphoton cryptography protocol for the case of low losses.

Distinguishing human normal or cancerous esophagus tissue ex vivo using multiphoton microscopy

NASA Astrophysics Data System (ADS)

Liu, N. R.; Chen, G. N.; Wu, S. S.; Chen, R.

2014-02-01

Application of multiphoton microscopy (MPM) to clinical cancer research has greatly developed over the last few years. In this paper, we mainly focus on two-photon excitation fluorescence (TPEF) and second harmonic generation (SHG) for investigating esophageal cancer. We chiefly discuss the SHG/TPEF image and spectral characteristics of normal and cancerous esophagus submucosa with the combined multi-channel imaging mode and Lambda mode of a multiphoton microscope (LSM 510 META). Great differences can be detected, such as collagen content and morphology, glandular-shaped cancer cells, TPEF/SHG intensity ratio, and so on, which demonstrate that the multiphoton imaging technique has the potential ability for minimally-invasive early cancer diagnosis.

Photodissociation of Non-Covalent Peptide-Crown Ether Complexes

PubMed Central

Wilson, Jeffrey J.; Kirkovits, Gregory J.; Sessler, Jonathan L.; Brodbelt, Jennifer S.

2008-01-01

Highly chromogenic 18-crown-6-dipyrrolylquinoxaline coordinates primary amines of peptides, forming non-covalent complexes that can be transferred to the gas phase by electrospray ionization. The appended chromogenic crown ether facilitates efficient energy transfer to the peptide upon ultraviolet irradiation in the gas phase, resulting in diagnostic peptide fragmentation. Collisional activated dissociation (CAD) and infrared multiphoton dissociation (IRMPD) of these non-covalent complexes results only in their disassembly with the charge retained on either the peptide or crown ether, yielding no sequence ions. Upon UV photon absorption the intermolecular energy transfer is facilitated by the fast activation time scale of UVPD (< 10 ns) and by the collectively strong hydrogen bonding between the crown ether and peptide, thus allowing effective transfer of energy to the peptide moiety prior to disruption of the intermolecular hydrogen bonds. PMID:18077179

Fingerprints of Both Watson-Crick and Hoogsteen Isomers of the Isolated (Cytosine-Guanine)H+ Pair.

PubMed

Cruz-Ortiz, Andrés F; Rossa, Maximiliano; Berthias, Francis; Berdakin, Matías; Maitre, Philippe; Pino, Gustavo A

2017-11-16

 Gas phase protonated guanine-cytosine (CGH + ) pair was generated using an electrospray ionization source from solutions at two different pH (5.8 and 3.2). Consistent evidence from MS/MS fragmentation patterns and differential ion mobility spectra (DIMS) point toward the presence of two isomers of the CGH + pair, whose relative populations depend strongly on the pH of the solution. Gas phase infrared multiphoton dissociation (IRMPD) spectroscopy in the 900-1900 cm -1 spectral range further confirms that the Watson-Crick isomer is preferentially produced (91%) at pH = 5.8, while the Hoogsteen isomer predominates (66%) at pH = 3.2). These fingerprint signatures are expected to be useful for the development of new analytical methodologies and to trigger isomer selective photochemical studies of protonated DNA base pairs.

Torsional, Vibrational and Vibration-Torsional Levels in the S_{1} and Ground Cationic D_{0}^{+} States of Para-Fluorotoluene

NASA Astrophysics Data System (ADS)

Gardner, Adrian M.; Tuttle, William Duncan; Whalley, Laura E.; Claydon, Andrew; Carter, Joseph H.; Wright, Timothy G.

2017-06-01

The S_{1} electronic state and ground state of the cation of para-fluorotoluene (pFT) have been investigated using resonance-enhanced multiphoton ionization (REMPI) spectroscopy and zero-kinetic-energy (ZEKE) spectroscopy. Here we focus on the low wavenumber region where a number of "pure" torsional, fundamental vibrational and vibration-torsional levels are expected; assignments of observed transitions are discussed, which are compared to results of published work on toluene (methylbenzene) from the Lawrance group. The similarity in the activity observed in the excitation spectrum of the two molecules is striking. A. M. Gardner, W. D. Tuttle, L. Whalley, A. Claydon, J. H. Carter and T. G. Wright, J. Chem. Phys., 145, 124307 (2016). J. R. Gascooke, E. A. Virgo, and W. D. Lawrance J. Chem. Phys., 143, 044313 (2015).

Strong Field Theories beyond Dipole Approximations in Nonrelativistic Regimes

NASA Astrophysics Data System (ADS)

He, Pei-Lun; Lao, Di; He, Feng

2017-04-01

The exact nondipole Volkov solutions to the Schrödinger equation and Pauli equation are found, based on which a strong field theory beyond the dipole approximation is built for describing the nondipole effects in nonrelativistic laser driven electron dynamics. This theory is applied to investigate momentum partition laws for multiphoton and tunneling ionization and explicitly shows that the complex interplay of a laser field and Coulomb action may reverse the expected photoelectron momentum along the laser propagation direction. The magnetic-spin coupling does not bring observable effects on the photoelectron momentum distribution and can be neglected. Compared to the strong field approximation within the dipole approximation, this theory works in a much wider range of laser parameters and lays a solid foundation for describing nonrelativistic electron dynamics in both short wavelength and midinfrared regimes where nondipole effects are unavoidable.

Photoelectron spectrometer for liquid and gas-phase attosecond spectroscopy with field-free and magnetic bottle operation modes

NASA Astrophysics Data System (ADS)

Jordan, Inga; Jain, Arohi; Gaumnitz, Thomas; Ma, Jun; Wörner, Hans Jakob

2018-05-01

A compact time-of-flight spectrometer for applications in attosecond spectroscopy in the liquid and gas phases is presented. It allows for altering the collection efficiency by transitioning between field-free and magnetic-bottle operation modes. High energy resolution (ΔE/E = 0.03 for kinetic energies >20 eV) is achieved despite the short flight-tube length through a homogeneous deceleration potential at the beginning of the flight tube. A closing mechanism allows isolating the vacuum system of the flight tube from the interaction region in order to efficiently perform liquid-microjet experiments. The capabilities of the instrument are demonstrated through photoelectron spectra from multiphoton ionization of argon and xenon, as well as photoelectron spectra of liquid and gaseous water generated by an attosecond pulse train.

Physical processes associated with current collection by plasma contactors

NASA Technical Reports Server (NTRS)

Katz, Ira; Davis, Victoria A.

1990-01-01

Recent flight data confirms laboratory observations that the release of neutral gas increases plasma sheath currents. Plasma contactors are devices which release a partially ionized gas in order to enhance the current flow between a spacecraft and the space plasma. Ionization of the expellant gas and the formation of a double layer between the anode plasma and the space plasma are the dominant physical processes. A theory is presented of the interaction between the contactor plasma and the background plasma. The conditions for formation of a double layer between the two plasmas are derived. Double layer formation is shown to be a consequence of the nonlinear response of the plasmas to changes in potential. Numerical calculations based upon this model are compared with laboratory measurements of current collection by hollow cathode-based plasma contactors.

State-resolved three-dimensional electron-momentum correlation in nonsequential double ionization of benzene

NASA Astrophysics Data System (ADS)

Winney, Alexander H.; Lin, Yun Fei; Lee, Suk Kyoung; Adhikari, Pradip; Li, Wen

2016-03-01

We report state-resolved electron-momentum correlation measurement of strong-field nonsequential double ionization in benzene. With a novel coincidence detection apparatus, highly efficient triple coincidence (electron-electron dication) and quadruple coincidence (electron-electron-cation-cation) are used to resolve the final ionic states and to characterize three-dimensional (3D) electron-momentum correlation. The primary states associated with dissociative and nondissociative dications are assigned. A 3D momentum anticorrelation is observed for the electrons in coincidence with dissociative benzene dication states whereas such a correlation is absent for nondissociative dication states.

Double ionization of neon in elliptically polarized femtosecond laser fields

NASA Astrophysics Data System (ADS)

Kang, HuiPeng; Henrichs, Kevin; Wang, YanLan; Hao, XiaoLei; Eckart, Sebastian; Kunitski, Maksim; Schöffler, Markus; Jahnke, Till; Liu, XiaoJun; Dörner, Reinhard

2018-06-01

We present a joint experimental and theoretical investigation of the correlated electron momentum spectra from strong-field double ionization of neon induced by elliptically polarized laser pulses. A significant asymmetry of the electron momentum distributions along the major polarization axis is reported. This asymmetry depends sensitively on the laser ellipticity. Using a three-dimensional semiclassical model, we attribute this asymmetry pattern to the ellipticity-dependent probability distributions of recollision time. Our work demonstrates that, by simply varying the ellipticity, the correlated electron emission can be two-dimensionally controlled and the recolliding electron trajectories can be steered on a subcycle time scale.

Diode-laser-based RIMS measurements of strontium-90

NASA Astrophysics Data System (ADS)

Bushaw, B. A.; Cannon, B. D.

1998-12-01

Double- and triple-resonance excitation schemes for the ionization of strontium are presented. Use of single-mode diode lasers for the resonance excitations provides a high degree of optical isotopic selectivity: with double-resonance, selectivity of >104 for 90Sr against the stable Sr isotopes has been demonstrated. Measurement of lineshapes and stable isotope shifts in the triple-resonance process indicate that optical selectivity should increase to ˜109. When combined with mass spectrometer selectivity this is sufficient for measurement of 90Sr at background environmental levels. Additionally, autoionizing resonances have been investigated for improving ionization efficiency with lower power lasers.

Self-referenced axial chromatic dispersion measurement in multiphoton microscopy through 2-color THG imaging.

PubMed

Du, Yu; Zhuang, Ziwei; He, Jiexing; Liu, Hongji; Qiu, Ping; Wang, Ke

2018-05-16

With tunable excitation light, multiphoton microscopy (MPM) is widely used for imaging biological structures at subcellular resolution. Axial chromatic dispersion, present in virtually every transmissive optical system including the multiphoton microscope, leads to focal (and the resultant image) plane separation. Here we demonstrate experimentally a technique to measure the axial chromatic dispersion in a multiphoton microscope, using simultaneous 2-color third-harmonic generation (THG) imaging excited by a 2-color soliton source with tunable wavelength separation. Our technique is self-referenced, eliminating potential measurement error when 1-color tunable excitation light is used which necessitates reciprocating motion of the mechanical translation stage. Using this technique, we demonstrate measured axial chromatic dispersion with 2 different objective lenses in a multiphoton microscope. Further measurement in a biological sample also indicates that this axial chromatic dispersion, in combination with 2-color imaging, may open up opportunity for simultaneous imaging of two different axial planes. This article is protected by copyright. All rights reserved. This article is protected by copyright. All rights reserved.

Spatiotemporal focusing-based widefield multiphoton microscopy for fast optical sectioning of thick tissues

NASA Astrophysics Data System (ADS)

Cheng, Li-Chung; Chang, Chia-Yuan; Yen, Wei-Chung; Chen, Shean-Jen

2012-10-01

Conventional multiphoton microscopy employs beam scanning; however, in this study a microscope based on spatiotemporal focusing offering widefield multiphoton excitation has been developed to provide fast optical sectioning images. The microscope integrates a 10 kHz repetition rate ultrafast amplifier featuring strong instantaneous peak power (maximum 400 μJ/pulse at 90 fs pulse width) with a TE-cooled, ultra-sensitive photon detecting, electron multiplying charge-coupled device camera. This configuration can produce multiphoton excited images with an excitation area larger than 200 × 100 μm2 at a frame rate greater than 100 Hz. Brownian motions of fluorescent microbeads as small as 0.5 μm have been instantaneously observed with a lateral spatial resolution of less than 0.5 μm and an axial resolution of approximately 3.5 μm. Moreover, we combine the widefield multiphoton microscopy with structure illuminated technique named HiLo to reject the background scattering noise to get better quality for bioimaging.

Nanoparticle-assisted-multiphoton microscopy for in vivo brain imaging of mice

NASA Astrophysics Data System (ADS)

Qian, Jun

2015-03-01

Neuro/brain study has attracted much attention during past few years, and many optical methods have been utilized in order to obtain accurate and complete neural information inside the brain. Relying on simultaneous absorption of two or more near-infrared photons by a fluorophore, multiphoton microscopy can achieve deep tissue penetration and efficient light detection noninvasively, which makes it very suitable for thick-tissue and in vivo bioimaging. Nanoparticles possess many unique optical and chemical properties, such as anti-photobleaching, large multiphoton absorption cross-section, and high stability in biological environment, which facilitates their applications in long-term multiphoton microscopy as contrast agents. In this paper, we will introduce several typical nanoparticles (e.g. organic dye doped polymer nanoparticles and gold nanorods) with high multiphoton fluorescence efficiency. We further applied them in two- and three-photon in vivo functional brain imaging of mice, such as brain-microglia imaging, 3D architecture reconstruction of brain blood vessel, and blood velocity measurement.

Imaging of cardiovascular structures using near-infrared femtosecond multiphoton laser scanning microscopy.

PubMed

Schenke-Layland, Katja; Riemann, Iris; Stock, Ulrich A; König, Karsten

2005-01-01

Multiphoton imaging represents a novel and very promising medical diagnostic technology for the high-resolution analysis of living biological tissues. We performed multiphoton imaging to analyzed structural features of extracellular matrix (ECM) components, e.g., collagen and elastin, of vital pulmonary and aortic heart valves. High-resolution autofluorescence images of collagenous and elastic fibers were demonstrated using multifluorophore, multiphoton excitation at two different wavelengths and optical sectioning, without the requirement of embedding, fixation, or staining. Collagenous structures were selectively imaged by detection of second harmonic generation (SHG). Additionally, routine histology and electron microscopy were integrated to verify the observed results. In comparison with pulmonary tissues, aortic heart valve specimens show very similar matrix formations. The quality of the resulting three-dimensional (3-D) images enabled the differentiation between collagenous and elastic fibers. These experimental results indicate that multiphoton imaging with near-infrared (NIR) femtosecond laser pulses may prove to be a useful tool for the nondestructive monitoring and characterization of cardiovascular structures. Copyright 2005 Society of Photo-Optical Instrumentation Engineers.

Application of Multiphoton Microscopy in Dermatological Studies: a Mini-Review

PubMed Central

Yew, Elijah; Rowlands, Christopher

2014-01-01

This review summarizes the historical and more recent developments of multiphoton microscopy, as applied to dermatology. Multiphoton microscopy offers several advantages over competing microscopy techniques: there is an inherent axial sectioning, penetration depths that compete well with confocal microscopy on account of the use of near-infrared light, and many two-photon contrast mechanisms, such as second-harmonic generation, have no analogue in one-photon microscopy. While the penetration depths of photons into tissue are typically limited on the order of hundreds of microns, this is of less concern in dermatology, as the skin is thin and readily accessible. As a result, multiphoton microscopy in dermatology has generated a great deal of interest, much of which is summarized here. The review covers the interaction of light and tissue, as well as the various considerations that must be made when designing an instrument. The state of multiphoton microscopy in imaging skin cancer and various other diseases is also discussed, along with the investigation of aging and regeneration phenomena, and finally, the use of multiphoton microscopy to analyze the transdermal transport of drugs, cosmetics and other agents is summarized. The review concludes with a look at potential future research directions, especially those that are necessary to push these techniques into widespread clinical acceptance. PMID:25075226

Structure of multiphoton quantum optics. I. Canonical formalism and homodyne squeezed states

NASA Astrophysics Data System (ADS)

dell'Anno, Fabio; de Siena, Silvio; Illuminati, Fabrizio

2004-03-01

We introduce a formalism of nonlinear canonical transformations for general systems of multiphoton quantum optics. For single-mode systems the transformations depend on a tunable free parameter, the homodyne local-oscillator angle; for n -mode systems they depend on n heterodyne mixing angles. The canonical formalism realizes nontrivial mixing of pairs of conjugate quadratures of the electromagnetic field in terms of homodyne variables for single-mode systems, and in terms of heterodyne variables for multimode systems. In the first instance the transformations yield nonquadratic model Hamiltonians of degenerate multiphoton processes and define a class of non-Gaussian, nonclassical multiphoton states that exhibit properties of coherence and squeezing. We show that such homodyne multiphoton squeezed states are generated by unitary operators with a nonlinear time evolution that realizes the homodyne mixing of a pair of conjugate quadratures. Tuning of the local-oscillator angle allows us to vary at will the statistical properties of such states. We discuss the relevance of the formalism for the study of degenerate (up-)down-conversion processes. In a companion paper [

Structure of multiphoton quantum optics. I. Canonical formalism and homodyne squeezed states

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

Dell'Anno, Fabio; De Siena, Silvio; Illuminati, Fabrizio

2004-03-01

We introduce a formalism of nonlinear canonical transformations for general systems of multiphoton quantum optics. For single-mode systems the transformations depend on a tunable free parameter, the homodyne local-oscillator angle; for n-mode systems they depend on n heterodyne mixing angles. The canonical formalism realizes nontrivial mixing of pairs of conjugate quadratures of the electromagnetic field in terms of homodyne variables for single-mode systems, and in terms of heterodyne variables for multimode systems. In the first instance the transformations yield nonquadratic model Hamiltonians of degenerate multiphoton processes and define a class of non-Gaussian, nonclassical multiphoton states that exhibit properties of coherencemore » and squeezing. We show that such homodyne multiphoton squeezed states are generated by unitary operators with a nonlinear time evolution that realizes the homodyne mixing of a pair of conjugate quadratures. Tuning of the local-oscillator angle allows us to vary at will the statistical properties of such states. We discuss the relevance of the formalism for the study of degenerate (up-)down-conversion processes. In a companion paper [F. Dell'Anno, S. De Siena, and F. Illuminati, 69, 033813 (2004)], we provide the extension of the nonlinear canonical formalism to multimode systems, we introduce the associated heterodyne multiphoton squeezed states, and we discuss their possible experimental realization.« less

DNA Damage by Ionizing Radiation: Tandem Double Lesions by Charged Particles

NASA Technical Reports Server (NTRS)

Huo, Winifred M.; Chaban, Galina M.; Wang, Dunyou; Dateo, Christopher E.

2005-01-01

Oxidative damages by ionizing radiation are the source of radiation-induced carcinogenesis, damage to the central nervous system, lowering of the immune response, as well as other radiation-induced damages to human health. Monte Carlo track simulations and kinetic modeling of radiation damages to the DNA employ available molecular and cellular data to simulate the biological effect of high and low LET radiation io the DNA. While the simulations predict single and double strand breaks and base damages, so far all complex lesions are the result of stochastic coincidence from independent processes. Tandem double lesions have not yet been taken into account. Unlike the standard double lesions that are produced by two separate attacks by charged particles or radicals, tandem double lesions are produced by one single attack. The standard double lesions dominate at the high dosage regime. On the other hand, tandem double lesions do not depend on stochastic coincidences and become important at the low dosage regime of particular interest to NASA. Tandem double lesions by hydroxyl radical attack of guanine in isolated DNA have been reported at a dosage of radiation as low as 10 Gy. The formation of two tandem base lesions was found to be linear with the applied doses, a characteristic of tandem lesions. However, tandem double lesions from attack by a charged particle have not been reported.

Electron-Atom Ionization Calculations using Propagating Exterior Complex Scaling

NASA Astrophysics Data System (ADS)

Bartlett, Philip

2007-10-01

The exterior complex scaling method (Science 286 (1999) 2474), pioneered by Rescigno, McCurdy and coworkers, provided highly accurate ab initio solutions for electron-hydrogen collisions by directly solving the time-independent Schr"odinger equation in coordinate space. An extension of this method, propagating exterior complex scaling (PECS), was developed by Bartlett and Stelbovics (J. Phys. B 37 (2004) L69, J. Phys. B 39 (2006) R379) and has been demonstrated to provide computationally efficient and accurate calculations of ionization and scattering cross sections over a large range of energies below, above and near the ionization threshold. An overview of the PECS method for three-body collisions and the computational advantages of its propagation and iterative coupling techniques will be presented along with results of: (1) near-threshold ionization of electron-hydrogen collisions and the Wannier threshold laws, (2) scattering cross section resonances below the ionization threshold, and (3) total and differential cross sections for electron collisions with excited targets and hydrogenic ions from low through to high energies. Recently, the PECS method has been extended to solve four-body collisions using time-independent methods in coordinate space and has initially been applied to the s-wave model for electron-helium collisions. A description of the extensions made to the PECS method to facilitate these significantly more computationally demanding calculations will be given, and results will be presented for elastic, single-excitation, double-excitation, single-ionization and double-ionization collisions.

Clustered DNA damages induced in isolated DNA and in human cells by low doses of ionizing radiation

NASA Technical Reports Server (NTRS)

Sutherland, B. M.; Bennett, P. V.; Sidorkina, O.; Laval, J.; Lowenstein, D. I. (Principal Investigator)

2000-01-01

Clustered DNA damages-two or more closely spaced damages (strand breaks, abasic sites, or oxidized bases) on opposing strands-are suspects as critical lesions producing lethal and mutagenic effects of ionizing radiation. However, as a result of the lack of methods for measuring damage clusters induced by ionizing radiation in genomic DNA, neither the frequencies of their production by physiological doses of radiation, nor their repairability, nor their biological effects are known. On the basis of methods that we developed for quantitating damages in large DNAs, we have devised and validated a way of measuring ionizing radiation-induced clustered lesions in genomic DNA, including DNA from human cells. DNA is treated with an endonuclease that induces a single-strand cleavage at an oxidized base or abasic site. If there are two closely spaced damages on opposing strands, such cleavage will reduce the size of the DNA on a nondenaturing gel. We show that ionizing radiation does induce clustered DNA damages containing abasic sites, oxidized purines, or oxidized pyrimidines. Further, the frequency of each of these cluster classes is comparable to that of frank double-strand breaks; among all complex damages induced by ionizing radiation, double-strand breaks are only about 20%, with other clustered damage constituting some 80%. We also show that even low doses (0.1-1 Gy) of high linear energy transfer ionizing radiation induce clustered damages in human cells.

A pragmatic guide to multiphoton microscope design

PubMed Central

Young, Michael D.; Field, Jeffrey J.; Sheetz, Kraig E.; Bartels, Randy A.; Squier, Jeff

2016-01-01

Multiphoton microscopy has emerged as a ubiquitous tool for studying microscopic structure and function across a broad range of disciplines. As such, the intent of this paper is to present a comprehensive resource for the construction and performance evaluation of a multiphoton microscope that will be understandable to the broad range of scientific fields that presently exploit, or wish to begin exploiting, this powerful technology. With this in mind, we have developed a guide to aid in the design of a multiphoton microscope. We discuss source selection, optical management of dispersion, image-relay systems with scan optics, objective-lens selection, single-element light-collection theory, photon-counting detection, image rendering, and finally, an illustrated guide for building an example microscope. PMID:27182429

Generation of single- and two-mode multiphoton states in waveguide QED

NASA Astrophysics Data System (ADS)

Paulisch, V.; Kimble, H. J.; Cirac, J. I.; González-Tudela, A.

2018-05-01

Single- and two-mode multiphoton states are the cornerstone of many quantum technologies, e.g., metrology. In the optical regime, these states are generally obtained combining heralded single photons with linear optics tools and post-selection, leading to inherent low success probabilities. In a recent paper [A. González-Tudela et al., Phys. Rev. Lett. 118, 213601 (2017), 10.1103/PhysRevLett.118.213601], we design several protocols that harness the long-range atomic interactions induced in waveguide QED to improve fidelities and protocols of single-mode multiphoton emission. Here, we give full details of these protocols, revisit them to simplify some of their requirements, and also extend them to generate two-mode multiphoton states, such as Yurke or NOON states.

Ex-vivo multiphoton analysis of rabbit corneal wound healing following photorefractive keratectomy

NASA Astrophysics Data System (ADS)

Wang, Tsung-Jen; Lo, Wen; Dong, Chen-Yuan; Hu, Fung-Rong

2008-02-01

The aim of this study is to assess the application of multiphoton autofluorescence and second harmonic generation (SHG) microscopy for investigating corneal wound healing after high myopic (-10.0D) photorefractive keratectomy (PRK) procedures on the rabbit eyes. The effect of PRK on the morphology and distribution of keratocytes were investigated using multiphoton excited autofluorescence imaging, while the effect of PRK on the arrangement of collagen fibers was monitored by second-harmonic generation imaging. Without histological processing, multiphoton microscopy is able to characterize corneal damage and wound healing from PRK. Our results show that this technique has potential application in the clinical evaluation of corneal damage due to refractive surgery, and may be used to study the unwanted side effects of these procedures.

Non-thermal near-infrared exposure photobiomodulates cellular responses to ionizing radiation in human full thickness skin models.

PubMed

König, Anke; Zöller, Nadja; Kippenberger, Stefan; Bernd, August; Kaufmann, Roland; Layer, Paul G; Heselich, Anja

2018-01-01

Ionizing and near-infrared radiation are both part of the therapeutic spectrum in cancer treatment. During cancer therapy ionizing radiation is typically used for non-invasive reduction of malignant tissue, while near-infrared photobiomodulation is utilized in palliative medical approaches, e.g. for pain reduction or impairment of wound healing. Furthermore, near-infrared is part of the solar wavelength spectrum. A combined exposure of these two irradiation qualities - either intentionally during medical treatment or unintentionally due to solar exposure - is therefore presumable for cancer patients. Several studies in different model organisms and cell cultures show a strong impact of near-infrared pretreatment on ionizing radiation-induced stress response. To investigate the risks of non-thermal near-infrared (NIR) pretreatment in patients, a human in vitro full thickness skin models (FTSM) was evaluated for radiation research. FTSM were pretreated with therapy-relevant doses of NIR followed by X-radiation, and then examined for DNA-double-strand break (DSB) repair, cell proliferation and apoptosis. Double-treated FTSM revealed a clear influence of NIR on X-radiation-induced stress responses in cells in their typical tissue environment. Furthermore, over a 24h time period, double-treated FTSM presented a significant persistence of DSBs, as compared to samples exclusively irradiated by X-rays. In addition, NIR pretreatment inhibited apoptosis induction of integrated fibroblasts, and counteracted the radiation-induced proliferation inhibition of basal keratinocytes. Our work suggests that cancer patients treated with X-rays should be prevented from uncontrolled NIR irradiation. On the other hand, controlled double-treatment could provide an alternative therapy approach, exposing the patient to less radiation. Copyright © 2017. Published by Elsevier B.V.

Hugoniot measurements of double-shocked precompressed dense xenon plasmas

NASA Astrophysics Data System (ADS)

Zheng, J.; Chen, Q. F.; Gu, Y. J.; Chen, Z. Y.

2012-12-01

The current partially ionized plasmas models for xenon show substantial differences since the description of pressure and thermal ionization region becomes a formidable task, prompting the need for an improved understanding of dense xenon plasmas behavior at above 100 GPa. We performed double-shock compression experiments on dense xenon to determine accurately the Hugoniot up to 172 GPa using a time-resolved optical radiation method. The planar strong shock wave was produced using a flyer plate impactor accelerated up to ˜6 km/s with a two-stage light-gas gun. The time-resolved optical radiation histories were acquired by using a multiwavelength channel optical transience radiance pyrometer. Shock velocity was measured and mass velocity was determined by the impedance-matching methods. The experimental equation of state of dense xenon plasmas are compared with the self-consistent fluid variational calculations of dense xenon in the region of partial ionization over a wide range of pressures and temperatures.

Note: a novel vacuum ultraviolet light source assembly with aluminum-coated electrodes for enhancing the ionization efficiency of photoionization mass spectrometry.

PubMed

Zhu, Zhixiang; Wang, Jian; Qiu, Keqing; Liu, Chengyuan; Qi, Fei; Pan, Yang

2014-04-01

A novel vacuum ultraviolet (VUV) light source assembly (VUVLSA) for enhancing the ionization efficiency of photoionization mass spectrometer has been described. The VUVLSA composes of a Krypton lamp and a pair of disk electrodes with circular center cavities. The two interior surfaces that face the photoionization region were aluminum-coated. VUV light can be reflected back and forth in the photoionization region between the electrodes, thus the photoionization efficiency can be greatly enhanced. The performances of two different shaped electrodes, the coated double flat electrodes (DFE), and double conical electrodes, were studied. We showed that the signal amplification of coated DFE is around 4 times higher than that of uncoated electrodes without VUV light reflection. The relationship between the pressure of ionization chamber and mass signal enhancement has also been studied.

Deep Tissue Fluorescent Imaging in Scattering Specimens Using Confocal Microscopy

PubMed Central

Clendenon, Sherry G.; Young, Pamela A.; Ferkowicz, Michael; Phillips, Carrie; Dunn, Kenneth W.

2015-01-01

In scattering specimens, multiphoton excitation and nondescanned detection improve imaging depth by a factor of 2 or more over confocal microscopy; however, imaging depth is still limited by scattering. We applied the concept of clearing to deep tissue imaging of highly scattering specimens. Clearing is a remarkably effective approach to improving image quality at depth using either confocal or multiphoton microscopy. Tissue clearing appears to eliminate the need for multiphoton excitation for deep tissue imaging. PMID:21729357

In vivo 3D measurement of moxifloxacin and gatifloxacin distributions in the mouse cornea using multiphoton microscopy

NASA Astrophysics Data System (ADS)

Lee, Seunghun; Lee, Jun Ho; Park, Jin Hyoung; Yoon, Yeoreum; Chung, Wan Kyun; Tchah, Hungwon; Kim, Myoung Joon; Kim, Ki Hean

2016-05-01

Moxifloxacin and gatifloxacin are fourth-generation fluoroquinolone antibiotics used in the clinic to prevent or treat ocular infections. Their pharmacokinetics in the cornea is usually measured from extracted ocular fluids or tissues, and in vivo direct measurement is difficult. In this study multiphoton microscopy (MPM), which is a 3D optical microscopic technique based on multiphoton fluorescence, was applied to the measurement of moxifloxacin and gatifloxacin distribution in the cornea. Intrinsic multiphoton fluorescence properties of moxifloxacin and gatifloxacin were characterized, and their distributions in mouse cornea in vivo were measured by 3D MPM imaging. Both moxifloxacin and gatifloxacin had similar multiphoton spectra, while moxifloxacin had stronger fluorescence than gatifloxacin. MPM imaging of mouse cornea in vivo showed (1) moxifloxacin had good penetration through the superficial corneal epithelium, while gatifloxacin had relatively poor penetration, (2) both ophthalmic solutions had high intracellular distribution. In vivo MPM results were consistent with previous studies. This study demonstrates the feasibility of MPM as a method for in vivo direct measurement of moxifloxacin and gatifloxacin in the cornea.

In vivo 3D measurement of moxifloxacin and gatifloxacin distributions in the mouse cornea using multiphoton microscopy

PubMed Central

Lee, Seunghun; Lee, Jun Ho; Park, Jin Hyoung; Yoon, Yeoreum; Chung, Wan Kyun; Tchah, Hungwon; Kim, Myoung Joon; Kim, Ki Hean

2016-01-01

Moxifloxacin and gatifloxacin are fourth-generation fluoroquinolone antibiotics used in the clinic to prevent or treat ocular infections. Their pharmacokinetics in the cornea is usually measured from extracted ocular fluids or tissues, and in vivo direct measurement is difficult. In this study multiphoton microscopy (MPM), which is a 3D optical microscopic technique based on multiphoton fluorescence, was applied to the measurement of moxifloxacin and gatifloxacin distribution in the cornea. Intrinsic multiphoton fluorescence properties of moxifloxacin and gatifloxacin were characterized, and their distributions in mouse cornea in vivo were measured by 3D MPM imaging. Both moxifloxacin and gatifloxacin had similar multiphoton spectra, while moxifloxacin had stronger fluorescence than gatifloxacin. MPM imaging of mouse cornea in vivo showed (1) moxifloxacin had good penetration through the superficial corneal epithelium, while gatifloxacin had relatively poor penetration, (2) both ophthalmic solutions had high intracellular distribution. In vivo MPM results were consistent with previous studies. This study demonstrates the feasibility of MPM as a method for in vivo direct measurement of moxifloxacin and gatifloxacin in the cornea. PMID:27138688

Multiphoton imaging microscopy at deeper layers with adaptive optics control of spherical aberration.

PubMed

Bueno, Juan M; Skorsetz, Martin; Palacios, Raquel; Gualda, Emilio J; Artal, Pablo

2014-01-01

Despite the inherent confocality and optical sectioning capabilities of multiphoton microscopy, three-dimensional (3-D) imaging of thick samples is limited by the specimen-induced aberrations. The combination of immersion objectives and sensorless adaptive optics (AO) techniques has been suggested to overcome this difficulty. However, a complex plane-by-plane correction of aberrations is required, and its performance depends on a set of image-based merit functions. We propose here an alternative approach to increase penetration depth in 3-D multiphoton microscopy imaging. It is based on the manipulation of the spherical aberration (SA) of the incident beam with an AO device while performing fast tomographic multiphoton imaging. When inducing SA, the image quality at best focus is reduced; however, better quality images are obtained from deeper planes within the sample. This is a compromise that enables registration of improved 3-D multiphoton images using nonimmersion objectives. Examples on ocular tissues and nonbiological samples providing different types of nonlinear signal are presented. The implementation of this technique in a future clinical instrument might provide a better visualization of corneal structures in living eyes.

Characterization of Nuclear Recoils in High Pressure Xenon Gas: Towards a Simultaneous Search for WIMP Dark Matter and Neutrinoless Double Beta Decay

DOE PAGES

Renner, J.; Gehman, V. M.; Goldschmidt, A.; ...

2015-03-24

Xenon has recently been the medium of choice in several large scale detectors searching for WIMP dark matter and neutrinoless double beta decay. Though present-day large scale experiments use liquid xenon, the gas phase offers advantages favorable to both types of searches such as improved intrinsic energy resolution and fewer fluctuations in the partition of deposited energy between scintillation and ionization channels. We recently constructed a high pressure xenon gas TPC as a prototype for the NEXT (Neutrino Experiment with a Xenon TPC) neutrinoless double beta decay experiment and have demonstrated the feasibility of 0.5% FWHM energy resolution at themore » 136Xe double beta Q-value with 3-D tracking capabilities. We now present results from this prototype on the simultaneous observation of scintillation and ionization produced by nuclear recoils at approximately 14 bar pressure. The recoils were produced by neutrons of approximately 2-6 MeV emitted from a radioisotope plutonium-beryllium source, and primary scintillation (S1) and electroluminescent photons produced by ionization (S2) were observed. We discuss the potential of gaseous xenon to distinguish between electron and nuclear recoils through the ratio of these two signals S2/S1. From these results combined with the possibility of using columnar recombination to sense nuclear recoil directionality at high pressures we envision a dual-purpose, ton-scale gaseous xenon detector capable of a combined search for WIMP dark matter and neutrinoless double beta decay. This work has been performed within the context of the NEXT collaboration.« less

Barium Tagging from nEXO Using Resonance Ionization Spectroscopy

NASA Astrophysics Data System (ADS)

Twelker, K.; Kravitz, S.

nEXO is a 5-ton liquid enriched-xenon time projection chamber (TPC) to search for neutrinoless double-beta decay, designed to have the sensitivity to completely probe the inverted mass hierarchy of Majorana neutrinos. The detector will accommodate-as a background reduction technique-a system to recover and identify the barium decay product. This upgrade will allow a background-free measurement of neutrinoless double-beta decay and increase the half-life sensitivity of the experiment by at least one order of magnitude. Ongoing research and development includes a system to test barium extraction from liquid xenon using surface adsorption and Resonance Ionization Spectroscopy (RIS).

Characterizing lamina propria of human gastric mucosa by multiphoton microscopy

NASA Astrophysics Data System (ADS)

Liu, Y. C.; Yang, H. Q.; Chen, G.; Zhuo, S. M.; Chen, J. X.; Yan, J.

2011-01-01

Lamina propria (LP) of gastric mucosa plays an important role in progression of gastric cancer because of the site at where inflammatory reactions occur. Multiphoton imaging has been recently employed for microscopic examination of intact tissue. In this paper, using multiphoton microscopy (MPM) based on two-photon excited fluorescence (TPEF) and second harmonic generation (SHG), high resolution multiphoton microscopic images of lamina propria (LP) are obtained in normal human gastric mucosa at excitation wavelength λex = 800 nm. The main source of tissue TPEF originated from the cells of gastric glands, and loose connective tissue, collagen, produced SHG signals. Our results demonstrated that MPM can be effective for characterizing the microstructure of LP in human gastric mucosa. The findings will be helpful for diagnosing and staging early gastric cancer in the clinics.

In vivo microscopy of the mouse brain using multiphoton laser scanning techniques

NASA Astrophysics Data System (ADS)

Yoder, Elizabeth J.

2002-06-01

The use of multiphoton microscopy for imaging mouse brain in vivo offers several advantages and poses several challenges. This tutorial begins by briefly comparing multiphoton microscopy with other imaging modalities used to visualize the brain and its activity. Next, an overview of the techniques for introducing fluorescence into whole animals to generate contrast for in vivo microscopy using two-photon excitation is presented. Two different schemes of surgically preparing mice for brain imaging with multiphoton microscopy are reviewed. Then, several issues and problems with in vivo microscopy - including motion artifact, respiratory and cardiac rhythms, maintenance of animal health, anesthesia, and the use of fiducial markers - are discussed. Finally, examples of how these techniques have been applied to visualize the cerebral vasculature and its response to hypercapnic stimulation are provided.

A review of biomedical multiphoton microscopy and its laser sources

NASA Astrophysics Data System (ADS)

Lefort, Claire

2017-10-01

Multiphoton microscopy (MPM) has been the subject of major development efforts for about 25 years for imaging biological specimens at micron scale and presented as an elegant alternative to classical fluorescence methods such as confocal microscopy. In this topical review, the main interests and technical requirements of MPM are addressed with a focus on the crucial role of excitation source for optimization of multiphoton processes. Then, an overview of the different sources successfully demonstrated in literature for MPM is presented, and their physical parameters are inventoried. A classification of these sources in function with their ability to optimize multiphoton processes is proposed, following a protocol found in literature. Starting from these considerations, a suggestion of a possible identikit of the ideal laser source for MPM concludes this topical review. Dedicated to Martin.

Effects of ultrashort laser pulses on angular distributions of photoionization spectra.

PubMed

Ooi, C H Raymond; Ho, W L; Bandrauk, A D

2017-07-27

We study the photoelectron spectra by intense laser pulses with arbitrary time dependence and phase within the Keldysh framework. An efficient semianalytical approach using analytical transition matrix elements for hydrogenic atoms in any initial state enables efficient and accurate computation of the photoionization probability at any observation point without saddle point approximation, providing comprehensive three dimensional photoelectron angular distribution for linear and elliptical polarizations, that reveal the intricate features and provide insights on the photoionization characteristics such as angular dispersions, shift and splitting of photoelectron peaks from the tunneling or above threshold ionization(ATI) regime to non-adiabatic(intermediate) and multiphoton ionization(MPI) regimes. This facilitates the study of the effects of various laser pulse parameters on the photoelectron spectra and their angular distributions. The photoelectron peaks occur at multiples of 2ħω for linear polarization while  odd-ordered peaks are suppressed in the direction perpendicular to the electric field. Short pulses create splitting and angular dispersion where the peaks are strongly correlated to the angles. For MPI and elliptical polarization with shorter pulses the peaks split into doublets and the first peak vanishes. The carrier envelope phase(CEP) significantly affects the ATI spectra while the Stark effect shifts the spectra of intermediate regime to higher energies due to interference.

Reaction dynamics of Al + O₂ → AlO + O studied by a crossed-beam velocity map imaging technique: vib-rotational state selected angular-kinetic energy distribution.

PubMed

Honma, Kenji; Miyashita, Kazuki; Matsumoto, Yoshiteru

2014-06-07

Oxidation reaction of a gas-phase aluminum atom by a molecular oxygen was studied by a crossed-beam condition at 12.4 kJ/mol of collision energy. A (1+1) resonance-enhanced multiphoton ionization (REMPI) via the D(2)Σ(+)-X(2)Σ(+) transition of AlO was applied to ionize the product. The REMPI spectrum was analyzed to determine rotational state distributions for v = 0-2 of AlO. For several vib-rotational states of AlO, state selected angular and kinetic energy distributions were determined by a time-sliced ion imaging technique for the first time. Kinetic energy distributions were well represented by that taken into account initial energy spreads of collision energy and the population of the spin-orbit levels of the counter product O((3)P(J)) determined previously. All angular distributions showed forward and backward peaks, and the forward peaks were more pronounced than the backward one for the states of low internal energy. The backward peak intensity became comparable to the forward one for the states of high internal energy. These results and the rotational state distributions suggested that the reaction proceeds via an intermediate which has a lifetime comparable to or shorter than its rotational period.

Laser Ionization Studies of Hydrocarbon Flames.

NASA Astrophysics Data System (ADS)

Bernstein, Jeffrey Scott

Resonance-enhanced multiphoton ionization (REMPI) and laser induced fluorescence (LIF) are applied as laser based flame diagnostics for studies of hydrocarbon combustion chemistry. rm CH_4/O_2, C _2H_4/O_2, and rm C_2H_6/O_2 low pressure ( ~20 Torr), stoichiometric burner stabilized flat flames are studied. Density profiles of intermediate flame species, existing at ppm concentrations, are mapped out as a function of distance from the burner head. Profiles resulting from REMPI and LIF detection are obtained for HCO, CH_3, H, O, OH, CH, and CO flame radicals. The above flame systems are computer modeled against currently accepted combustion mechanisms using the Chemkin and Premix flame codes developed at Sandia National Laboratories. The modeled profile densities show good agreement with the experimental results of the CH_4/O_2 flame system, thus confirming the current C1 kinetic flame mechanism. Discrepancies between experimental and modeled results are found with the C2 flames. These discrepancies are partially amended by modifying the rate constant of the rm C_2H_3+rm O_2 to H_2CO + HCO reaction. The modeled results computed with the modified rate constant strongly suggest that the kinetics of several or possibly many reactions in the C2 mechanism need refinement.

Laser spectroscopy on organic molecules.

PubMed

Imasaka, T

1996-06-01

Various laser spectrometric methods have been developed until now. Especially, laser fluorometry is most sensitive and is frequently combined with a separation technique such as capillary electrophoresis. For non-fluorescent compounds, photothermal spectrometry may be used instead. A diode laser is potentially useful for practical trace analysis, because of its low cost and long-term trouble-free operation. On the other hand, monochromaticity of the laser is essential in high-resolution spectrometry, e.g. in low temperature spectrometry providing a very sharp spectral feature. Closely-related compounds such as isomers can easily be differentiated, and information for assignment is obtained from the spectrum. Multiphoton ionization mass spectrometry is useful for soft ionization, providing additional information concerned with molecular weight and chemical structure. A short laser pulse with a sufficient energy is suitable for rapid heating of the solid surface. A matrix-assisted laser desorption/ion-ization technique is recently employed for introduction of a large biological molecule into a vacuum for mass analysis. In the future, laser spectrometry will be developed by a combination with state-of-the-art laser technology. In the 21st century, new laser spectrometry will be developed, which may be based on revolutionary ideas or unexpected discoveries. Such studies will open new frontiers in analytical laser spectroscopy.

Lifetime of inner-shell hole states of Ar (2p) and Kr (3d) using equation-of-motion coupled cluster method

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

Ghosh, Aryya; Vaval, Nayana, E-mail: np.vaval@ncl.res.in; Pal, Sourav

2015-07-14

Auger decay is an efficient ultrafast relaxation process of core-shell or inner-shell excited atom or molecule. Generally, it occurs in femto-second or even atto-second time domain. Direct measurement of lifetimes of Auger process of single ionized and double ionized inner-shell state of an atom or molecule is an extremely difficult task. In this paper, we have applied the highly correlated complex absorbing potential-equation-of-motion coupled cluster (CAP-EOMCC) approach which is a combination of CAP and EOMCC approach to calculate the lifetime of the states arising from 2p inner-shell ionization of an Ar atom and 3d inner-shell ionization of Kr atom. Wemore » have also calculated the lifetime of Ar{sup 2+}(2p{sup −1}3p{sup −1}) {sup 1}D, Ar{sup 2+}(2p{sup −1}3p{sup −1}) {sup 1}S, and Ar{sup 2+}(2p{sup −1}3s{sup −1}) {sup 1}P double ionized states. The predicted results are compared with the other theoretical results as well as experimental results available in the literature.« less

Low-energy electron-impact single ionization of helium

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

Colgan, J.; Pindzola, M. S.; Childers, G.

2006-04-15

A study is made of low-energy electron-impact single ionization of ground-state helium. The time-dependent close-coupling method is used to calculate total integral, single differential, double differential, and triple differential ionization cross sections for impact electron energies ranging from 32 to 45 eV. For all quantities, the calculated cross sections are found to be in very good agreement with experiment, and for the triple differential cross sections, good agreement is also found with calculations made using the convergent close-coupling technique.

Rotationally resolved pulsed field ionization photoelectron study of CO[sup +](X[sup 2][Sigma][sup +],v[sup +]=0[endash]42) in the energy range of 13. 98[endash]21. 92 eV

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

Evans, M.; Ng, C.Y.

1999-11-01

We have obtained rotationally resolved pulsed field ionization[endash]photoelectron (PFI-PE) spectra of CO in the energy range of 13.98[endash]21.92 eV, covering the ionization transitions CO[sup +](X hthinsp;[sup 2][Sigma][sup +],v[sup +]=0[endash]42,N[sup +])[l arrow]CO(X hthinsp;[sup 1][Sigma][sup +],v[sup [double prime

In vivo multiphoton microscopy of deep tissue with gradient index lenses

NASA Astrophysics Data System (ADS)

Levene, Michael J.; Dombeck, Daniel A.; Williams, Rebecca M.; Skoch, Jesse; Hickey, Gregory A.; Kasischke, Karl A.; Molloy, Raymond P.; Ingelsson, Martin; Stern, Edward A.; Klucken, Jochen; Bacskai, Brian J.; Zipfel, Warren R.; Hyman, Bradley T.; Webb, Watt W.

2004-06-01

Gradient index lenses enable multiphoton microscopy of deep tissues in the intact animal. In order to assess their applicability to clinical research, we present in vivo multiphoton microscopy with gradient index lenses in brain regions associated with Alzheimer's disease and Parkinson's disease in both transgenic and wild-type mice. We also demonstrate microscopy of ovary in wild type mouse using only intrinsic fluorescence and second harmonic generation, signal sources which may prove useful for both the study and diagnosis of cancer.

In vivo multiphoton microscopy beyond 1 mm in the brain

NASA Astrophysics Data System (ADS)

Miller, David R.; Medina, Flor A.; Hassan, Ahmed; Perillo, Evan P.; Hagan, Kristen; Kazmi, S. M. Shams; Zemelman, Boris V.; Dunn, Andrew K.

2017-02-01

We perform high-resolution, non-invasive, in vivo deep-tissue imaging of the mouse neocortex using multiphoton microscopy with a high repetition rate optical parametric amplifier laser source tunable between λ=1,100 and 1,400 nm. We demonstrate an imaging depth of 1,200 μm in vasculature and 1,160 μm in neurons. We also demonstrate deep-tissue imaging using Indocyanine Green (ICG), which is FDA approved and a promising route to translate multiphoton microscopy to human applications.

Measurements of the Activation Energies for Atomic Hydrogen Diffusion on Pure Solid CO

NASA Astrophysics Data System (ADS)

Kimura, Y.; Tsuge, M.; Pirronello, V.; Kouchi, A.; Watanabe, N.

2018-05-01

The diffusion of hydrogen atoms on dust grains is a key process in the formation of interstellar H2 and some hydrogenated molecules such as formaldehyde and methanol. We investigate the adsorption and diffusion of H atoms on pure solid CO as an analog of dust surfaces observed toward some cold interstellar regions. Using a combination of photostimulated desorption and resonance-enhanced multiphoton ionization methods to detect H atoms directly, the relative adsorption probabilities and diffusion coefficients of the H atoms are measured on pure solid CO at 8, 12, and 15 K. There is little difference between the diffusion coefficients of the hydrogen and deuterium atoms, indicating that the diffusion is limited by thermal hopping. The activation energies controlling the H-atom diffusion depend on the surface temperature, and values of 22, 30, and ∼37 meV were obtained for 8, 12, and 15 K, respectively.

Spectroscopic study on deuterated benzenes. II. High-resolution laser spectroscopy and rotational structure in the S{sub 1} state

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

Kunishige, Sachi; Katori, Toshiharu; Baba, Masaaki, E-mail: baba@kuchem.kyoto-u.ac.jp

High-resolution spectra of the S{sub 1}←S{sub 0} transition in jet-cooled deuterated benzenes were observed using pulse dye amplification of single-mode laser light and mass-selective resonance enhanced multiphoton ionization (REMPI) detection. The vibrational and rotational structures were accurately analyzed for the vibronic levels in the S{sub 1} state. The degenerate 6{sup 1} levels of C{sub 6}H{sub 6} or C{sub 6}D{sub 6} are split into 6a{sup 1} and 6b{sup 1} in many of deuterated benzenes. The rigid-rotor rotational constants were assessed and found to be slightly different between 6a and 6b because of different mean molecular structures. Their rotational levels are significantlymore » shifted by Coriolis interactions. It was found that the Coriolis parameter proportionally changed with the number of substituted D atoms.« less

Ultrafast dynamics of electrons in ammonia.

PubMed

Vöhringer, Peter

2015-04-01

Solvated electrons were first discovered in solutions of metals in liquid ammonia. The physical and chemical properties of these species have been studied extensively for many decades using an arsenal of electrochemical, spectroscopic, and theoretical techniques. Yet, in contrast to their hydrated counterpart, the ultrafast dynamics of ammoniated electrons remained completely unexplored until quite recently. Femtosecond pump-probe spectroscopy on metal-ammonia solutions and femtosecond multiphoton ionization spectroscopy on the neat ammonia solvent have provided new insights into the optical properties and the reactivities of this fascinating species. This article reviews the nature of the optical transition, which gives the metal-ammonia solutions their characteristic blue appearance, in terms of ultrafast relaxation processes involving bound and continuum excited states. The recombination processes following the injection of an electron via photoionization of the solvent are discussed in the context of the electronic structure of the liquid and the anionic defect associated with the solvated electron.

Mass-Selective Chiral Analysis

NASA Astrophysics Data System (ADS)

Boesl, Ulrich; Kartouzian, Aras

2016-06-01

Three ways of realizing mass-selective chiral analysis are reviewed. The first is based on the formation of diastereomers that are of homo- and hetero- type with respect to the enantiomers of involved chiral molecules. This way is quite well-established with numerous applications. The other two ways are more recent developments, both based on circular dichroism (CD). In one, conventional or nonlinear electronic CD is linked to mass spectrometry (MS) by resonance-enhanced multiphoton ionization. The other is based on CD in the angular distribution of photoelectrons, which is measured in combination with MS via photoion photoelectron coincidence. Among the many important applications of mass-selective chiral analysis, this review focuses on its use as an analytical tool for the development of heterogeneous enantioselective chemical catalysis. There exist other approaches to combine chiral analysis and mass-selective detection, such as chiral chromatography MS, which are not discussed here.

Polycyclic aromatic hydrocarbons in the atmospheres of Titan and Jupiter

NASA Technical Reports Server (NTRS)

Sagan, Carl; Khare, B. N.; Thompson, W. R.; Mcdonald, G. D.; Wing, Michael R.; Bada, Jeffrey L.; Vo-Dinh, Tuan; Arakawa, E. T.

1993-01-01

PAHs are important components of the interstellar medium and carbonaceous chondrites, but have never been identified in the reducing atmospheres of the outer solar system. Incompletely characterized complex organic solids (tholins) produced by irradiating simulated Titan atmospheres reproduce well the observed UV/visible/IR optical constants of the Titan stratospheric haze. Titan tholin and a tholin generated in a crude simulation of the atmosphere of Jupiter are examined by two-step laser desorption/multiphoton ionization mass spectrometry. A range of two- to four-ring PAHs, some with one to four alkylation sites, are identified, with a net abundance of about 0.0001 g/g (grams per gram) of tholins produced. Synchronous fluorescence techniques confirm this detection. Titan tholins have proportionately more one- and two-ring PAHs than do Jupiter tholins, which in turn have more four-ring and larger PAHs. The four-ringed PAH chrysene, prominent in some discussions of interstellar grains, is found in Jupiter tholins.

Strong Field Optical and Quantum Control

NASA Astrophysics Data System (ADS)

Schumacher, Douglass William

1995-01-01

This work presents the results of an effort to use unique forms of optical radiation to better probe and control matter. Results are presented of a study of intense field photo-ionization of krypton and xenon in a two-color field. The use of a two-color field provides a valuable probe, the relative optical phase, into the dynamics of the ionization process. It is found that phase dependent tunneling character is preserved even though the photoelectron spectra indicate that the experiments performed were well into the multi-photon regime of ionization. Evidence for core scattering of the departing electrons is seen in the changes to the phase dependent spectra as the polarization of the exciting light is varied from linear to slightly elliptical. To further control the optical field, a pulse shaper was constructed using liquid crystal modulators that allowed either spectral phase or spectral amplitude shaping of a short pulse. The results were characterized using cross-correlations. The shaped light was then subsequently amplified in a chirped pulse amplifier. This light was characterized using Frequency Resolved Optical Gating, a newly developed technique for the complete determination of the optical field in a short pulse. The shaped pulses were then used to tailor atomic radial wavepackets in cesium. The evolution of the wavepackets was monitored by measuring atomic auto-interferograms for the case of amplitude shaping, which was used to control the atomic states excited. Cross -interferograms were used for phase shaping, which was used to select the initial phase of the atomic states. The cross-interferograms required the simultaneous amplification of a shaped and an unshaped pulse in our amplifier.

Simulation of deleterious processes in a static-cell diode pumped alkali laser

NASA Astrophysics Data System (ADS)

Oliker, Benjamin Q.; Haiducek, John D.; Hostutler, David A.; Pitz, Greg A.; Rudolph, Wolfgang; Madden, Timothy J.

2014-02-01

The complex interactions in a diode pumped alkali laser (DPAL) gain cell provide opportunities for multiple deleterious processes to occur. Effects that may be attributable to deleterious processes have been observed experimentally in a cesium static-cell DPAL at the United States Air Force Academy [B.V. Zhdanov, J. Sell, R.J. Knize, "Multiple laser diode array pumped Cs laser with 48 W output power," Electronics Letters, 44, 9 (2008)]. The power output in the experiment was seen to go through a "roll-over"; the maximum power output was obtained with about 70 W of pump power, then power output decreased as the pump power was increased beyond this point. Research to determine the deleterious processes that caused this result has been done at the Air Force Research Laboratory utilizing physically detailed simulation. The simulations utilized coupled computational fluid dynamics (CFD) and optics solvers, which were three-dimensional and time-dependent. The CFD code used a cell-centered, conservative, finite-volume discretization of the integral form of the Navier-Stokes equations. It included thermal energy transport and mass conservation, which accounted for chemical reactions and state kinetics. Optical models included pumping, lasing, and fluorescence. The deleterious effects investigated were: alkali number density decrease in high temperature regions, convective flow, pressure broadening and shifting of the absorption lineshape including hyperfine structure, radiative decay, quenching, energy pooling, off-resonant absorption, Penning ionization, photoionization, radiative recombination, three-body recombination due to free electron and buffer gas collisions, ambipolar diffusion, thermal aberration, dissociative recombination, multi-photon ionization, alkali-hydrocarbon reactions, and electron impact ionization.

Partial cross sections of helium satellites at medium photon energies

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

Wehlitz, R.; Sellin, I.A.; Hemmers, O.

1997-04-01

Still of current interest is the important role of single ionization with excitation compared to single ionization alone. The coupling between the electrons and the incoming photon is a single-particle operator. Thus, an excitation in addition to an ionization, leading to a so-called satellite line in a photoelectron spectrum, is entirely due to electron-electron interaction and probes the electron correlation in the ground and final state. Therefore the authors have undertaken the study of the intensity of helium satellites He{sup +}nl (n = 2 - 6) relative to the main photoline (n = 1) as a function of photon energymore » at photon energies well above threshold up to 900 eV. From these results they could calculate the partial cross-sections of the helium satellites. In order to test the consistency of their satellite-to-1s ratios with published double-to-single photoionization ratios, the authors calculated the double-to-single photoionization ratio from their measured ratios using the theoretical energy-distribution curves of Chang and Poe and Le Rouzo and Dal Cappello which proved to be valid for photon energies below 120 eV. These calculated double-to-single ionization ratios agree fairly well with recent ion measurements. In the lower photon energy range the authors ratios agree better with the ratios of Doerner et al. while for higher photon energies the agreement is better with the values of Levin et al.« less

Fast volumetric imaging with patterned illumination via digital micro-mirror device-based temporal focusing multiphoton microscopy.

PubMed

Chang, Chia-Yuan; Hu, Yvonne Yuling; Lin, Chun-Yu; Lin, Cheng-Han; Chang, Hsin-Yu; Tsai, Sheng-Feng; Lin, Tzu-Wei; Chen, Shean-Jen

2016-05-01

Temporal focusing multiphoton microscopy (TFMPM) has the advantage of area excitation in an axial confinement of only a few microns; hence, it can offer fast three-dimensional (3D) multiphoton imaging. Herein, fast volumetric imaging via a developed digital micromirror device (DMD)-based TFMPM has been realized through the synchronization of an electron multiplying charge-coupled device (EMCCD) with a dynamic piezoelectric stage for axial scanning. The volumetric imaging rate can achieve 30 volumes per second according to the EMCCD frame rate of more than 400 frames per second, which allows for the 3D Brownian motion of one-micron fluorescent beads to be spatially observed. Furthermore, it is demonstrated that the dynamic HiLo structural multiphoton microscope can reject background noise by way of the fast volumetric imaging with high-speed DMD patterned illumination.

Imaging rat esophagus using combination of reflectance confocal and multiphoton microscopy

NASA Astrophysics Data System (ADS)

Zhuo, S. M.; Chen, J. X.; Jiang, X. S.; Lu, K. C.; Xie, S. S.

2008-08-01

We combine reflectance confocal microscopy (RCM) with multiphoton microscopy (MPM) to image rat esophagus. The two imaging modalities allow detection of layered-resolved complementary information from esophagus. In the keratinizing layer, the keratinocytes boundaries can be characterized by RCM, while the keratinocytes cytoplasm (keratin) can be further imaged by multiphoton autofluorescence signal. In the epithelium, the epithelial cellular boundaries and nucleus can be detected by RCM, and MPM can be used for imaging epithelial cell cytoplasm and monitoring metabolic state of epithelium. In the stroma, multiphoton autofluorescence signal is used to image elastin and second harmonic generation signal is utilized to detect collagen, while RCM is used to determine the optical property of stroma. Overall, these results suggest that the combination of RCM and MPM has potential to provide more important and comprehensive information for early diagnosis of esophageal cancer.

Sequential double photodetachment of He- in elliptically polarized laser fields

NASA Astrophysics Data System (ADS)

Génévriez, Matthieu; Dunseath, Kevin M.; Terao-Dunseath, Mariko; Urbain, Xavier

2018-02-01

Four-photon double detachment of the helium negative ion is investigated experimentally and theoretically for photon energies where the transient helium atom is in the 1 s 2 s 3S or 1 s 2 p P3o states, which subsequently ionize by absorption of three photons. Ionization is enhanced by intermediate resonances, giving rise to series of peaks in the He+ spectrum, which we study in detail. The He+ yield is measured in the wavelength ranges from 530 to 560 nm and from 685 to 730 nm and for various polarizations of the laser light. Double detachment is treated theoretically as a sequential process, within the framework of R -matrix theory for the first step and effective Hamiltonian theory for the second step. Experimental conditions are accurately modeled, and the measured and simulated yields are in good qualitative and, in some cases, quantitative agreement. Resonances in the double detachment spectra can be attributed to well-defined Rydberg states of the transient atom. The double detachment yield exhibits a strong dependence on the laser polarization which can be related to the magnetic quantum number of the intermediate atomic state. We also investigate the possibility of nonsequential double detachment with a two-color experiment but observe no evidence for it.

EDITORIAL: Theory of Quantum Gases and Quantum Coherence: The Cortona BEC Workshop, 29 October-2 November 2005

NASA Astrophysics Data System (ADS)

Capuzzi, Pablo; Chitra, R.; Menotti, Chiara; Minguzz, Anna; Vignolo, Patrizia

2006-05-01

Nonlinear, or multiphoton, interaction of intense laser radiation with matter has been a key research subject for about four decades. Every three years, the International Conference on Multiphoton Processes (ICOMP) covers the latest advances in the field. Intense-field physics has seen phenomenal progress over the last decade. What looked like dreams in the mid-nineties have become routine today. Major theoretical, experimental and technological advances in fundamental science and applications of multiphoton processes cover such diverse areas as precision measurements, femtosecond and now attosecond metrology, quantum control of atomic and molecular dynamics, laser machining of solid state materials, laser acceleration of electrons and protons, and medical applications. This special issue of Journal of Physics B: Atomic, Molecular and Optical Physics (J. Phys. B) contains a collection of articles originating from the Tenth International Conference on Multiphoton Processes (ICOMP 2005) held on 9-14 October 2005 in Orford, Quebec, Canada (general chair Lou DiMauro, Ohio State University, program co-chairs Paul Corkum and Misha Ivanov, National Research Council of Canada). The conference focused on atoms and molecules in strong fields, femtosecond and attosecond processes, propagation of intense pulses, and of course multiphoton processes which lie at the foundation of all these subjects. Articles presented in this issue cover several key areas of intense-field physics. These include strong field ionization of atoms, molecules and inside transparent dielectric materials, methods of generation and characterization of attosecond XUV pulses and pulse trains, and new approaches to using intense laser fields and/or attosecond pulses for studying entangled systems and imaging electronic and nuclear dynamics with sub-Ångstrom spatial and sub-femtosecond temporal resolution. We have tried to group the papers according to these general areas. We would like to use this opportunity to thank all the participants of ICOMP-X, and in particular the contributors to this issue, for the high quality of science presented at the conference and in this journal. The success of the conference would not have been possible without the program committee which included D Charalambidis, L Cocke, R Freeman, Y Fujimura, S Goreslavsky, A L'Huillier, F Krausz, R Levis, S H Lin, A Maquet, J Marangos, K Midorikawa, G Mourou, P Salieres, W Sandner, K Schafer, A Scrinzi, A M Sergeev, H Stapelfeldt, A Starace, J Ullrich, M Vrakking, and K Yamanouchi. A particularly lively atmosphere in the discussions was ensured by many students who were able to participate in the conference, in part due to generous support of the Canadian Institute for Photonic Innovations (CIPI) to the Canadian, and of the US Department of Energy Office of Basic Energy Sciences to the American students. Additional support to the conference was provided by the Natural Sciences and Engineering Research Council (NSERC), the National Research Council of Canada (NRC), Pfeiffer Vacuum, Femtolasers Produktions GmbH, Roentdek Handels GmbH, Coherent Laser Products, and Amplitude Technologies. Last but not least, the guest editors of this special issue would like to acknowledge the tremendous amount of work done by the staff of J. Phys. B in handling all aspects of the publication process. In particular, we would like to thank Isabelle Auffret-Babak, Alice Malhador and Joanna Dingley from the editorial team, Katie Gerrard in production and the Editor-in-Chief, Professor J-M Rost.

Time and Space Resolved High Harmonic Imaging of Electron Tunnelling from Molecules

NASA Astrophysics Data System (ADS)

Smirnova, O.

2009-05-01

High harmonic generation in intense laser fields carries the promise of combining sub-Angstrom spatial and attosecond temporal resolution of electronic structures and dynamics in molecules, see e.g. [1-3]. High harmonic emission occurs when an electron detached from a molecule by an intense laser field recombines with the parent ion [4]. Similar to Young's double-slit experiment, recombination to several ``lobes'' of the same molecular orbital can produce interference minima and maxima in harmonic intensities [1]. These minima (maxima) carry structural information -- they occur when the de-Broglie wavelength of the recombining electron matches distances between the centers. We demonstrate both theoretically and experimentally that amplitude minima (maxima) in the harmonic spectra can also have dynamical origin, reflecting multi-electron dynamics in the molecule. We use high harmonic spectra to record this dynamics and reconstruct the position of the hole left in the molecule after ionization. Experimental data are consistent with the hole starting in different places as the ionization dynamics changes from tunnelling to the multi-photon regime. Importantly, hole localization and subsequent attosecond dynamics are induced even in the tunnelling limit. Thus, even ``static'' tunnelling induced by a tip of a tunnelling microscope will generate similar attosecond dynamics in a sample. We anticipate that our approach will become standard in disentangling spatial and temporal information from high harmonic spectra of molecules.[4pt] In collaboration with Serguei Patchkovskii, National Research Council, 100 Sussex Drive, Ottawa, Ontario K1A 0R6, Canada; Yann Mairesse, NRC Canada and CELIA, Universit'e Bordeaux I, UMR 5107 (CNRS, Bordeaux 1, CEA), 351 Cours de la Lib'eration, 33405 Talence Cedex, France; Nirit Dudovich, NRC Canada and Department of Physics of Complex Systems, Weizmann Institute of Science, Rehovot 76100, Israel; David Villeneuve, Paul Corkum, NRC Canada; and Misha Yu. Ivanov, NRC Canada and Imperial College of Science, Technology and Medicine, London SW7 2BW, United Kingdom. [4pt] [1] Lein, M., et al. Phys. Rev. Lett. 88, 183903 (2002).[0pt] [2] Itatani, J. et al. Nature 432, 834 (2004).[0pt] [3] Baker, S. et al Science 312, 424 (2006).[0pt] [4] Corkum, P. B.Phys. Rev. Lett. 71, 1994 (1993).

Transverse correlations in multiphoton entanglement

NASA Astrophysics Data System (ADS)

Wen, Jianming; Rubin, Morton H.; Shih, Yanhua

2007-10-01

We have analyzed the transverse correlation in multiphoton entanglement. The generalization of quantum ghost imaging is extended to the N -photon state. The Klyshko’s two-photon advanced-wave picture is generalized to the N -photon case.

Ionization compression impact on dense gas distribution and star formation. Probability density functions around H II regions as seen by Herschel

NASA Astrophysics Data System (ADS)

Tremblin, P.; Schneider, N.; Minier, V.; Didelon, P.; Hill, T.; Anderson, L. D.; Motte, F.; Zavagno, A.; André, Ph.; Arzoumanian, D.; Audit, E.; Benedettini, M.; Bontemps, S.; Csengeri, T.; Di Francesco, J.; Giannini, T.; Hennemann, M.; Nguyen Luong, Q.; Marston, A. P.; Peretto, N.; Rivera-Ingraham, A.; Russeil, D.; Rygl, K. L. J.; Spinoglio, L.; White, G. J.

2014-04-01

Aims: Ionization feedback should impact the probability distribution function (PDF) of the column density of cold dust around the ionized gas. We aim to quantify this effect and discuss its potential link to the core and initial mass function (CMF/IMF). Methods: We used Herschel column density maps of several regions observed within the HOBYS key program in a systematic way: M 16, the Rosette and Vela C molecular clouds, and the RCW 120 H ii region. We computed the PDFs in concentric disks around the main ionizing sources, determined their properties, and discuss the effect of ionization pressure on the distribution of the column density. Results: We fitted the column density PDFs of all clouds with two lognormal distributions, since they present a "double-peak" or an enlarged shape in the PDF. Our interpretation is that the lowest part of the column density distribution describes the turbulent molecular gas, while the second peak corresponds to a compression zone induced by the expansion of the ionized gas into the turbulent molecular cloud. Such a double peak is not visible for all clouds associated with ionization fronts, but it depends on the relative importance of ionization pressure and turbulent ram pressure. A power-law tail is present for higher column densities, which are generally ascribed to the effect of gravity. The condensations at the edge of the ionized gas have a steep compressed radial profile, sometimes recognizable in the flattening of the power-law tail. This could lead to an unambiguous criterion that is able to disentangle triggered star formation from pre-existing star formation. Conclusions: In the context of the gravo-turbulent scenario for the origin of the CMF/IMF, the double-peaked or enlarged shape of the PDF may affect the formation of objects at both the low-mass and the high-mass ends of the CMF/IMF. In particular, a broader PDF is required by the gravo-turbulent scenario to fit the IMF properly with a reasonable initial Mach number for the molecular cloud. Since other physical processes (e.g., the equation of state and the variations among the core properties) have already been said to broaden the PDF, the relative importance of the different effects remains an open question. Herschel is an ESA space observatory with science instruments provided by European-led Principal Investigator consortia and with important participation from NASA.

Inhibition of APOBEC3G activity impedes double-stranded DNA repair.

PubMed

Prabhu, Ponnandy; Shandilya, Shivender M D; Britan-Rosich, Elena; Nagler, Adi; Schiffer, Celia A; Kotler, Moshe

2016-01-01

The cellular cytidine deaminase APOBEC3G (A3G) was first described as an anti-HIV-1 restriction factor, acting by directly deaminating reverse transcripts of the viral genome. HIV-1 Vif neutralizes the activity of A3G, primarily by mediating degradation of A3G to establish effective infection in host target cells. Lymphoma cells, which express high amounts of A3G, can restrict Vif-deficient HIV-1. Interestingly, these cells are more stable in the face of treatments that result in double-stranded DNA damage, such as ionizing radiation and chemotherapies. Previously, we showed that the Vif-derived peptide (Vif25-39) efficiently inhibits A3G deamination, and increases the sensitivity of lymphoma cells to ionizing radiation. In the current study, we show that additional peptides derived from Vif, A3G, and APOBEC3F, which contain the LYYF motif, inhibit deamination activity. Each residue in the Vif25-39 sequence moderately contributes to the inhibitory effect, whereas replacing a single residue in the LYYF motif completely abrogates inhibition of deamination. Treatment of A3G-expressing lymphoma cells exposed to ionizing radiation with the new inhibitory peptides reduces double-strand break repair after irradiation. Incubation of cultured irradiated lymphoma cells with peptides that inhibit double-strand break repair halts their propagation. These results suggest that A3G may be a potential therapeutic target that is amenable to peptide and peptidomimetic inhibition. © 2015 FEBS.

Quantum cryptography with perfect multiphoton entanglement.

PubMed

Luo, Yuhui; Chan, Kam Tai

2005-05-01

Multiphoton entanglement in the same polarization has been shown theoretically to be obtainable by type-I spontaneous parametric downconversion (SPDC), which can generate bright pulses more easily than type-II SPDC. A new quantum cryptographic protocol utilizing polarization pairs with the detected type-I entangled multiphotons is proposed as quantum key distribution. We calculate the information capacity versus photon number corresponding to polarization after considering the transmission loss inside the optical fiber, the detector efficiency, and intercept-resend attacks at the level of channel error. The result compares favorably with all other schemes employing entanglement.

Remote focusing for programmable multi-layer differential multiphoton microscopy

PubMed Central

Hoover, Erich E.; Young, Michael D.; Chandler, Eric V.; Luo, Anding; Field, Jeffrey J.; Sheetz, Kraig E.; Sylvester, Anne W.; Squier, Jeff A.

2010-01-01

We present the application of remote focusing to multiphoton laser scanning microscopy and utilize this technology to demonstrate simultaneous, programmable multi-layer imaging. Remote focusing is used to independently control the axial location of multiple focal planes that can be simultaneously imaged with single element detection. This facilitates volumetric multiphoton imaging in scattering specimens and can be practically scaled to a large number of focal planes. Further, it is demonstrated that the remote focusing control can be synchronized with the lateral scan directions, enabling imaging in orthogonal scan planes. PMID:21326641

Hybrid reflecting objectives for functional multiphoton microscopy in turbid media

PubMed Central

Vučinić, Dejan; Bartol, Thomas M.; Sejnowski, Terrence J.

2010-01-01

Most multiphoton imaging of biological specimens is performed using microscope objectives optimized for high image quality under wide-field illumination. We present a class of objectives designed de novo without regard for these traditional constraints, driven exclusively by the needs of fast multiphoton imaging in turbid media: the delivery of femtosecond pulses without dispersion and the efficient collection of fluorescence. We model the performance of one such design optimized for a typical brain-imaging setup and show that it can greatly outperform objectives commonly used for this task. PMID:16880851

Laser resonance ionization spectroscopy of antimony

NASA Astrophysics Data System (ADS)

Li, R.; Lassen, J.; Ruczkowski, J.; Teigelhöfer, A.; Bricault, P.

2017-02-01

The resonant ionization laser ion source is an element selective, efficient and versatile ion source to generate radioactive ion beams at on-line mass separator facilities. For some elements with complex atomic structures and incomplete spectroscopic data, laser spectroscopic investigations are required for ionization scheme development. Laser resonance ionization spectroscopy using Ti:Sa lasers has been performed on antimony (Sb) at TRIUMF's off-line laser ion source test stand. Laser light of 230.217 nm (vacuum wavelength) as the first excitation step and light from a frequency-doubled Nd:YVO4 laser (532 nm) as the nonresonant ionization step allowed to search for suitable second excitation steps by continuous wavelength scans from 720 nm to 920 nm across the wavelength tuning range of a grating-tuned Ti:Sa laser. Upon the identification of efficient SES, the third excitation steps for resonance ionization were investigated by laser scans across Rydberg states, the ionization potential and autoionizing states. One Rydberg state and six AI states were found to be well suitable for efficient resonance ionization.

Coherence-Gated Sensorless Adaptive Optics Multiphoton Retinal Imaging

PubMed Central

Cua, Michelle; Wahl, Daniel J.; Zhao, Yuan; Lee, Sujin; Bonora, Stefano; Zawadzki, Robert J.; Jian, Yifan; Sarunic, Marinko V.

2016-01-01

Multiphoton microscopy enables imaging deep into scattering tissues. The efficient generation of non-linear optical effects is related to both the pulse duration (typically on the order of femtoseconds) and the size of the focused spot. Aberrations introduced by refractive index inhomogeneity in the sample distort the wavefront and enlarge the focal spot, which reduces the multiphoton signal. Traditional approaches to adaptive optics wavefront correction are not effective in thick or multi-layered scattering media. In this report, we present sensorless adaptive optics (SAO) using low-coherence interferometric detection of the excitation light for depth-resolved aberration correction of two-photon excited fluorescence (TPEF) in biological tissue. We demonstrate coherence-gated SAO TPEF using a transmissive multi-actuator adaptive lens for in vivo imaging in a mouse retina. This configuration has significant potential for reducing the laser power required for adaptive optics multiphoton imaging, and for facilitating integration with existing systems. PMID:27599635

Phase Sensitive Demodulation in Multiphoton Microscopy

NASA Astrophysics Data System (ADS)

Fisher, Walt G.; Piston, David W.; Wachter, Eric A.

2002-06-01

Multiphoton laser scanning microscopy offers advantages in depth of penetration into intact samples over other optical sectioning techniques. To achieve these advantages it is necessary to detect the emitted light without spatial filtering. In this nondescanned (nonconfocal) approach, ambient room light can easily contaminate the signal, forcing experiments to be performed in absolute darkness. For multiphoton microscope systems employing mode-locked lasers, signal processing can be used to reduce such problems by taking advantage of the pulsed characteristics of such lasers. Specifically, by recovering fluorescence generated at the mode-locked frequency, interference from stray light and other ambient noise sources can be significantly reduced. This technology can be adapted to existing microscopes by inserting demodulation circuitry between the detector and data collection system. The improvement in signal-to-noise ratio afforded by this approach yields a more robust microscope system and opens the possibility of moving multiphoton microscopy from the research lab to more demanding settings, such as the clinic.

Processing multiphoton states through operation on a single photon: Methods and applications

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

Lin Qing; He Bing; Bergou, Janos A.

2009-10-15

Multiphoton states are widely applied in quantum information technology. By the methods presented in this paper, the structure of a multiphoton state in the form of multiple single-photon qubit products can be mapped to a single-photon qudit, which could also be in a separable product with other photons. This makes possible the manipulation of such multiphoton states by processing single-photon states. The optical realization of unknown qubit discrimination [B. He, J. A. Bergou, and Y.-H. Ren, Phys. Rev. A 76, 032301 (2007)] is simplified with the transformation methods. Another application is the construction of quantum logic gates, where the inversemore » transformations back to the input state spaces are also necessary. We especially show that the modified setups to implement the transformations can realize the deterministic multicontrol gates (including Toffoli gate) operating directly on the products of single-photon qubits.« less

Coherence-Gated Sensorless Adaptive Optics Multiphoton Retinal Imaging.

PubMed

Cua, Michelle; Wahl, Daniel J; Zhao, Yuan; Lee, Sujin; Bonora, Stefano; Zawadzki, Robert J; Jian, Yifan; Sarunic, Marinko V

2016-09-07

Multiphoton microscopy enables imaging deep into scattering tissues. The efficient generation of non-linear optical effects is related to both the pulse duration (typically on the order of femtoseconds) and the size of the focused spot. Aberrations introduced by refractive index inhomogeneity in the sample distort the wavefront and enlarge the focal spot, which reduces the multiphoton signal. Traditional approaches to adaptive optics wavefront correction are not effective in thick or multi-layered scattering media. In this report, we present sensorless adaptive optics (SAO) using low-coherence interferometric detection of the excitation light for depth-resolved aberration correction of two-photon excited fluorescence (TPEF) in biological tissue. We demonstrate coherence-gated SAO TPEF using a transmissive multi-actuator adaptive lens for in vivo imaging in a mouse retina. This configuration has significant potential for reducing the laser power required for adaptive optics multiphoton imaging, and for facilitating integration with existing systems.

Dissociative double-photoionization of butadiene in the 25-45 eV energy range using 3-D multi-coincidence ion momentum imaging spectrometry

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

Oghbaie, Shabnam; Gisselbrecht, Mathieu; Laksman, Joakim

Dissociative double-photoionization of butadiene in the 25-45 eV energy range has been studied with tunable synchrotron radiation using full three-dimensional ion momentum imaging. Using ab initio calculations, the electronic states of the molecular dication below 33 eV are identified. The results of the measurement and calculation show that double ionization from π orbitals selectively triggers twisting about the terminal or central C–C bonds. We show that this conformational rearrangement depends upon the dication electronic state, which effectively acts as a gateway for the dissociation reaction pathway. For photon energies above 33 eV, three-body dissociation channels where neutral H-atom evaporation precedesmore » C–C charge-separation in the dication species appear in the correlation map. The fragment angular distributions support a model where the dication species is initially aligned with the molecular backbone parallel to the polarization vector of the light, indicating a high probability for double-ionization to the “gateway states” for molecules with this orientation.« less

Polymer dots enable deep in vivo multiphoton fluorescence imaging of cerebrovascular architecture

NASA Astrophysics Data System (ADS)

Hassan, Ahmed M.; Wu, Xu; Jarrett, Jeremy W.; Xu, Shihan; Miller, David R.; Yu, Jiangbo; Perillo, Evan P.; Liu, Yen-Liang; Chiu, Daniel T.; Yeh, Hsin-Chih; Dunn, Andrew K.

2018-02-01

Deep in vivo imaging of vasculature requires small, bright, and photostable fluorophores suitable for multiphoton microscopy (MPM). Although semiconducting polymer dots (pdots) are an emerging class of highly fluorescent contrast agents with favorable advantages for the next generation of in vivo imaging, their use for deep multiphoton imaging has never before been demonstrated. Here we characterize the multiphoton properties of three pdot variants (CNPPV, PFBT, and PFPV) and demonstrate deep imaging of cortical microvasculature in C57 mice. Specifically, we measure the two- versus three-photon power dependence of these pdots and observe a clear three-photon excitation signature at wavelengths longer than 1300 nm, and a transition from two-photon to three-photon excitation within a 1060 - 1300 nm excitation range. Furthermore, we show that pdots enable in vivo two-photon imaging of cerebrovascular architecture in mice up to 850 μm beneath the pial surface using 800 nm excitation. In contrast with traditional multiphoton probes, we also demonstrate that the broad multiphoton absorption spectrum of pdots permits imaging at longer wavelengths (λex = 1,060 and 1225 nm). These wavelengths approach an ideal biological imaging wavelength near 1,300 nm and confer compatibility with a high-power ytterbium-fiber laser and a high pulse energy optical parametric amplifier, resulting in substantial improvements in signal-to-background ratio (>3.5-fold) and greater cortical imaging depths of 900 μm and 1300 μm. Ultimately, pdots are a versatile tool for MPM due to their extraordinary brightness and broad absorption, which will undoubtedly unlock the ability to interrogate deep structures in vivo.

Coupled Cluster Studies of Ionization Potentials and Electron Affinities of Single-Walled Carbon Nanotubes

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

Peng, Bo; Govind, Niranjan; Aprà, Edoardo

In this paper we apply equation-of-motion coupled cluster (EOMCC) methods in studies of vertical ionization potentials (IP) and electron affinities (EA) for sin- gled walled carbon nanotubes. EOMCC formulations for ionization potentials and electron affinities employing excitation manifolds spanned by single and double ex- citations (IP/EA-EOMCCSD) are used to study IPs and EAs of nanotubes as a function of nanotube length. Several armchair nanotubes corresponding to C20nH20 models with n = 2 - 6 have been used in benchmark calculations. In agreement with previous studies, we demonstrate that the electronegativity of C20nH20 systems remains, to a large extent, independent ofmore » nanotube length. We also compare IP/EA- EOMCCSD results with those obtained with the coupled cluster models with single and double excitations corrected by perturbative triples, CCSD(T), and density func- tional theory (DFT) using global and range-separated hybrid exchange-correlation functionals.« less

Multiphoton microscopic imaging of human normal and cancerous oesophagus tissue.

PubMed

Chen, W S; Wang, Y; Liu, N R; Zhang, J X; Chen, R

2014-01-01

In this paper, microstructures of human oesophageal submucosa are evaluated using multiphoton microscopy, based on two-photon excited fluorescence and second harmonic generation. The content and distribution of collagen, elastic fibers and cancer cells in normal and cancerous submucosa layer have been distinctly obtained and briefly discussed. The variation of these components is very relevant to the pathology in oesophagus, especially in early oesophageal cancer. Our results further indicate that the multiphoton microscopy technique has the potential application in vivo in clinical diagnosis and monitoring of early oesophageal cancer. © 2013 The Authors Journal of Microscopy © 2013 Royal Microscopical Society.

Multiphoton microscopy for the in-situ investigation of cellular processes and integrity in cryopreservation.

PubMed

Doerr, Daniel; Stark, Martin; Ehrhart, Friederike; Zimmermann, Heiko; Stracke, Frank

2009-08-01

In this study we demonstrate a new noninvasive imaging method to monitor freezing processes in biological samples and to investigate life in the frozen state. It combines a laser scanning microscope with a computer-controlled cryostage. Nearinfrared (NIR) femtosecond laser pulses evoke the fluorescence of endogenous fluorophores and fluorescent labels due to multiphoton absorption.The inherent optical nonlinearity of multiphoton absorption allows 3D fluorescence imaging for optical tomography of frozen biological material in-situ. As an example for functional imaging we use fluorescence lifetime imaging (FLIM) to create images with chemical and physical contrast.

Multiphoton microscopy can visualize zonal damage and decreased cellular metabolic activity in hepatic ischemia-reperfusion injury in rats

NASA Astrophysics Data System (ADS)

Thorling, Camilla A.; Liu, Xin; Burczynski, Frank J.; Fletcher, Linda M.; Gobe, Glenda C.; Roberts, Michael S.

2011-11-01

Ischemia-reperfusion (I/R) injury is a common occurrence in liver surgery. In orthotopic transplantation, the donor liver is exposed to periods of ischemia and when oxygenated blood is reintroduced to the liver, oxidative stress may develop and lead to graft failure. The aim of this project was to investigate whether noninvasive multiphoton and fluorescence lifetime imaging microscopy, without external markers, were useful in detecting early liver damage caused by I/R injury. Localized hepatic ischemia was induced in rats for 1 h followed by 4 h reperfusion. Multiphoton and fluorescence lifetime imaging microscopy was conducted prior to ischemia and up to 4 h of reperfusion and compared to morphological and biochemical assessment of liver damage. Liver function was significantly impaired at 2 and 4 h of reperfusion. Multiphoton microscopy detected liver damage at 1 h of reperfusion, manifested by vacuolated cells and heterogeneous spread of damage over the liver. The damage was mainly localized in the midzonal region of the liver acinus. In addition, fluorescence lifetime imaging showed a decrease in cellular metabolic activity. Multiphoton and fluorescence lifetime imaging microscopy detected evidence of early I/R injury both structurally and functionally. This provides a simple noninvasive technique useful for following progressive liver injury without external markers.

Laser spectroscopic study of the Rydberg state structure of atomic lithium

NASA Astrophysics Data System (ADS)

Ballard, M. Kent

1998-07-01

Pulsed laser induced fluorescence spectroscopy was performed on both isotopic species of atomic lithium. Nonresonant multiphoton excitation spectra were recorded. The laser induced fluorescence of the lithium vapor was measured following excitation with a tunable, pulsed, nanosecond laser. Both two- and three-photon allowed transitions were observed resulting in four different transition series originating from the 22S and 22P levels, the latter likely originating from photodissociation products of the lithium dimer, Li2. Forty-seven identifiable transitions were assigned for 6Li. Evidence for a parity forbidden multiphoton transition is also present. For 7Li, fifty-three identifiable transitions were assigned including an additional series of parity forbidden multiphoton transitions. Laser polarization and power dependencies were measured and found to be consistent with the multiphoton transition probabilities. Due to the intense laser fields needed to produce the nonresonant multiphoton excitations, the lithium vapor was subjected to the laser induced ac Stark effect. The Autler-Townes doublets observed for the nF gets 2P transition series were found to exhibit normal asymmetry. The observed asymmetrical Autler-Townes profiles are explained in terms of the two-level and the three-level atomic systems which are based on different excitation schemes. A new computerized data acquisition system was developed as well as associated computer programs needed to analyze spectra.

Structure of multiphoton quantum optics. II. Bipartite systems, physical processes, and heterodyne squeezed states

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

Dell'Anno, Fabio; De Siena, Silvio; Illuminati, Fabrizio

2004-03-01

Extending the scheme developed for a single mode of the electromagnetic field in the preceding paper [F. Dell'Anno, S. De Siena, and F. Illuminati, Phys. Rev. A 69, 033812 (2004)], we introduce two-mode nonlinear canonical transformations depending on two heterodyne mixing angles. They are defined in terms of Hermitian nonlinear functions that realize heterodyne superpositions of conjugate quadratures of bipartite systems. The canonical transformations diagonalize a class of Hamiltonians describing nondegenerate and degenerate multiphoton processes. We determine the coherent states associated with the canonical transformations, which generalize the nondegenerate two-photon squeezed states. Such heterodyne multiphoton squeezed states are defined asmore » the simultaneous eigenstates of the transformed, coupled annihilation operators. They are generated by nonlinear unitary evolutions acting on two-mode squeezed states. They are non-Gaussian, highly nonclassical, entangled states. For a quadratic nonlinearity the heterodyne multiphoton squeezed states define two-mode cubic phase states. The statistical properties of these states can be widely adjusted by tuning the heterodyne mixing angles, the phases of the nonlinear couplings, as well as the strength of the nonlinearity. For quadratic nonlinearity, we study the higher-order contributions to the susceptibility in nonlinear media and we suggest possible experimental realizations of multiphoton conversion processes generating the cubic-phase heterodyne squeezed states.« less

Structure of multiphoton quantum optics. II. Bipartite systems, physical processes, and heterodyne squeezed states

NASA Astrophysics Data System (ADS)

dell'Anno, Fabio; de Siena, Silvio; Illuminati, Fabrizio

2004-03-01

Extending the scheme developed for a single mode of the electromagnetic field in the preceding paper [

Detection of the multiphoton signals in stained tissue using nonlinear optical microscopy

NASA Astrophysics Data System (ADS)

Zeng, Yaping; Xu, Jian; Kang, Deyong; Lin, Jiangbo; Chen, Jianxin

2016-10-01

Multiphoton microscopy (MPM) based on two-photon excited fluorescence (TPEF) and second harmonic generation (SHG) imaging, has become a powerful, important tool for tissue imaging at the molecular level. Recently, MPM is also used to image hematoxylin and eosin (H and E)-stained sections in cancer diagnostics. However, several studies have showed that the MPM images of tissue stained with H and E are significantly different from unstained tissue sections. Our aim was to detect of the multiphoton signals in stained tissue by using MPM. In this paper, MPM was used to image histological sections of esophageal invasive carcinoma tissues stained with H, E, H and E and fresh tissue. To detect of the multiphoton signals in stained tissue, the emission spectroscopic of tissue stained with H, E, H and E were obtained. For comparison, the fresh tissues were also investigated. Our results showed that the tissue stained with H, E, H and E could be detected by their TPEF signals. While the tissue stained with H and fresh tissue could be detected by their TPEF and SHG signals. In this work, we detect of the multiphoton signals in stained tissue. These findings will be useful for choosing suitable staining method so to improve the quality of MPM imaging in the future.

Multi-Wavelength Laser Transmitter for the Two-Step Laser Time-of-Flight Mass Spectrometer

NASA Technical Reports Server (NTRS)

Yu, Anthony W.; Li, Steven X.; Fahey, Molly E.; Grubisic, Andrej; Farcy, Benjamin J.; Uckert, Kyle; Li, Xiang; Getty, Stephanie

2017-01-01

Missions to diverse Outer Solar System bodies will require investigations that can detect a wide range of organics in complex mixtures, determine the structure of selected molecules, and provide powerful insights into their origin and evolution. Previous studies from remote spectroscopy of the Outer Solar System showed a diverse population of macromolecular species that are likely to include aromatic and conjugated hydrocarbons with varying degrees of methylation and nitrile incorporation. In situ exploration of Titan's upper atmosphere via mass and plasma spectrometry has revealed a complex mixture of organics. Similar material is expected on the Ice Giants, their moons, and other Outer Solar System bodies, where it may subsequently be deposited onto surface ices. It is evident that the detection of organics on other planetary surfaces provides insight into the chemical and geological evolution of a Solar System body of interest and can inform our understanding of its potential habitability. We have developed a prototype two-step laser desorption/ionization time-of-flight mass spectrometer (L2MS) instrument by exploiting the resonance-enhanced desorption of analyte. We have successfully demonstrated the ability of the L2MS to detect hydrocarbons in organically-doped analog minerals, including cryogenic Ocean World-relevant ices and mixtures. The L2MS instrument operates by generating a neutral plume of desorbed analyte with an IR desorption laser pulse, followed at a delay by a ultraviolet (UV) laser pulse, ionizing the plume. Desorption of the analyte, including trace organic species, may be enhanced by selecting the wavelength of the IR desorption laser to coincide with IR absorption features associated with vibration transitions of minerals or organic functional groups. In this effort, a preliminary laser developed for the instrument uses a breadboard mid-infrared (MIR) desorption laser operating at a discrete 3.475 µm wavelength, and a breadboard UV ionization laser operating at a wavelength of 266 nm. The MIR wavelength was selected to overlap the C-H stretch vibrational transition of certain aromatic hydrocarbons, and the UV wavelength provides additional selectivity to aromatic species via UV resonance-enhanced multiphoton ionization effects. The use of distinct laser wavelengths allows efficient coupling to the vibrational and electronic spectra of the analyte in independent desorption and ionization steps, mitigating excess energy that can lead to fragmentation during the ionization process and leading to selectivity that can aid in data interpretation.

Autoionizing resonances in electron-impact ionization of O5+ ions

NASA Astrophysics Data System (ADS)

Müller, A.; Teng, H.; Hofmann, G.; Phaneuf, R. A.; Salzborn, E.

2000-12-01

We report on a detailed experimental and theoretical study of electron-impact ionization of O5+ ions. A high-resolution scan measurement of the K-shell excitation threshold region has been performed with statistical uncertainties as low as 0.03%. At this level of precision a wealth of features in the cross section arising from indirect ionization processes becomes visible, and even interference of direct ionization with resonant-excitation/auto-double-ionization (READI) is clearly observed. The experimental results are compared with R-matrix calculations that include both direct and indirect processes in a unified way. Radiative damping of autoionizing Li-like states is found to be about 10-15 %. The calculations almost perfectly reproduce most of the experimental resonance features found in the present measurement including READI. They also agree with the direct-ionization converged close-coupling results of I. Bray [J. Phys. B 28, L247 (1995)] and the absolute total ionization cross section measurement of K. Rinn et al. [Phys. Rev. A 36, 595 (1987)].

Theoretical study of geometry relaxation following core excitation: H2O, NH3, and CH4

NASA Astrophysics Data System (ADS)

Takahashi, Osamu; Kunitake, Naoto; Takaki, Saya

2015-10-01

Single core-hole (SCH) and double core-hole excited state molecular dynamics (MD) calculations for neutral and cationic H2O, NH3, and CH4 have been performed to examine geometry relaxation after core excitation. We observed faster X-H (X = C, N, O) bond elongation for the core-ionized state produced from the valence cationic molecule and the double-core-ionized state produced from the ground and valence cationic molecules than for the first resonant SCH state. Using the results of SCH MD simulations of the ground and valence cationic molecules, Auger decay spectra calculations were performed. We found that fast bond scission leads to peak broadening of the spectra.

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.

Experimental and theoretical double differential cross sections for electron impact ionization of methane

NASA Astrophysics Data System (ADS)

Yavuz, Murat; Ozer, Zehra Nur; Ulu, Melike; Champion, Christophe; Dogan, Mevlut

2016-04-01

Experimental and theoretical double differential cross sections (DDCSs) for electron-induced ionization of methane (CH4) are here reported for primary energies ranging from 50 eV to 350 eV and ejection angles between 25° and 130°. Experimental DDCSs are compared with theoretical predictions performed within the first Born approximation Coulomb wave. In this model, the initial molecular state is described by using single center wave functions, the incident (scattered) electron being described by a plane wave, while a Coulomb wave function is used for modeling the secondary ejected electron. A fairly good agreement may be observed between theory and experiment with nevertheless an expected systematic overestimation of the theory at low-ejection energies (<50 eV).

Ultrafast Structural Dynamics in Combustion Relevant Model Systems

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

Weber, Peter M.

2014-03-31

The research project explored the time resolved structural dynamics of important model reaction system using an array of novel methods that were developed specifically for this purpose. They include time resolved electron diffraction, time resolved relativistic electron diffraction, and time resolved Rydberg fingerprint spectroscopy. Toward the end of the funding period, we also developed time-resolved x-ray diffraction, which uses ultrafast x-ray pulses at LCLS. Those experiments are just now blossoming, as the funding period expired. In the following, the time resolved Rydberg Fingerprint Spectroscopy is discussed in some detail, as it has been a very productive method. The binding energymore » of an electron in a Rydberg state, that is, the energy difference between the Rydberg level and the ground state of the molecular ion, has been found to be a uniquely powerful tool to characterize the molecular structure. To rationalize the structure sensitivity we invoke a picture from electron diffraction: when it passes the molecular ion core, the Rydberg electron experiences a phase shift compared to an electron in a hydrogen atom. This phase shift requires an adjustment of the binding energy of the electron, which is measurable. As in electron diffraction, the phase shift depends on the molecular, geometrical structure, so that a measurement of the electron binding energy can be interpreted as a measurement of the molecule’s structure. Building on this insight, we have developed a structurally sensitive spectroscopy: the molecule is first elevated to the Rydberg state, and the binding energy is then measured using photoelectron spectroscopy. The molecule’s structure is read out as the binding energy spectrum. Since the photoionization can be done with ultrafast laser pulses, the technique is inherently capable of a time resolution in the femtosecond regime. For the purpose of identifying the structures of molecules during chemical reactions, and for the analysis of molecular species in the hot environments of combustion processes, there are several features that make the Rydberg ionization spectroscopy uniquely useful. First, the Rydberg electron’s orbit is quite large and covers the entire molecule for most molecular structures of combustion interest. Secondly, the ionization does not change vibrational quantum numbers, so that even complicated and large molecules can be observed with fairly well resolved spectra. In fact, the spectroscopy is blind to vibrational excitation of the molecule. This has the interesting consequence for the study of chemical dynamics, where the molecules are invariably very energetic, that the molecular structures are observed unobstructed by the vibrational congestion that dominates other spectroscopies. This implies also that, as a tool to probe the time-dependent structural dynamics of chemically interesting molecules, Rydberg spectroscopy may well be better suited than electron or x-ray diffraction. With recent progress in calculating Rydberg binding energy spectra, we are approaching the point where the method can be evolved into a structure determination method. To implement the Rydberg ionization spectroscopy we use a molecular beam based, time-resolved pump-probe multi-photon ionization/photoelectron scheme in which a first laser pulse excites the molecule to a Rydberg state, and a probe pulse ionizes the molecule. A time-of-flight detector measures the kinetic energy spectrum of the photoelectrons. The photoelectron spectrum directly provides the binding energy of the electron, and thereby reveals the molecule’s time-dependent structural fingerprint. Only the duration of the laser pulses limits the time resolution. With a new laser system, we have now reached time resolutions better than 100 fs, although very deep UV wavelengths (down to 190 nm) have slightly longer instrument functions. The structural dynamics of molecules in Rydberg-excited states is obtained by delaying the probe ionization photon from the pump photon; the structural dynamics of molecules in their ground state or excited valence states is measured by inducing the dynamics using a near UV laser pulse, and employing a multi-photon ionization scheme via the Rydberg states as a probe process. Thus, the technique is capable of measuring the reaction dynamics in any electronic state of neutral molecules.« less

The Ar-NO van der Waals complex studied by resonant multiphoton ionization spectroscopy involving photoion and photoelectron measurements

NASA Astrophysics Data System (ADS)

Sato, Kenji; Achiba, Yohji; Kimura, Katsumi

1984-07-01

Using a 5% mixture of NO in Ar in a supersonic free jet, in the present work we have carried out measurements of the total ion current in the 380-385 nm laser wavelength region. We have also measured photoelectron kinetic energy spectra at individual ion current peaks. In the ion-current spectrum we have observed a new vibrational progression which consists of four peaks in the wavelength region longer than the peak of the two-photon transition of the free NO molecule NO(X, v″=0) →2hν NO(C,v'=0). It has been concluded that the new ion-current peaks are attributed to bound-to-bound transitions of the Ar-NO van der Waals complex from its ground state to the two-photon resonant state expressed by Ar-NO*(C 2Π, v'=0), in which the NO component is in the 3p Rydberg state. The whole resonant ionization process studied may be expressed by Ar-NO(X, v″=0) →2hνAr-NO*(C, v'=0) →hν Ar-NO+(X, v+=0). Each ion-current peak separation is about 50 cm-1, which may correspond to the frequency of the Ar-NO intermolecular stretching vibration, showing a strong anharmonicity. The dissociation energy (D0) of the Ar-NO*(C 2Π) state has been found to be 0.055±0.001 eV. From the photoelectron spectra, we also conclude that the adiabatic ionization energy of Ar-NO is Ia =9.148±0.005 eV and the dissociation energy of the Ar-NO+(X 1Σ) ion is D0=0.129±0.005 eV.

A novel flexible clinical multiphoton tomograph for early melanoma detection, skin analysis, testing of anti-age products, and in situ nanoparticle tracking

NASA Astrophysics Data System (ADS)

Weinigel, Martin; Breunig, Hans Georg; Gregory, Axel; Fischer, Peter; Kellner-Höfer, Marcel; Bückle, Rainer; König, Karsten

2010-02-01

High-resolution 3D microscopy based on multiphoton induced autofluorescence and second harmonic generation have been introduced in 1990. 13 years later, CE-marked clinical multiphoton systems for 3D imaging of human skin with subcellular resolution have first been launched by JenLab company with the tomography DermaInspect®. This year, the second generation of clinical multiphoton tomographs was introduced. The novel multiphoton tomograph MPTflex, equipped with a flexible articulated optical arm, provides an increased flexibility and accessibility especially for clinical and cosmetical examinations. Improved image quality and signal to noise ratio (SNR) are achieved by a very short source-drain spacing, by larger active areas of the detectors and by single photon counting (SPC) technology. Shorter image acquisition time due to improved image quality reduces artifacts and simplifies the operation of the system. The compact folded optical design and the light-weight structure of the optical head eases the handling. Dual channel detectors enable to distinguish between intratissue elastic fibers and collagenous structures simultaneously. Through the use of piezo-driven optics a stack of optical cross-sections (optical sectioning) can be acquired and 3D imaging can be performed. The multiphoton excitation of biomolecules like NAD(P)H, flavins, porphyrins, elastin, and melanin is done by picojoule femtosecond laser pulses from an tunable turn-key femtosescond near infrared laser system. The ability for rapid high-quality image acquisition, the user-friendly operation of the system and the compact and flexible design qualifies this system to be used for melanoma detection, diagnostics of dermatological disorders, cosmetic research and skin aging measurements as well as in situ drug monitoring and animal research.

Spin Multiphoton Antiresonance at Finite Temperatures

NASA Astrophysics Data System (ADS)

Hicke, Christian; Dykman, Mark

2007-03-01

Weakly anisotropic S>1 spin systems display multiphoton antiresonance. It occurs when an Nth overtone of the radiation frequency coincides with the distance between the ground and the Nth excited energy level (divided by ). The coherent response of the spin displays a sharp minimum or maximum as a function of frequency, depending on which state was initially occupied. We find the spectral shape of the response dips/peaks. We also study the stationary response for zero and finite temperatures. The response changes dramatically with increasing temperature, when excited states become occupied even in the absence of radiation. The change is due primarily to the increasing role of single-photon resonances between excited states, which occur at the same frequencies as multiphoton resonances. Single-photon resonances are broad, because the single-photon Rabi frequencies largely exceed the multi-photon ones. This allows us to separate different resonances and to study their spectral shape. We also study the change of the spectrum due to relaxational broadening of the peaks, with account taken of both decay and phase modulation.

High speed multiphoton imaging

NASA Astrophysics Data System (ADS)

Li, Yongxiao; Brustle, Anne; Gautam, Vini; Cockburn, Ian; Gillespie, Cathy; Gaus, Katharina; Lee, Woei Ming

2016-12-01

Intravital multiphoton microscopy has emerged as a powerful technique to visualize cellular processes in-vivo. Real time processes revealed through live imaging provided many opportunities to capture cellular activities in living animals. The typical parameters that determine the performance of multiphoton microscopy are speed, field of view, 3D imaging and imaging depth; many of these are important to achieving data from in-vivo. Here, we provide a full exposition of the flexible polygon mirror based high speed laser scanning multiphoton imaging system, PCI-6110 card (National Instruments) and high speed analog frame grabber card (Matrox Solios eA/XA), which allows for rapid adjustments between frame rates i.e. 5 Hz to 50 Hz with 512 × 512 pixels. Furthermore, a motion correction algorithm is also used to mitigate motion artifacts. A customized control software called Pscan 1.0 is developed for the system. This is then followed by calibration of the imaging performance of the system and a series of quantitative in-vitro and in-vivo imaging in neuronal tissues and mice.

Tuning single-photon sources for telecom multi-photon experiments.

PubMed

Greganti, Chiara; Schiansky, Peter; Calafell, Irati Alonso; Procopio, Lorenzo M; Rozema, Lee A; Walther, Philip

2018-02-05

Multi-photon state generation is of great interest for near-future quantum simulation and quantum computation experiments. To-date spontaneous parametric down-conversion is still the most promising process, even though two major impediments still exist: accidental photon noise (caused by the probabilistic non-linear process) and imperfect single-photon purity (arising from spectral entanglement between the photon pairs). In this work, we overcome both of these difficulties by (1) exploiting a passive temporal multiplexing scheme and (2) carefully optimizing the spectral properties of the down-converted photons using periodically-poled KTP crystals. We construct two down-conversion sources in the telecom wavelength regime, finding spectral purities of > 91%, while maintaining high four-photon count rates. We use single-photon grating spectrometers together with superconducting nanowire single-photon detectors to perform a detailed characterization of our multi-photon source. Our methods provide practical solutions to produce high-quality multi-photon states, which are in demand for many quantum photonics applications.

ARTICLES: Variation of the absorption cross section of high-power infrared laser radiation in homologous series of CnH2n+1OH molecules

NASA Astrophysics Data System (ADS)

Bagratashvili, Viktor N.; Brodskaya, E. A.; Vereshchagina, Lyudmila N.; Kuz'min, M. V.; Osmanov, R. R.; Putilin, F. N.; Stuchebryukhov, A. A.

1984-11-01

An experimental investigation was made of variation of the characteristics of infrared multiphoton absorption in a homologous series of CnH2n+1OH alcohols (n = 1-5) excited with CO2 laser pulses. The dependences of the energy absorbed by the molecules on the frequency and energy density of laser radiation were determined by the optoacoustic method. It was found that the multiphoton absorption cross section decreases on increase in the radiation energy density at a rate which becomes slower on increase in the molecular size. A model is proposed for multiphoton excitation of molecules in a homologous series. This model is based on an analysis of a resonant mode interacting with the infrared radiation field and coupled to a reservoir of modes that do not interact with the field. The model predicts correctly the change in the multiphoton absorption cross section on increase in the number of the degrees of freedom of a molecule.

Spatiotemporal focusing-based widefield multiphoton microscopy for fast optical sectioning.

PubMed

Cheng, Li-Chung; Chang, Chia-Yuan; Lin, Chun-Yu; Cho, Keng-Chi; Yen, Wei-Chung; Chang, Nan-Shan; Xu, Chris; Dong, Chen Yuan; Chen, Shean-Jen

2012-04-09

In this study, a microscope based on spatiotemporal focusing offering widefield multiphoton excitation has been developed to provide fast optical sectioning images. Key features of this microscope are the integrations of a 10 kHz repetition rate ultrafast amplifier featuring high instantaneous peak power (maximum 400 μJ/pulse at a 90 fs pulse width) and a TE-cooled, ultra-sensitive photon detecting, electron multiplying charge-coupled camera into a spatiotemporal focusing microscope. This configuration can produce multiphoton images with an excitation area larger than 200 × 100 μm² at a frame rate greater than 100 Hz (current maximum of 200 Hz). Brownian motions of fluorescent microbeads as small as 0.5 μm were observed in real-time with a lateral spatial resolution of less than 0.5 μm and an axial resolution of approximately 3.5 μm. Furthermore, second harmonic images of chicken tendons demonstrate that the developed widefield multiphoton microscope can provide high resolution z-sectioning for bioimaging.

Focal switching of photochromic fluorescent proteins enables multiphoton microscopy with superior image contrast.

PubMed

Kao, Ya-Ting; Zhu, Xinxin; Xu, Fang; Min, Wei

2012-08-01

Probing biological structures and functions deep inside live organisms with light is highly desirable. Among the current optical imaging modalities, multiphoton fluorescence microscopy exhibits the best contrast for imaging scattering samples by employing a spatially confined nonlinear excitation. However, as the incident laser power drops exponentially with imaging depth into the sample due to the scattering loss, the out-of-focus background eventually overwhelms the in-focus signal, which defines a fundamental imaging-depth limit. Herein we significantly improve the image contrast for deep scattering samples by harnessing reversibly switchable fluorescent proteins (RSFPs) which can be cycled between bright and dark states upon light illumination. Two distinct techniques, multiphoton deactivation and imaging (MPDI) and multiphoton activation and imaging (MPAI), are demonstrated on tissue phantoms labeled with Dronpa protein. Such a focal switch approach can generate pseudo background-free images. Conceptually different from wave-based approaches that try to reduce light scattering in turbid samples, our work represents a molecule-based strategy that focused on imaging probes.

Focal switching of photochromic fluorescent proteins enables multiphoton microscopy with superior image contrast

PubMed Central

Kao, Ya-Ting; Zhu, Xinxin; Xu, Fang; Min, Wei

2012-01-01

Probing biological structures and functions deep inside live organisms with light is highly desirable. Among the current optical imaging modalities, multiphoton fluorescence microscopy exhibits the best contrast for imaging scattering samples by employing a spatially confined nonlinear excitation. However, as the incident laser power drops exponentially with imaging depth into the sample due to the scattering loss, the out-of-focus background eventually overwhelms the in-focus signal, which defines a fundamental imaging-depth limit. Herein we significantly improve the image contrast for deep scattering samples by harnessing reversibly switchable fluorescent proteins (RSFPs) which can be cycled between bright and dark states upon light illumination. Two distinct techniques, multiphoton deactivation and imaging (MPDI) and multiphoton activation and imaging (MPAI), are demonstrated on tissue phantoms labeled with Dronpa protein. Such a focal switch approach can generate pseudo background-free images. Conceptually different from wave-based approaches that try to reduce light scattering in turbid samples, our work represents a molecule-based strategy that focused on imaging probes. PMID:22876358

Spectroscopic imaging of self-organization in high power impulse magnetron sputtering plasmas

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

Andersson, Joakim; Centre for Quantum Technologies, National University of Singapore, 3 Science Drive 2, 117543 Singapore; Ni, Pavel

Excitation and ionization conditions in traveling ionization zones of high power impulse magnetron sputtering plasmas were investigated using fast camera imaging through interference filters. The images, taken in end-on and side-on views using light of selected gas and target atom and ion spectral lines, suggest that ionization zones are regions of enhanced densities of electrons, and excited atoms and ions. Excited atoms and ions of the target material (Al) are strongly concentrated near the target surface. Images from the highest excitation energies exhibit the most localized regions, suggesting localized Ohmic heating consistent with double layer formation.

Spectroscopic imaging of self-organization in high power impulse magnetron sputtering plasmas

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

Centre for Quantum Technologies, National University of Singapore, 3 Science Drive 2, 117543 Singapore, Singapore; Andersson, Joakim; Ni, Pavel

Excitation and ionization conditions in traveling ionization zones of high power impulse magnetron sputtering plasmas were investigated using fast camera imaging through interference filters. The images, taken in end-on and side on views using light of selected gas and target atom and ion spectral lines, suggest that ionization zones are regions of enhanced densities of electrons, and excited atoms and ions. Excited atoms and ions of the target material (Al) are strongly concentrated near the target surface. Images from the highest excitation energies exhibit the most localized regions, suggesting localized Ohmic heating consistent with double layer formation.

The ArDM experiment

DOE PAGES

Harańczyk, M.; Amsler, C.; Badertscher, A.; ...

2010-08-24

The aim of the ArDM project is the development and operation of a one ton double-phase liquid argon detector for direct Dark Matter searches. The detector measures both the scintillation light and the ionization charge from ionizing radiation using two independent readout systems. This paper briefly describes the detector concept and presents preliminary results from the ArDM R & D program, including a 3 l prototype developed to test the charge readout system.

Quantum interference in laser-induced nonsequential double ionization

NASA Astrophysics Data System (ADS)

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

2017-09-01

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

High-resolution multiphoton microscopy with a low-power continuous wave laser pump.

PubMed

Chen, Xiang-Dong; Li, Shen; Du, Bo; Dong, Yang; Wang, Ze-Hao; Guo, Guang-Can; Sun, Fang-Wen

2018-02-15

Multiphoton microscopy (MPM) has been widely used for three-dimensional biological imaging. Here, based on the photon-induced charge state conversion process, we demonstrated a low-power high-resolution MPM with a nitrogen vacancy (NV) center in diamond. Continuous wave green and orange lasers were used to pump and detect the two-photon charge state conversion, respectively. The power of the laser for multiphoton excitation was 40 μW. Both the axial and lateral resolutions were improved approximately 1.5 times compared with confocal microscopy. The results can be used to improve the resolution of the NV center-based quantum sensing and biological imaging.

Clinical combination of multiphoton tomography and high frequency ultrasound imaging for evaluation of skin diseases

NASA Astrophysics Data System (ADS)

König, K.; Speicher, M.; Koehler, M. J.; Scharenberg, R.; Elsner, P.; Kaatz, M.

2010-02-01

For the first time, high frequency ultrasound imaging, multiphoton tomography, and dermoscopy were combined in a clinical study. Different dermatoses such as benign and malign skin cancers, connective tissue diseases, inflammatory skin diseases and autoimmune bullous skin diseases have been investigated with (i) state-of-the-art and highly sophisticated ultrasound systems for dermatology, (ii) the femtosecond-laser multiphoton tomograph DermaInspectTM and (iii) dermoscopes. Dermoscopy provides two-dimensional color imaging of the skin surface with a magnification up to 70x. Ultrasound images are generated from reflections of the emitted ultrasound signal, based on inhomogeneities of the tissue. These echoes are converted to electrical signals. Depending on the ultrasound frequency the penetration depth varies from about 1 mm to 16 mm in dermatological application. The 100-MHz-ultrasound system provided an axial resolution down to 16 μm and a lateral resolution down to 32 μm. In contrast to the wide-field ultrasound images, multiphoton tomography provided horizontal optical sections of 0.36×0.36 mm2 down to 200 μm tissue depth with submicron resolution. The autofluorescence of mitochondrial coenzymes, melanin, and elastin as well as the secondharmonic- generation signal of the collagen network were imaged. The combination of ultrasound and multiphoton tomography provides a novel opportunity for diagnostics of skin disorders.

USE OF MULTIPHOTON LASER SCANNING MICROSCOPY TO IMAGE BENZO[A]PYRENE AND METABOLITES IN FISH EGGS

EPA Science Inventory

Multiphoton laser scanning microscopy (MPLSM) is a promising tool to study the tissue distribution of environmental chemical contaminants during fish early life stages. One such chemical for which this is possible is benzo[a]pyrene (BaP), a polycyclic aromatic hydrocarbon that a...

Multiphoton Imaging of Rabbit Cornea Treated with Mitomycin C after Photorefractive Keratectomy

NASA Astrophysics Data System (ADS)

Hsueh, Chiu-Mei; Lo, Wen; Wang, Tsung-Jen; Hu, Fung-Rong; Dong, Chen-Yuan

2007-07-01

In this work we use multiphoton microscopy to observe the post surgery structure variation of rabbit cornea after photorefractive keratectomy (PRK). In addition, we added mitomycin C (MMC) to the post surgery rabbit cornea in order to investigate the effect of MMC treatment on the postoperative regeneration.

Scaling Laws of the Two-Electron Sum-Energy Spectrum in Strong-Field Double Ionization.

PubMed

Ye, Difa; Li, Min; Fu, Libin; Liu, Jie; Gong, Qihuang; Liu, Yunquan; Ullrich, J

2015-09-18

The sum-energy spectrum of two correlated electrons emitted in nonsequential strong-field double ionization (SFDI) of Ar was studied for intensities of 0.3 to 2×10^{14} W/cm^{2}. We find the mean sum energy, the maximum of the distributions as well as the high-energy tail of the scaled (to the ponderomotive energy) spectra increase with decreasing intensity below the recollision threshold (BRT). At higher intensities the spectra collapse into a single distribution. This behavior can be well explained within a semiclassical model providing clear evidence of the importance of multiple recollisions in the BRT regime. Here, ultrafast thermalization between both electrons is found occurring within three optical cycles only and leaving its clear footprint in the sum-energy spectra.

Nonlinear Dichroism in Back-to-Back Double Ionization of He by an Intense Elliptically Polarized Few-Cycle Extreme Ultraviolet Pulse.

PubMed

Ngoko Djiokap, J M; Manakov, N L; Meremianin, A V; Hu, S X; Madsen, L B; Starace, Anthony F

2014-11-28

Control of double ionization of He by means of the polarization and carrier-envelope phase (CEP) of an intense, few-cycle extreme ultraviolet (XUV) pulse is demonstrated numerically by solving the six-dimensional two-electron, time-dependent Schrödinger equation for He interacting with an elliptically polarized XUV pulse. Guided by perturbation theory (PT), we predict the existence of a nonlinear dichroic effect (∝I^{3/2}) that is sensitive to the CEP, ellipticity, peak intensity I, and temporal duration of the pulse. This dichroic effect (i.e., the difference of the two-electron angular distributions for opposite helicities of the ionizing XUV pulse) originates from interference of first- and second-order PT amplitudes, allowing one to probe and control S- and D-wave channels of the two-electron continuum. We show that the back-to-back in-plane geometry with unequal energy sharing is an ideal one for observing this dichroic effect that occurs only for an elliptically polarized, few-cycle attosecond pulse.

Application of Laser Mass Spectrometry to Art and Archaeology

NASA Technical Reports Server (NTRS)

Gulian, Lase Lisa E.; Callahan, Michael P.; Muliadi, Sarah; Owens, Shawn; McGovern, Patrick E.; Schmidt, Catherine M.; Trentelman, Karen A.; deVries, Mattanjah S.

2011-01-01

REMPI laser mass spectrometry is a combination of resonance enhanced multiphoton ionization spectroscopy and time of flight mass spectrometry, This technique enables the collection of mass specific optical spectra as well as of optically selected mass spectra. Analytes are jet-cooled by entrainment in a molecular beam, and this low temperature gas phase analysis has the benefit of excellent vibronic resolution. Utilizing this method, mass spectrometric analysis of historically relevant samples can be simplified and improved; Optical selection of targets eliminates the need for chromatography while knowledge of a target's gas phase spectroscopy allows for facile differentiation of molecules that are in the aqueous phase considered spectroscopically indistinguishable. These two factors allow smaller sample sizes than commercial MS instruments, which in turn will require less damage to objects of antiquity. We have explored methods to optimize REMPI laser mass spectrometry as an analytical tool to archaeology using theobromine and caffeine as molecular markers in Mesoamerican pottery, and are expanding this approach to the field of art to examine laccaic acid in shellacs.

Enantiomer-specific analysis of multi-component mixtures by correlated electron imaging-ion mass spectrometry

NASA Astrophysics Data System (ADS)

Fanood, Mohammad M. Rafiee; Ram, N. Bhargava; Lehmann, C. Stefan; Powis, Ivan; Janssen, Maurice H. M.

2015-06-01

Simultaneous, enantiomer-specific identification of chiral molecules in multi-component mixtures is extremely challenging. Many established techniques for single-component analysis fail to provide selectivity in multi-component mixtures and lack sensitivity for dilute samples. Here we show how enantiomers may be differentiated by mass-selected photoelectron circular dichroism using an electron-ion coincidence imaging spectrometer. As proof of concept, vapours containing ~1% of two chiral monoterpene molecules, limonene and camphor, are irradiated by a circularly polarized femtosecond laser, resulting in multiphoton near-threshold ionization with little molecular fragmentation. Large chiral asymmetries (2-4%) are observed in the mass-tagged photoelectron angular distributions. These asymmetries switch sign according to the handedness (R- or S-) of the enantiomer in the mixture and scale with enantiomeric excess of a component. The results demonstrate that mass spectrometric identification of mixtures of chiral molecules and quantitative determination of enantiomeric excess can be achieved in a table-top instrument.

Dramatic enhancement of supercontinuum generation in elliptically-polarized laser filaments

PubMed Central

Rostami, Shermineh; Chini, Michael; Lim, Khan; Palastro, John P.; Durand, Magali; Diels, Jean-Claude; Arissian, Ladan; Baudelet, Matthieu; Richardson, Martin

2016-01-01

Broadband laser sources based on supercontinuum generation in femtosecond laser filamentation have enabled applications from stand-off sensing and spectroscopy to the generation and self-compression of high-energy few-cycle pulses. Filamentation relies on the dynamic balance between self-focusing and plasma defocusing – mediated by the Kerr nonlinearity and multiphoton or tunnel ionization, respectively. The filament properties, including the supercontinuum generation, are therefore highly sensitive to the properties of both the laser source and the propagation medium. Here, we report the anomalous spectral broadening of the supercontinuum for filamentation in molecular gases, which is observed for specific elliptical polarization states of the input laser pulse. The resulting spectrum is accompanied by a modification of the supercontinuum polarization state and a lengthening of the filament plasma column. Our experimental results and accompanying simulations suggest that rotational dynamics of diatomic molecules play an essential role in filamentation-induced supercontinuum generation, which can be controlled with polarization ellipticity. PMID:26847427

Photoemission of Energetic Hot Electrons Produced via Up-Conversion in Doped Quantum Dots.

PubMed

Dong, Yitong; Parobek, David; Rossi, Daniel; Son, Dong Hee

2016-11-09

The benefits of the hot electrons from semiconductor nanostructures in photocatalysis or photovoltaics result from their higher energy compared to that of the band-edge electrons facilitating the electron-transfer process. The production of high-energy hot electrons usually requires short-wavelength UV or intense multiphoton visible excitation. Here, we show that highly energetic hot electrons capable of above-threshold ionization are produced via exciton-to-hot-carrier up-conversion in Mn-doped quantum dots under weak band gap excitation (∼10 W/cm 2 ) achievable with the concentrated solar radiation. The energy of hot electrons is as high as ∼0.4 eV above the vacuum level, much greater than those observed in other semiconductor or plasmonic metal nanostructures, which are capable of performing energetically and kinetically more-challenging electron transfer. Furthermore, the prospect of generating solvated electron is unique for the energetic hot electrons from up-conversion, which can open a new door for long-range electron transfer beyond short-range interfacial electron transfer.

Enantiomer-specific analysis of multi-component mixtures by correlated electron imaging–ion mass spectrometry

PubMed Central

Fanood, Mohammad M Rafiee; Ram, N. Bhargava; Lehmann, C. Stefan; Powis, Ivan; Janssen, Maurice H. M.

2015-01-01

Simultaneous, enantiomer-specific identification of chiral molecules in multi-component mixtures is extremely challenging. Many established techniques for single-component analysis fail to provide selectivity in multi-component mixtures and lack sensitivity for dilute samples. Here we show how enantiomers may be differentiated by mass-selected photoelectron circular dichroism using an electron–ion coincidence imaging spectrometer. As proof of concept, vapours containing ∼1% of two chiral monoterpene molecules, limonene and camphor, are irradiated by a circularly polarized femtosecond laser, resulting in multiphoton near-threshold ionization with little molecular fragmentation. Large chiral asymmetries (2–4%) are observed in the mass-tagged photoelectron angular distributions. These asymmetries switch sign according to the handedness (R- or S-) of the enantiomer in the mixture and scale with enantiomeric excess of a component. The results demonstrate that mass spectrometric identification of mixtures of chiral molecules and quantitative determination of enantiomeric excess can be achieved in a table-top instrument. PMID:26104140

Below-threshold harmonic generation from strong non-uniform fields

NASA Astrophysics Data System (ADS)

Yavuz, I.

2017-10-01

Strong-field photoemission below the ionization threshold is a rich/complex region where atomic emission and harmonic generation may coexist. We studied the mechanism of below-threshold harmonics (BTH) from spatially non-uniform local fields near the metallic nanostructures. Discrete harmonics are generated due to the broken inversion symmetry, suggesting enriched coherent emission in the vuv frequency range. Through the numerical solution of the time-dependent Schrödinger equation, we investigate wavelength and intensity dependence of BTH. Wavelength dependence identifies counter-regular resonances; individual contributions from the multi-photon emission and channel-closing effects due to quantum path interferences. In order to understand the underlying mechanism of BTH, we devised a generalized semi-classical model, including the influence of Coulomb and non-uniform field interactions. As in uniform fields, Coulomb potential in non-uniform fields is the determinant of BTH; we observed that the generation of BTH are due to returning trajectories with negative energies. Due to large distance effectiveness of the non-uniformity, only long trajectories are noticeably affected.

Analytical model for atomic resonant attosecond transient absorption

NASA Astrophysics Data System (ADS)

Cariker, C.; Kjellson, T.; Lindroth, E.; Argenti, L.

2017-04-01

Recent advancements in ultrafast laser technology have made it possible to probe electron dynamics in highly excited atomic states that autoionize on a femtosecond timescale, thus giving insight into the dynamics of Auger decay and its interference with the continuum. These experiments provide a stringent test for time-resolved analytical models of autoionization. Here we present a finite-pulse, multi-photon perturbative model which is used in conjunction with ab-initio structure calculations to predict the attosecond transient absorption spectrum (ATAS) of an atom above the ionization threshold. We apply this model to compute the ATAS of argon in the vicinity of the 3s-1 4 p resonance as a function of the time delay between an extreme ultraviolet (XUV) and an infrared (IR) pulse, as well as of the angle between their polarization. We show that by modulating the parameters of the IR pulse it is possible to control the dipolar coupling between neighboring states and hence the lineshape of the 3s-1 4 p resonance. NSF Grant No. 1607588.

Enhancing nonlinear energy deposition into transparent solids with an elliptically polarized and mid-IR heating laser pulse under two-color femtosecond impact

NASA Astrophysics Data System (ADS)

Potemkin, F. V.; Mareev, E. I.; Bezsudnova, Yu I.; Platonenko, V. T.; Bravy, B. G.; Gordienko, V. M.

2017-06-01

We report on an enhancement of deposited energy density of up to 10 kJ cm-3 inside transparent solids (fused silica and quartz) from using two-color µJ energy level tightly focused (NA  =  0.5) co-propagating linearly polarized seeding (visible, 0.62 µm) and elliptically polarized heating (near-IR, 1.24 µm) femtosecond laser pulses. The rise in temperature under constant volume causes pressure of up to 12 GPa. It has been shown experimentally and theoretically that the production of seeding electrons through multiphoton ionization by visible laser pulse paves the way for controllability of the energy deposition and laser-induced micromodification via carrier heating by delayed infrared laser pulses inside the material. The developed theoretical approach predicts that the deposited energy density will be enhanced by up to 14 kJ cm-3 when using longer (up to 5 µm) wavelengths for heating laser pulses inside transparent solids.

High-precision laser spectroscopy of the CO A(1)Π - X(1)Σ(+) (2,0), (3,0), and (4,0) bands.

PubMed

Niu, M L; Ramirez, F; Salumbides, E J; Ubachs, W

2015-01-28

High-precision two-photon Doppler-free frequency measurements have been performed on the CO A(1)Π - X(1)Σ(+) fourth-positive system (2,0), (3,0), and (4,0) bands. Absolute frequencies of forty-three transitions, for rotational quantum numbers up to J = 5, have been determined at an accuracy of 1.6 × 10(-3) cm(-1), using advanced techniques of two-color 2  +  1' resonance-enhanced multi-photon ionization, Sagnac interferometry, frequency-chirp analysis on the laser pulses, and correction for AC-Stark shifts. The accurate transition frequencies of the CO A(1)Π - X(1)Σ(+) system are of relevance for comparison with astronomical data in the search for possible drifts of fundamental constants in the early universe. The present accuracies in laboratory wavelengths of Δλ/λ = 2 × 10(-8) may be considered exact for the purpose of such comparisons.

Experiment and simulation of novel liquid crystal plasma mirrors for high contrast, intense laser pulses

PubMed Central

Poole, P. L.; Krygier, A.; Cochran, G. E.; Foster, P. S.; Scott, G. G.; Wilson, L. A.; Bailey, J.; Bourgeois, N.; Hernandez-Gomez, C.; Neely, D.; Rajeev, P. P.; Freeman, R. R.; Schumacher, D. W.

2016-01-01

We describe the first demonstration of plasma mirrors made using freely suspended, ultra-thin films formed dynamically and in-situ. We also present novel particle-in-cell simulations that for the first time incorporate multiphoton ionization and dielectric models that are necessary for describing plasma mirrors. Dielectric plasma mirrors are a crucial component for high intensity laser applications such as ion acceleration and solid target high harmonic generation because they greatly improve pulse contrast. We use the liquid crystal 8CB and introduce an innovative dynamic film formation device that can tune the film thickness so that it acts as its own antireflection coating. Films can be formed at a prolonged, high repetition rate without the need for subsequent realignment. High intensity reflectance above 75% and low-field reflectance below 0.2% are demonstrated, as well as initial ion acceleration experimental results that demonstrate increased ion energy and yield on shots cleaned with these plasma mirrors. PMID:27557592

Electron-hydrogen collisions in a laser field. (Reannouncement with new availability information)

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

Smith, P.H.; Flannery, M.R.

1991-12-31

The Floquet treatment has already been successfully employed (Chu, Potvliege and Shakeshaft) in calculations of laser-induced multiphoton ionizations, where it provides dressed states for an atom in a laser field. The (perturbative) dressing of target states can have important consequences in laser-assisted scattering was illustrated by Byron and Joachain. These dressed states are useful, not only for laser-induced phenomena, but also as a collisional basis set for laser-assisted collisions. In this role they are in fact very appealing, since the Floquet treatment naturally lends itself to a time-independent analysis, and hence are compatible with present field-free scattering theories. Despite themore » apparent applicability of this approach, work along these lines has only just recently appeared (Sharma and Mohan, Smith and Flannery, Burke et al). Byron and Joachain have illustrated that perturbative dressing of the target states can have important consequences in laser-assisted scattering. Floquet dressing however provides a more complete description (Smith and Flannery).« less

Experiment and simulation of novel liquid crystal plasma mirrors for high contrast, intense laser pulses

DOE PAGES

Poole, P. L.; Krygier, A.; Cochran, G. E.; ...

2016-08-25

Here, we describe the first demonstration of plasma mirrors made using freely suspended, ultra-thin films formed dynamically and in-situ. We also present novel particle-in-cell simulations that for the first time incorporate multiphoton ionization and dielectric models that are necessary for describing plasma mirrors. Dielectric plasma mirrors are a crucial component for high intensity laser applications such as ion acceleration and solid target high harmonic generation because they greatly improve pulse contrast. We use the liquid crystal 8CB and introduce an innovative dynamic film formation device that can tune the film thickness so that it acts as its own antireflection coating.more » Films can be formed at a prolonged, high repetition rate without the need for subsequent realignment. High intensity reflectance above 75% and low-field reflectance below 0.2% are demonstrated, as well as initial ion acceleration experimental results that demonstrate increased ion energy and yield on shots cleaned with these plasma mirrors.« less

Infrared laser dissociation of single megadalton polymer ions in a gated electrostatic ion trap: the added value of statistical analysis of individual events.

PubMed

Halim, Mohammad A; Clavier, Christian; Dagany, Xavier; Kerleroux, Michel; Dugourd, Philippe; Dunbar, Robert C; Antoine, Rodolphe

2018-05-07

In this study, we report the unimolecular dissociation mechanism of megadalton SO 3 -containing poly(2-acrylamido-2-methyl-1-propanesulfonic acid) (PAMPS) polymer cations and anions with the aid of infrared multiphoton dissociation coupled to charge detection ion trap mass spectrometry. A gated electrostatic ion trap ("Benner trap") is used to store and detect single gaseous polymer ions generated by positive and negative polarity in an electrospray ionization source. The trapped ions are then fragmented due to the sequential absorption of multiple infrared photons produced from a continuous-wave CO 2 laser. Several fragmentation pathways having distinct signatures are observed. Highly charged parent ions characteristically adopt a distinctive "stair-case" pattern (assigned to the "fission" process) whereas low charge species take on a "funnel like" shape (assigned to the "evaporation" process). Also, the log-log plot of the dissociation rate constants as a function of laser intensity between PAMPS positive and negative ions is significantly different.

Exploration of the Dissociative Recombination following DNA ionization to DNA+ due to ionizing radiation

NASA Astrophysics Data System (ADS)

Strom, Richard A.; Zimmerly, Andrew T.; Andrianarijaona, Vola M.

2014-05-01

It is known that ionizing radiation generates low-energy secondary electrons, which may interact with the surrounding area, including biomolecules, such as triggering DNA single strand and double strand breaks as demonstrated by Sanche and coworkers (Radiat. Res. 157, 227(2002)). The bio-effects of low-energy electrons are currently a topic of high interest. Most of the studies are dedicated to dissociative electron attachments; however, the area is still mostly unexplored and still not well understood. We are computationally investigating the effect of ionizing radiation on DNA, such as its ionization to DNA+. More specifically, we are exploring the possibility of the dissociative recombination of the temporary DNA+ with one of the low-energy secondary electrons, produced by the ionizing radiation, to be another process of DNA strand breaks. Our preliminary results, which are performed with the binaries of ORCA, will be presented. Authors wish to give special thanks to Pacific Union College Student Senate in Angwin, California, for their financial support.

Ionization Cross Sections and Dissociation Channels of the DNA Sugar-Phosphate Backbone by Electron Collisions

NASA Technical Reports Server (NTRS)

Dateo, Christopher; Huo, Winifred M.; Fletcher, Graham D.

2004-01-01

It has been suggested that the genotoxic effects of ionizing radiation in living cells are not caused by the highly energetic incident radiation, but rather are induced by less energetic secondary species generated, the most abundant of which are free electrons.' The secondary electrons will further react to cause DNA damage via indirect and direct mechanisms. Detailed knowledge of these mechanisms is ultimately important for the development of global models of cellular radiation damage. We are studying one possible mechanism for the formation cf DNA strand breaks involving dissociative ionization of the DNA sugar-phosphate backbone induced by secondary electron co!lisions. We will present ionization cross sections at electron collision energies between threshold and 10 KeV using the improved binary encounter dipole (iBED) formulation' Preliminary results of the possible dissociative ionization pathways will be presented. It is speculated that radical fragments produced from the dissociative ionization can further react, providing a possible mechanism for double strand breaks and base damage.

Cross sections for ionization of tetrahydrofuran by protons at energies between 300 and 3000 keV

NASA Astrophysics Data System (ADS)

Wang, Mingjie; Rudek, Benedikt; Bennett, Daniel; de Vera, Pablo; Bug, Marion; Buhr, Ticia; Baek, Woon Yong; Hilgers, Gerhard; Rabus, Hans

2016-05-01

Double-differential cross sections for ionization of tetrahydrofuran by protons with energies from 300 to 3000 keV were measured at the Physikalisch-Technische Bundesanstalt ion accelerator facility. The electrons emitted at angles between 15∘ and 150∘ relative to the ion-beam direction were detected with an electrostatic hemispherical electron spectrometer. Single-differential and total ionization cross sections have been derived by integration. The experimental results are compared to the semiempirical Hansen-Kocbach-Stolterfoht model as well as to the recently reported method based on the dielectric formalism. The comparison to the latter showed good agreement with experimental data in a broad range of emission angles and energies of secondary electrons. The scaling property of ionization cross sections for tetrahydrofuran was also investigated. Compared to molecules of different size, the ionization cross sections of tetrahydrofuran were found to scale with the number of valence electrons at large impact parameters.

A method of coupling the Paternò-Büchi reaction with direct infusion ESI-MS/MS for locating the C[double bond, length as m-dash]C bond in glycerophospholipids.

PubMed

Stinson, Craig A; Xia, Yu

2016-06-21

Tandem mass spectrometry (MS/MS) coupled with soft ionization is established as an essential platform for lipid analysis; however, determining high order structural information, such as the carbon-carbon double bond (C[double bond, length as m-dash]C) location, remains challenging. Recently, our group demonstrated a method for sensitive and confident lipid C[double bond, length as m-dash]C location determination by coupling online the Paternò-Büchi (PB) reaction with nanoelectrospray ionization (nanoESI) and MS/MS. Herein, we aimed to expand the scope of the PB reaction for lipid analysis by enabling the reaction with infusion ESI-MS/MS at much higher flow rates than demonstrated in the nanoESI setup (∼20 nL min(-1)). In the new design, the PB reaction was effected in a fused silica capillary solution transfer line, which also served as a microflow UV reactor, prior to ESI. This setup allowed PB reaction optimization and kinetics studies. Under optimized conditions, a maximum of 50% PB reaction yield could be achieved for a standard glycerophosphocholine (PC) within 6 s of UV exposure over a wide flow rate range (0.1-10 μL min(-1)). A solvent composition of 7 : 3 acetone : H2O (with 1% acid or base modifier) allowed the highest PB yields and good lipid ionization, while lower yields were obtained with an addition of a variety of organic solvents. Radical induced lipid peroxidation was identified to induce undesirable side reactions, which could be effectively suppressed by eliminating trace oxygen in the solution via N2 purge. Finally, the utility of coupling the PB reaction with infusion ESI-MS/MS was demonstrated by analyzing a yeast polar lipid extract where C[double bond, length as m-dash]C bond locations were revealed for 35 glycerophospholipids (GPs).

Tunable multiphoton Rabi oscillations in an electronic spin system

NASA Astrophysics Data System (ADS)

Bertaina, S.; Groll, N.; Chen, L.; Chiorescu, I.

2011-10-01

We report on multiphoton Rabi oscillations and controlled tuning of a multilevel system at room temperature (S=5/2 for Mn2+:MgO) in and out of a quasiharmonic level configuration. The anisotropy is much smaller than the Zeeman splittings, e.g., the six-level scheme shows only a small deviation from an equidistant diagram. This allows us to tune the spin dynamics by compensating for the cubic anisotropy with either a precise static-field orientation or a microwave field intensity. Using the rotating-frame approximation, the experiments are explained very well by both an analytical model and a generalized numerical model. The calculated multiphoton Rabi frequencies are in excellent agreement with the experimental data.

Moxifloxacin: Clinically compatible contrast agent for multiphoton imaging

NASA Astrophysics Data System (ADS)

Wang, Taejun; Jang, Won Hyuk; Lee, Seunghun; Yoon, Calvin J.; Lee, Jun Ho; Kim, Bumju; Hwang, Sekyu; Hong, Chun-Pyo; Yoon, Yeoreum; Lee, Gilgu; Le, Viet-Hoan; Bok, Seoyeon; Ahn, G.-One; Lee, Jaewook; Gho, Yong Song; Chung, Euiheon; Kim, Sungjee; Jang, Myoung Ho; Myung, Seung-Jae; Kim, Myoung Joon; So, Peter T. C.; Kim, Ki Hean

2016-06-01

Multiphoton microscopy (MPM) is a nonlinear fluorescence microscopic technique widely used for cellular imaging of thick tissues and live animals in biological studies. However, MPM application to human tissues is limited by weak endogenous fluorescence in tissue and cytotoxicity of exogenous probes. Herein, we describe the applications of moxifloxacin, an FDA-approved antibiotic, as a cell-labeling agent for MPM. Moxifloxacin has bright intrinsic multiphoton fluorescence, good tissue penetration and high intracellular concentration. MPM with moxifloxacin was demonstrated in various cell lines, and animal tissues of cornea, skin, small intestine and bladder. Clinical application is promising since imaging based on moxifloxacin labeling could be 10 times faster than imaging based on endogenous fluorescence.

Applications of multiphoton microscopy in the field of colorectal cancer

NASA Astrophysics Data System (ADS)

Wang, Shu; Li, Lianhuang; Zhu, Xiaoqin; Zheng, Liqin; Zhuo, Shuangmu; Chen, Jianxin

2018-06-01

Multiphoton microscopy (MPM) is a powerful tool for visualizing cellular and subcellular details within living tissue by its unique advantages of being label-free, its intrinsic optical sectioning ability, near-infrared excitation for deep penetration depth into tissue, reduced photobleaching and phototoxicity in the out-of-focus regions, and being capable of providing quantitative information. In this review, we focus on applications of MPM in the field of colorectal cancer, including monitoring cancer progression, detecting tumor metastasis and microenvironment, evaluating the cancer therapy response, and visualizing and ablating pre-invasive cancer cells. We also present one of the major challenges and the future research direction to exploit a colorectal multiphoton endoscope.

Electrofluidic gating of a chemically reactive surface.

PubMed

Jiang, Zhijun; Stein, Derek

2010-06-01

We consider the influence of an electric field applied normal to the electric double layer at a chemically reactive surface. Our goal is to elucidate how surface chemistry affects the potential for field-effect control over micro- and nanofluidic systems, which we call electrofluidic gating. The charging of a metal-oxide-electrolyte (MOE) capacitor is first modeled analytically. We apply the Poisson-Boltzmann description of the double layer and impose chemical equilibrium between the ionizable surface groups and the solution at the solid-liquid interface. The chemically reactive surface is predicted to behave as a buffer, regulating the charge in the double layer by either protonating or deprotonating in response to the applied field. We present the dependence of the charge density and the electrochemical potential of the double layer on the applied field, the density, and the dissociation constants of ionizable surface groups and the ionic strength and the pH of the electrolyte. We simulate the responses of SiO(2) and Al(2)O(3), two widely used oxide insulators with different surface chemistries. We also consider the limits to electrofluidic gating imposed by the nonlinear behavior of the double layer and the dielectric strength of oxide materials, which were measured for SiO(2) and Al(2)O(3) films in MOE configurations. Our results clarify the response of chemically reactive surfaces to applied fields, which is crucial to understanding electrofluidic effects in real devices.

Determination of phospholipid regiochemistry by Ag(I) adduction and tandem mass spectrometry.

PubMed

Yoo, Hyun Ju; Håkansson, Kristina

2011-02-15

Collision-activated dissociation (CAD) and infrared multiphoton dissociation (IRMPD) of Ag-adducted phospholipids were investigated as structural tools. Previously, determination of the acyl chains at the two phospholipid esterification sites has been performed based on the R(1)COO(-)/R(2)COO(-) ratio in negative ion mode CAD tandem mass spectrometry. However, the observed product ion ratio is dependent on the extent of unsaturation of the fatty acyl group at sn-2 as well as on the total chain length. Similarly, in positive ion mode CAD with/without alkaline or alkaline earth metal adduction, the ratio of product ions resulting from either R(1)COOH or R(2)COOH neutral losses is dependent on the nature of the phospholipid polar headgroup. Ag(+) ion chromatography, in which silver ions are part of the stationary phase, can provide information on double bond number/distribution as well as double bond configuration (cis/trans) because of interaction between Ag(+) ions and olefinic π electrons of fatty acids and lipids. We hypothesized that interactions between double bonds and Ag(+) may be utilized to also reveal phospholipid esterification site information in tandem mass spectrometry. CAD and IRMPD of Ag-adducted phospholipids with unsaturated fatty acids (R(x)COOH, x = 1 or 2) provided characteristic product ions, [R(x)COOH + Ag](+), and their neutral losses. The characteristic product ions and their abundances do not depend on the type of polar headgroup or the number of double bonds of unsaturated acyl chains. Tandem mass spectrometry of Cu-adducted phospholipids was also performed for comparison based on the Lewis acid and base properties of Cu(+) and phospholipid double bonds, respectively.

The Multiphoton Interaction of Lambda Model Atom and Two-Mode Fields

NASA Technical Reports Server (NTRS)

Liu, Tang-Kun

1996-01-01

The system of two-mode fields interacting with atom by means of multiphotons is addressed, and the non-classical statistic quality of two-mode fields with interaction is discussed. Through mathematical calculation, some new rules of non-classical effects of two-mode fields which evolue with time, are established.

USE OF MULTIPHOTON LASER SCANNING MICROSCOPY TO IMAGE BENZO[A]PYRENE AND METABOLITES IN FISH EARLY LIFE STAGES

EPA Science Inventory

Multiphoton laser scanning micrsocopy holds promise as a tool to study the tissue distribution of environmental chemical contaminants during fish early life stage development. One such chemical for which this is possible is benzo[a]pyrene (BaP), a polyaromatic hydrocarbon that a...

Multi-Photon Absorption Spectra: A Comparison Between Transmittance Change and Fluorescence Methods

DTIC Science & Technology

2015-05-21

AFRL-OSR-VA-TR-2015-0134 multi-photon absorption spectra Cleber Mendonca INSTITUTO DE FISICA DE SAO CARLOS Final Report 05/21/2015 DISTRIBUTION A...5f. WORK UNIT NUMBER 7. PERFORMING ORGANIZATION NAME(S) AND ADDRESS(ES) Instituto de Fisica de Sao Carlos - Universidade de Sao Paulo Av

Real-time digital signal processing in multiphoton and time-resolved microscopy

NASA Astrophysics Data System (ADS)

Wilson, Jesse W.; Warren, Warren S.; Fischer, Martin C.

2016-03-01

The use of multiphoton interactions in biological tissue for imaging contrast requires highly sensitive optical measurements. These often involve signal processing and filtering steps between the photodetector and the data acquisition device, such as photon counting and lock-in amplification. These steps can be implemented as real-time digital signal processing (DSP) elements on field-programmable gate array (FPGA) devices, an approach that affords much greater flexibility than commercial photon counting or lock-in devices. We will present progress toward developing two new FPGA-based DSP devices for multiphoton and time-resolved microscopy applications. The first is a high-speed multiharmonic lock-in amplifier for transient absorption microscopy, which is being developed for real-time analysis of the intensity-dependence of melanin, with applications in vivo and ex vivo (noninvasive histopathology of melanoma and pigmented lesions). The second device is a kHz lock-in amplifier running on a low cost (50-200) development platform. It is our hope that these FPGA-based DSP devices will enable new, high-speed, low-cost applications in multiphoton and time-resolved microscopy.

Direct comparison between confocal and multiphoton microscopy for rapid histopathological evaluation of unfixed human breast tissue.

PubMed

Yoshitake, Tadayuki; Giacomelli, Michael G; Cahill, Lucas C; Schmolze, Daniel B; Vardeh, Hilde; Faulkner-Jones, Beverly E; Connolly, James L; Fujimoto, James G

2016-12-01

Rapid histopathological examination of surgical specimen margins using fluorescence microscopy during breast conservation therapy has the potential to reduce the rate of positive margins on postoperative histopathology and the need for repeat surgeries. To assess the suitability of imaging modalities, we perform a direct comparison between confocal fluorescence microscopy and multiphoton microscopy for imaging unfixed tissue and compare to paraffin-embedded histology. An imaging protocol including dual channel detection of two contrast agents to implement virtual hematoxylin and eosin images is introduced that provides high quality imaging under both one and two photon excitation. Corresponding images of unfixed human breast tissue show that both confocal and multiphoton microscopy can reproduce the appearance of conventional histology without the need for physical sectioning. We further compare normal breast tissue and invasive cancer specimens imaged at multiple magnifications, and assess the effects of photobleaching for both modalities using the staining protocol. The results demonstrate that confocal fluorescence microscopy is a promising and cost-effective alternative to multiphoton microscopy for rapid histopathological evaluation of ex vivo breast tissue.

Direct comparison between confocal and multiphoton microscopy for rapid histopathological evaluation of unfixed human breast tissue

PubMed Central

Yoshitake, Tadayuki; Giacomelli, Michael G.; Cahill, Lucas C.; Schmolze, Daniel B.; Vardeh, Hilde; Faulkner-Jones, Beverly E.; Connolly, James L.; Fujimoto, James G.

2016-01-01

Abstract. Rapid histopathological examination of surgical specimen margins using fluorescence microscopy during breast conservation therapy has the potential to reduce the rate of positive margins on postoperative histopathology and the need for repeat surgeries. To assess the suitability of imaging modalities, we perform a direct comparison between confocal fluorescence microscopy and multiphoton microscopy for imaging unfixed tissue and compare to paraffin-embedded histology. An imaging protocol including dual channel detection of two contrast agents to implement virtual hematoxylin and eosin images is introduced that provides high quality imaging under both one and two photon excitation. Corresponding images of unfixed human breast tissue show that both confocal and multiphoton microscopy can reproduce the appearance of conventional histology without the need for physical sectioning. We further compare normal breast tissue and invasive cancer specimens imaged at multiple magnifications, and assess the effects of photobleaching for both modalities using the staining protocol. The results demonstrate that confocal fluorescence microscopy is a promising and cost-effective alternative to multiphoton microscopy for rapid histopathological evaluation of ex vivo breast tissue. PMID:28032121

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

PubMed

Seemann, K M; Kuhn, B

2014-07-01

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

Ultralow-threshold multiphoton-pumped lasing from colloidal nanoplatelets in solution

PubMed Central

Li, Mingjie; Zhi, Min; Zhu, Hai; Wu, Wen-Ya; Xu, Qing-Hua; Jhon, Mark Hyunpong; Chan, Yinthai

2015-01-01

Although multiphoton-pumped lasing from a solution of chromophores is important in the emerging fields of nonlinear optofluidics and bio-photonics, conventionally used organic dyes are often rendered unsuitable because of relatively small multiphoton absorption cross-sections and low photostability. Here, we demonstrate highly photostable, ultralow-threshold multiphoton-pumped biexcitonic lasing from a solution of colloidal CdSe/CdS nanoplatelets within a cuvette-based Fabry–Pérot optical resonator. We find that colloidal nanoplatelets surprisingly exhibit an optimal lateral size that minimizes lasing threshold. These nanoplatelets possess very large gain cross-sections of 7.3 × 10−14 cm2 and ultralow lasing thresholds of 1.2 and 4.3 mJ cm−2 under two-photon (λexc=800 nm) and three-photon (λexc=1.3 μm) excitation, respectively. The highly polarized emission from the nanoplatelet laser shows no significant photodegradation over 107 laser shots. These findings constitute a more comprehensive understanding of the utility of colloidal semiconductor nanoparticles as the gain medium in high-performance frequency-upconversion liquid lasers. PMID:26419950

Direct comparison between confocal and multiphoton microscopy for rapid histopathological evaluation of unfixed human breast tissue

NASA Astrophysics Data System (ADS)

Yoshitake, Tadayuki; Giacomelli, Michael G.; Cahill, Lucas C.; Schmolze, Daniel B.; Vardeh, Hilde; Faulkner-Jones, Beverly E.; Connolly, James L.; Fujimoto, James G.

2016-12-01

Rapid histopathological examination of surgical specimen margins using fluorescence microscopy during breast conservation therapy has the potential to reduce the rate of positive margins on postoperative histopathology and the need for repeat surgeries. To assess the suitability of imaging modalities, we perform a direct comparison between confocal fluorescence microscopy and multiphoton microscopy for imaging unfixed tissue and compare to paraffin-embedded histology. An imaging protocol including dual channel detection of two contrast agents to implement virtual hematoxylin and eosin images is introduced that provides high quality imaging under both one and two photon excitation. Corresponding images of unfixed human breast tissue show that both confocal and multiphoton microscopy can reproduce the appearance of conventional histology without the need for physical sectioning. We further compare normal breast tissue and invasive cancer specimens imaged at multiple magnifications, and assess the effects of photobleaching for both modalities using the staining protocol. The results demonstrate that confocal fluorescence microscopy is a promising and cost-effective alternative to multiphoton microscopy for rapid histopathological evaluation of ex vivo breast tissue.

Comparison of higher-order multiphoton signal generation and collection at the 1700-nm window based on transmittance measurement of objective lenses.

PubMed

Wen, Wenhui; Wang, Yuxin; Liu, Hongji; Wang, Kai; Qiu, Ping; Wang, Ke

2018-01-01

One benefit of excitation at the 1700-nm window is the more accessible modalities of multiphoton signal generation. It is demonstrated here that the transmittance performance of the objective lens is of vital importance for efficient higher-order multiphoton signal generation and collection excited at the 1700-nm window. Two commonly used objective lenses for multiphoton microscopy (MPM) are characterized and compared, one with regular coating and the other with customized coating for high transmittance at the 1700-nm window. Our results show that, fourth harmonic generation imaging of mouse tail tendon and 5-photon fluorescence of carbon quantum dots using the regular objective lens shows an order of magnitude signal higher than those using the customized objective lens. Besides, the regular objective lens also enables a 3-photon fluorescence imaging depth of >1600 μm in mouse brain in vivo. Our results will provide guidelines for objective lens selection for MPM at the 1700-nm window. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Amonia gas: an improved reagent for chemical ionization mass spectrometry of bile acid methyl ester acetates

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

DeMark, B.R.; Klein, P.D.

1981-01-01

The ammonia chemical ionization mass spectra of 28 methyl ester acetate derivatives of bile acids and related compounds have been determined by gas-liquid chromatography-mass spectrometry. Advantages of ammonia ionization over the previously studied isobutane ionization include a 130 to 270% enhancement in the sensitivity of base peak monitoring, and direct determination of molecular weight from the base peak (M + NH/sub 4//sup +/) in the mass spectrum of any of the derivatives. Minor ions in the ammonia spectra also allow selective detection of 3-keto compounds and can indicate unsaturation or double bond conjugation in the molecule. The significance of thesemore » studies for the detection and quantitation of bile acids is discussed. 2 tables.« less

Raman Microscopy: A Noninvasive Method to Visualize the Localizations of Biomolecules in the Cornea.

PubMed

Kaji, Yuichi; Akiyama, Toshihiro; Segawa, Hiroki; Oshika, Tetsuro; Kano, Hideaki

2017-11-01

In vivo and in situ visualization of biomolecules without pretreatment will be important for diagnosis and treatment of ocular disorders in the future. Recently, multiphoton microscopy, based on the nonlinear interactions between molecules and photons, has been applied to reveal the localizations of various molecules in tissues. We aimed to use multimodal multiphoton microscopy to visualize the localizations of specific biomolecules in rat corneas. Multiphoton images of the corneas were obtained from nonlinear signals of coherent anti-Stokes Raman scattering, third-order sum frequency generation, and second-harmonic generation. The localizations of the adhesion complex-containing basement membrane and Bowman layer were clearly visible in the third-order sum frequency generation images. The fine structure of type I collagen was observed in the corneal stroma in the second-harmonic generation images. The localizations of lipids, proteins, and nucleic acids (DNA/RNA) was obtained in the coherent anti-Stokes Raman scattering images. Imaging technologies have progressed significantly and been applied in medical fields. Optical coherence tomography and confocal microscopy are widely used but do not provide information on the molecular structure of the cornea. By contrast, multiphoton microscopy provides information on the molecular structure of living tissues. Using this technique, we successfully visualized the localizations of various biomolecules including lipids, proteins, and nucleic acids in the cornea. We speculate that multiphoton microscopy will provide essential information on the physiological and pathological conditions of the cornea, as well as molecular localizations in tissues without pretreatment.

Multi-photon transitions and Rabi resonance in continuous wave EPR.

PubMed

Saiko, Alexander P; Fedaruk, Ryhor; Markevich, Siarhei A

2015-10-01

The study of microwave-radiofrequency multi-photon transitions in continuous wave (CW) EPR spectroscopy is extended to a Rabi resonance condition, when the radio frequency of the magnetic-field modulation matches the Rabi frequency of a spin system in the microwave field. Using the non-secular perturbation theory based on the Bogoliubov averaging method, the analytical description of the response of the spin system is derived for all modulation frequency harmonics. When the modulation frequency exceeds the EPR linewidth, multi-photon transitions result in sidebands in absorption EPR spectra measured with phase-sensitive detection at any harmonic. The saturation of different-order multi-photon transitions is shown to be significantly different and to be sensitive to the Rabi resonance. The noticeable frequency shifts of sidebands are found to be the signatures of this resonance. The inversion of two-photon lines in some spectral intervals of the out-of-phase first-harmonic signal is predicted under passage through the Rabi resonance. The inversion indicates the transition from absorption to stimulated emission or vice versa, depending on the sideband. The manifestation of the primary and secondary Rabi resonance is also demonstrated in the time evolution of steady-state EPR signals formed by all harmonics of the modulation frequency. Our results provide a theoretical framework for future developments in multi-photon CW EPR spectroscopy, which can be useful for samples with long spin relaxation times and extremely narrow EPR lines. Copyright © 2015 Elsevier Inc. All rights reserved.

Multiphoton fluorescence lifetime imaging of chemotherapy distribution in solid tumors

NASA Astrophysics Data System (ADS)

Carlson, Marjorie; Watson, Adrienne L.; Anderson, Leah; Largaespada, David A.; Provenzano, Paolo P.

2017-11-01

Doxorubicin is a commonly used chemotherapeutic employed to treat multiple human cancers, including numerous sarcomas and carcinomas. Furthermore, doxorubicin possesses strong fluorescent properties that make it an ideal reagent for modeling drug delivery by examining its distribution in cells and tissues. However, while doxorubicin fluorescence and lifetime have been imaged in live tissue, its behavior in archival samples that frequently result from drug and treatment studies in human and animal patients, and murine models of human cancer, has to date been largely unexplored. Here, we demonstrate imaging of doxorubicin intensity and lifetimes in archival formalin-fixed paraffin-embedded sections from mouse models of human cancer with multiphoton excitation and multiphoton fluorescence lifetime imaging microscopy (FLIM). Multiphoton excitation imaging reveals robust doxorubicin emission in tissue sections and captures spatial heterogeneity in cells and tissues. However, quantifying the amount of doxorubicin signal in distinct cell compartments, particularly the nucleus, often remains challenging due to strong signals in multiple compartments. The addition of FLIM analysis to display the spatial distribution of excited state lifetimes clearly distinguishes between signals in distinct compartments such as the cell nuclei versus cytoplasm and allows for quantification of doxorubicin signal in each compartment. Furthermore, we observed a shift in lifetime values in the nuclei of transformed cells versus nontransformed cells, suggesting a possible diagnostic role for doxorubicin lifetime imaging to distinguish normal versus transformed cells. Thus, data here demonstrate that multiphoton FLIM is a highly sensitive platform for imaging doxorubicin distribution in normal and diseased archival tissues.

Intravital multiphoton fluorescence imaging and optical manipulation of spinal cord in mice, using a compact fiber laser system.

PubMed

Oshima, Yusuke; Horiuch, Hideki; Honkura, Naoki; Hikita, Atsuhiko; Ogata, Tadanori; Miura, Hiromasa; Imamura, Takeshi

2014-09-01

Near-infrared ultrafast lasers are widely used for multiphoton excited fluorescence microscopy in living animals. Ti:Sapphire lasers are typically used for multiphoton excitation, but their emission wavelength is restricted below 1,000 nm. The aim of this study is to evaluate the performance of a compact Ytterbium-(Yb-) fiber laser at 1,045 nm for multiphoton excited fluorescence microscopy in spinal cord injury. In this study, we employed a custom-designed microscopy system with a compact Yb-fiber laser and evaluated the performance of this system in in vivo imaging of brain cortex and spinal cord in YFP-H transgenic mice. For in vivo imaging of brain cortex, sharp images of basal dendrites, and pyramidal cells expressing EYFP were successfully captured using the Yb-fiber laser in our microscopy system. We also performed in vivo imaging of axon fibers of spinal cord in the transgenic mice. The obtained images were almost as sharp as those obtained using a conventional ultrafast laser system. In addition, laser ablation and multi-color imaging could be performed simultaneously using the Yb-fiber laser. The high-peak pulse Yb-fiber laser is potentially useful for multimodal bioimaging methods based on a multiphoton excited fluorescence microscopy system that incorporates laser ablation techniques. Our results suggest that microscopy systems of this type could be utilized in studies of neuroscience and clinical use in diagnostics and therapeutic tool for spinal cord injury in the future. © 2014 Wiley Periodicals, Inc.

Improvement of depth resolution on photoacoustic imaging using multiphoton absorption

NASA Astrophysics Data System (ADS)

Yamaoka, Yoshihisa; Fujiwara, Katsuji; Takamatsu, Tetsuro

2007-07-01

Commercial imaging systems, such as computed tomography and magnetic resonance imaging, are frequently used powerful tools for observing structures deep within the human body. However, they cannot precisely visualized several-tens micrometer-sized structures for lack of spatial resolution. In this presentation, we propose photoacoustic imaging using multiphoton absorption technique to generate ultrasonic waves as a means of improving depth resolution. Since the multiphoton absorption occurs at only the focus point and the employed infrared pulses deeply penetrate living tissues, it enables us to extract characteristic features of structures embedded in the living tissue. When nanosecond pulses from a 1064-nm Nd:YAG laser were focused on Rhodamine B/chloroform solution (absorption peak: 540 nm), the peak intensity of the generated photoacoustic signal was proportional to the square of the input pulse energy. This result shows that the photoacoustic signals can be induced by the two-photon absorption of infrared nanosecond pulse laser and also can be detected by a commercial low-frequency MHz transducer. Furthermore, in order to evaluate the depth resolution of multiphoton-photoacoustic imaging, we investigated the dependence of photoacoustic signal on depth position using a 1-mm-thick phantom in a water bath. We found that the depth resolution of two-photon photoacoustic imaging (1064 nm) is greater than that of one-photon photoacoustic imaging (532 nm). We conclude that evolving multiphoton-photoacoustic imaging technology renders feasible the investigation of biomedical phenomena at the deep layer in living tissue.

Clinical multiphoton FLIM tomography

NASA Astrophysics Data System (ADS)

König, Karsten

2012-03-01

This paper gives an overview on current clinical high resolution multiphoton fluorescence lifetime imaging in volunteers and patients. Fluorescence lifetime imaging (FLIM) in Life Sciences was introduced in Jena/Germany in 1988/89 based on a ZEISS confocal picosecond dye laser scanning microscope equipped with a single photon counting unit. The porphyrin distribution in living cells and living tumor-bearing mice was studied with high spatial, temporal, and spectral resolution. Ten years later, time-gated cameras were employed to detect dental caries in volunteers based on one-photon excitation of autofluorescent bacteria with long fluorescence lifetimes. Nowadays, one-photon FLIM based on picosecond VIS laser diodes are used to study ocular diseases in humans. Already one decade ago, first clinical twophoton FLIM images in humans were taken with the certified clinical multiphoton femtosecond laser tomograph DermaInspectTM. Multiphoton tomographs with FLIM modules are now operating in hospitals at Brisbane, Tokyo, Berlin, Paris, London, Modena and other European cities. Multiple FLIM detectors allow spectral FLIM with a temporal resolution down to 20 ps (MCP) / 250 ps (PMT) and a spectral resolution of 10 nm. Major FLIM applications include the detection of intradermal sunscreen and tattoo nanoparticles, the detection of different melanin types, the early diagnosis of dermatitis and malignant melanoma, as well as the measurement of therapeutic effects in pateints suffering from dermatitis. So far, more than 1,000 patients and volunteers have been investigated with the clinical multiphoton FLIM tomographs DermaInspectTM and MPTflexTM.

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

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

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

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{sup -1} (390more » nm) and 48 500 cm{sup -1} (206 nm). We did not observe a (1+1) REMPI signal through the optically bright {sup 1}B{sub 2} ({pi}{pi}*) and {sup 1}A{sub 1} ({pi}{pi}*) states in pyrrole due to ultrafast deactivation via conical intersections with the dissociative {sup 1}A{sub 2} ({pi}{sigma}*) and {sup 1}B{sub 1} ({pi}{sigma}{sup *}) states. However, we did observe (2+1) REMPI through Rydberg states with a dominant feature at 27 432 cm{sup -1} (two-photon energy, 54 864 cm{sup -1}) assigned to a 3d(leftarrow){pi} transition. In contrast, 2,5-dimethylpyrrole has a broad and structured (1+1) REMPI spectrum between 36 000 and 42 500 cm{sup -1} as a result of vibronic transitions to the {sup 1}B{sub 2} ({pi}{pi}*) state, and it does not show the 3d(leftarrow){pi} 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 {sup 1}{pi}{sigma}* states (dissociative) and optically bright {sup 1}{pi}{pi}* states well, predicting the barrierless deactivation of the {sup 1}B{sub 2} ({pi}{pi}*) state of pyrrole and the bound minimum of the {sup 1}B{sub 2} ({pi}{pi}*) state in 2,5-dimethylpyrrole. However, the quantitative agreement between vibronic transition energies and the excited-state frequencies calculated by TD-DFT was hampered by inaccurate modeling of Rydberg orbital mixing with the valence states, caused by the lack of an asymptotic correction to the exchange-correlation functionals used.« less

The Lamont--Doherty Geological Observatory Isolab 54 isotope ratio mass spectrometer

NASA Astrophysics Data System (ADS)

England, J. G.; Zindler, A.; Reisberg, L. C.; Rubenstone, J. L.; Salters, V.; Marcantonio, F.; Bourdon, B.; Brueckner, H.; Turner, P. J.; Weaver, S.; Read, P.

1992-12-01

The Lamont--Doherty Geological Observatory (LDGO) Isolab 54 is a double focussing isotope ratio mass spectrometer that allows the measurement of thermal ions produced on a hot filament, (thermal-ionization mass spectrometry (TIMS)), secondary ions produced by sputtering a sample using a primary ion beam, (secondary ion mass spectrometry (SIMS)), and sputtered neutrals resonantly ionized using laser radiation, (sputter-induced resonance ionization mass spectrometry (SIRIMS)). Sputtering is carried out using an Ar primary beam generated in a duoplasmatron and focussed onto the sample using a two-lens column. Resonance ionization is accomplished using a frequency-doubled dye laser pumped by an excimer laser. The Isolab's forward geometry analyzer, consisting of an electrostatic followed by a magnetic sector, allows the simultaneous collection of different isotopes of the same element. This instrument is the first to have a multicollector that contains an ion-counting system based on a microchannel plate as well as traditional Faraday cups. A second electrostatic sector after the multicollector is equipped with an ion-counting Daly detector to allow high abundance sensitivity for measurements of large dynamics range. Selectable source, collector, [alpha] and energy slits on the instrument allow analyses to be made over a range of mass resolving powers and analyzer acceptances. Recent applications of the instrument have included the analyses of U by TIMS, Hf, Th and Re by SIMS and Re and Os by SIRIMS.

Technical note: A new wedge-shaped ionization chamber component module for BEAMnrc to model the integral quality monitoring system®

NASA Astrophysics Data System (ADS)

Oderinde, Oluwaseyi Michael; du Plessis, FCP

2017-12-01

The purpose of this study was to develop a new component module (CM) namely IQM to accurately model the integral quality monitoring (IQM) system® to be used in the BEAMnrc Monte Carlo (MC) code. The IQM is essentially a double wedge ionization chamber with the central electrode plate bisecting the wedge. The IQM CM allows the user to characterize the double wedge of this ionization chamber and BEAMnrc can then accurately calculate the dose in this CM including its enclosed air regions. This has been verified against measured data. The newly created CM was added into the standard BEAMnrc CMs, and it will be made available through the NRCC website. The BEAMnrc graphical user interface (GUI) and particle ray-tracing techniques were used to validate the IQM geometry. In subsequent MC simulations, the dose scored in the IQM was verified against measured data over a range of square fields ranging from 1 × 1-30 × 30 cm2. The IQM system is designed for the present day need for a device that could verify beam output in real-time during treatment. This CM is authentic, and it can serve as a basis for researchers that have an interest in real-time beam delivery checking using wedge-shaped ionization chamber based instruments like the IQM.

VUV and soft x-ray ionization of a plant volatile: Vanillin (C{sub 8}H{sub 8}O{sub 3})

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

Betancourt, A. Moreno; Moura, C. E. V. de; Rocha, A. B.

2016-03-21

Plant volatiles are emitted by plants in response to several forms of stress, including interaction with energetic photons. In the present work, we discuss the interaction of extreme UV and soft X-ray photons with a plant volatile, vanillin. The single and double (multiple) ionization of the vanillin molecule have been studied for the first time using time-of-flight mass spectrometry and VUV and soft X-ray photons (synchrotron radiation, at 12.0 eV, 21.2 eV, 130 eV, 310 eV, 531 eV, and 550 eV). At 12.0 and 21.2 eV, only singly charged species are observed and the parent ion, C{sub 8}H{sub 8}O{sub 3}{supmore » +}, is the dominant species. Energy differences for some selected fragments were calculated theoretically in this energy region. At 130 eV, direct double and triple ionization of the valence electrons may occur. The fragmentation increases and CHO{sup +} becomes one of the main cations in the mass spectrum. The molecular ion is still the dominant species, but other fragments, such as C{sub 6}H{sub 5}O{sup +}, begin to present similar intensities. At 310 eV, C 1s electrons may be ionized and Auger processes give rise to dissociative doubly ionized cations. Ionization around the O 1s edge has been studied both at the 531 eV resonance and above the ionization edge. Resonant and normal Auger processes play a significant role in each case and a large fragmentation of the molecule is observed at both photon energies, with intense fragments such as CHO{sup +} and CH{sub 3}{sup +} being clearly observed. A near edge X-ray absorption fine structure spectrum of the vanillin molecule was obtained around the O 1s ionization threshold. In addition, the fragmentation of vanillin has also been studied using a fast beam of electrons (800 eV), for the sake of comparison.« less

Recruitment of TRF2 to laser-induced DNA damage sites.

PubMed

Huda, Nazmul; Abe, Satoshi; Gu, Ling; Mendonca, Marc S; Mohanty, Samarendra; Gilley, David

2012-09-01

Several lines of evidence suggest that the telomere-associated protein TRF2 plays critical roles in the DNA damage response. TRF2 is rapidly and transiently phosphorylated by an ATM-dependent pathway in response to DNA damage and this DNA damage-induced phosphoryation is essential for the DNA-PK-dependent pathway of DNA double-strand break repair (DSB). However, the type of DNA damage that induces TRF2 localization to the damage sites, the requirement for DNA damage-induced phosphorylation of TRF2 for its recruitment, as well as the detailed kinetics of TRF2 accumulation at DNA damage sites have not been fully investigated. In order to address these questions, we used an ultrafast femtosecond multiphoton laser and a continuous wave 405-nm single photon laser to induce DNA damage at defined nuclear locations. Our results showed that DNA damage produced by a femtosecond multiphoton laser was sufficient for localization of TRF2 to these DNA damage sites. We also demonstrate that ectopically expressed TRF2 was recruited to DNA lesions created by a 405-nm laser. Our data suggest that ATM and DNA-PKcs kinases are not required for TRF2 localization to DNA damage sites. Furthermore, we found that phosphorylation of TRF2 at residue T188 was not essential for its recruitment to laser-induced DNA damage sites. Thus, we provide further evidence that a protein known to function in telomere maintenance, TRF2, is recruited to sites of DNA damage and plays critical roles in the DNA damage response. Copyright © 2012 Elsevier Inc. All rights reserved.

Human cytomegalovirus inhibits a DNA damage response by mislocalizing checkpoint proteins

NASA Astrophysics Data System (ADS)

Gaspar, Miguel; Shenk, Thomas

2006-02-01

The DNA damage checkpoint pathway responds to DNA damage and induces a cell cycle arrest to allow time for DNA repair. Several viruses are known to activate or modulate this cellular response. Here we show that the ataxia-telangiectasia mutated checkpoint pathway, which responds to double-strand breaks in DNA, is activated in response to human cytomegalovirus DNA replication. However, this activation does not propagate through the pathway; it is blocked at the level of the effector kinase, checkpoint kinase 2 (Chk2). Late after infection, several checkpoint proteins, including ataxia-telangiectasia mutated and Chk2, are mislocalized to a cytoplasmic virus assembly zone, where they are colocalized with virion structural proteins. This colocalization was confirmed by immunoprecipitation of virion proteins with an antibody that recognizes Chk2. Virus replication was resistant to ionizing radiation, which causes double-strand breaks in DNA. We propose that human CMV DNA replication activates the checkpoint response to DNA double-strand breaks, and the virus responds by altering the localization of checkpoint proteins to the cytoplasm and thereby inhibiting the signaling pathway. ionizing radiation | ataxia-telangiectasia mutated pathway

Intertwined electron-nuclear motion in frustrated double ionization in driven heteronuclear molecules

NASA Astrophysics Data System (ADS)

Vilà, A.; Zhu, J.; Scrinzi, A.; Emmanouilidou, A.

2018-03-01

We study frustrated double ionization (FDI) in a strongly-driven heteronuclear molecule HeH+ and compare with H2. We compute the probability distribution of the sum of the final kinetic energies of the nuclei for strongly-driven HeH+. We find that this distribution has more than one peak for strongly-driven HeH+, a feature we do not find to be present for strongly-driven H2. Moreover, we compute the probability distribution of the principal quantum number n of FDI. We find that this distribution has several peaks for strongly-driven HeH+, while the respective distribution has one main peak and a ‘shoulder’ at lower principal quantum numbers n for strongly-driven H2. Surprisingly, we find this feature to be a clear signature of the intertwined electron-nuclear motion.

Lanthanide heterometallic terephthalates: Concentration quenching and the principles of the "multiphotonic emission"

NASA Astrophysics Data System (ADS)

Utochnikova, V. V.; Grishko, A. Yu.; Koshelev, D. S.; Averin, A. A.; Lepnev, L. S.; Kuzmina, N. P.

2017-12-01

The principles of the "multiphotonic emission", i.e. multiple emission from one lanthanide ion, in heterometallic lanthanide terephthalates were determined. Thanks to it, another system with the same effect, namely EuxY1-x(dbm)3(Phen) (Hdbm - dibenzoylmethanate, Phen - o-phenanthroline (mistape)) was found. The criteria for concentration quenching appearance were formulated and demonstrated.

Hong-Ou-Mandel Interference with a Single Atom.

PubMed

Ralley, K A; Lerner, I V; Yurkevich, I V

2015-09-14

The Hong-Ou-Mandel (HOM) effect is widely regarded as the quintessential quantum interference phenomenon in optics. In this work we examine how nonlinearity can smear statistical photon bunching in the HOM interferometer. We model both the nonlinearity and a balanced beam splitter with a single two-level system and calculate a finite probability of anti-bunching arising in this geometry. We thus argue that the presence of such nonlinearity would reduce the visibility in the standard HOM setup, offering some explanation for the diminution of the HOM visibility observed in many experiments. We use the same model to show that the nonlinearity affects a resonant two-photon propagation through a two-level impurity in a waveguide due to a "weak photon blockade" caused by the impossibility of double-occupancy and argue that this effect might be stronger for multi-photon propagation.

Nanostructure and surface activation of mayenite (12CaO·7Al2O3) ceramics via femtosecond laser irradiation in solvents

NASA Astrophysics Data System (ADS)

Visbal, Heidy; Hirano, Minami; Omura, Takuya; Shimizu, Masahiro; Takaishi, Taigo; Hirao, Kazuyuki

2017-07-01

Mayenite (12CaO·7Al2O3) is a highly interesting functional material due to the wide variety of its possible future applications. In this study, we used femtosecond laser irradiation in several solvents with varying polarities to increase the specific surface area of 12CaO·7Al2O3 ceramics and reduce their particle size without any structural degradation or loss of crystallinity. We observed that when femtosecond laser irradiation was applied to solvents bearing hydroxyl groups, a smaller particle size was obtained with the particle size decreasing as the polarity of the solvent increased. Using infrared spectroscopy, we confirmed the presence of hydroxyl and carbonyl surface functional groups at the surface of 12CaO·7Al2O3 ceramics after femtosecond laser irradiation. This is attributed to the direct chemical bonds breaking of the solvent via multiphoton ionization and/or tunneling ionization, followed by the Coulomb explosion and the subsequent production of ions that are adsorbed on the surfaces of 12CaO·7Al2O3 ceramics. Femtosecond laser irradiation in polar solvents with hydroxyl groups can reduce the particle size and increase the specific surface area without degradation or loss of crystallinity of 12CaO·7Al2O3 ceramics. Additionally, this method can be used for the surface modification and introduction of functional groups on the 12CaO·7Al2O3 ceramics surface.

Ionization of elements in medium power capacitively coupled argon plasma torch with single and double ring electrodes.

PubMed

Ponta, Michaela; Frentiu, Maria; Frentiu, Tiberiu

2012-06-01

A medium power, low Ar consumption capacitively coupled plasma torch (275 W, 0.4 L min-1) with molybdenum tubular electrode and single or two ring electrodes in non-local thermodynamic equilibrium (LTE) was characterized with respect to its ability to achieve element ionization. Ionization degrees of Ca, Mg, Mn and Cd were determined from ionic-to-atomic emission ratio and ionization equilibrium according to Saha's equation. The ionization degrees resulted from the Saha equation were higher by 9-32% than those obtained from spectral lines intensity in LTE regime and closer to reality. A linear decrease of ionization with increase of ionization energy of elements was observed. Plasma torch with two ring electrodes provided higher ionization degrees (85 ± 7% Ca, 79 ± 7% Mn, 80 ± 7% Mg and 73 ± 8% Cd) than those in single ring arrangement (70 ± 6% Ca, 57 ± 7% Mn, 57 ± 8% Mg and 42 ± 9% Cd). The Ca ionization decreased linearly by up to 79 ± 4% and 53 ± 6% in plasma with two ring electrodes and single ring respectively in the presence of up to 400 µg mL-1 Na as interferent. The studied plasma was effective in element ionization and could be a potential ion source in mass spectrometry.

Shock-wave structure in a partially ionized gas

NASA Technical Reports Server (NTRS)

Lu, C. S.; Huang, A. B.

1974-01-01

The structure of a steady plane shock in a partially ionized gas has been investigated using the Boltzmann equation with a kinetic model as the governing equation and the discrete ordinate method as a tool. The effects of the electric field induced by the charge separation on the shock structure have also been studied. Although the three species of an ionized gas travel with approximately the same macroscopic velocity, the individual distribution functions are found to be very different. In a strong shock the atom distribution function may have double peaks, while the ion distribution function has only one peak. Electrons are heated up much earlier than ions and atoms in a partially ionized gas. Because the interactions of electrons with atoms and with ions are different, the ion temperature can be different from the atom temperature.

Wave-packet continuum-discretization approach to ion-atom collisions including rearrangement: Application to differential ionization in proton-hydrogen scattering

NASA Astrophysics Data System (ADS)

Abdurakhmanov, I. B.; Bailey, J. J.; Kadyrov, A. S.; Bray, I.

2018-03-01

In this work, we develop a wave-packet continuum-discretization approach to ion-atom collisions that includes rearrangement processes. The total scattering wave function is expanded using a two-center basis built from wave-packet pseudostates. The exact three-body Schrödinger equation is converted into coupled-channel differential equations for time-dependent expansion coefficients. In the asymptotic region these time-dependent coefficients represent transition amplitudes for all processes including elastic scattering, excitation, ionization, and electron capture. The wave-packet continuum-discretization approach is ideal for differential ionization studies as it allows one to generate pseudostates with arbitrary energies and distribution. The approach is used to calculate the double differential cross section for ionization in proton collisions with atomic hydrogen. Overall good agreement with experiment is obtained for all considered cases.

Enabling high-precision nonlinear three-dimensional photoprocessing of premeditated designs on a conventional multiphoton imaging system

NASA Astrophysics Data System (ADS)

Garsha, Karl E.

2004-06-01

There is an increasing amount of interest in functionalized microstructural, microphotonic and microelectromechanical systems (MEMS) for use in biological applications. By scanning a tightly focused ultra-short pulsed laser beam inside a wide variety of commercially available polymer systems, the flexibility of the multiphoton microscope can be extended to include routine manufacturing of micro-devices with feature sizes well below the diffraction limit. Compared with lithography, two-photon polymerization has the unique ability to additively realize designs with high resolution in three dimensions; this permits the construction of cross-linked components and structures with hollow cavities. In light of the increasing availability of multiphoton imaging systems at research facilities, femtosecond laser manufacturing becomes particularly attractive in that the modality provides a readily accessible, rapid and high-accuracy 3-D processing capability to biological investigators interested in culture scaffolds and biomimetic tissue engineering, bio-MEMS, biomicrophotonics and microfluidics applications. This manuscript overviews recent efforts towards to enabling user accessible 3-D micro-manufacturing capabilities on a conventional proprietary-based imaging system. Software which permits the off-line design of microstructures and leverages the extensibility of proprietary LCSM image acquisition software to realize designs is introduced. The requirements for multiphoton photo-disruption (ablation) are in some ways analogous to those for multiphoton polymerization. Hence, "beam-steering" also facilitates precision photo-disruption of biological tissues with 3-D resolution, and applications involving tissue microdissection and intracellular microsurgery or three-dimensionally resolved fluorescence recovery after photobleaching (FRAP) studies can benefit from this work as well.

IR and visible luminescence studies in the infrared multiphoton dissociation of 1,2-dibromo-1,1-difluoroethane

NASA Astrophysics Data System (ADS)

Pushpa, K. K.; Kumar, Awadhesh; Vatsa, R. K.; Naik, P. D.; Annaji Rao, K.; Mittal, J. P.; Parthasarathy, V.; Sarkar, S. K.

1995-07-01

The infrared multiphoton dissociation of 1,2-dibromo-1,1-difluoroethane gives rise to IR and visible luminescence. Vibrationally excited parent molecules dissociate via two primary channels yielding bromine and vibrationally excited HBr. The strong visible emission observed between 350 to 750 nm has been assigned to electronically excited carbene CF 2Br CH.

Mitochondrial Permeability Transition in Pathogenesis of Hemorrhagic Injury: Targeted Therapy with Minocycline

DTIC Science & Technology

2012-03-01

minocy- cline treatment (Figures 1-4). Minocycline also improved mitochondrial function as assessed by intravital multiphoton imaging of the...will make direct measurements by intravital multiphoton microscopy to determine whether onset of the mitochondrial permeability transition and...oxidative stress were assessed 6 h after resuscitation. Mitochondrial polarization were assessed by intravital microscopy. After H/R with vehicle or

Visualizing Viral Infection In Vivo by Multi-Photon Intravital Microscopy.

PubMed

Sewald, Xaver

2018-06-20

Viral pathogens have adapted to the host organism to exploit the cellular machinery for virus replication and to modulate the host cells for efficient systemic dissemination and immune evasion. Much of our knowledge of the effects that virus infections have on cells originates from in vitro imaging studies using experimental culture systems consisting of cell lines and primary cells. Recently, intravital microscopy using multi-photon excitation of fluorophores has been applied to observe virus dissemination and pathogenesis in real-time under physiological conditions in living organisms. Critical steps during viral infection and pathogenesis could be studied by direct visualization of fluorescent virus particles, virus-infected cells, and the immune response to viral infection. In this review, I summarize the latest research on in vivo studies of viral infections using multi-photon intravital microscopy (MP-IVM). Initially, the underlying principle of multi-photon microscopy is introduced and experimental challenges during microsurgical animal preparation and fluorescent labeling strategies for intravital imaging are discussed. I will further highlight recent studies that combine MP-IVM with optogenetic tools and transcriptional analysis as a powerful approach to extend the significance of in vivo imaging studies of viral pathogens.

Multiphoton fluorescence imaging of NADH to quantify metabolic changes in epileptic tissue in vitro

NASA Astrophysics Data System (ADS)

Chia, Thomas H.; Zinter, Joseph; Spencer, Dennis D.; Williamson, Anne; Levene, Michael J.

2007-02-01

A powerful advantage of multiphoton microscopy is its ability to image endogenous fluorophores such as the ubiquitous coenzyme NADH in discrete cellular populations. NADH is integral in both oxidative and non-oxidative cellular metabolism. NADH loses fluorescence upon oxidation to NAD +; thus changes in NADH fluorescence can be used to monitor metabolism. Recent studies have suggested that hypo metabolic astrocytes play an important role in cases of temporal lobe epilepsy (TLE). Current theories suggest this may be due to defective and/or a reduced number of mitochondria or dysfunction of the neuronal-astrocytic metabolic coupling. Measuring NADH fluorescence changes following chemical stimulation enables the quantification of the cellular distribution of metabolic anomalies in epileptic brain tissue compared to healthy tissue. We present what we believe to be the first multiphoton microscopy images of NADH from the human brain. We also present images of NADH fluorescence from the hippocampus of the kainate-treated rat TLE model. In some experiments, human and rat astrocytes were selectively labeled with the fluorescent dye sulforhodamine 101 (SR101). Our results demonstrate that multiphoton microscopy is a powerful tool for assaying the metabolic pathologies associated with temporal lobe epilepsy in humans and in rodent models.

Equation-of-motion coupled-cluster method for doubly ionized states with spin-orbit coupling.

PubMed

Wang, Zhifan; Hu, Shu; Wang, Fan; Guo, Jingwei

2015-04-14

In this work, we report implementation of the equation-of-motion coupled-cluster method for doubly ionized states (EOM-DIP-CC) with spin-orbit coupling (SOC) using a closed-shell reference. Double ionization potentials (DIPs) are calculated in the space spanned by 2h and 3h1p determinants with the EOM-DIP-CC approach at the CC singles and doubles level (CCSD). Time-reversal symmetry together with spatial symmetry is exploited to reduce computational effort. To circumvent the problem of unstable dianion references when diffuse basis functions are included, nuclear charges are scaled. Effect of this stabilization potential on DIPs is estimated based on results from calculations using a small basis set without diffuse basis functions. DIPs and excitation energies of some low-lying states for a series of open-shell atoms and molecules containing heavy elements with two unpaired electrons have been calculated with the EOM-DIP-CCSD approach. Results show that this approach is able to afford a reliable description on SOC splitting. Furthermore, the EOM-DIP-CCSD approach is shown to provide reasonable excitation energies for systems with a dianion reference when diffuse basis functions are not employed.

Equation-of-motion coupled-cluster method for doubly ionized states with spin-orbit coupling

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

Wang, Zhifan; Hu, Shu; Guo, Jingwei

2015-04-14

In this work, we report implementation of the equation-of-motion coupled-cluster method for doubly ionized states (EOM-DIP-CC) with spin-orbit coupling (SOC) using a closed-shell reference. Double ionization potentials (DIPs) are calculated in the space spanned by 2h and 3h1p determinants with the EOM-DIP-CC approach at the CC singles and doubles level (CCSD). Time-reversal symmetry together with spatial symmetry is exploited to reduce computational effort. To circumvent the problem of unstable dianion references when diffuse basis functions are included, nuclear charges are scaled. Effect of this stabilization potential on DIPs is estimated based on results from calculations using a small basis setmore » without diffuse basis functions. DIPs and excitation energies of some low-lying states for a series of open-shell atoms and molecules containing heavy elements with two unpaired electrons have been calculated with the EOM-DIP-CCSD approach. Results show that this approach is able to afford a reliable description on SOC splitting. Furthermore, the EOM-DIP-CCSD approach is shown to provide reasonable excitation energies for systems with a dianion reference when diffuse basis functions are not employed.« less

Classical trajectory studies on the dynamics of one-photon double photionization of H2O

NASA Astrophysics Data System (ADS)

Streeter, Zachary; Yip, Frank; Reedy, Dylan P.; Landers, Allen; McCurdy, C. William

2017-04-01

Recent momentum imaging experiments at the Advanced Light Source have opened the possibility of measuring the complete triple differential cross section (TDCS) for one-photon double ionization of H2O in the molecular frame. The measurements depend on the complete breakup process, H2O + hν -> 2e-+ H+ + H+ +O. At the 57 eV photon energy of the experiment this process could proceed via any of the nine energetically accessible electronic states of H2O++. To discover which ionization channels contribute to the observed TDCS for the electrons measured in coincidence with different kinetic energy releases, we have carried out classical trajectory studies for breakup of the water dication on all nine potential surfaces, sampling from a Wigner phase space distribution for the vibrational ground state of H2O. The final momentum distributions of the protons and branching ratios between two- and three-body breakup are then analyzed and the results are compared with experiment to identify which ionization channels contribute to the TDCS observed in coincidence measurements of the ejected electrons. Office of Basic Energy Sciences, U.S. DOE.

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

Müller, Alfred; Bernhardt, Dietrich; Borovik, Alexander

Single, double, and triple photoionization of Ne + ions by single photons have been investigated at the synchrotron radiation source PETRA III in Hamburg, Germany. Absolute cross-sections were measured by employing the photon-ion merged-beams technique. Photon energies were between about 840 and 930 eV, covering the range from the lowest-energy resonances associated with the excitation of one single K-shell electron up to double excitations involving one K- and one L-shell electron, well beyond the K-shell ionization threshold. Also, photoionization of neutral Ne was investigated just below the K edge. The chosen photon energy bandwidths were between 32 and 500 meV,more » facilitating the determination of natural line widths. The uncertainty of the energy scale is estimated to be 0.2 eV. For comparison with existing theoretical calculations, astrophysically relevant photoabsorption cross-sections were inferred by summing the measured partial ionization channels. Discussion of the observed resonances in the different final ionization channels reveals the presence of complex Auger-decay mechanisms. The ejection of three electrons from the lowest K-shell-excited Ne + (1s2s 2p 6 2S 1/2) level, for example, requires cooperative interaction of at least four electrons.« less

Use of near infrared femtosecond lasers as sub-micron radiation microbeam for cell DNA damage and repair studies.

PubMed

Botchway, S W; Reynolds, P; Parker, A W; O'Neill, P

2010-01-01

Laser induced radiation microbeam technology for radiobiology research is undergoing rapid growth because of the increased availability and ease of use of femtosecond laser sources. The main processes involved are multiphoton absorption and/or plasma formation. The high peak powers these lasers generate make them ideal tools for depositing sub-micrometer size radiant energy within a region of a living cell nucleus to activate ionising and/or photochemically driven processes. The technique allows questions relating to the effects of low doses of radiation, the propagation and treatment of deoxyribonucleic acid (DNA) damage and repair in individual live cells as well as non-targeted cell to cell effects to be addressed. This mini-review focuses on the use of near infrared (NIR) ca. 800nm radiation to induce damage that is radically different from the early and subsequent ultraviolet microbeam techniques. Ultrafast pulsed NIR instrumentation has many benefits including the ability to eliminate issues of unspecific UV absorption by the many materials prevalent within cells. The multiphoton interaction volume also permits energy deposition beyond the diffraction limit. Work has established that the fundamental process of the damage induced by the ultrashort laser pulses is different to those induced from continuous wave light sources. Pioneering work has demonstrated that NIR laser microbeam radiation can mimic ionising radiation via multiphoton absorption within the 3D femtolitre volume of the highly focused Gaussian beam. This light-matter interaction phenomenon provides a novel optical microbeam probe for mimicking both complex ionising and UV radiation-type cell damage including double strand breaks (DSBs) and base damage. A further advantage of the pulsed laser technique is that it provides further scope for time-resolved experiments. Recently the NIR laser microbeam technique has been used to investigate the recruitment of repair proteins to the sub-micrometre size area of damage in viable cells using both immuno-fluorescent staining of gamma-H2AX (a marker for DSBs) and real-time imaging of GFP-labelled repair proteins including ATM, p53 binding protein 1 (53BP1), RAD51 and Ku 70/80 to elucidate the interaction of the two DNA DSB repair pathways, homologous recombination and the non-homologous end joining pathway. 2010 Elsevier B.V. All rights reserved.

Nonlinear optical properties, upconversion and lasing in metal-organic frameworks.

PubMed

Medishetty, Raghavender; Zaręba, Jan K; Mayer, David; Samoć, Marek; Fischer, Roland A

2017-08-14

The building block modular approach that lies behind coordination polymers (CPs) and metal-organic frameworks (MOFs) results not only in a plethora of materials that can be obtained but also in a vast array of material properties that could be aimed at. Optical properties appear to be particularly predetermined by the character of individual structural units and by the intricate interplay between them. Indeed, the "design principles" shaping the optical properties of these materials seem to be well explored for luminescence and second-harmonic generation (SHG) phenomena; these have been covered in numerous previous reviews. Herein, we shine light on CPs and MOFs as optical media for state-of-the-art photonic phenomena such as multi-photon absorption, triplet-triplet annihilation (TTA) and stimulated emission. In the first part of this review we focus on the nonlinear optical (NLO) properties of CPs and MOFs, with a closer look at the two-photon absorption property. We discuss the scope of applicability of most commonly used measurement techniques (Z-scan and two-photon excited fluorescence (TPEF)) that can be applied for proper determination of the NLO properties of these materials; in particular, we suggest recommendations for their use, along with a discussion of the best reporting practices of NLO parameters. We also outline design principles, employing both intramolecular and intermolecular strategies, that are necessary for maximizing the NLO response. A review of recent literature on two-, three- and multi-photon absorption in CPs and MOFs is further supplemented with application-oriented processes such as two-photon 3D patterning and data storage. Additionally, we provide an overview of the latest achievements in the field of frequency doubling (SHG) and tripling (third-harmonic generation, THG) in these materials. Apart from nonlinear processes, in the next sections we also target the photonic properties of MOFs that benefit from their porosity, and resulting from this their ability to serve as containers for optically-active molecules. Thus, we survey dye@MOF composites as novel media in which efficient upconversion via triplet energy migration (TEM) occurs as well as materials for stimulated emission and multi-photon pumped lasing. Prospects for producing lasing as an intrinsic property of MOFs has also been discussed. Overall, further development of the optical processes highlighted herein should allow for realization of various photonic, data storage, biomedical and optoelectronic applications.

Multiphoton tomography of intratissue tattoo nanoparticles

NASA Astrophysics Data System (ADS)

König, Karsten

2012-02-01

Most of today's intratissue tattoo pigments are unknown nanoparticles. So far, there was no real control of their use due to the absence of regulations. Some of the tattoo pigments contain carcinogenic amines e.g. azo pigment Red 22. Nowadays, the European Union starts to control the administration of tattoo pigments. There is an interest to obtain information on the intratissue distribution, their interaction with living cells and the extracellular matrix, and the mechanisms behind laser tattoo removal. Multiphoton tomographs are novel biosafety and imaging tools that can provide such information non-invasively and without further labeling. When using the spectral FLIM module, spatially-resolved emission spectra, excitation spectra, and fluorescence lifetimes can pr provided. Multiphoton tomographs are used by all major cosmetic comapanies to test the biosafety of sunscreen nanoparticles.

Multiphoton tomography to detect chemo- and biohazards

NASA Astrophysics Data System (ADS)

König, Karsten

2015-03-01

In vivo high-resolution multiphoton/CARS tomography provides optical biopsies with 300 nm lateral resolution with chemical fingerprints. Thousands of volunteers and patients have been investigated for early cancer diagnosis, evaluation of anti-ageing cosmetic products, and changes of cellular metabolism by UV exposure and decreased oxygen supply. The skin as the outermost and largest organ is also the major target of CB agents. Current UV-based sensors are useful for bio-aerosol sensing but not for evaluating exposed in vivo skin. Here we evaluate the use of 4D multiphoton/CARS tomographs based on near infrared femtosecond laser radiation, time-correlated single photon counting (FLIM) and white light generation by photonic crystal fibers to detect bio- and chemohazards in human in vivo skin using twophoton fluorescence, SHG, and Raman signals.

Targeting Protein for Xenopus Kinesin-like Protein 2 (TPX2) Regulates γ-Histone 2AX (γ-H2AX) Levels upon Ionizing Radiation*

PubMed Central

Neumayer, Gernot; Helfricht, Angela; Shim, Su Yeon; Le, Hoa Thi; Lundin, Cecilia; Belzil, Camille; Chansard, Mathieu; Yu, Yaping; Lees-Miller, Susan P.; Gruss, Oliver J.; van Attikum, Haico; Helleday, Thomas; Nguyen, Minh Dang

2012-01-01

The microtubule-associated protein targeting protein for Xenopus kinesin-like protein 2 (TPX2) plays a key role in spindle assembly and is required for mitosis in human cells. In interphase, TPX2 is actively imported into the nucleus to prevent its premature activity in microtubule organization. To date, no function has been assigned to nuclear TPX2. We now report that TPX2 plays a role in the cellular response to DNA double strand breaks induced by ionizing radiation. Loss of TPX2 leads to inordinately strong and transient accumulation of ionizing radiation-dependent Ser-139-phosphorylated Histone 2AX (γ-H2AX) at G0 and G1 phases of the cell cycle. This is accompanied by the formation of increased numbers of high intensity γ-H2AX ionizing radiation-induced foci. Conversely, cells overexpressing TPX2 have reduced levels of γ-H2AX after ionizing radiation. Consistent with a role for TPX2 in the DNA damage response, we found that the protein accumulates at DNA double strand breaks and associates with the mediator of DNA damage checkpoint 1 (MDC1) and the ataxia telangiectasia mutated (ATM) kinase, both key regulators of γ-H2AX amplification. Pharmacologic inhibition or depletion of ATM or MDC1, but not of DNA-dependent protein kinase (DNA-PK), antagonizes the γ-H2AX phenotype caused by TPX2 depletion. Importantly, the regulation of γ-H2AX signals by TPX2 is not associated with apoptosis or the mitotic functions of TPX2. In sum, our study identifies a novel and the first nuclear function for TPX2 in the cellular responses to DNA damage. PMID:23045526

Near-K -edge single, double, and triple photoionization of C+ ions

NASA Astrophysics Data System (ADS)

Müller, A.; Borovik, A.; Buhr, T.; Hellhund, J.; Holste, K.; Kilcoyne, A. L. D.; Klumpp, S.; Martins, M.; Ricz, S.; Viefhaus, J.; Schippers, S.

2018-01-01

Single, double, and triple ionization of the C+ ion by a single photon have been investigated in the energy range 286 to 326 eV around the K -shell single-ionization threshold at an unprecedented level of detail. At energy resolutions as low as 12 meV, corresponding to a resolving power of 24 000, natural linewidths of the most prominent resonances could be determined. From the measurement of absolute cross sections, oscillator strengths, Einstein coefficients, multielectron Auger decay rates, and other transition parameters of the main K -shell excitation and decay processes are derived. The cross sections are compared to results of previous theoretical calculations. Mixed levels of agreement are found despite the relatively simple atomic structure of the C+ ion with only five electrons. This paper is a followup to a previous Letter [A. Müller et al., Phys. Rev. Lett. 114, 013002 (2015), 10.1103/PhysRevLett.114.013002].

Influence of XRCC1 Genetic Polymorphisms on Ionizing Radiation-Induced DNA Damage and Repair.

PubMed

Sterpone, Silvia; Cozzi, Renata

2010-07-25

It is well known that ionizing radiation (IR) can damage DNA through a direct action, producing single- and double-strand breaks on DNA double helix, as well as an indirect effect by generating oxygen reactive species in the cells. Mammals have evolved several and distinct DNA repair pathways in order to maintain genomic stability and avoid tumour cell transformation. This review reports important data showing a huge interindividual variability on sensitivity to IR and in susceptibility to developing cancer; this variability is principally represented by genetic polymorphisms, that is, DNA repair gene polymorphisms. In particular we have focussed on single nucleotide polymorphisms (SNPs) of XRCC1, a gene that encodes for a scaffold protein involved basically in Base Excision Repair (BER). In this paper we have reported and presented recent studies that show an influence of XRCC1 variants on DNA repair capacity and susceptibility to breast cancer.

Multi-Photon Micro-Spectroscopy of Biological Specimens

DTIC Science & Technology

2000-07-01

Micro-spectroscopy, multi-photon fluorescence spectroscopy, second harmonic generation, plant tissues, stem, chloroplast, protoplast, maize, Arabidopsis...harmonic generation (SHG) in the plant cell 5wall. In this case, micro-spectroscopy provides a means of verification that, indeed, SHG occurs in plant ...fluorescence microscopy -the response of plant cells to high intensity illumination," Micron (in press) 2000. 3. H.-C. Huang and C. -C Chen, "Genome

Monte Carlo event generators in atomic collisions: A new tool to tackle the few-body dynamics

NASA Astrophysics Data System (ADS)

Ciappina, M. F.; Kirchner, T.; Schulz, M.

2010-04-01

We present a set of routines to produce theoretical event files, for both single and double ionization of atoms by ion impact, based on a Monte Carlo event generator (MCEG) scheme. Such event files are the theoretical counterpart of the data obtained from a kinematically complete experiment; i.e. they contain the momentum components of all collision fragments for a large number of ionization events. Among the advantages of working with theoretical event files is the possibility to incorporate the conditions present in a real experiment, such as the uncertainties in the measured quantities. Additionally, by manipulating them it is possible to generate any type of cross sections, specially those that are usually too complicated to compute with conventional methods due to a lack of symmetry. Consequently, the numerical effort of such calculations is dramatically reduced. We show examples for both single and double ionization, with special emphasis on a new data analysis tool, called four-body Dalitz plots, developed very recently. Program summaryProgram title: MCEG Catalogue identifier: AEFV_v1_0 Program summary URL:http://cpc.cs.qub.ac.uk/summaries/AEFV_v1_0.html Program obtainable from: CPC Program Library, Queen's University, Belfast, N. Ireland Licensing provisions: Standard CPC licence, http://cpc.cs.qub.ac.uk/licence/licence.html No. of lines in distributed program, including test data, etc.: 2695 No. of bytes in distributed program, including test data, etc.: 18 501 Distribution format: tar.gz Programming language: FORTRAN 77 with parallelization directives using scripting Computer: Single machines using Linux and Linux servers/clusters (with cores with any clock speed, cache memory and bits in a word) Operating system: Linux (any version and flavor) and FORTRAN 77 compilers Has the code been vectorised or parallelized?: Yes RAM: 64-128 kBytes (the codes are very cpu intensive) Classification: 2.6 Nature of problem: The code deals with single and double ionization of atoms by ion impact. Conventional theoretical approaches aim at a direct calculation of the corresponding cross sections. This has the important shortcoming that it is difficult to account for the experimental conditions when comparing results to measured data. In contrast, the present code generates theoretical event files of the same type as are obtained in a real experiment. From these event files any type of cross sections can be easily extracted. The theoretical schemes are based on distorted wave formalisms for both processes of interest. Solution method: The codes employ a Monte Carlo Event Generator based on theoretical formalisms to generate event files for both single and double ionization. One of the main advantages of having access to theoretical event files is the possibility of adding the conditions present in real experiments (parameter uncertainties, environmental conditions, etc.) and to incorporate additional physics in the resulting event files (e.g. elastic scattering or other interactions absent in the underlying calculations). Additional comments: The computational time can be dramatically reduced if a large number of processors is used. Since the codes has no communication between processes it is possible to achieve an efficiency of a 100% (this number certainly will be penalized by the queuing waiting time). Running time: Times vary according to the process, single or double ionization, to be simulated, the number of processors and the type of theoretical model. The typical running time is between several hours and up to a few weeks.

Application of hollow anodes in a Hall thruster with double-peak magnetic fields

NASA Astrophysics Data System (ADS)

Ding, Yongjie; Sun, Hezhi; Li, Peng; Wei, Liqiu; Su, Hongbo; Peng, Wuji; Li, Hong; Yu, Daren

2017-08-01

A low-power Hall thruster was designed with two permanent magnet rings. Unlike conventional Hall thrusters, this one has a symmetrical double-peak magnetic field with a larger gradient. Moreover, the highest magnetic field strength appears in the plume region; hence, the distance from the zero-magnetic region to the channel outlet is shorter than that of other Hall thrusters. This paper presents the law and mechanism of the effect of a U-shaped hollow anode with the front end in the zero-magnetic region and anodes at the first magnetic peak and zero-magnetic point (corresponding to the front and rear end faces of the U-shaped anode, respectively) on the discharge characteristics of the thruster. The study shows that the overall performance of the hollow anode under the same operating conditions is the highest. For the anode at the magnetic peak, although the ionization rate is the highest, most of the ions generated by ionization collide with the walls, causing greater energy loss and minimizing its performance. For the anode at the zero-magnetic point, although its maximum ionization rate is higher than that of the hollow anode, and the power deposition on the walls is slightly smaller, its propellant utilization and voltage utilization are lower than those of the hollow anode; furthermore, its overall performance is poorer than that of the hollow anode because of the short channel and shorter ionization region.

Raman-Scattering Line Profiles of the Symbiotic Star AG Peg

NASA Astrophysics Data System (ADS)

Lee, Seong-Jae; Hyung, Siek

2017-06-01

The high dispersion Hα and Hβ line profiles of the Symbiotic star AG Peg consist of top double Gaussian and bottom components. We investigated the formation of the broad wings with Raman scattering mechanism. Adopting the same physical parameters from the photo-ionization study of Kim and Hyung (2008) for the white dwarf and the ionized gas shell, Monte Carlo simulations were carried out for a rotating accretion disk geometry of non-symmetrical latitude angles from -7° < θ < +7° to -16° < θ < +16°. The smaller latitude angle of the disk corresponds to the approaching side of the disk responsible for weak blue Gaussian profile, while the wider latitude angle corresponds to the other side of the disk responsible for the strong red Gaussian profile. We confirmed that the shell has the high gas density ˜ 109.85 cm-3 in the ionized zone of AG Peg derived in the previous photo-ionization model study. The simulation with various HI shell column densities (characterized by a thickness ΔD × gas number density nH) shows that the HI gas shell with a column density Hhi ≈ 3 - 5 × 1019 cm-2 fits the observed line profiles well. The estimated rotation speed of the accretion disk shell is in the range of 44 - 55 kms-1. We conclude that the kinematically incoherent structure involving the outflowing gas from the giant star caused an asymmetry of the disk and double Gaussian profiles found in AG Peg.

Infrared Multiphoton Dissociation Spectroscopy of a Gas-Phase Complex of Uranyl and 3-Oxa-Glutaramide: An Extreme Red-Shift of the [O=U=O]²⁺ Asymmetric Stretch

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

Gibson, John K.; Hu, Hanshi; Van Stipdonk, Michael J.

2015-04-09

The gas-phase complex UO₂(TMOGA)₂²⁺ (TMOGA = tetramethyl-3-oxa-glutaramide) prepared by electrospray ionization was characterized by infrared multiphoton dissociation (IRMPD) spectroscopy. The IRMPD spectrum from 700–1800 cm⁻¹ was interpreted using a computational study based on density functional theory. The predicted vibrational frequencies are in good agreement with the measured values, with an average deviation of only 8 cm⁻¹ (<1%) and a maximum deviation of 21 cm⁻¹ (<2%). The only IR peak assigned to the linear uranyl moiety was the asymmetric ν₃ mode, which appeared at 965 cm⁻¹ and was predicted by DFT as 953 cm⁻¹. This ν₃ frequency is red-shifted relative tomore » bare uranyl, UO₂²⁺, by ca. 150 cm⁻¹ due to electron donation from the TMOGA ligands. Based on the degree of red-shifting, it is inferred that two TMOGA oxygen-donor ligands have a greater effective gas basicity than the four monodentate acetone ligands in UO₂(acetone)₄²⁺. The uranyl ν₃ frequency was also computed for uranyl coordinated by two TMGA ligands, in which the central Oether of TMOGA has been replaced by CH₂. The computed ν₃ for UO₂(TMGA)₂²⁺, 950 cm⁻¹, is essentially the same as that for UO₂(TMOGA)₂²⁺, suggesting that electron donation to uranyl from the Oether of TMOGA is minor. The computed ν₃ asymmetric stretching frequencies for the three actinyl complexes, UO₂(TMOGA)₂²⁺, NpO₂(TMOGA)₂²⁺ and PuO₂(TMOGA)₂²⁺, are comparable. This similarity is discussed in the context of the relationship between ν₃ and intrinsic actinide-oxygen bond energies in actinyl complexes.« less

Correlated multielectron dynamics in mid-infrared laser pulse interactions with neon atoms.

PubMed

Tang, Qingbin; Huang, Cheng; Zhou, Yueming; Lu, Peixiang

2013-09-09

The multielectron dynamics in nonsequential triple ionization (NSTI) of neon atoms driven by mid-infrared (MIR) laser pulses is investigated with the three-dimensional classical ensemble model. In consistent with the experimental result, our numerical result shows that in the MIR regime, the triply charged ion longitudinal momentum spectrum exhibits a pronounced double-hump structure at low laser intensity. Back analysis reveals that as the intensity increases, the responsible triple ionization channels transform from direct (e, 3e) channel to the various mixed channels. This transformation of the NSTI channels leads to the results that the shape of ion momentum spectra becomes narrow and the distinct maxima shift towards low momenta with the increase of the laser intensity. By tracing the triply ionized trajectories, the various ionization channels at different laser intensities are clearly identified and these results provide an insight into the complex dynamics of the correlated three electrons in NSTI.

Clustered DNA damages induced in human hematopoietic cells by low doses of ionizing radiation

NASA Technical Reports Server (NTRS)

Sutherland, Betsy M.; Bennett, Paula V.; Cintron-Torres, Nela; Hada, Megumi; Trunk, John; Monteleone, Denise; Sutherland, John C.; Laval, Jacques; Stanislaus, Marisha; Gewirtz, Alan

2002-01-01

Ionizing radiation induces clusters of DNA damages--oxidized bases, abasic sites and strand breaks--on opposing strands within a few helical turns. Such damages have been postulated to be difficult to repair, as are double strand breaks (one type of cluster). We have shown that low doses of low and high linear energy transfer (LET) radiation induce such damage clusters in human cells. In human cells, DSB are about 30% of the total of complex damages, and the levels of DSBs and oxidized pyrimidine clusters are similar. The dose responses for cluster induction in cells can be described by a linear relationship, implying that even low doses of ionizing radiation can produce clustered damages. Studies are in progress to determine whether clusters can be produced by mechanisms other than ionizing radiation, as well as the levels of various cluster types formed by low and high LET radiation.

Ionization, evaporation and fragmentation of C60 in collisions with highly charged C, O and F ions—effect of projectile charge state.

NASA Astrophysics Data System (ADS)

Kelkar, A. H.; Misra, D.; Tribedi, L. C.

2007-09-01

We study the various inelastic processes such ionization, fragmentation and evaporation of C60 molecule in collisions with fast heavy ions. We have used 2.33 MeV/u C, O and F projectile ion beams. Various ionization and fragmentation products were detected using time-of-flight mass spectrometer. The multiply charged C60r+ ions were detected for maximum r = 4. The projectile charge state (qp) dependence of the single and double ionization cross sections is well reproduced by a model based on the giant dipole plasmon resonance (GDPR). The qp-dependence of the fragmentation yields, was found to be linear. Variation of relative yields of the evaporation products of C602+ (i.e. C582+, C562+ etc) and C603+ (i.e. C583+, C563+ etc) with qp has also been investigated for various projectiles.

The inception of pulsed discharges in air: simulations in background fields above and below breakdown

NASA Astrophysics Data System (ADS)

Sun, Anbang; Teunissen, Jannis; Ebert, Ute

2014-11-01

We investigate discharge inception in air, in uniform background electric fields above and below the breakdown threshold. We perform 3D particle simulations that include a natural level of background ionization in the form of positive and \\text{O}2- ions. In background fields below breakdown, we use a strongly ionized seed of electrons and positive ions to enhance the field locally. In the region of enhanced field, we observe the growth of positive streamers, as in previous simulations with 2D plasma fluid models. The inclusion of background ionization has little effect in this case. When the background field is above the breakdown threshold, the situation is very different. Electrons can then detach from \\text{O}2- and start ionization avalanches in the whole volume. These avalanches together create one extended discharge, in contrast to the ‘double-headed’ streamers found in many fluid simulations.

Measurement of scintillation and ionization yield with high-pressure gaseous mixtures of Xe and TMA for improved neutrinoless double beta decay and dark matter searches

DOE PAGES

Nakajima, Y.; Goldschmidt, A.; Matis, H. S.; ...

2016-03-18

The gaseous Xenon(Xe) time projection chamber (TPC) is an attractive detector technique for neutrinoless double beta decay and WIMP dark matter searches. While it is less dense compared to Liquid Xe detectors, it has intrinsic advantages in tracking capability and better energy resolution. The performance of gaseous Xe can be further improved by molecular additives such as trimethylamine(TMA), which is expected to (1) cool down the ionization electrons, (2) convert Xe excitation energy to TMA ionizations through Penning transfer, and (3) produce scintillation and electroluminescence light in a more easily detectable wavelength (300 nm). In order to test the feasibilitymore » of the performance improvements with TMA, in this paper we made the first direct measurement of Penning and fluorescence transfer efficiency with gaseous mixtures of Xe and TMA. While we observed a Penning transfer efficiency up to ~35%, we found strong suppression of primary scintillation light with TMA. We also found that the primary scintillation light with Xe and TMA mixture can be well characterized by ~3% fluorescence transfer from Xe to TMA, with further suppression due to TMA self-quenching. No evidence of the scintillation light produced by recombination of TMA ions was found. This strong suppression of scintillation light makes dark matter searches quite challenging, while the possibility of improved neutrinoless double beta decay searches remains open. Finally, this work has been carried out within the context of the NEXT collaboration.« less

Single- and multi-photon ionization studies of organosulfur species

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

Cheung, Yu -San

1999-02-12

Accurate ionization energies (IE`s) for molecular species are used for prediction of chemical reactivity and are of fundamental importance to chemists. The IE of a gaseous molecule can be determined routinely in a photoionization or a photoelectron experiment. IE determinations made in conventional photoionization and photoelectron studies have uncertainties in the range of 3--100 meV (25--250 cm -1). In the past decade, the most exciting development in the field of photoionization and photoelectron spectroscopy has been the availability of high resolution, tunable ultraviolet (UV) and vacuum ultraviolet (VUV) laser sources. The laser pulsed field ionization photoelectron (PFI-PE) scheme is currentlymore » the state-of-the-art photoelectron spectroscopic technique and is capable of providing photoelectron energy resolution close to the optical resolution. The author has focused attention on the photoionization processes of some sulfur-containing species. The studies of the photoionization and photodissociation on sulfur-containing compounds [such as CS 2, CH 3SH, CH 3SSCH 3, CH 3CH 2SCH 2CH 3, HSCH 2CH 2SH and C 4H 4S (thiophene) and sulfur-containing radicals, such as HS, CS, CH 3S, CH 3CH 2S and CH 3SS], have been the major subjects in the group because sulfur is an important species contributing to air pollution in the atmosphere. The modeling of the combustion and oxidation of sulfur compounds represents important steps for the control of both the production and the elimination of sulfur-containing pollutants. Chapter 1 is a general introduction of the thesis. Chapters 2 and 6 contain five papers published in, or accepted for publication in, academic periodicals. In Chapter 7, the progress of the construction in the laboratory of a new vacuum ultraviolet laser system equipped with a reflectron mass spectrometer is presented. Chapters 2 through 7 have been removed for separate processing. A general conclusion of these studies are given in Chapter 8 followed by an appendix.« less

Observation of fullerenes (C60-C70) associated with LDEF crater number 31

NASA Technical Reports Server (NTRS)

Radicatidibrozolo, Filippo; Fleming, R. H.; Bunch, T. E.

1992-01-01

The presence of fullerenes in and around the LDEF crater number 31 is reported. This crater has a high C level associated with it, and is interpreted as having been produced by the impact of a C-rich micrometeoroid. Fullerenes are large 3-D C structures, among which the species C sub 60 (MW 720) and C sub 70 (MW 840) are preeminent. Fullerenes have several UV absorption bands, hence fullerenes should be detectable using UV laser ionization time-of-flight mass spectrometry. We use a LIMA-2A instrument with pulsed UV laser (266 nm) to search for high mass C species associated with LDEF crater number 31. The mass range was 0 to 1200 amu. Low ablating laser power levels were used (less than or = 5 x 10 exp 7 W/sq. cm); 200 mass spectra were acquired and summed. We observed high mass signals near m/z 720, exhibiting 24 amu separation, which is characteristic of fullerenes. Alkali ion signals were also observed. Little or no C clusters of intermediate mass were observed. We interpret the signals around m/z 720 as fullerenes, mainly C sub 60+ with lower levels of C sub 70+. We propose that the mechanism that produces these signals is resonant multiphoton ionization (REMPI). This selective mechanism explains why low mass C cluster ions are not observed along with the fullerenes, since they have much higher ionization potentials. This finding is unexpected, since up to now the search for fullerenes in extraterrestrial materials has not been successful. We conclude that the fullerenes became associated with crater number 31 in space. Two alternative (and exciting) scenarios are being considered at this time: either the fullerenes were carried by the C-rich projectile that formed crater number 31, or the fullerenes formed upon impact with the LDEF. We show the results of experiments at the ARC Vertical Gun Facility, which may establish some constraints on the origin of the fullerenes.

SALI chemical analysis of provided samples

NASA Technical Reports Server (NTRS)

Becker, Christopher H.

1993-01-01

SRI has completed the chemical analysis of all the samples supplied by NASA. The final batch of four samples consisted of: one inch diameter MgF2 mirror, control 1200-ID-FL3; one inch diameter neat resin, PMR-15, AO171-IV-55, half exposed and half unexposed; one inch diameter chromic acid anodized, EOIM-3 120-47 aluminum disc; and AO-exposed and unexposed samples of fullerene extract material in powdered form, pressed into In foil for analysis. Chemical analyses of the surfaces were performed by the surface analysis by laser ionization (SALI) method. The analyses emphasize surface contamination or general organic composition. SALI uses nonselective photoionization of sputtered or desorbed atoms and molecules above but close (approximately one mm) to the surface, followed by time-of-flight (TOF) mass spectrometry. In these studies, we used laser-induced desorption by 5-ns pulse-width 355-nm light (10-100 mJ/sq cm) and single-photon ionization (SPI) by coherent 118-nm radiation (at approximately 5 x 10(exp 5) W/sq cm). SPI was chosen primarily for its ability to obtain molecular information, whereas multiphoton ionization (not used in the present studies) is intended primarily for elemental and small molecule information. In addition to these four samples, the Au mirror (EOIM-3 200-11, sample four) was depth profiled again. Argon ion sputtering was used together with photoionization with intense 355-nm radiation (35-ps pulsewidths). Depth profiles are similar to those reported earlier, showing reproducibility. No chromium was found in the sample above noise level; its presence could at most be at the trace level. Somewhat more Ni appears to be present in the Au layer in the unexposed side, indicating thermal diffusion without chemical enhancement. The result of the presence of oxygen is apparently to tie-up/draw out the Ni as an oxide at the surface. The exposed region has a brownish tint appearance to the naked eye.

The accuracy of seminumerical reionization models in comparison with radiative transfer simulations

NASA Astrophysics Data System (ADS)

Hutter, Anne

2018-06-01

We have developed a modular seminumerical code that computes the time and spatially dependent ionization of neutral hydrogen (H I), neutral (He I), and single-ionized helium (He II) in the intergalactic medium (IGM). The model accounts for recombinations and provides different descriptions for the photoionization rate that are used to calculate the residual H I fraction in ionized regions. We compare different seminumerical reionization schemes to a radiative transfer (RT) simulation. We use the RT simulation as a benchmark, and find that the seminumerical approaches produce similar H II and He II morphologies and power spectra of the H I 21 cm signal throughout reionization. As we do not track partial ionization of He II, the extent of the double-ionized helium (He III) regions is consistently smaller. In contrast to previous comparison projects, the ionizing emissivity in our seminumerical scheme is not adjusted to reproduce the redshift evolution of the RT simulation, but directly derived from the RT simulation spectra. Among schemes that identify the ionized regions by the ratio of the number of ionization and absorption events on different spatial smoothing scales, we find those that mark the entire sphere as ionized when the ionization criterion is fulfilled to result in significantly accelerated reionization compared to the RT simulation. Conversely, those that flag only the central cell as ionized yield very similar but slightly delayed redshift evolution of reionization, with up to 20 per cent ionizing photons lost. Despite the overall agreement with the RT simulation, our results suggest that constraining ionizing emissivity-sensitive parameters from seminumerical galaxy formation-reionization models are subject to photon nonconservation.

The accuracy of semi-numerical reionization models in comparison with radiative transfer simulations

NASA Astrophysics Data System (ADS)

Hutter, Anne

2018-03-01

We have developed a modular semi-numerical code that computes the time and spatially dependent ionization of neutral hydrogen (H I), neutral (He I) and singly ionized helium (He II) in the intergalactic medium (IGM). The model accounts for recombinations and provides different descriptions for the photoionization rate that are used to calculate the residual H I fraction in ionized regions. We compare different semi-numerical reionization schemes to a radiative transfer (RT) simulation. We use the RT simulation as a benchmark, and find that the semi-numerical approaches produce similar H II and He II morphologies and power spectra of the H I 21cm signal throughout reionization. As we do not track partial ionization of He II, the extent of the double ionized helium (He III) regions is consistently smaller. In contrast to previous comparison projects, the ionizing emissivity in our semi-numerical scheme is not adjusted to reproduce the redshift evolution of the RT simulation, but directly derived from the RT simulation spectra. Among schemes that identify the ionized regions by the ratio of the number of ionization and absorption events on different spatial smoothing scales, we find those that mark the entire sphere as ionized when the ionization criterion is fulfilled to result in significantly accelerated reionization compared to the RT simulation. Conversely, those that flag only the central cell as ionized yield very similar but slightly delayed redshift evolution of reionization, with up to 20% ionizing photons lost. Despite the overall agreement with the RT simulation, our results suggests that constraining ionizing emissivity sensitive parameters from semi-numerical galaxy formation-reionization models are subject to photon nonconservation.

Dissociative and double photoionization cross sections of NO from threshold to 120 A

NASA Technical Reports Server (NTRS)

Samson, J. A. R.; Masuoka, T.; Pareek, P. N.

1985-01-01

The partial photoionization cross sections for producing the NO(+) parent ion and the O(+), N(+), and NO(2+) fragmentations from neutral NO are presented from 120 to 614 A. The results indicate predissociation of the 3 pi (21.72 eV) and B-prime 1Sigma(+) (22.73 eV) electronic states of NO(+). The photoionization threshold for double ionization was found to be 39.4 + or - 0.12 eV.

Non-invasive imaging of skin cancer with fluorescence lifetime imaging using two photon tomography

NASA Astrophysics Data System (ADS)

Patalay, Rakesh; Talbot, Clifford; Alexandrov, Yuriy; Munro, Ian; Breunig, Hans Georg; König, Karsten; Warren, Sean; Neil, Mark A. A.; French, Paul M. W.; Chu, Anthony; Stamp, Gordon W.; Dunsby, Christopher

2011-07-01

Multispectral fluorescence lifetime imaging (FLIM) using two photon microscopy as a non-invasive technique for the diagnosis of skin lesions is described. Skin contains fluorophores including elastin, keratin, collagen, FAD and NADH. This endogenous contrast allows tissue to be imaged without the addition of exogenous agents and allows the in vivo state of cells and tissues to be studied. A modified DermaInspect® multiphoton tomography system was used to excite autofluorescence at 760 nm in vivo and on freshly excised ex vivo tissue. This instrument simultaneously acquires fluorescence lifetime images in four spectral channels between 360-655 nm using time-correlated single photon counting and can also provide hyperspectral images. The multispectral fluorescence lifetime images were spatially segmented and binned to determine lifetimes for each cell by fitting to a double exponential lifetime model. A comparative analysis between the cellular lifetimes from different diagnoses demonstrates significant diagnostic potential.

Towards in vivo breast skin characterization using multiphoton microscopy

NASA Astrophysics Data System (ADS)

Batista, Ana; Uchugonova, Aisada; Breunig, Hans Georg; König, Karsten

2017-02-01

Breast cancer, the most common type of cancer in women worldwide, as well as its treatment (e.g. radiation therapy) can affect the human skin. Multiphoton imaging could provide new insights into these skin alterations non-invasively and with high-resolution. As a preparation for a later investigation involving patients, areas of the breast and forearm skin of healthy volunteers were imaged using the clinically certified multiphoton imaging tomograph MPTflex based on endogenous skin autofluorescence and second-harmonic signals. Depth-resolved image stacks were acquired in consecutive weeks to explore the influence of hormonal variations on the skin properties. Both breasts were considered and up to three different areas were imaged per session. Acquisition parameters were optimized to minimize artifacts caused by breathing-motion. As a first result, skin properties, such as the epidermal thickness, appear to be influenced by hormonal variations.

Dirac Equation in (1 +1 )-Dimensional Curved Spacetime and the Multiphoton Quantum Rabi Model

NASA Astrophysics Data System (ADS)

Pedernales, J. S.; Beau, M.; Pittman, S. M.; Egusquiza, I. L.; Lamata, L.; Solano, E.; del Campo, A.

2018-04-01

We introduce an exact mapping between the Dirac equation in (1 +1 )-dimensional curved spacetime (DCS) and a multiphoton quantum Rabi model (QRM). A background of a (1 +1 )-dimensional black hole requires a QRM with one- and two-photon terms that can be implemented in a trapped ion for the quantum simulation of Dirac particles in curved spacetime. We illustrate our proposal with a numerical analysis of the free fall of a Dirac particle into a (1 +1 )-dimensional black hole, and find that the Zitterbewegung effect, measurable via the oscillatory trajectory of the Dirac particle, persists in the presence of gravity. From the duality between the squeezing term in the multiphoton QRM and the metric coupling in the DCS, we show that gravity generates squeezing of the Dirac particle wave function.

Assessing and benchmarking multiphoton microscopes for biologists

PubMed Central

Corbin, Kaitlin; Pinkard, Henry; Peck, Sebastian; Beemiller, Peter; Krummel, Matthew F.

2017-01-01

Multiphoton microscopy has become staple tool for tracking cells within tissues and organs due to superior depth of penetration, low excitation volumes, and reduced phototoxicity. Many factors, ranging from laser pulse width to relay optics to detectors and electronics, contribute to the overall ability of these microscopes to excite and detect fluorescence deep within tissues. However, we have found that there are few standard ways already described in the literature to distinguish between microscopes or to benchmark existing microscopes to measure the overall quality and efficiency of these instruments. Here, we discuss some simple parameters and methods that can either be used within a multiphoton facility or by a prospective purchaser to benchmark performance. This can both assist in identifying decay in microscope performance and in choosing features of a scope that are suited to experimental needs. PMID:24974026

Rapid in vivo vertical tissue sectioning by multiphoton tomography

NASA Astrophysics Data System (ADS)

Batista, Ana; Breunig, Hans Georg; König, Karsten

2018-02-01

A conventional tool in the pathological field is histology which involves the analysis of thin sections of tissue in which specific cellular structures are stained with different dyes. The process to obtain these stained tissue sections is time consuming and invasive as it requires tissue removal, fixation, sectioning, and staining. Moreover, imaging of live tissue is not possible. We demonstrate that multiphoton tomography can provide within seconds, non-invasive, label-free, vertical images of live tissue which are in quality similar to conventional light micrographs of histologic stained specimen. In contrast to conventional setups based on laser scanning which image horizontally sections, the vertical in vivo images are directly recorded by combined line scanning and timed adjustments of the height of the focusing optics. In addition, multiphoton tomography provides autofluorescence lifetimes which can be used to determine the metabolic states of cells.

Hybrid label-free multiphoton and optoacoustic microscopy (MPOM)

NASA Astrophysics Data System (ADS)

Soliman, Dominik; Tserevelakis, George J.; Omar, Murad; Ntziachristos, Vasilis

2015-07-01

Many biological applications require a simultaneous observation of different anatomical features. However, unless potentially harmful staining of the specimens is employed, individual microscopy techniques do generally not provide multi-contrast capabilities. We present a hybrid microscope integrating optoacoustic microscopy and multiphoton microscopy, including second-harmonic generation, into a single device. This combined multiphoton and optoacoustic microscope (MPOM) offers visualization of a broad range of structures by employing different contrast mechanisms and at the same time enables pure label-free imaging of biological systems. We investigate the relative performance of the two microscopy modalities and demonstrate their multi-contrast abilities through the label-free imaging of a zebrafish larva ex vivo, simultaneously visualizing muscles and pigments. This hybrid microscopy application bears great potential for developmental biology studies, enabling more comprehensive information to be obtained from biological specimens without the necessity of staining.

Double Electron Processes in Collisions of Partially Stripped Ions Cq+(q = 1-4) with Helium

NASA Astrophysics Data System (ADS)

Ding, Bao-Wei; Chen, Xi-Meng; Yu, De-Yang; Fu, Hong-Bin; Liu, Zhao-Yuan; Sun, Guang-Zhi; Liu, Yu-Wen; Lu, Yan-Xia; Xie, Jiang-Shan; Du, Juan; Gao, Zhi-Min; Chen, Lin; Cui, Ying; Shao, Jian-Xiong; He, Zi-Feng; Cai, Xiao-Hong

2007-01-01

The multi-electron processes are investigated for 17.9-120 keV/u C1+, 30-323 keV/u C2+, 120-438 keV/u C3+, 287-480 keV/u C4+ incident on a helium target. The cross-section ratios of double electron (DE) process to the total of the single electron (SE) and the double electron process (i.e. SE+DE), the direct double electron (DDI) to the direct single ionization (DSI) as well as the contributions of DDI to DE and of TI to DE are measured using coincidence techniques. The energy and charge state dependences of the measured cross-section ratios are studied and discussed.

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

Baalrud, S. D.; Lafleur, T.; Boswell, R. W.

Current-free double layers of the type reported in plasmas in the presence of an expanding magnetic field [C. Charles and R. W. Boswell, Appl. Phys. Lett. 82, 1356 (2003)] are modeled theoretically and with particle-in-cell/Monte Carlo simulations. Emphasis is placed on determining what mechanisms affect the electron velocity distribution function (EVDF) and how the EVDF influences the double layer. A theoretical model is developed based on depletion of electrons in certain velocity intervals due to wall losses and repletion of these intervals due to ionization and elastic electron scattering. This model is used to predict the range of neutral pressuresmore » over which a double layer can form and the electrostatic potential drop of the double layer. These predictions are shown to compare well with simulation results.« less

Metabolic Mapping of Breast Cancer with Multiphoton Spectral and Lifetime Imaging

DTIC Science & Technology

2007-03-01

spectral and lifetime characterization of NADH may be used to reveal metabolic changes in vivo and has potential to be used as an early diagnostic...combined spectral lifetime imaging modality will help for 5 characterization of breast cancer cells from cell culture based models to a relevant in... spectral and lifetime system and integrated into a multiphoton fluorescence excitation microscopy system 7 • Calibrated and characterized this

Continuum generation in ultra high numerical aperture fiber with application to multiphoton microscopy

NASA Astrophysics Data System (ADS)

Sayler, Nicholas

Nonlinear microscopy benefits from broadband laser sources, enabling efficient excitation of an array of fluorophores, for example. This work demonstrates broadening of a narrow band input pulse (6 nm to 40 nm) centered at 1040 nm with excellent shot-to-shot stability. In a preliminary demonstration, multiphoton imaging with pulses from the fiber is performed. In particular second harmonic imaging of corn starch is performed.

First multiphoton tomography of brain in man

NASA Astrophysics Data System (ADS)

König, Karsten; Kantelhardt, Sven R.; Kalasauskas, Darius; Kim, Ella; Giese, Alf

2016-03-01

We report on the first two-photon in vivo brain tissue imaging study in man. High resolution in vivo histology by multiphoton tomography (MPT) including two-photon FLIM was performed in the operation theatre during neurosurgery to evaluate the feasibility to detect label-free tumor borders with subcellular resolution. This feasibility study demonstrates, that MPT has the potential to identify tumor borders on a cellular level in nearly real-time.

Label-free multiphoton microscopy reveals altered tissue architecture in hippocampal sclerosis.

PubMed

Uckermann, Ortrud; Galli, Roberta; Leupold, Susann; Coras, Roland; Meinhardt, Matthias; Hallmeyer-Elgner, Susanne; Mayer, Thomas; Storch, Alexander; Schackert, Gabriele; Koch, Edmund; Blümcke, Ingmar; Steiner, Gerald; Kirsch, Matthias

2017-01-01

The properties and structure of tissue can be visualized without labeling or preparation by multiphoton microscopy combining coherent anti-Stokes Raman scattering (CARS), addressing lipid content, second harmonic generation (SHG) showing collagen, and two-photon excited fluorescence (TPEF) of endogenous fluorophores. We compared samples of sclerotic and nonsclerotic human hippocampus to detect pathologic changes in the brain of patients with pharmacoresistant temporomesial epilepsy (n = 15). Multiphoton microscopy of cryosections and bulk tissue revealed hippocampal layering and micromorphologic details in accordance with reference histology: CARS displayed white and gray matter layering and allowed the assessment of axonal myelin. SHG visualized blood vessels based on adventitial collagen. In addition, corpora amylacea (CoA) were found to be SHG-active. Pyramidal cell bodies were characterized by intense cytoplasmic endogenous TPEF. Furthermore, diffuse TPEF around blood vessels was observed that co-localized with positive albumin immunohistochemistry and might indicate degeneration-associated vascular leakage. We present a label-free and fast optical approach that analyzes pathologic aspects of HS. Hippocampal layering, loss of pyramidal cells, and presence of CoA indicative of sclerosis are visualized. Label-free multiphoton microscopy has the potential to extend the histopathologic armamentarium for ex vivo assessment of changes of the hippocampal formation on fresh tissue and prospectively in vivo. Wiley Periodicals, Inc. © 2016 International League Against Epilepsy.

Multiphoton microscopy in every lab: the promise of ultrafast semiconductor disk lasers

NASA Astrophysics Data System (ADS)

Emaury, Florian; Voigt, Fabian F.; Bethge, Philipp; Waldburger, Dominik; Link, Sandro M.; Carta, Stefano; van der Bourg, Alexander; Helmchen, Fritjof; Keller, Ursula

2017-07-01

We use an ultrafast diode-pumped semiconductor disk laser (SDL) to demonstrate several applications in multiphoton microscopy. The ultrafast SDL is based on an optically pumped Vertical External Cavity Surface Emitting Laser (VECSEL) passively mode-locked with a semiconductor saturable absorber mirror (SESAM) and generates 170-fs pulses at a center wavelength of 1027 nm with a repetition rate of 1.63 GHz. We demonstrate the suitability of this laser for structural and functional multiphoton in vivo imaging in both Drosophila larvae and mice for a variety of fluorophores (including mKate2, tdTomato, Texas Red, OGB-1, and R-CaMP1.07) and for endogenous second-harmonic generation in muscle cell sarcomeres. We can demonstrate equivalent signal levels compared to a standard 80-MHz Ti:Sapphire laser when we increase the average power by a factor of 4.5 as predicted by theory. In addition, we compare the bleaching properties of both laser systems in fixed Drosophila larvae and find similar bleaching kinetics despite the large difference in pulse repetition rates. Our results highlight the great potential of ultrafast diode-pumped SDLs for creating a cost-efficient and compact alternative light source compared to standard Ti:Sapphire lasers for multiphoton imaging.

Clinical optical coherence tomography combined with multiphoton tomography for evaluation of several skin disorders

NASA Astrophysics Data System (ADS)

König, Karsten; Speicher, Marco; Bückle, Rainer; Reckfort, Julia; McKenzie, Gordon; Welzel, Julia; Koehler, Martin J.; Elsner, Peter; Kaatz, Martin

2010-02-01

The first clinical trial of optical coherence tomography (OCT) combined with multiphoton tomography (MPT) and dermoscopy is reported. State-of-the-art (i) OCT systems for dermatology (e.g. multibeam swept source OCT), (ii) the femtosecond laser multiphoton tomograph DermaInspectTM, and (iii) digital dermoscopes were applied to 47 patients with a diversity of skin diseases and disorders such as skin cancer, psoriasis, hemangioma, connective tissue diseases, pigmented lesions, and autoimmune bullous skin diseases. Dermoscopy, also called 'epiluminescent microscopy', provides two-dimensional color images of the skin surface. OCT imaging is based on the detection of optical reflections within the tissue measured interferometrically whereas nonlinear excitation of endogenous fluorophores and the second harmonic generation are the bases of MPT images. OCT cross sectional "wide field" image provides a typical field of view of 5 x 2 mm2 and offers fast information on the depth and the volume of the investigated lesion. In comparison, multiphoton tomography presents 0.36 x 0.36 mm2 horizontal or diagonal sections of the region of interest within seconds with submicron resolution and down to a tissue depth of 200 μm. The combination of OCT and MPT provides a synergistic optical imaging modality for early detection of skin cancer and other skin diseases.

Multiphoton in vivo imaging with a femtosecond semiconductor disk laser

PubMed Central

Voigt, Fabian F.; Emaury, Florian; Bethge, Philipp; Waldburger, Dominik; Link, Sandro M.; Carta, Stefano; van der Bourg, Alexander; Helmchen, Fritjof; Keller, Ursula

2017-01-01

We use an ultrafast diode-pumped semiconductor disk laser (SDL) to demonstrate several applications in multiphoton microscopy. The ultrafast SDL is based on an optically pumped Vertical External Cavity Surface Emitting Laser (VECSEL) passively mode-locked with a semiconductor saturable absorber mirror (SESAM) and generates 170-fs pulses at a center wavelength of 1027 nm with a repetition rate of 1.63 GHz. We demonstrate the suitability of this laser for structural and functional multiphoton in vivo imaging in both Drosophila larvae and mice for a variety of fluorophores (including mKate2, tdTomato, Texas Red, OGB-1, and R-CaMP1.07) and for endogenous second-harmonic generation in muscle cell sarcomeres. We can demonstrate equivalent signal levels compared to a standard 80-MHz Ti:Sapphire laser when we increase the average power by a factor of 4.5 as predicted by theory. In addition, we compare the bleaching properties of both laser systems in fixed Drosophila larvae and find similar bleaching kinetics despite the large difference in pulse repetition rates. Our results highlight the great potential of ultrafast diode-pumped SDLs for creating a cost-efficient and compact alternative light source compared to standard Ti:Sapphire lasers for multiphoton imaging. PMID:28717563

Clinical optical coherence tomography combined with multiphoton tomography of patients with skin diseases.

PubMed

König, Karsten; Speicher, Marco; Bückle, Rainer; Reckfort, Julia; McKenzie, Gordon; Welzel, Julia; Koehler, Martin J; Elsner, Peter; Kaatz, Martin

2009-07-01

We report on the first clinical study based on optical coherence tomography (OCT) in combination with multiphoton tomography (MPT) and dermoscopy. 47 patients with a variety of skin diseases and disorders such as skin cancer, psoriasis, hemangioma, connective tissue diseases, pigmented lesions, and autoimmune bullous skin diseases have been investigated with (i) state-of-the-art OCT systems for dermatology including multibeam swept source OCT, (ii) the femtosecond laser multiphoton tomograph, and (iii) dermoscopes. Dermoscopy provides two-dimensional color images of the skin surface. OCT images reflect modifications of the intratissue refractive index whereas MPT is based on nonlinear excitation of endogenous fluorophores and second harmonic generation. A stack of cross-sectional OCT "wide field" images with a typical field of view of 5 x 2 mm(2) gave fast information on the depth and the volume of the lesion. Multiphoton tomography provided 0.36 x 0.36 mm(2) horizontal/diagonal optical sections within seconds of a particular region of interest with superior submicron resolution down to a tissue depth of 200 mum. The combination of OCT and MPT provides a unique powerful optical imaging modality for early detection of skin cancer and other skin diseases as well as for the evaluation of the efficiency of treatments.

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

NASA Astrophysics Data System (ADS)

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

2009-06-01

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

Comparison of Cornea Module and DermaInspect for noninvasive imaging of ocular surface pathologies

NASA Astrophysics Data System (ADS)

Steven, Philipp; Müller, Maya; Koop, Norbert; Rose, Christian; Hüttmann, Gereon

2009-11-01

Minimally invasive imaging of ocular surface pathologies aims at securing clinical diagnosis without actual tissue probing. For this matter, confocal microscopy (Cornea Module) is in daily use in ophthalmic practice. Multiphoton microscopy is a new optical technique that enables high-resolution imaging and functional analysis of living tissues based on tissue autofluorescence. This study was set up to compare the potential of a multiphoton microscope (DermaInspect) to the Cornea Module. Ocular surface pathologies such as pterygia, papillomae, and nevi were investigated in vivo using the Cornea Module and imaged immediately after excision by DermaInspect. Two excitation wavelengths, fluorescence lifetime imaging and second-harmonic generation (SHG), were used to discriminate different tissue structures. Images were compared with the histopathological assessment of the samples. At wavelengths of 730 nm, multiphoton microscopy exclusively revealed cellular structures. Collagen fibrils were specifically demonstrated by second-harmonic generation. Measurements of fluorescent lifetimes enabled the highly specific detection of goblet cells, erythrocytes, and nevus-cell clusters. At the settings used, DermaInspect reaches higher resolutions than the Cornea Module and obtains additional structural information. The parallel detection of multiphoton excited autofluorescence and confocal imaging could expand the possibilities of minimally invasive investigation of the ocular surface toward functional analysis at higher resolutions.

Weak-field multiphoton femtosecond coherent control in the single-cycle regime.

PubMed

Chuntonov, Lev; Fleischer, Avner; Amitay, Zohar

2011-03-28

Weak-field coherent phase control of atomic non-resonant multiphoton excitation induced by shaped femtosecond pulses is studied theoretically in the single-cycle regime. The carrier-envelope phase (CEP) of the pulse, which in the multi-cycle regime does not play any control role, is shown here to be a new effective control parameter that its effect is highly sensitive to the spectral position of the ultrabroad spectrum. Rationally chosen position of the ultrabroadband spectrum coherently induces several groups of multiphoton transitions from the ground state to the excited state of the system: transitions involving only absorbed photons as well as Raman transitions involving both absorbed and emitted photons. The intra-group interference is controlled by the relative spectral phase of the different frequency components of the pulse, while the inter-group interference is controlled jointly by the CEP and the relative spectral phase. Specifically, non-resonant two- and three-photon excitation is studied in a simple model system within the perturbative frequency-domain framework. The developed intuition is then applied to weak-field multiphoton excitation of atomic cesium (Cs), where the simplified model is verified by non-perturbative numerical solution of the time-dependent Schrödinger equation. We expect this work to serve as a basis for a new line of femtosecond coherent control experiments.

Ultrafast breakdown of dielectrics: new insight from double pump-probe experiments (Conference Presentation)

NASA Astrophysics Data System (ADS)

Guizard, Stéphane; Mouskeftaras, Alexandros; Bildé, Allan; Klimentov, Sergey M.; Fedorov, Nikita

2017-05-01

We investigate the mechanisms involved in the modification of dielectric materials by ultrashort laser pulses. We show that the use of a double pulse (fundamental and second harmonic of a Ti-Sa laser) excitation scheme allows getting new insight in the fundamental processes that occur during the interaction. We first measure the optical breakdown (OB) threshold map (intensity of first pulse versus intensity of second pulse) in various materials (Al2O3, MgO, α-SiO2). Using a simple model that includes multiphoton excitation followed by carrier heating in the conduction band, and assuming that OB occurs when a critical amount of energy is deposited in the material, we can satisfactorily reproduce this evolution of optical breakdown thresholds. The results demonstrate the dominant role of carrier heating in the energy transfer from the laser pulse to the solid. This important phenomenon is also highlighted by the kinetic energy distribution of photoelectrons observed in a photoemission experiment performed under similar conditions of double pulse excitation. Furthermore, we show, in the case of α-SiO2, that the formation of self-trapped exciton is in competition with the heating mechanism and thus play an important role especially when the pulse duration exceeds a few 100 fs. Finally, also in quartz or silica, we observe that the initial electronic excitation plays a key role in the formation of surface ripples and that their characteristics are determined by the first pulse, even at intensities well below OB threshold. The consequence of all these experimental results in the domain of UV or VUV induce damage will be discussed. In particular we demonstrate the possibility to dramatically increase the ablation efficiency by VUV light by using such double pulse scheme.