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Sample records for femtosecond pump-probe photoionization

  1. Femtosecond pump-probe photoionization-photofragmentation spectroscopy: photoionization-induced twisting and coherent vibrational motion of azobenzene cation.

    PubMed

    Ho, Jr-Wei; Chen, Wei-Kan; Cheng, Po-Yuan

    2009-10-01

    We report studies of ultrafast dynamics of azobenzene cation using femtosecond photoionization-photofragmentation spectroscopy. In our experiments, a femtosecond pump pulse first produces an ensemble of azobenzene cations via photoionization of the neutrals. A delayed probe pulse then brings the evolving ionic system to excited states that ultimately undergo ion fragmentation. The dynamics is followed by monitoring either the parent-ion depletion or fragment-ion formation as a function of the pump-probe delay time. The observed transients for azobenzene cation are characterized by a constant ion depletion modulated by a rapidly damped oscillatory signal with a period of about 1 ps. Theoretical calculations suggest that the oscillation arises from a vibration motion along the twisting inversion coordinate involving displacements in CNNC and phenyl-ring torsions. The oscillation is damped rapidly with a time constant of about 1.2 ps, suggesting that energy dissipation from the active mode to bath modes takes place in this time scale. PMID:19814554

  2. Spectroscopy of triplet states of Rb{sub 2} by femtosecond pump-probe photoionization of doped helium nanodroplets

    SciTech Connect

    Mudrich, M.; Heister, Ph.; Hippler, T.; Giese, Ch.; Stienkemeier, F.; Dulieu, O.

    2009-10-15

    The dynamics of vibrational wave packets in triplet states of rubidium dimers (Rb{sub 2}) formed on helium nanodroplets are studied using femtosecond pump-probe photoionization spectroscopy. Due to fast desorption of the excited Rb{sub 2} molecules off the droplets and due to their low internal temperature, wave-packet oscillations can be followed up to very long pump-probe delay times > or approx. 1.5 ns. In the first-excited triplet state (1){sup 3}{sigma}{sub g}{sup +}, full and fractional revivals are observed with high contrast. Fourier analysis provides high-resolution vibrational spectra which are in excellent agreement with ab initio calculations.

  3. Femtosecond Pump-Probe Microspectroscopy of Single Perylene Nanoparticles.

    PubMed

    Ishibashi, Yukihide; Asahi, Tsuyoshi

    2016-08-01

    We have developed a femtosecond pump-probe light scattering microspectroscopic system in which the output of a femtosecond Ti:sapphire oscillator (1 W, 82 MHz) was used as a light source; the pump light is the second harmonics (395 nm) of the laser output, and the probe light is a femtosecond white-light continuum (490-900 nm) generated with a photonic crystal fiber. Detection of the backscattered light from single nanoparticle on a glass substrate allowed us to obtain higher gain of the transient signals by ∼20 times in comparison with the conventional transmittance-mode experiment. This high-sensitivity of the backscattering detection makes it possible to examine ultrafast relaxation dynamics of excited states in organic nanoparticles, which, in general, are lower photodurability than the inorganic one. We applied the system to single nanocrystals of α-form perylene and then succeeded in direct observation of the excimer formation dynamics on a picosecond time scale. Single nanoparticle measurements for the perylene nanocrystals having a size range of 100 to 500 nm suggested that the excimer formation time became short from 2 ps to <0.3 ps for decreasing of the size. PMID:27420175

  4. Nonlinear femtosecond pump-probe spectroscopy using a power-encoded soliton delay line.

    PubMed

    Saint-Jalm, Sarah; Andresen, Esben Ravn; Bendahmane, Abdelkrim; Kudlinski, Alexandre; Rigneault, Hervé

    2016-01-01

    We show femtosecond time-resolved nonlinear pump-probe spectroscopy using a fiber soliton as the probe pulse. Furthermore, we exploit soliton dynamics to record an entire transient trace with a power-encoded delay sweep. The power-encoded delay line takes advantage of the dependency of the soliton trajectory in the (λ,z) space upon input power; the difference in accumulated group delay between trajectories converts a fast power sweep into a fast delay sweep. We demonstrate the concept by performing transient absorption spectroscopy in a test sample and validate it against a conventional pump-probe setup. PMID:26696172

  5. Femtosecond pump-probe microscopy generates virtual cross-sections in historic artwork

    PubMed Central

    Villafana, Tana Elizabeth; Brown, William P.; Delaney, John K.; Palmer, Michael; Warren, Warren S.; Fischer, Martin C.

    2014-01-01

    The layering structure of a painting contains a wealth of information about the artist's choice of materials and working methods, but currently, no 3D noninvasive method exists to replace the taking of small paint samples in the study of the stratigraphy. Here, we adapt femtosecond pump-probe imaging, previously shown in tissue, to the case of the color palette in paintings, where chromophores have much greater variety. We show that combining the contrasts of multispectral and multidelay pump-probe spectroscopy permits nondestructive 3D imaging of paintings with molecular and structural contrast, even for pigments with linear absorption spectra that are broad and relatively featureless. We show virtual cross-sectioning capabilities in mockup paintings, with pigment separation and nondestructive imaging on an intact 14th century painting (The Crucifixion by Puccio Capanna). Our approach makes it possible to extract microscopic information for a broad range of applications to cultural heritage. PMID:24449855

  6. Hetero-site-specific X-ray pump-probe spectroscopy for femtosecond intramolecular dynamics

    DOE PAGESBeta

    Picón, A.; Lehmann, C. S.; Bostedt, C.; Rudenko, A.; Marinelli, A.; Osipov, T.; Rolles, D.; Berrah, N.; Bomme, C.; Bucher, M.; et al

    2016-05-23

    New capabilities at X-ray free-electron laser facilities allow the generation of two-colour femtosecond X-ray pulses, opening the possibility of performing ultrafast studies of X-ray-induced phenomena. Specifically, the experimental realization of hetero-site-specific X-ray-pump/X-ray-probe spectroscopy is of special interest, in which an X-ray pump pulse is absorbed at one site within a molecule and an X-ray probe pulse follows the X-ray-induced dynamics at another site within the same molecule. In this paper, we show experimental evidence of a hetero-site pump-probe signal. By using two-colour 10-fs X-ray pulses, we are able to observe the femtosecond time dependence for the formation of F ionsmore » during the fragmentation of XeF2 molecules following X-ray absorption at the Xe site.« less

  7. Hetero-site-specific X-ray pump-probe spectroscopy for femtosecond intramolecular dynamics.

    PubMed

    Picón, A; Lehmann, C S; Bostedt, C; Rudenko, A; Marinelli, A; Osipov, T; Rolles, D; Berrah, N; Bomme, C; Bucher, M; Doumy, G; Erk, B; Ferguson, K R; Gorkhover, T; Ho, P J; Kanter, E P; Krässig, B; Krzywinski, J; Lutman, A A; March, A M; Moonshiram, D; Ray, D; Young, L; Pratt, S T; Southworth, S H

    2016-01-01

    New capabilities at X-ray free-electron laser facilities allow the generation of two-colour femtosecond X-ray pulses, opening the possibility of performing ultrafast studies of X-ray-induced phenomena. Particularly, the experimental realization of hetero-site-specific X-ray-pump/X-ray-probe spectroscopy is of special interest, in which an X-ray pump pulse is absorbed at one site within a molecule and an X-ray probe pulse follows the X-ray-induced dynamics at another site within the same molecule. Here we show experimental evidence of a hetero-site pump-probe signal. By using two-colour 10-fs X-ray pulses, we are able to observe the femtosecond time dependence for the formation of F ions during the fragmentation of XeF2 molecules following X-ray absorption at the Xe site. PMID:27212390

  8. Hetero-site-specific X-ray pump-probe spectroscopy for femtosecond intramolecular dynamics

    NASA Astrophysics Data System (ADS)

    Picón, A.; Lehmann, C. S.; Bostedt, C.; Rudenko, A.; Marinelli, A.; Osipov, T.; Rolles, D.; Berrah, N.; Bomme, C.; Bucher, M.; Doumy, G.; Erk, B.; Ferguson, K. R.; Gorkhover, T.; Ho, P. J.; Kanter, E. P.; Krässig, B.; Krzywinski, J.; Lutman, A. A.; March, A. M.; Moonshiram, D.; Ray, D.; Young, L.; Pratt, S. T.; Southworth, S. H.

    2016-05-01

    New capabilities at X-ray free-electron laser facilities allow the generation of two-colour femtosecond X-ray pulses, opening the possibility of performing ultrafast studies of X-ray-induced phenomena. Particularly, the experimental realization of hetero-site-specific X-ray-pump/X-ray-probe spectroscopy is of special interest, in which an X-ray pump pulse is absorbed at one site within a molecule and an X-ray probe pulse follows the X-ray-induced dynamics at another site within the same molecule. Here we show experimental evidence of a hetero-site pump-probe signal. By using two-colour 10-fs X-ray pulses, we are able to observe the femtosecond time dependence for the formation of F ions during the fragmentation of XeF2 molecules following X-ray absorption at the Xe site.

  9. Hetero-site-specific X-ray pump-probe spectroscopy for femtosecond intramolecular dynamics

    PubMed Central

    Picón, A.; Lehmann, C. S.; Bostedt, C.; Rudenko, A.; Marinelli, A.; Osipov, T.; Rolles, D.; Berrah, N.; Bomme, C.; Bucher, M.; Doumy, G.; Erk, B.; Ferguson, K. R.; Gorkhover, T.; Ho, P. J.; Kanter, E. P.; Krässig, B.; Krzywinski, J.; Lutman, A. A.; March, A. M.; Moonshiram, D.; Ray, D.; Young, L.; Pratt, S. T.; Southworth, S. H.

    2016-01-01

    New capabilities at X-ray free-electron laser facilities allow the generation of two-colour femtosecond X-ray pulses, opening the possibility of performing ultrafast studies of X-ray-induced phenomena. Particularly, the experimental realization of hetero-site-specific X-ray-pump/X-ray-probe spectroscopy is of special interest, in which an X-ray pump pulse is absorbed at one site within a molecule and an X-ray probe pulse follows the X-ray-induced dynamics at another site within the same molecule. Here we show experimental evidence of a hetero-site pump-probe signal. By using two-colour 10-fs X-ray pulses, we are able to observe the femtosecond time dependence for the formation of F ions during the fragmentation of XeF2 molecules following X-ray absorption at the Xe site. PMID:27212390

  10. Investigation of electronically excited indole relaxation dynamics via photoionization and fragmentation pump-probe spectroscopy

    SciTech Connect

    Godfrey, T. J.; Yu, Hui; Ullrich, Susanne

    2014-07-28

    The studies herein investigate the involvement of the low-lying {sup 1}L{sub a} and {sup 1}L{sub b} states with {sup 1}ππ{sup *} character and the {sup 1}πσ{sup *} state in the deactivation process of indole following photoexcitation at 201 nm. Three gas-phase, pump-probe spectroscopic techniques are employed: (1) Time-resolved photoelectron spectroscopy (TR-PES), (2) hydrogen atom (H-atom) time-resolved kinetic energy release (TR-KER), and (3) time-resolved ion yield (TR-IY). Each technique provides complementary information specific to the photophysical processes in the indole molecule. In conjunction, a thorough examination of the electronically excited states in the relaxation process, with particular focus on the involvement of the {sup 1}πσ{sup *} state, is afforded. Through an extensive analysis of the TR-PES data presented here, it is deduced that the initial excitation of the {sup 1}B{sub b} state decays to the {sup 1}L{sub a} state on a timescale beyond the resolution of the current experimental setup. Relaxation proceeds on the {sup 1}L{sub a} state with an ultrafast decay constant (<100 femtoseconds (fs)) to the lower-lying {sup 1}L{sub b} state, which is found to possess a relatively long lifetime of 23 ± 5 picoseconds (ps) before regressing to the ground state. These studies also manifest an additional component with a relaxation time of 405 ± 76 fs, which is correlated with activity along the {sup 1}πσ{sup *} state. TR-KER and TR-IY experiments, both specifically probing {sup 1}πσ{sup *} dynamics, exhibit similar decay constants, further validating these observations.

  11. 5-Femtosecond Laser-Electron Synchronization for Pump-Probe Crystallography and Diffraction

    NASA Astrophysics Data System (ADS)

    Walbran, Matthew; Gliserin, Alexander; Jung, Kwangyun; Kim, Jungwon; Baum, Peter

    2015-10-01

    For improving the temporal resolution in ultrafast pump-probe electron or x-ray diffraction, we report a laser-electron synchronization concept via direct microwave extraction from the laser frequency comb combined with phase detection by fiber-loop interferometry, in situ drift correction via electron-energy analysis, and laser-electron streaking for final timing metrology. We achieve a laser-electron jitter below 5 fs (rms) integrated between 8 min and Nyquist period (400 ns). Slower drifts are also below 5 fs (rms) after active compensation. This result helps advance femtosecond crystallography with electrons or x rays to the regime of fundamental atomic-scale dynamics and light-matter interaction.

  12. Femtosecond pump-probe studies of actinic-wavelength dependence in aqueous chlorine dioxide photochemistry

    NASA Astrophysics Data System (ADS)

    Bixby, Teresa J.; Bolinger, Joshua C.; Patterson, Joshua D.; Reid, Philip J.

    2009-04-01

    The actinic or photolysis-wavelength dependence of aqueous chlorine dioxide (OClO) photochemistry is investigated using femtosecond pump-probe spectroscopy. Following photoexcitation at 310, 335, and 410 nm the photoinduced evolution in optical density is measured from the UV to the near IR. Analysis of the optical-density evolution illustrates that the quantum yield for atomic chlorine production (ΦCl) increases with actinic energy, with ΦCl=0.16±0.02 for 410 nm excitation and increasing to 0.25±0.01 and 0.54±0.10 for 335 and 310 nm excitations, respectively. Consistent with previous studies, the production of Cl occurs through two channels, with one channel corresponding to prompt (<5 ps) Cl formation and the other corresponding to the thermal decomposition of ClOO formed by OClO photoisomerization. The partitioning between Cl production channels is dependent on actinic energy, with prompt Cl production enhanced with an increase in actinic energy. Limited evidence is found for enhanced ClO production with an increase in actinic energy. Stimulated emission and excited-state absorption features associated with OClO populating the optically prepared A22 surface decrease with an increase in actinic energy suggesting that the excited-state decay dynamics are also actinic energy dependent. The studies presented here provide detailed information on the actinic-wavelength dependence of OClO photochemistry in aqueous solution.

  13. Excited-State Vibrational Coherence in Perylene Bisimide Probed by Femtosecond Broadband Pump-Probe Spectroscopy.

    PubMed

    Son, Minjung; Park, Kyu Hyung; Yoon, Min-Chul; Kim, Pyosang; Kim, Dongho

    2015-06-18

    Broadband laser pulses with ultrashort duration are capable of triggering impulsive excitation of the superposition of vibrational eigenstates, giving rise to quantum beating signals originating from coherent wave packet motions along the potential energy surface. In this work, coherent vibrational wave packet dynamics of an N,N'-bis(2,6-dimethylphenyl)perylene bisimide (DMP-PBI) were investigated by femtosecond broadband pump-probe spectroscopy which features fast and balanced data acquisition with a wide spectral coverage of >200 nm. Clear modulations were observed in the envelope of the stimulated emission decay profiles of DMP-PBI with the oscillation frequencies of 140 and 275 cm(-1). Fast Fourier transform analysis of each oscillatory mode revealed characteristic phase jumps near the maxima of the steady-state fluorescence, indicating that the observed vibrational coherence originates from an excited-state wave packet motion. Quantum calculations of the normal modes at the low-frequency region suggest that low-frequency C-C (C═C) stretching motions accompanied by deformation of the dimethylphenyl substituents are responsible for the manifestation of such coherent wave packet dynamics. PMID:25992707

  14. Femtosecond pump-probe studies of actinic-wavelength dependence in aqueous chlorine dioxide photochemistry

    SciTech Connect

    Bixby, Teresa J.; Bolinger, Joshua C.; Patterson, Joshua D.; Reid, Philip J.

    2009-04-21

    The actinic or photolysis-wavelength dependence of aqueous chlorine dioxide (OClO) photochemistry is investigated using femtosecond pump-probe spectroscopy. Following photoexcitation at 310, 335, and 410 nm the photoinduced evolution in optical density is measured from the UV to the near IR. Analysis of the optical-density evolution illustrates that the quantum yield for atomic chlorine production ({Phi}{sub Cl}) increases with actinic energy, with {Phi}{sub Cl}=0.16{+-}0.02 for 410 nm excitation and increasing to 0.25{+-}0.01 and 0.54{+-}0.10 for 335 and 310 nm excitations, respectively. Consistent with previous studies, the production of Cl occurs through two channels, with one channel corresponding to prompt (<5 ps) Cl formation and the other corresponding to the thermal decomposition of ClOO formed by OClO photoisomerization. The partitioning between Cl production channels is dependent on actinic energy, with prompt Cl production enhanced with an increase in actinic energy. Limited evidence is found for enhanced ClO production with an increase in actinic energy. Stimulated emission and excited-state absorption features associated with OClO populating the optically prepared {sup 2}A{sub 2} surface decrease with an increase in actinic energy suggesting that the excited-state decay dynamics are also actinic energy dependent. The studies presented here provide detailed information on the actinic-wavelength dependence of OClO photochemistry in aqueous solution.

  15. Pump-probe imaging of the fs-ps-ns dynamics during femtosecond laser Bessel beam drilling in PMMA.

    PubMed

    Yu, Yanwu; Jiang, Lan; Cao, Qiang; Xia, Bo; Wang, Qingsong; Lu, Yongfeng

    2015-12-14

    A pump-probe shadowgraph imaging technique was used to reveal the femtosecond-picosecond-nanosecond multitimescale fundamentals of high-quality, high-aspect-ratio (up to 287:1) microhole drilling in poly-methyl-meth-acrylate (PMMA) by a single-shot femtosecond laser Bessel beam. The propagation of Bessel beam in PMMA (at 1.98 × 10⁸ m/s) and it induced cylindrical pressure wave expansion (at 3000-3950 m/s in radius) were observed during drilling processes. Also, it was unexpectedly found that the expansion of the cylindrical pressure wave in PMMA showed a linear relation with time and was insensitive to the laser energy fluctuation, quite different from the case in air. It was assumed that the energy insensitivity was due to the anisotropy of wave expansion in PMMA and the ambient air. PMID:26699062

  16. Femtosecond-precision synchronization of the pump-probe optical laser for user experiments at FLASH

    NASA Astrophysics Data System (ADS)

    Schulz, S.; Czwalinna, M. K.; Felber, M.; Predki, P.; Schefer, S.; Schlarb, H.; Wegner, U.

    2013-05-01

    In this paper, we present the long-term stable synchronization of the FLASH pump-probe Ti:sapphire oscillator to an optical reference with sub-10 fs (rms) timing jitter employing a balanced optical cross-correlator. The reference pulse train, transmitted over an actively transit time-stabilized 500m long fiber link, is generated by the FLASH master laser oscillator. This laser also provides the reference for several electron bunch arrival time monitors with sub-10 fs resolution, which in turn enables a longitudinal feedback reducing the electron bunch arrival time jitter to below 25 fs (rms). Combining the precise synchronization of the laser and the longitudinal accelerator feedback enabled a proof-of-principle pump-probe experiment at FLASH, ultimately showing a significant reduction of the timing jitter between the optical laser and the XUV pulses generated by the FEL, compared to the present standard operation.

  17. All-reflective femtosecond optical pump-probe setup for transient grating spectroscopy.

    PubMed

    Cucini, R; Bencivenga, F; Masciovecchio, C

    2011-04-01

    We developed a pump-probe setup that can be used for free electron lasers based four-wave mixing experiments in the extreme ultraviolet/soft x-ray spectral range. The main feature of the proposed optical layout is the absence of transmission optics. Test measurements on liquid and solid samples carried out using the transient grating technique in both transmission and reflection geometry demonstrate the reliability of the setup. PMID:21478973

  18. Dual Femtosecond TITANIUM:SAPPHIRE Laser for Ultrafast Optical Sampling Two-Color Pump/probe Studies.

    NASA Astrophysics Data System (ADS)

    Luo, Ningyi Daniel

    A pair of self-synchronous Ti:Sapphire lasers have been setup for two-color pump/probe detection in the sub-picosecond time regime. The two 75 femtosecond self -mode-locked Ti:Sapphire lasers are operated asynchronously at slightly different repetition rates to provide continuously varying dynamic delay times. They are tunable at 700-890 nm. The shorter wavelength pulses from one laser are used as a pump source, while the longer wavelength pulses are used as a probe. The sum-frequency pulses generated by the cross-correlation of the two laser pulses are used to define the "time-zero" position and trigger the pump/probe process. The experiment is triggered at the difference frequency, and the signal can be averaged many times allowing a weak signal to build up. Dual-time scale is involved with the interpretation of the signal, which allows the experiment to be carried on the real time scale and the signal to be recorded on a much reduced equivalent time scale. Excited state lifetime measurement of laser HITCI has proven that this technology is practically feasible. Several advantages have been seen: (1) independent wavelength tunability of the pump and probe lasers; (2) variable femto- to nano -second pump/probe time delay; (3) fast (mu s-ms) data collection time; (4) compact optical layout, without the need for optical delay lines and modulators, and thus, simple optical alignment. This study sheds light on the development of a novel compact high speed optical instrument.

  19. A split-beam probe-pump-probe scheme for femtosecond time resolved protein X-ray crystallography.

    PubMed

    van Thor, Jasper J; Madsen, Anders

    2015-01-01

    In order to exploit the femtosecond pulse duration of X-ray Free-Electron Lasers (XFEL) operating in the hard X-ray regime for ultrafast time-resolved protein crystallography experiments, critical parameters that determine the crystallographic signal-to-noise (I/σI) must be addressed. For single-crystal studies under low absorbed dose conditions, it has been shown that the intrinsic pulse intensity stability as well as mode structure and jitter of this structure, significantly affect the crystallographic signal-to-noise. Here, geometrical parameters are theoretically explored for a three-beam scheme: X-ray probe, optical pump, X-ray probe (or "probe-pump-probe") which will allow experimental determination of the photo-induced structure factor amplitude differences, ΔF, in a ratiometric manner, thereby internally referencing the intensity noise of the XFEL source. In addition to a non-collinear split-beam geometry which separates un-pumped and pumped diffraction patterns on an area detector, applying an additional convergence angle to both beams by focusing leads to integration over mosaic blocks in the case of well-ordered stationary protein crystals. Ray-tracing X-ray diffraction simulations are performed for an example using photoactive yellow protein crystals in order to explore the geometrical design parameters which would be needed. The specifications for an X-ray split and delay instrument that implements both an offset angle and focused beams are discussed, for implementation of a probe-pump-probe scheme at the European XFEL. We discuss possible extension of single crystal studies to serial femtosecond crystallography, particularly in view of the expected X-ray damage and ablation due to the first probe pulse. PMID:26798786

  20. Observation of femtosecond X-ray interactions with matter using an X-ray-X-ray pump-probe scheme.

    PubMed

    Inoue, Ichiro; Inubushi, Yuichi; Sato, Takahiro; Tono, Kensuke; Katayama, Tetsuo; Kameshima, Takashi; Ogawa, Kanade; Togashi, Tadashi; Owada, Shigeki; Amemiya, Yoshiyuki; Tanaka, Takashi; Hara, Toru; Yabashi, Makina

    2016-02-01

    Resolution in the X-ray structure determination of noncrystalline samples has been limited to several tens of nanometers, because deep X-ray irradiation required for enhanced resolution causes radiation damage to samples. However, theoretical studies predict that the femtosecond (fs) durations of X-ray free-electron laser (XFEL) pulses make it possible to record scattering signals before the initiation of X-ray damage processes; thus, an ultraintense X-ray beam can be used beyond the conventional limit of radiation dose. Here, we verify this scenario by directly observing femtosecond X-ray damage processes in diamond irradiated with extraordinarily intense (∼10(19) W/cm(2)) XFEL pulses. An X-ray pump-probe diffraction scheme was developed in this study; tightly focused double-5-fs XFEL pulses with time separations ranging from sub-fs to 80 fs were used to excite (i.e., pump) the diamond and characterize (i.e., probe) the temporal changes of the crystalline structures through Bragg reflection. It was found that the pump and probe diffraction intensities remain almost constant for shorter time separations of the double pulse, whereas the probe diffraction intensities decreased after 20 fs following pump pulse irradiation due to the X-ray-induced atomic displacement. This result indicates that sub-10-fs XFEL pulses enable conductions of damageless structural determinations and supports the validity of the theoretical predictions of ultraintense X-ray-matter interactions. The X-ray pump-probe scheme demonstrated here would be effective for understanding ultraintense X-ray-matter interactions, which will greatly stimulate advanced XFEL applications, such as atomic structure determination of a single molecule and generation of exotic matters with high energy densities. PMID:26811449

  1. Ultrafast dynamics in thiophene investigated by femtosecond pump probe photoelectron spectroscopy and theory.

    PubMed

    Weinkauf, R; Lehr, L; Schlag, E W; Salzmann, S; Marian, C M

    2008-01-21

    A hybrid of a time-of-flight mass spectrometer and a time-of-flight "magnetic-bottle type" photoelectron (PE) spectrometer is used for fs pump-probe investigations of the excited state dynamics of thiophene. A resonant two-photon ionization spectrum of the onset of the excited states has been recorded with a tunable UV laser of 190 fs pulse width. With the pump laser set to the first intense transition we find by UV probe ionization first a small time shift of the maxima in the PE spectrum and then a fast decay to a low constant intensity level. The fitted time constants are 80+/-10 fs, and 25+/-10 fs, respectively. Theoretical calculations show that upon geometry relaxation the electronic state order changes and conical intersections between excited states exist. We use the vertical state order S1, S2, S3 to define the terms S1, S2, and S3 for the characterization of the electron configuration of these states. On the basis of our theoretical result we discuss the electronic state order in the UV spectra and identify in the photoelectron spectrum the origin of the first cation excited state D1. The fast excited state dynamics agrees best with a vibrational dynamics in the photo-excited S1 (80+/-10 fs) and an ultrafast decay via a conical intersection, presumably a ring opening to the S3 state (25+/-10 fs). The subsequently observed weak constant signal is taken as an indication, that in the gas phase the ring-closure to S0 is slower than 50 ps. An ultrafast equilibrium between S1 and S2 before ring opening is not supported by our data. PMID:18174981

  2. Water Hydrogen-Bonding Network Structure and Dynamics at Phospholipid Multibilayer Surface: Femtosecond Mid-IR Pump-Probe Spectroscopy.

    PubMed

    Kundu, Achintya; Błasiak, Bartosz; Lim, Joon-Hyung; Kwak, Kyungwon; Cho, Minhaeng

    2016-03-01

    The water hydrogen-bonding network at a lipid bilayer surface is crucial to understanding membrane structures and its functional activities. With a phospholipid multibilayer mimicking a biological membrane, we study the temperature dependence of water hydrogen-bonding structure, distribution, and dynamics at a lipid multibilayer surface using femtosecond mid-IR pump-probe spectroscopy. We observe two distinguished vibrational lifetime components. The fast component (0.6 ps) is associated with water interacting with a phosphate part, whereas the slow component (1.9 ps) is with bulk-like choline-associated water. With increasing temperature, the vibrational lifetime of phosphate-associated water remains constant though its relative fraction dramatically increases. The OD stretch vibrational lifetime of choline-bound water slows down in a sigmoidal fashion with respect to temperature, indicating a noticeable change of the water environment upon the phase transition. The water structure and dynamics are thus shown to be in quantitative correlation with the structural change of liquid multibilayer upon the gel-to-liquid crystal phase transition. PMID:26859047

  3. A split-beam probe-pump-probe scheme for femtosecond time resolved protein X-ray crystallography

    DOE PAGESBeta

    van Thor, Jasper J.; Madsen, Anders

    2015-01-01

    In order to exploit the femtosecond pulse duration of X-ray Free-Electron Lasers (XFEL) operating in the hard X-ray regime for ultrafast time-resolved protein crystallography experiments, critical parameters that determine the crystallographic signal-to-noise (I/σI) must be addressed. For single-crystal studies under low absorbed dose conditions, it has been shown that the intrinsic pulse intensity stability as well as mode structure and jitter of this structure, significantly affect the crystallographic signal-to-noise. Here, geometrical parameters are theoretically explored for a three-beam scheme: X-ray probe, optical pump, X-ray probe (or “probe-pump-probe”) which will allow experimental determination of the photo-induced structure factor amplitude differences, ΔF,more » in a ratiometric manner, thereby internally referencing the intensity noise of the XFEL source. In addition to a non-collinear split-beam geometry which separates un-pumped and pumped diffraction patterns on an area detector, applying an additional convergence angle to both beams by focusing leads to integration over mosaic blocks in the case of well-ordered stationary protein crystals. Ray-tracing X-ray diffraction simulations are performed for an example using photoactive yellow protein crystals in order to explore the geometrical design parameters which would be needed. The specifications for an X-ray split and delay instrument that implements both an offset angle and focused beams are discussed, for implementation of a probe-pump-probe scheme at the European XFEL. We discuss possible extension of single crystal studies to serial femtosecond crystallography, particularly in view of the expected X-ray damage and ablation due to the first probe pulse.« less

  4. A split-beam probe-pump-probe scheme for femtosecond time resolved protein X-ray crystallography

    SciTech Connect

    van Thor, Jasper J.; Madsen, Anders

    2015-01-01

    In order to exploit the femtosecond pulse duration of X-ray Free-Electron Lasers (XFEL) operating in the hard X-ray regime for ultrafast time-resolved protein crystallography experiments, critical parameters that determine the crystallographic signal-to-noise (I/σI) must be addressed. For single-crystal studies under low absorbed dose conditions, it has been shown that the intrinsic pulse intensity stability as well as mode structure and jitter of this structure, significantly affect the crystallographic signal-to-noise. Here, geometrical parameters are theoretically explored for a three-beam scheme: X-ray probe, optical pump, X-ray probe (or “probe-pump-probe”) which will allow experimental determination of the photo-induced structure factor amplitude differences, ΔF, in a ratiometric manner, thereby internally referencing the intensity noise of the XFEL source. In addition to a non-collinear split-beam geometry which separates un-pumped and pumped diffraction patterns on an area detector, applying an additional convergence angle to both beams by focusing leads to integration over mosaic blocks in the case of well-ordered stationary protein crystals. Ray-tracing X-ray diffraction simulations are performed for an example using photoactive yellow protein crystals in order to explore the geometrical design parameters which would be needed. The specifications for an X-ray split and delay instrument that implements both an offset angle and focused beams are discussed, for implementation of a probe-pump-probe scheme at the European XFEL. We discuss possible extension of single crystal studies to serial femtosecond crystallography, particularly in view of the expected X-ray damage and ablation due to the first probe pulse.

  5. A split-beam probe-pump-probe scheme for femtosecond time resolved protein X-ray crystallography

    PubMed Central

    van Thor, Jasper J.; Madsen, Anders

    2015-01-01

    In order to exploit the femtosecond pulse duration of X-ray Free-Electron Lasers (XFEL) operating in the hard X-ray regime for ultrafast time-resolved protein crystallography experiments, critical parameters that determine the crystallographic signal-to-noise (I/σI) must be addressed. For single-crystal studies under low absorbed dose conditions, it has been shown that the intrinsic pulse intensity stability as well as mode structure and jitter of this structure, significantly affect the crystallographic signal-to-noise. Here, geometrical parameters are theoretically explored for a three-beam scheme: X-ray probe, optical pump, X-ray probe (or “probe-pump-probe”) which will allow experimental determination of the photo-induced structure factor amplitude differences, ΔF, in a ratiometric manner, thereby internally referencing the intensity noise of the XFEL source. In addition to a non-collinear split-beam geometry which separates un-pumped and pumped diffraction patterns on an area detector, applying an additional convergence angle to both beams by focusing leads to integration over mosaic blocks in the case of well-ordered stationary protein crystals. Ray-tracing X-ray diffraction simulations are performed for an example using photoactive yellow protein crystals in order to explore the geometrical design parameters which would be needed. The specifications for an X-ray split and delay instrument that implements both an offset angle and focused beams are discussed, for implementation of a probe-pump-probe scheme at the European XFEL. We discuss possible extension of single crystal studies to serial femtosecond crystallography, particularly in view of the expected X-ray damage and ablation due to the first probe pulse. PMID:26798786

  6. Photodissociation dynamics of iodocyclohexane upon UV excitation by femtosecond pump-probe technique

    NASA Astrophysics Data System (ADS)

    Hu, Chunlong; Wang, Lian; Wang, Yanmei; Tang, Ying; Long, Jinyou; Zhang, Bing

    2016-08-01

    The photodissociation dynamics of iodocyclohexane in the A-band and C-state have been investigated by femtosecond time-resolved time-of-flight mass spectroscopy. Iodocyclohexane was pumped by 266 nm pulse to its A-band. The following dissociation dynamics is prompt and direct. The time it takes for the progression of the wave packet from the dissociative state to the dissociating asymptotic region is around 180 fs. The C-state was excited by 200 nm pump pulse and it has predissociative character with predissociation time of about 600 fs, which may have contributions from multiple vibrational modes.

  7. Dependence of line shapes in femtosecond broadband stimulated Raman spectroscopy on pump-probe time delay

    PubMed Central

    Yoon, Sangwoon; McCamant, David W.; Kukura, Philipp; Mathies, Richard A.; Zhang, Donghui; Lee, Soo-Y.

    2005-01-01

    The effect of the time delay between the picosecond Raman pump and the femtosecond Stokes probe pulse on the Raman gain line shape in femtosecond broadband stimulated Raman spectroscopy (FSRS) is presented. Experimental data are obtained for cyclohexane to investigate the dependence of the FSRS line shape on this time delay. Theoretical simulations of the line shapes as a function of the time delay using the coupled wave theory agree well with experimental data, recovering broad line shapes at positive time delays and narrower bands with small Raman loss side wings at negative time delays. The analysis yields the lower bounds of the vibrational dephasing times of 2.0 ps and 0.65 ps for the 802 and 1027 cm−1 modes for cyclohexane, respectively. The theoretical description and simulation using the coupled wave theory are also consistent with the observed Raman gain intensity profile over time delay, reaching the maximum at a slightly negative time delay (∼−21 ps), and show that the coupled wave theory is a good model for describing FSRS. PMID:15638596

  8. Spectral relaxation in pump-probe transients

    NASA Astrophysics Data System (ADS)

    Farrow, Darcie A.; Yu, Anchi; Jonas, David M.

    2003-05-01

    The relationship between pump-probe transients and the transition frequency correlation function, M(t), is examined. Calculations of pump-probe transients are carried out with a full-quantum expression for a displaced harmonic oscillator coupled to a heat bath. Pump-probe transients for a slowly decaying, overdamped, Brownian oscillator are shown to resemble a power series in M(t), where the slowest time scale is always equal to the slowest decay in M(t). This equality is consistent with a semiclassical model of pump-probe and valid over the full range of temperature, pulse duration, and detuning explored. The contribution of time scales faster than M(t) to the pump-probe transient increases with increasing temperature, pulse duration, and detuning of the pulse center frequency below resonance. Pump-probe transients for a critically damped oscillator that decays on a femtosecond time scale also have faster early time decay at higher temperatures. Based on these calculations a bootstrap method is suggested for extracting M(t) from pump-probe data starting with the slowest decay. Comparisons are made between simulations of pump-probe and three pulse echo peak shift (3PEPS) transients for a single oscillator and for multiple oscillator systems. Additional fast relaxations similar to those in pump-probe are also present in the 3PEPS transients. For the models investigated, pump-probe is comparable to 3PEPS for the extraction of M(t).

  9. Femtosecond resolution timing jitter correction on a TW scale Ti:sapphire laser system for FEL pump-probe experiments.

    PubMed

    Csatari Divall, Marta; Mutter, Patrick; Divall, Edwin J; Hauri, Christoph P

    2015-11-16

    Intense ultrashort pulse lasers are used for fs resolution pump-probe experiments more and more at large scale facilities, such as free electron lasers (FEL). Measurement of the arrival time of the laser pulses and stabilization to the machine or other sub-systems on the target, is crucial for high time-resolution measurements. In this work we report on a single shot, spectrally resolved, non-collinear cross-correlator with sub-fs resolution. With a feedback applied we keep the output of the TW class Ti:sapphire amplifier chain in time with the seed oscillator to ~3 fs RMS level for several hours. This is well below the typical pulse duration used at FELs and supports fs resolution pump-probe experiments. Short term jitter and long term timing drift measurements are presented. Applicability to other wavelengths and integration into the timing infrastructure of the FEL are also covered to show the full potential of the device. PMID:26698475

  10. Femtosecond resolution timing jitter correction on a TW scale Ti:sapphire laser system for FEL pump-probe experiments

    NASA Astrophysics Data System (ADS)

    Csatari Divall, Marta; Mutter, Patrick; Divall, Edwin J.; Hauri, Christoph P.

    2015-11-01

    Intense ultrashort pulse lasers are used for fs resolution pumpprobe experiments more and more at large scale facilities, such as free electron lasers (FEL). Measurement of the arrival time of the laser pulses and stabilization to the machine or other sub-systems on the target, is crucial for high time-resolution measurements. In this work we report on a single shot, spectrally resolved, non-collinear cross-correlator with sub-fs resolution. With a feedback applied we keep the output of the TW class Ti:sapphire amplifier chain in time with the seed oscillator to ~3 fs RMS level for several hours. This is well below the typical pulse duration used at FELs and supports fs resolution pump-probe experiments. Short term jitter and long term timing drift measurements are presented. Applicability to other wavelengths and integration into the timing infrastructure of the FEL are also covered to show the full potential of the device.

  11. Femtosecond pump-probe measurements of non-radiative relaxation in LiAlO(2):V(3+).

    PubMed

    Wells, Jon-Paul R; Grinberg, Marek; Wynne, Klaas; Han, T P J

    2006-04-26

    We report on time-resolved studies of non-radiative relaxation of V(3+) ions in LiAlO(2) by means of a two-beam, pump-probe saturation experiment performed with the 150 fs pulsed output of a Ti-sapphire laser. Exciting into the vibronically broadened [Formula: see text] transition at 800 nm, a (3)T(1) relaxation time of 199 ps has been measured at 4 K. This value decreases to 82 ps at room temperature, representing a reduction in the lifetime of a factor of 2.5 due to internal-conversion processes. The relative probabilities for non-radiative, phonon-assisted barrier hopping and quantum mechanical tunnelling through the potential barrier to the (3)A(2) ground state have been obtained using Mott's expression, yielding best-fit parameters of W(0) = (5.2 ± 1) × 10(9) Hz and W(1) = (7.5 ± 1) × 10(10) Hz for a potential barrier of E(nr) = 530 ± 50 cm(-1). PMID:21690751

  12. In-Situ Probing Plasmonic Energy Transfer in Cu(In, Ga)Se2 Solar Cells by Ultrabroadband Femtosecond Pump-Probe Spectroscopy

    NASA Astrophysics Data System (ADS)

    Chen, Shih-Chen; Wu, Kaung-Hsiung; Li, Jia-Xing; Yabushita, Atsushi; Tang, Shih-Han; Luo, Chih Wei; Juang, Jenh-Yih; Kuo, Hao-Chung; Chueh, Yu-Lun

    2015-12-01

    In this work, we demonstrated a viable experimental scheme for in-situ probing the effects of Au nanoparticles (NPs) incorporation on plasmonic energy transfer in Cu(In, Ga)Se2 (CIGS) solar cells by elaborately analyzing the lifetimes and zero moment for hot carrier relaxation with ultrabroadband femtosecond pump-probe spectroscopy. The signals of enhanced photobleach (PB) and waned photoinduced absorption (PIA) attributable to surface plasmon resonance (SPR) of Au NPs were in-situ probed in transient differential absorption spectra. The results suggested that substantial carriers can be excited from ground state to lower excitation energy levels, which can reach thermalization much faster with the existence of SPR. Thus, direct electron transfer (DET) could be implemented to enhance the photocurrent of CIGS solar cells. Furthermore, based on the extracted hot carrier lifetimes, it was confirmed that the improved electrical transport might have been resulted primarily from the reduction in the surface recombination of photoinduced carriers through enhanced local electromagnetic field (LEMF). Finally, theoretical calculation for resonant energy transfer (RET)-induced enhancement in the probability of exciting electron-hole pairs was conducted and the results agreed well with the enhanced PB peak of transient differential absorption in plasmonic CIGS film. These results indicate that plasmonic energy transfer is a viable approach to boost high-efficiency CIGS solar cells.

  13. In-Situ Probing Plasmonic Energy Transfer in Cu(In, Ga)Se2 Solar Cells by Ultrabroadband Femtosecond Pump-Probe Spectroscopy.

    PubMed

    Chen, Shih-Chen; Wu, Kaung-Hsiung; Li, Jia-Xing; Yabushita, Atsushi; Tang, Shih-Han; Luo, Chih Wei; Juang, Jenh-Yih; Kuo, Hao-Chung; Chueh, Yu-Lun

    2015-01-01

    In this work, we demonstrated a viable experimental scheme for in-situ probing the effects of Au nanoparticles (NPs) incorporation on plasmonic energy transfer in Cu(In, Ga)Se2 (CIGS) solar cells by elaborately analyzing the lifetimes and zero moment for hot carrier relaxation with ultrabroadband femtosecond pump-probe spectroscopy. The signals of enhanced photobleach (PB) and waned photoinduced absorption (PIA) attributable to surface plasmon resonance (SPR) of Au NPs were in-situ probed in transient differential absorption spectra. The results suggested that substantial carriers can be excited from ground state to lower excitation energy levels, which can reach thermalization much faster with the existence of SPR. Thus, direct electron transfer (DET) could be implemented to enhance the photocurrent of CIGS solar cells. Furthermore, based on the extracted hot carrier lifetimes, it was confirmed that the improved electrical transport might have been resulted primarily from the reduction in the surface recombination of photoinduced carriers through enhanced local electromagnetic field (LEMF). Finally, theoretical calculation for resonant energy transfer (RET)-induced enhancement in the probability of exciting electron-hole pairs was conducted and the results agreed well with the enhanced PB peak of transient differential absorption in plasmonic CIGS film. These results indicate that plasmonic energy transfer is a viable approach to boost high-efficiency CIGS solar cells. PMID:26679958

  14. In-Situ Probing Plasmonic Energy Transfer in Cu(In, Ga)Se2 Solar Cells by Ultrabroadband Femtosecond Pump-Probe Spectroscopy

    PubMed Central

    Chen, Shih-Chen; Wu, Kaung-Hsiung; Li, Jia-Xing; Yabushita, Atsushi; Tang, Shih-Han; Luo, Chih Wei; Juang, Jenh-Yih; Kuo, Hao-Chung; Chueh, Yu-Lun

    2015-01-01

    In this work, we demonstrated a viable experimental scheme for in-situ probing the effects of Au nanoparticles (NPs) incorporation on plasmonic energy transfer in Cu(In, Ga)Se2 (CIGS) solar cells by elaborately analyzing the lifetimes and zero moment for hot carrier relaxation with ultrabroadband femtosecond pump-probe spectroscopy. The signals of enhanced photobleach (PB) and waned photoinduced absorption (PIA) attributable to surface plasmon resonance (SPR) of Au NPs were in-situ probed in transient differential absorption spectra. The results suggested that substantial carriers can be excited from ground state to lower excitation energy levels, which can reach thermalization much faster with the existence of SPR. Thus, direct electron transfer (DET) could be implemented to enhance the photocurrent of CIGS solar cells. Furthermore, based on the extracted hot carrier lifetimes, it was confirmed that the improved electrical transport might have been resulted primarily from the reduction in the surface recombination of photoinduced carriers through enhanced local electromagnetic field (LEMF). Finally, theoretical calculation for resonant energy transfer (RET)-induced enhancement in the probability of exciting electron-hole pairs was conducted and the results agreed well with the enhanced PB peak of transient differential absorption in plasmonic CIGS film. These results indicate that plasmonic energy transfer is a viable approach to boost high-efficiency CIGS solar cells. PMID:26679958

  15. A Dual-Colour Architecture for Pump-Probe Spectroscopy of Ultrafast Magnetization Dynamics in the Sub-10-femtosecond Range.

    PubMed

    Gonçalves, C S; Silva, A S; Navas, D; Miranda, M; Silva, F; Crespo, H; Schmool, D S

    2016-01-01

    Current time-resolution-limited dynamic measurements clearly show the need for improved techniques to access processes on the sub-10-femtosecond timescale. To access this regime, we have designed and constructed a state-of-the-art time-resolved magneto-optic Kerr effect apparatus, based on a new dual-color scheme, for the measurement of ultrafast demagnetization and precessional dynamics in magnetic materials. This system can operate well below the current temporal ranges reported in the literature, which typically lie in the region of around 50 fs and above. We have used a dual-colour scheme, based on ultra broadband hollow-core fibre and chirped mirror pulse compression techniques, to obtain unprecedented sub-8-fs pump and probe pulse durations at the sample plane. To demonstrate the capabilities of this system for ultrafast demagnetization and precessional dynamics studies, we have performed measurements in a ferrimagnetic GdFeCo thin film. Our study has shown that the magnetization shows a sudden drop within the first picosecond after the pump pulse, a fast recovery (remagnetization) within a few picoseconds, followed by a clear oscillation or precession during a slower magnetization recovery. Moreover, we have experimentally confirmed for the first time that a sub-10-fs pulse is able to efficiently excite a magnetic system such as GdFeCo. PMID:26976721

  16. A Dual-Colour Architecture for Pump-Probe Spectroscopy of Ultrafast Magnetization Dynamics in the Sub-10-femtosecond Range

    PubMed Central

    Gonçalves, C. S.; Silva, A. S.; Navas, D.; Miranda, M.; Silva, F.; Crespo, H.; Schmool, D. S.

    2016-01-01

    Current time-resolution-limited dynamic measurements clearly show the need for improved techniques to access processes on the sub-10-femtosecond timescale. To access this regime, we have designed and constructed a state-of-the-art time-resolved magneto-optic Kerr effect apparatus, based on a new dual-color scheme, for the measurement of ultrafast demagnetization and precessional dynamics in magnetic materials. This system can operate well below the current temporal ranges reported in the literature, which typically lie in the region of around 50 fs and above. We have used a dual-colour scheme, based on ultra broadband hollow-core fibre and chirped mirror pulse compression techniques, to obtain unprecedented sub-8-fs pump and probe pulse durations at the sample plane. To demonstrate the capabilities of this system for ultrafast demagnetization and precessional dynamics studies, we have performed measurements in a ferrimagnetic GdFeCo thin film. Our study has shown that the magnetization shows a sudden drop within the first picosecond after the pump pulse, a fast recovery (remagnetization) within a few picoseconds, followed by a clear oscillation or precession during a slower magnetization recovery. Moreover, we have experimentally confirmed for the first time that a sub-10-fs pulse is able to efficiently excite a magnetic system such as GdFeCo. PMID:26976721

  17. A Dual-Colour Architecture for Pump-Probe Spectroscopy of Ultrafast Magnetization Dynamics in the Sub-10-femtosecond Range

    NASA Astrophysics Data System (ADS)

    Gonçalves, C. S.; Silva, A. S.; Navas, D.; Miranda, M.; Silva, F.; Crespo, H.; Schmool, D. S.

    2016-03-01

    Current time-resolution-limited dynamic measurements clearly show the need for improved techniques to access processes on the sub-10-femtosecond timescale. To access this regime, we have designed and constructed a state-of-the-art time-resolved magneto-optic Kerr effect apparatus, based on a new dual-color scheme, for the measurement of ultrafast demagnetization and precessional dynamics in magnetic materials. This system can operate well below the current temporal ranges reported in the literature, which typically lie in the region of around 50 fs and above. We have used a dual-colour scheme, based on ultra broadband hollow-core fibre and chirped mirror pulse compression techniques, to obtain unprecedented sub-8-fs pump and probe pulse durations at the sample plane. To demonstrate the capabilities of this system for ultrafast demagnetization and precessional dynamics studies, we have performed measurements in a ferrimagnetic GdFeCo thin film. Our study has shown that the magnetization shows a sudden drop within the first picosecond after the pump pulse, a fast recovery (remagnetization) within a few picoseconds, followed by a clear oscillation or precession during a slower magnetization recovery. Moreover, we have experimentally confirmed for the first time that a sub-10-fs pulse is able to efficiently excite a magnetic system such as GdFeCo.

  18. Communication: State-to-state photodissociation study by the two-color VUV-VUV laser pump-probe time-slice velocity-map-imaging-photoion method

    NASA Astrophysics Data System (ADS)

    Gao, Hong; Song, Yu; Jackson, William M.; Ng, C. Y.

    2013-05-01

    We demonstrate that combining two independently tunable vacuum ultraviolet (VUV) lasers and the time-slice velocity-map-imaging-photoion (VMI-PI) method allows the rovibronically state-selected photodissociation study of CO in the VUV region along with the state-selective detection of product C(3P0,1,2) using the VUV-UV (1+1') resonance-enhanced photoionization and the VUV Rydberg autoionization methods. Both tunable VUV lasers are generated based on the two-photon resonance-enhanced four-wave mixing scheme using a pulsed rare gas jet as the nonlinear medium. The observed fine-structure distributions of product C(3PJ), J = 0, 1, and 2, are found to depend on the CO rovibronic state populated by VUV photoexcitation. The branching ratios for C(3P0) + O(3PJ): C(3P0) + O(1D2), C(3P1) + O(3PJ): C(3P1) + O(1D2), and C(3P2) + O(3PJ): C(3P2) + O(1D2), which were determined based on the time-slice VMI-PI measurements of C+ ions formed by J-state selective photoionization sampling of C(3P0,1,2), also reveal strong dependences on the spin-orbit state of C(3P0,1,2). By combining the measured branching ratios and fine-structure distributions of C(3P0,1,2), we have determined the correlated distributions of C(3P0,1,2) accompanying the formation of O(1D2) and O(3PJ) produced in the VUV photodissociation of CO. The success of this demonstration experiment shows that the VUV photodissociation pump-VUV photoionization probe method is promising for state-to-state photodissociation studies of many small molecules, which are relevant to planetary atmospheres as well as fundamental understanding of photodissociation dynamics.

  19. Communication: State-to-state photodissociation study by the two-color VUV-VUV laser pump-probe time-slice velocity-map-imaging-photoion method.

    PubMed

    Gao, Hong; Song, Yu; Jackson, William M; Ng, C Y

    2013-05-21

    We demonstrate that combining two independently tunable vacuum ultraviolet (VUV) lasers and the time-slice velocity-map-imaging-photoion (VMI-PI) method allows the rovibronically state-selected photodissociation study of CO in the VUV region along with the state-selective detection of product C((3)P(0,1,2)) using the VUV-UV (1+1') resonance-enhanced photoionization and the VUV Rydberg autoionization methods. Both tunable VUV lasers are generated based on the two-photon resonance-enhanced four-wave mixing scheme using a pulsed rare gas jet as the nonlinear medium. The observed fine-structure distributions of product C((3)P(J)), J = 0, 1, and 2, are found to depend on the CO rovibronic state populated by VUV photoexcitation. The branching ratios for C((3)P0) + O((3)P(J)): C((3)P0) + O((1)D2), C((3)P1) + O((3)P(J)): C((3)P1) + O((1)D2), and C((3)P2) + O((3)PJ): C((3)P2) + O((1)D2), which were determined based on the time-slice VMI-PI measurements of C(+) ions formed by J-state selective photoionization sampling of C((3)P(0,1,2)), also reveal strong dependences on the spin-orbit state of C((3)P(0,1,2)). By combining the measured branching ratios and fine-structure distributions of C((3)P(0,1,2)), we have determined the correlated distributions of C((3)P(0,1,2)) accompanying the formation of O((1)D2) and O((3)P(J)) produced in the VUV photodissociation of CO. The success of this demonstration experiment shows that the VUV photodissociation pump-VUV photoionization probe method is promising for state-to-state photodissociation studies of many small molecules, which are relevant to planetary atmospheres as well as fundamental understanding of photodissociation dynamics. PMID:23697402

  20. Relaxation dynamics of the LH2 complex from a photosynthetic purple bacterium Thiorhodospira sibirica studied by the near-IR femtosecond pump-probe method

    SciTech Connect

    Razjivin, A P; Pishchal'nikov, R Yu; Kozlovskii, V S; Kompanets, V O; Chekalin, Sergei V; Moskalenko, A A; Makhneva, Z K

    2005-01-31

    Photoinduced changes in the absorption spectrum of the LH2 (B800-830-850) complex from a Thiorhodospira sibirica (Trs. sibirica) bacterium are studied by the pump-probe method. The complex has the anomalous absorption spectrum exhibiting three bands in the near-IR region at 793, 826.5, and 846.5 nm. At room temperature, the excitation energy transfer from the B800, B830, and B859 bands was detected with the time constants {tau}{sub 1{approx}}0.5 ps, {tau}{sub 2{approx}}2.5 ps, and {tau}{sub 3} of the order of a few hundreds of picoseconds, respectively. A rapid energy transfer from the B830 band compared to energy transfer from the B850 band ({tau}{sub 2}||{tau}{sub 3}) suggests that all the three bands belong to the same complex (i.e., that the LH2 complex from Trs. sibirica is homogeneous). A slower energy transfer (by three - five times) from the B830 band of the LH2 complex from Trs. sibirica compared to energy transfer from the B800 band of the LH2 complexes (B800-850 and especially B800-820) from other purple bacteria suggests that the electronic structures of ensembles of bacteriochlorophyll molecules in these complexes are substantially different. (laser applications and other topics in quantum electronics)

  1. Primary charge separation in the photosystem II core from Synechocystis: a comparison of femtosecond visible/midinfrared pump-probe spectra of wild-type and two P680 mutants.

    PubMed

    Di Donato, Mariangela; Cohen, Rachel O; Diner, Bruce A; Breton, Jacques; van Grondelle, Rienk; Groot, Marie Louise

    2008-06-01

    It is now quite well accepted that charge separation in PS2 reaction centers starts predominantly from the accessory chlorophyll B(A) and not from the special pair P(680). To identify spectral signatures of B(A,) and to further clarify the process of primary charge separation, we compared the femtosecond-infrared pump-probe spectra of the wild-type (WT) PS2 core complex from the cyanobacterium Synechocystis sp. PCC 6803 with those of two mutants in which the histidine residue axially coordinated to P(B) (D2-His(197)) has been changed to Ala or Gln. By analogy with the structure of purple bacterial reaction centers, the mutated histidine is proposed to be indirectly H-bonded to the C(9)=O carbonyl of the putative primary donor B(A) through a water molecule. The constructed mutations are thus expected to perturb the vibrational properties of B(A) by modifying the hydrogen bond strength, possibly by displacing the H-bonded water molecule, and to modify the electronic properties and the charge localization of the oxidized donor P(680)(+). Analysis of steady-state light-induced Fourier transform infrared difference spectra of the WT and the D2-His(197)Ala mutant indeed shows that a modification of the axially coordinating ligand to P(B) induces a charge redistribution of P(680)(+). In addition, a comparison of the time-resolved visible/midinfrared spectra of the WT and mutants has allowed us to investigate the changes in the kinetics of primary charge separation induced by the mutations and to propose a band assignment identifying the characteristic vibrations of B(A). PMID:18326665

  2. Ultrafast Pump-Probe Experimental Studies of Heme Proteins

    NASA Astrophysics Data System (ADS)

    Wang, Wei; Demidov, Andrey; Ye, Xiong; Christian, James F.; Champion, Paul M.

    1998-03-01

    Femtosecond time-resovled spectroscopy has been applied to explore coherent dynamics of cytochrome c and myoglobin with different diatomic ligands (NO, O2, CO) using amplified 50fs laser pulses which are generated by a regenerative amplifier and optical parametric amplifier laser system at a repetition rate of 250KHz. Signals associated with ``field driven'' coherence and ``reaction driven'' coherence are studied using both single-color and two-color pump-probe schemes. The combination of the two schemes helps us to further understand electronic relaxation, ligand photodissociation and protein relaxation processes in heme proteins.

  3. Ultrafast pump-probe microscopy with high temporal dynamic range.

    PubMed

    Domke, Matthias; Rapp, Stephan; Schmidt, Michael; Huber, Heinz P

    2012-04-23

    Ultrafast pump-probe microscopy is a common method for time and space resolved imaging of short and ultra-short pulse laser ablation. The temporal delay between the ablating pump pulse and the illuminating probe pulse is tuned either by an optical delay, resulting in several hundred femtoseconds temporal resolution for delay times up to a few ns, or by an electronic delay, resulting in several nanoseconds resolution for longer delay times. In this work we combine both delay types for temporally high resolved observations of complete ablation processes ranging from femtoseconds to microseconds, while ablation is initiated by an ultrafast 660 fs laser pump pulse. For this purpose, we also demonstrate the calibration of the delay time zero point, the synchronization of both probe sources, as well as a method for image quality enhancing. In addition, we present for the first time to our knowledge pump-probe microscopy investigations of the complete substrate side selective ablation process of molybdenum films on glass. The initiation of mechanical film deformation is observed at about 400 ps, continues until approximately 15 ns, whereupon a Mo disk is sheared off free from thermal effects due to a directly induced laser lift-off ablation process. PMID:22535122

  4. Enantioselective femtosecond laser photoionization spectrometry of limonene using photoelectron circular dichroism.

    PubMed

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

    2015-04-14

    Limonene is ionized by circularly polarized 420 nm femtosecond laser pulses. Ion mass and photoelectron energy spectra identify the dominant (2 + 1) multiphoton ionization mechanism, aided by TDDFT calculations of the Rydberg excitations. Photoelectron circular dichroism measurements on pure enantiomers reveal a chiral asymmetry of ±4 %. PMID:25744283

  5. The X-ray Pump-Probe instrument at the Linac Coherent Light Source.

    PubMed

    Chollet, Matthieu; Alonso-Mori, Roberto; Cammarata, Marco; Damiani, Daniel; Defever, Jim; Delor, James T; Feng, Yiping; Glownia, James M; Langton, J Brian; Nelson, Silke; Ramsey, Kelley; Robert, Aymeric; Sikorski, Marcin; Song, Sanghoon; Stefanescu, Daniel; Srinivasan, Venkat; Zhu, Diling; Lemke, Henrik T; Fritz, David M

    2015-05-01

    The X-ray Pump-Probe instrument achieves femtosecond time-resolution with hard X-ray methods using a free-electron laser source. It covers a photon energy range of 4-24 keV. A femtosecond optical laser system is available across a broad spectrum of wavelengths for generating transient states of matter. The instrument is designed to emphasize versatility and the scientific goals encompass ultrafast physical, chemical and biological processes involved in the transformation of matter and transfer of energy at the atomic scale. PMID:25931060

  6. Improving Phase Measurement Procedures for Pump-Probe Experiments

    SciTech Connect

    Perkins, Cara P.; /Merrimack Coll. /SLAC

    2011-06-22

    Pump-probe experiments use a visible laser to excite an atom or molecule, while an X-ray pulse measures its shape. The phases and pulse times of each beam are used to calculate the object's positing at a given time - a moving picture of the chemical reaction. Currently, the fastest X-ray pulses can travel a time-length of five femtoseconds. However, present-day phase measurements can only be done as quickly as 50 femtoseconds. The purpose of this research is to explore ways in which phase-timing measurements can be improved. Three experiments are undergone to find the key factors in phase-timing. Different frequency mixers, the radio frequency (RF) components used for phase measurement, are tested for the highest sensitivity. These same mixers are then tested using two different power splitters for the lowest noise-to-sensitivity ratio. Lastly, the temperature dependency of phase is explored by testing each component at a range of temperatures to see how the phase is affected. This research demonstrated that certain mixers were more sensitive than others; on average, one mixer performed the best with a sensitivity of 0.0230 V/ps. The results also showed that same mixer combined with one splitter gave the best noise-to-sensitivity ratio overall with an average of 6.95E-04 fs/{radical}(Hz). All the components tested exhibited a temperature-dependent phase change (ranging from 1.69 to 81.6 fs/{sup o}C); the same mixer that performed at the highest sensitivity with the least noise had a significantly greater phase change than the other two. In conclusion, the experiments showed that a temperature-controlled environment is most appropriate for phase measurement. They also demonstrated that mixers are not significantly noisy and that certain types of mixers may perform better than others, which could be accounted for in their construction. The results of this research encourage further investigation into the study of different mixers and other RF components used in pump-probe

  7. Invited Review Article: Pump-probe microscopy

    NASA Astrophysics Data System (ADS)

    Fischer, Martin C.; Wilson, Jesse W.; Robles, Francisco E.; Warren, Warren S.

    2016-03-01

    Multiphoton microscopy has rapidly gained popularity in biomedical imaging and materials science because of its ability to provide three-dimensional images at high spatial and temporal resolution even in optically scattering environments. Currently the majority of commercial and home-built devices are based on two-photon fluorescence and harmonic generation contrast. These two contrast mechanisms are relatively easy to measure but can access only a limited range of endogenous targets. Recent developments in fast laser pulse generation, pulse shaping, and detection technology have made accessible a wide range of optical contrasts that utilize multiple pulses of different colors. Molecular excitation with multiple pulses offers a large number of adjustable parameters. For example, in two-pulse pump-probe microscopy, one can vary the wavelength of each excitation pulse, the detection wavelength, the timing between the excitation pulses, and the detection gating window after excitation. Such a large parameter space can provide much greater molecular specificity than existing single-color techniques and allow for structural and functional imaging without the need for exogenous dyes and labels, which might interfere with the system under study. In this review, we provide a tutorial overview, covering principles of pump-probe microscopy and experimental setup, challenges associated with signal detection and data processing, and an overview of applications.

  8. Invited Review Article: Pump-probe microscopy.

    PubMed

    Fischer, Martin C; Wilson, Jesse W; Robles, Francisco E; Warren, Warren S

    2016-03-01

    Multiphoton microscopy has rapidly gained popularity in biomedical imaging and materials science because of its ability to provide three-dimensional images at high spatial and temporal resolution even in optically scattering environments. Currently the majority of commercial and home-built devices are based on two-photon fluorescence and harmonic generation contrast. These two contrast mechanisms are relatively easy to measure but can access only a limited range of endogenous targets. Recent developments in fast laser pulse generation, pulse shaping, and detection technology have made accessible a wide range of optical contrasts that utilize multiple pulses of different colors. Molecular excitation with multiple pulses offers a large number of adjustable parameters. For example, in two-pulse pump-probe microscopy, one can vary the wavelength of each excitation pulse, the detection wavelength, the timing between the excitation pulses, and the detection gating window after excitation. Such a large parameter space can provide much greater molecular specificity than existing single-color techniques and allow for structural and functional imaging without the need for exogenous dyes and labels, which might interfere with the system under study. In this review, we provide a tutorial overview, covering principles of pump-probe microscopy and experimental setup, challenges associated with signal detection and data processing, and an overview of applications. PMID:27036751

  9. One-Photon and Two-Photon Pump-Probe Spectroscopy of Photoactive Yellow Protein

    NASA Astrophysics Data System (ADS)

    Lyngnes, O.; Gibbs, H. M.; Li, C. F.; Devanathan, S. B.; Meyer, T. E.; Tollin, G.; Cusanovich, M. A.

    We present the results of nonlinear optical pump-probe experiments on photoactive yellow protein (PYP). We are able to completely bleach the 446 nm absorption peak of PYP by one-photon excitation using a cw argon laser. We calculate the corresponding index change and find it to be similar to that of bacteriorhodopsin. We also determine an upper limit to the two photon absorption cross-section of PYP by looking for bleaching of the 446 nm absorption peak under irradiation by femtosecond pulses at 820-910 nm. No TPA signal is observed.

  10. Exciton dynamics in pentacene thin films studied by pump-probe spectroscopy

    NASA Astrophysics Data System (ADS)

    Jundt, C.; Klein, G.; Sipp, B.; Le Moigne, J.; Joucla, M.; Villaeys, A. A.

    1995-07-01

    Pentacene microcrystalline thin films have been investigated by pump-probe spectroscopy in the femtosecond regime. The competition between induced absorption in the singlet S 1 → S n and triplet T1 → T n excited electronic configurations and bleaching of the S 0 → S 1 transition has been observed. A theoretical description is proposed to explain the experimental results. The importance of the different contributions associated with the various competing processes are stressed. A very fast triplet exciton creation with rate constant 1.3 × 10 13 s -1 is attributed to a fission process from one S 1 exciton to a pair of lowest triplet T 1 excitons.

  11. Pump-Probe Noise Spectroscopy of Molecular Junctions.

    PubMed

    Ochoa, Maicol A; Selzer, Yoram; Peskin, Uri; Galperin, Michael

    2015-02-01

    The slow response of electronic components in junctions limits the direct applicability of pump-probe type spectroscopy in assessing the intramolecular dynamics. Recently the possibility of getting information on a sub-picosecond time scale from dc current measurements was proposed. We revisit the idea of picosecond resolution by pump-probe spectroscopy from dc measurements and show that any intramolecular dynamics not directly related to charge transfer in the current direction is missed by current measurements. We propose a pump-probe dc shot noise spectroscopy as a suitable alternative. Numerical examples of time-dependent and average responses of junctions are presented for generic models. PMID:26261965

  12. Theory of Floquet band formation and local pseudospin textures in pump-probe photoemission of graphene

    NASA Astrophysics Data System (ADS)

    Sentef, M. A.; Claassen, M.; Kemper, A. F.; Moritz, B.; Oka, T.; Freericks, J. K.; Devereaux, T. P.

    2015-05-01

    Ultrafast materials science promises optical control of physical properties of solids. Continuous-wave circularly polarized laser driving was predicted to induce a light-matter coupled state with an energy gap and a quantum Hall effect, coined Floquet topological insulator. Whereas the envisioned Floquet topological insulator requires high-frequency pumping to obtain well-separated Floquet bands, a follow-up question regards the creation of Floquet-like states in graphene with realistic low-frequency laser pulses. Here we predict that short optical pulses attainable in experiments can lead to local spectral gaps and novel pseudospin textures in graphene. Pump-probe photoemission spectroscopy can track these states by measuring sizeable energy gaps and Floquet band formation on femtosecond time scales. Analysing band crossings and pseudospin textures near the Dirac points, we identify new states with optically induced nontrivial changes of sublattice mixing that leads to Berry curvature corrections of electrical transport and magnetization.

  13. Femtosecond single-electron diffraction

    PubMed Central

    Lahme, S.; Kealhofer, C.; Krausz, F.; Baum, P.

    2014-01-01

    Ultrafast electron diffraction allows the tracking of atomic motion in real time, but space charge effects within dense electron packets are a problem for temporal resolution. Here, we report on time-resolved pump-probe diffraction using femtosecond single-electron pulses that are free from intra-pulse Coulomb interactions over the entire trajectory from the source to the detector. Sufficient average electron current is achieved at repetition rates of hundreds of kHz. Thermal load on the sample is avoided by minimizing the pump-probe area and by maximizing heat diffusion. Time-resolved diffraction from fibrous graphite polycrystals reveals coherent acoustic phonons in a nanometer-thick grain ensemble with a signal-to-noise level comparable to conventional multi-electron experiments. These results demonstrate the feasibility of pump-probe diffraction in the single-electron regime, where simulations indicate compressibility of the pulses down to few-femtosecond and attosecond duration. PMID:26798778

  14. Femtosecond probing of sodium cluster ion Na sub n sup + fragmentation

    SciTech Connect

    Baumert, T.; Roettgermann, C.; Rothenfusser, C.; Thalweiser, R.; Weiss, V.; Gerber, G. )

    1992-09-07

    We report on the first femtosecond time-resolved experiments in cluster physics. The photofragmentation dynamics of small sodium cluster ions Na{sub {ital n}}{sup +} have been studied with pump-probe techniques. Ultrashort laser pulses of 60-fs duration are employed to photoionize the sodium clusters and to probe the photofragments. We find that the ejection of neutral dimer Na{sub 2} and, observed for the first time, neutral trimer Na{sub 3} photofragments occur on ultrashort time scales of 2.5 and 0.4 ps, respectively. This and the absence of cluster heating reveals that direct photoinduced fragmentation processes are important at short times rather than the statistical unimolecular decay.

  15. Time- and frequency-resolved photoionization of the C (2)A(2) state of the benzyl radical, C(7)H(7).

    PubMed

    Margraf, Markus; Noller, Bastian; Schröter, Christian; Schultz, Thomas; Fischer, Ingo

    2010-08-21

    The structure and dynamics of the C (2)A(2) electronically excited state of the benzyl radical, C(7)H(7), were investigated by nanosecond and femtosecond pump-probe photoionization. A free jet of benzyl radicals was generated by flash pyrolysis from the precursors 2-phenylethyl nitrite and toluene. Nanosecond multiphoton ionization spectra show a number of vibronic bands that are excited in the wavelength range of 290-310 nm. At excitation wavelengths of 305, 301, and 298 nm, rapid biexponential decay of the excited states was observed. Lifetimes at the C-state origin (305 nm excitation) are 400 fs and 4.5 ps. The lifetimes decrease with increasing excitation energy. The dynamics can be understood within a two-step internal conversion to the electronic ground state. PMID:20726639

  16. Transmission pump-probe spectroscopy on multilayer black phosphorus

    NASA Astrophysics Data System (ADS)

    Suess, Ryan J.; Jadidi, Mohammad M.; Murphy, Thomas E.; Mittendorff, Martin

    Black phosphorus is a two-dimensional material that has recently attracted interest due to its high mobility and direct bandgap. In this work we examine the pump-induced change in optical transmission of mechanically exfoliated black phosphorus flakes using a two-color optical pump-probe measurement. The time-resolved data reveal a fast pump-induced transparency accompanied by a slower absorption that we attribute to Pauli blocking and free-carrier absorption, respectively. Polarization studies show that these effects are also highly anisotropic - underscoring the importance of crystal orientation in the design of optical devices based on this material. Ongoing work suggests that exploring the carrier density dependence of the pump-probe signals, which can be accessed experimentally via electrostatic gating, may allow for improved understanding of the optical response and carrier dynamics in the material. Supported by NSF and ONR-MURI.

  17. Phasor analysis for nonlinear pump-probe microscopy

    PubMed Central

    Robles, Francisco E.; Wilson, Jesse W.; Fischer, Martin C.; Warren, Warren S.

    2012-01-01

    Pump-probe microscopy provides molecular information by probing transient, excited state dynamic properties of pigmented samples. Analysis of the transient response is typically conducted using principal component analysis or multi-exponential fitting, however these methods are not always practical or feasible. Here, we show an adaptation of phasor analysis to provide an intuitive, robust, and efficient method for analyzing and displaying pump-probe images, thereby alleviating some of the challenges associated with differentiating multiple pigments. A theoretical treatment is given to understand how the complex transient signals map onto the phasor plot. Analyses of cutaneous and ocular pigmented tissue samples, as well as historical pigments in art demonstrate the utility of this approach.

  18. High-Precision Time Delay Control with Continuous Phase Shifter for Pump-Probe Experiments Using Synchrotron Radiation Pulses

    SciTech Connect

    Tanaka, Yoshihito; Ohshima, Takashi; Moritomo, Yutaka; Tanaka, Hitoshi; Takata, Masaki

    2010-06-23

    Brilliant pulsed x-ray synchrotron radiation (SR) is useful for pump-probe experiment such as time-resolved x-ray diffraction, x-ray absorption fine structure, and x-ray spectroscopy. For laser pump-SR x-ray probe experiments, short pulsed lasers are generally synchronized to the SR master oscillator controlling the voltage for acceleration of electron bunches in an accelerator, and the interval between the laser and the SR pulses is changed around the time scale of target phenomenon. Ideal delay control produces any time delay as keeping the time-precision and pointing-stability of optical pulses at a sample position. We constructed the time delay control module using a continuous phase shifter of radio frequency signal and a frequency divider, which can produce the delayed trigger pulses to the laser without degradation of the time precision and the pointing stability. A picoseconds time-resolved x-ray diffraction experiment was demonstrated at SPring-8 storage ring for fast lattice response by femtosecond pulsed laser irradiation, and suggested the possibility of accurate sound velocity measurement. A delay control unit operating with subpicosecond precision has also been designed for femtosecond pump-probe experiments using a free electron laser at SPring-8 campus.

  19. Coherence specific signal detection via chiral pump-probe spectroscopy.

    PubMed

    Holdaway, David I H; Collini, Elisabetta; Olaya-Castro, Alexandra

    2016-05-21

    We examine transient circular dichroism (TRCD) spectroscopy as a technique to investigate signatures of exciton coherence dynamics under the influence of structured vibrational environments. We consider a pump-probe configuration with a linearly polarized pump and a circularly polarized probe, with a variable angle θ between the two directions of propagation. In our theoretical formalism the signal is decomposed in chiral and achiral doorway and window functions. Using this formalism, we show that the chiral doorway component, which beats during the population time, can be isolated by comparing signals with different values of θ. As in the majority of time-resolved pump-probe spectroscopy, the overall TRCD response shows signatures of both excited and ground state dynamics. However, we demonstrate that the chiral doorway function has only a weak ground state contribution, which can generally be neglected if an impulsive pump pulse is used. These findings suggest that the pump-probe configuration of optical TRCD in the impulsive limit has the potential to unambiguously probe quantum coherence beating in the excited state. We present numerical results for theoretical signals in an example dimer system. PMID:27208941

  20. Time resolved EUV pump-probe microscopy of fs-LASER induced nanostructure formation

    NASA Astrophysics Data System (ADS)

    Freiberger, R.; Hauck, J.; Reininghaus, M.; Wortmann, D.; Juschkin, L.

    2011-05-01

    We report on our efforts in design and construction of a compact Extreme Ultraviolet (EUV)-pump-probe microscope. The goal is the observation of formation of nanostructures, induced by a femtosecond (fs)-laser pulse. The unique interaction processes of fs-laser radiation with matter open up new markets in laser material processing and, therefore, are actively investigated in the last decade. The resulting "sub 100 nm"-structures offer vast potential benefits in photonics, biotechnology, tribological surface design, plasmonic applications and production of nanoparticles. Focused fs-laser radiation causes a local modification resulting in nanostructures of high precision and reproducibility. However the formation dynamics is not well understood. Research in this field requires high temporal and spatial resolution. A combination of fs-laser and EUV-microscope provides a tool for "in situ"-observation of the formation dynamics. As exemplary structures to be investigated, we use nanojets on thin gold films and periodic surface structures (ripples) on dielectrics. In the future, the EUV-pump-probe microscope can become a versatile tool to observe physical or biological processes. Microscopy using EUV-light is capable of detecting structures on a scale down to several tens of nanometers. For detailed investigations a compact EUV-microscope has been realized utilizing OVI Balmer-alpha radiation at 17.3 nm coming from a discharge produced oxygen plasma. As optical elements a grazing incidence elliptical collector and a zone plate with a width of outermost zone of 50 nm and a spectral filter to avoid chromatic aberrations are used. The detector is a fast gated microchannel plate with a pore size of 2 microns contacted by a low impedance transmission line. The expected spatial resolution of the setup is better than 100 nm and the time resolution is better than 1 ns. The newly developed EUV-microscope is a powerful tool for a wide field of investigations that need high time

  1. Femtosecond dynamics of exciton bleaching in bulk GaN at room temperature

    NASA Astrophysics Data System (ADS)

    Huang, Yin-Chieh; Chern, Gia-Wei; Lin, Kung-Hsuan; Liang, Jian-Chin; Sun, Chi-Kuang; Hsu, Chia-Chen; Keller, Stacia; DenBaars, Steven P.

    2002-07-01

    Femtosecond transient transmission pump-probe technique was used to investigate exciton dynamics in a nominally undoped GaN thin film at room temperature. An exciton ionization time of 100-250 femtoseconds was observed by the time-resolved pump-probe measurement. A comparison experiment with pre-excited free carriers also confirmed the observation of the exciton ionization process in bulk GaN.

  2. Femtosecond carrier dynamics and modelocking in monolithic CPM lasers

    SciTech Connect

    Brorson, S.D.; Moerk, J.; Moeller-Larsen, A.; Nielsen, J.M.; Bischoff, S.

    1996-10-01

    Femtosecond pump-probe measurements of the dynamics in both forward- and reverse-biased semiconductor optical waveguides are presented. Slow (nanosecond) as well as ultrafast (femtosecond) dynamics are observed in both kinds of structures. These measurements imply that the slow saturable absorber theory of modelocking in monolithic CPM devices is incomplete.

  3. Pump-probe study of atoms and small molecules with laser driven high order harmonics

    NASA Astrophysics Data System (ADS)

    Cao, Wei

    A commercially available modern laser can emit over 1015 photons within a time window of a few tens of femtoseconds (10-15second), which can be focused into a spot size of about 10 mum, resulting in a peak intensity above 1014W/cm2. This paves the way for table-top strong field physics studies such as above threshold ionization (ATI), non-sequential double ionization (NSDI), high order harmonic generation (HHG), etc.. Among these strong laser-matter interactions, high order harmonic generation, which combines many photons of the fundamental laser field into a single photon, offers a unique way to generate light sources in the vacuum ultraviolet (VUV) or extreme ultraviolet (EUV) region. High order harmonic photons are emitted within a short time window from a few tens of femtoseconds down to a few hundreds of attoseconds (10 -18second). This highly coherent nature of HHG allows it to be synchronized with an infrared (IR) laser pulse, and the pump-probe technique can be adopted to study ultrafast dynamic processes in a quantum system. The major work of this thesis is to develop a table-top VUV(EUV) light source based on HHG, and use it to study dynamic processes in atoms and small molecules with the VUV(EUV)-pump IR-probe method. A Cold Target Recoil Ion Momentum Spectroscopy (COLTRIMS) apparatus is used for momentum imaging of the interaction products. Two types of high harmonic pump pulses are generated and applied for pump-probe studies. The first one consists of several harmonics forming a short attosecond pulse train (APT) in the EUV regime (around 40 eV). We demonstrate that, (1) the auto-ionization process triggered by the EUV in cation carbon-monoxide and oxygen molecules can be modified by scanning the EUV-IR delay, (2) the phase information of quantum trajectories in bifurcated high harmonics can be extracted by performing an EUV-IR cross-correlation experiment, thus disclosing the macroscopic quantum control in HHG. The second type of high harmonic source

  4. Photoacoustic imaging of fluorophores using pump-probe excitation

    PubMed Central

    Märk, Julia; Schmitt, Franz-Josef; Theiss, Christoph; Dortay, Hakan; Friedrich, Thomas; Laufer, Jan

    2015-01-01

    A pump-probe technique for the detection of fluorophores in tomographic PA images is introduced. It is based on inducing stimulated emission in fluorescent molecules, which in turn modulates the amount of thermalized energy, and hence the PA signal amplitude. A theoretical model of the PA signal generation in fluorophores is presented and experimentally validated on cuvette measurements made in solutions of Rhodamine 6G, a fluorophore of known optical and molecular properties. The application of this technique to deep tissue tomographic PA imaging is demonstrated by determining the spatial distribution of a near-infrared fluorophore in a tissue phantom. PMID:26203378

  5. Pump probe spectroscopy of quasiparticle dynamics in cuprate superconductors

    SciTech Connect

    Segre, Gino P.

    2001-05-01

    Pump probe spectroscopy is used to examine the picosecond response of a BSCCO thin film, and two YBCO crystals in the near infrared. The role of pump fluence and temperature have been closely examined in an effort to clarify the mechanism by which the quasiparticles rejoin the condensate. BSCCO results suggest that the recombination behavior is consistent with the d-wave density of states in that quasiparticles appear to relax to the nodes immediately before they rejoin the condensate. The first substantial investigation of polarized pump probe response in detwinned YBCO crystals is also reported. Dramatic doping dependent anisotropies along the a and b axes are observed in time and temperature resolved studies. Among many results, we highlight the discovery of an anomalous temperature and time dependence of a- axis response in optimally doped YBCO. We also report on the first observation of the photoinduced response in a magnetic field. We find the amplitude of the response, and in some cases, the dynamics considerably changed with the application of a 6T field. Finally, we speculate on two of the many theoretical directions stimulated by our results. We find that the two-fluid model suggests a mechanism to explain how changes at very low energies are visible to a high-energy probe. Also discussed are basic recombination processes which may play a role in the observed decay.

  6. Optical afterburner for an x-ray free electron laser as a tool for pump-probe experiments

    NASA Astrophysics Data System (ADS)

    Saldin, E. L.; Schneidmiller, E. A.; Yurkov, M. V.

    2010-03-01

    We propose a new scheme for two-color operation of an x-ray self-amplified spontaneous emission free electron laser (SASE FEL). The scheme is based on an intrinsic feature of such a device: chaotic modulations of electron beam energy and energy spread on the scale of FEL coherence length are converted into large density modulations on the same scale with the help of a dispersion section, installed behind the x-ray undulator. Powerful radiation is then generated with the help of a dedicated radiator (like an undulator that selects a narrow spectral line), or one can simply use, for instance, broadband edge radiation. A typical radiation wavelength can be as short as a FEL coherence length, and can be redshifted by increasing the dispersion section strength. In practice it means the wavelength ranges from vacuum ultraviolet to infrared. The long-wavelength radiation pulse is naturally synchronized with the x-ray pulse and can be either directly used in pump-probe experiments or cross correlated with a high-power pulse from a conventional laser system. In this way experimenters overcome jitter problems and can perform pump-probe experiments with femtosecond resolution. Additional possibilities like on-line monitoring of x-ray pulse duration (making “optical replica” of an x-ray pulse) are also discussed in the paper. The proposed scheme is very simple, cheap, and robust, and therefore can be easily realized in facilities like FLASH, European XFEL, LCLS, and SCSS.

  7. Non-degenerate pump-probe spectroscopy of single GaN nanowires

    SciTech Connect

    Upadhya, Prashanth C; Taylor, Antoinette J; Prasankumar, Rohiy P; Wang, George T; Martinez, Julio A; Li, Qiming; Swartzentruber, Brian S

    2010-01-01

    Spatially-resolved ultrafast transient absorption measurements on a single GaN nanowire give insight into carrier relaxation dynamics as a function of the probe polarization and position on the nanowire on a femtosecond timescale. The synthesis and optical characterization of semiconductor nanowires (NWs) has gained considerable attention in recent years owing to their unique electronic and optical properties that arise from their anisotropic geometry, large surface to volume ratio and two-dimensional quasiparticle confinement, Post-growth characterization of their properties is crucial in understanding the fundamental physical processes that can lead to enhanced functionality of NW-based devices, In particular, it is important to understand the carrier relaxation pathways in individual NWs, since the geometry of these nanostructures can significantly influence carrier recombination and/or trapping. In this respect, ultrafast optical techniques offer reliable and non-contact spectroscopic tools to study carrier dynamics in semiconductor nanostructures. In summary, time-resolved optical pump-probe spectroscopy was performed on single GaN NWs. These measurements give insight into the different processes that govern carrier capture, particularly at surface states, and relaxation in individual nanostructures. Our experiments thus demonstrate the value of single-particle ultrafast optical spectroscopy in understanding the physical processes that govern the properties of semiconductor NWs, while suggesting approaches to optimize NW-based devices for nanophotonic applications.

  8. Synchronized pulses generated at 20 eV and 90 eV for attosecond pump-probe experiments

    NASA Astrophysics Data System (ADS)

    Fabris, D.; Witting, T.; Okell, W. A.; Walke, D. J.; Matia-Hernando, P.; Henkel, J.; Barillot, T. R.; Lein, M.; Marangos, J. P.; Tisch, J. W. G.

    2015-06-01

    The development of attosecond pulses across different photon energies is an essential precursor to performing pump-probe attosecond experiments in complex systems, where the potential of attosecond science can be further developed. We report the generation and characterization of synchronized extreme ultraviolet (90 eV) and vacuum ultraviolet (20 eV) pulses, generated simultaneously via high-harmonic generation. The vacuum ultraviolet pulses are well suited for pump-probe experiments that exploit the high photo-ionization cross-sections of many molecules in this spectral region as well as the higher photon flux due to the higher conversion efficiency of the high harmonic generation process at these energies. We temporally characterized all pulses using the attosecond streaking technique and the FROG-CRAB retrieval method. We report 576 ± 16 as pulses at 20 eV and 257 ± 21 as pulses at 90 eV. Our demonstration of synchronized attosecond pulses at different photon energies, which are inherently jitter-free due to the common-path geometry implemented, offers unprecedented possibilities for pump-probe studies.

  9. Excited state dynamics of metastable phthalocyanine-tetrasulfonate tetra-anions probed by pump/probe photoelectron spectroscopy

    SciTech Connect

    Ehrler, Oli T.; Yang Jiping; Sugiharto, Albert B.; Unterreiner, Andreas N.; Kappes, Manfred M.

    2007-11-14

    Femtosecond time-resolved pump-probe photoelectron spectroscopy was used to study elementary relaxation processes occurring in isolated phthalocyanine-tetrasulfonate tetra-anions ([MPc(SO{sub 3}){sub 4}]{sup 4-}, M=Cu,Ni, and ''free-base'' [H{sub 2}Pc(SO{sub 3}){sub 4}]{sup 4-}) following Q band excitation by one-photon absorption at 775 nm. Whereas the Cu and Ni systems decay rapidly by means of internal conversion without electron loss, the free-base phthalocyanine primarily undergoes excited state tunneling electron emission. This reflects less efficient coupling to lower lying states within the corresponding spin manifold. Results are interpreted in terms of (time-dependent) density functional theory calculations of ground and electronically excited states and kinetically modeled to yield the associated rates.

  10. Broadband pump-probe spectroscopy at 20-MHz modulation frequency.

    PubMed

    Preda, Fabrizio; Kumar, Vikas; Crisafi, Francesco; Figueroa Del Valle, Diana Gisell; Cerullo, Giulio; Polli, Dario

    2016-07-01

    We introduce an innovative high-sensitivity broadband pump-probe spectroscopy system, based on Fourier-transform detection, operating at 20-MHz modulation frequency. A common-mode interferometer employing birefringent wedges creates two phase-locked delayed replicas of the broadband probe pulse, interfering at a single photodetector. A single-channel lock-in amplifier demodulates the interferogram, whose Fourier transform provides the differential transmission spectrum. Our approach combines broad spectral coverage with high sensitivity, due to high-frequency modulation and detection. We demonstrate its performances by measuring two-dimensional differential transmission maps of a carbon nanotubes sample, simultaneously acquiring the signal over the entire 950-1350 nm range with 2.7·10-6  rms noise over 1.5 s integration time. PMID:27367078

  11. Quantum Dynamics Simulations for Modeling Experimental Pump-Probe Measurements

    NASA Astrophysics Data System (ADS)

    Pearson, Brett; Nayyar, Sahil; Liss, Kyle; Weinacht, Thomas

    2016-05-01

    Time-resolved studies of quantum dynamics have benefited greatly from developments in ultrafast table-top and free electron lasers. Advances in computer software and hardware have lowered the barrier for performing calculations such that relatively simple simulations allow for direct comparison with experimental results. We describe here a set of quantum dynamics calculations in low-dimensional molecular systems. The calculations incorporate coupled electronic-nuclear dynamics, including two interactions with an applied field and nuclear wave packet propagation. The simulations were written and carried out by undergraduates as part of a senior research project, with the specific goal of allowing for detailed interpretation of experimental pump-probe data (in additional to the pedagogical value).

  12. Probing calculated O2+ potential-energy curves with an XUV-IR pump-probe experiment

    NASA Astrophysics Data System (ADS)

    Cörlin, Philipp; Fischer, Andreas; Schönwald, Michael; Sperl, Alexander; Mizuno, Tomoya; Thumm, Uwe; Pfeifer, Thomas; Moshammer, Robert

    2015-04-01

    We study dissociative photoionization of molecular oxygen in a kinematically complete XUV-IR pump-probe experiment. Detecting charged fragments and photoelectrons in coincidence using a reaction microscope, we observe a pump-probe delay-dependent yield of very low energetic O+ ions which oscillates with a period of 40 fs . This feature is caused by a time-dependent vibrational wave packet in the potential of the binding O2+(a Π4u) state, which is probed by resonant absorption of a single infrared photon to the weakly repulsive O2+(f Π4g) state. By quantitative comparison of the experimental kinetic-energy-release (KER) and quantum-beat (QB) spectra with the results of a coupled-channel simulation, we are able to discriminate between the calculated adiabatic O2+ potential-energy curves (PECs) of Marian et al. [Marian, Marian, Peyerimhoff, Hess, Buenker, and Seger, Mol. Phys. 46, 779 (1982), 10.1080/00268978200101591] and Magrakvelidze et al. [Magrakvelidze, Aikens, and Thumm, Phys. Rev. A 86, 023402 (2012), 10.1103/PhysRevA.86.023402]. In general, we find a good agreement between experimental and simulated KER and QB spectra. However, we could not reproduce all features of the experimental data with these PECs. In contrast, adjusting a Morse potential to the experimental data, most features of the experimental spectra are well reproduced by our simulation. By comparing this Morse potential to theoretically predicted PECs, we demonstrate the sensitivity of our experimental method to small changes in the shape of the binding potential.

  13. Time-resolved pump-probe experiments at the LCLS

    SciTech Connect

    Glownia, James; Cryan, J.; Andreasson, J.; Belkacem, A.; Berrah, N.; Blaga, C.L.; Bostedt, C.; Bozek, J.; DiMauro, L.F.; Fang, L.; Frisch, J.; Gessner, O.; Guhr, M.; Hajdu, J.; Hertlein, M.P.; Hoener, M.; Huang, G.; Kornilov, O.; Marangos, J.P.; March, A.M.; McFarland, B.K.; /SLAC /Stanford U., Phys. Dept. /SLAC /IRAMIS, Saclay /Stanford U., Phys. Dept. /Georgia Tech /Argonne /Kansas State U. /SLAC /Stanford U., Phys. Dept. /SLAC /Stanford U., Appl. Phys. Dept. /Stanford U., Appl. Phys. Dept. /SLAC /LBNL /Argonne /SLAC /SLAC /Stanford U., Appl. Phys. Dept. /Stanford U., Phys. Dept.

    2011-08-12

    The first time-resolved x-ray/optical pump-probe experiments at the SLAC Linac Coherent Light Source (LCLS) used a combination of feedback methods and post-analysis binning techniques to synchronize an ultrafast optical laser to the linac-based x-ray laser. Transient molecular nitrogen alignment revival features were resolved in time-dependent x-ray-induced fragmentation spectra. These alignment features were used to find the temporal overlap of the pump and probe pulses. The strong-field dissociation of x-ray generated quasi-bound molecular dications was used to establish the residual timing jitter. This analysis shows that the relative arrival time of the Ti:Sapphire laser and the x-ray pulses had a distribution with a standard deviation of approximately 120 fs. The largest contribution to the jitter noise spectrum was the locking of the laser oscillator to the reference RF of the accelerator, which suggests that simple technical improvements could reduce the jitter to better than 50 fs.

  14. Pump-probe Kelvin-probe force microscopy: Principle of operation and resolution limits

    SciTech Connect

    Murawski, J.; Graupner, T.; Milde, P. Raupach, R.; Zerweck-Trogisch, U.; Eng, L. M.

    2015-10-21

    Knowledge on surface potential dynamics is crucial for understanding the performance of modern-type nanoscale devices. We describe an electrical pump-probe approach in Kelvin-probe force microscopy that enables a quantitative measurement of dynamic surface potentials at nanosecond-time and nanometer-length scales. Also, we investigate the performance of pump-probe Kelvin-probe force microscopy with respect to the relevant experimental parameters. We exemplify a measurement on an organic field effect transistor that verifies the undisturbed functionality of our pump-probe approach in terms of simultaneous and quantitative mapping of topographic and electronic information at a high lateral and temporal resolution.

  15. Chemical-contrast imaging with pulse-shaping based pump-probe spectroscopy

    NASA Astrophysics Data System (ADS)

    Flynn, Daniel C.; Bhagwat, Amar R.; Ogilvie, Jennifer P.

    2013-02-01

    Ultrafast pump-probe spectroscopy and pulse-shaping techniques are providing new modes of contrast for the field of multiphoton microscopy. Endogenous species such as heme proteins show rich nonlinear spectroscopic signatures of excited state absorption, stimulated emission and ground-state bleaching. Commercially available octave-spanning Ti:sapphire oscillators offer new opportunities for imaging based on pump-probe contrast. Spatial light modulators take advantage of this large bandwidth, shaping pulses of light to selectively excite molecular structures with similar spectral properties. We present two-color pump-probe imaging of heme proteins solutions and red blood cells.

  16. Ultrafast pump-probe dynamics of iron oxide based earth pigments for applications to ancient pottery manufacture

    NASA Astrophysics Data System (ADS)

    Villafana, Tana E.; Brown, William; Warren, Warren S.; Fischer, Martin

    2015-06-01

    We demonstrate that ultrafast pump-probe microscopy provides unique dynamics for natural iron oxide and iron hydroxide earth pigments, despite their chemical similarity. First, we conducted a pump-probe spectroscopy study on heat-treated hematite (the pure red iron oxide mineral) and found the pump-probe dynamics to be temperature dependent. Second, we investigated pottery fired under known conditions and observed firing dependent pump-probe dynamics. Finally, we imaged a New World potshard from the North Carolina Museum of Art. Our results indicate that pump-probe microscopy could be a useful tool in elucidating pottery manufacture.

  17. Exciton dynamics in pentacene and tetracene studied using optical pump-probe spectroscopy

    NASA Astrophysics Data System (ADS)

    Thorsmølle, V. K.; Averitt, R. D.; Demsar, J.; Chi, X.; Smith, D. L.; Ramirez, A. P.; Taylor, A. J.

    We present room temperature photoinduced reflection and transmission measurements in pentacene and tetracene single crystals using optical pump-probe spectroscopy. Singlet exciton recombination, singlet-triplet fission, excited singlet, and triplet state absorption is observed.

  18. Exciton dynamics in pentacene and tetracene studied using optical pump-probe spectroscopy

    SciTech Connect

    Thorsmølle, V. K.; Averitt, R. D.; Demsar, J.; Chi, X.; Smith, D. L.; Ramirez, A. P.; Taylor, Antoinette J.,

    2004-01-01

    We present room temperature photoinduced reflection and transmission measurements in pentacene and tetracene single crystals using optical pump-probe spectroscopy. Singlet exciton recombination, singlet-triplet fission, excited singlet, and triplet state absorption is observed.

  19. Rubidium pump-probe spectroscopy: Comparison between ab initio theory and experiment

    SciTech Connect

    Himsworth, M.; Freegarde, T.

    2010-02-15

    We present a simple, analytic model for pump-probe spectroscopy in dilute atomic gases. Our model treats multilevel atoms, takes several broadening mechanisms into account and, with no free parameters, shows excellent agreement with experimentally observed spectra.

  20. Femtosecond pump-probe measurements of solvation by hydrogen-bonding interactions.

    PubMed

    Pines, Ehud; Pines, Dina; Ma, Ying-Zhong; Fleming, Graham R

    2004-09-20

    An additional ultrafast blue shift in the transient absorption spectra of hydrogen-bonding complexes of a strong photoacid, 8-hydroxypyrene 1,3,6-trisdimethylsulfonamide (HPTA), over the solvation response of the uncomplexed HPTA and also over that of the methoxy derivative of the photoacid (MPTA) in the presence of the hydrogen-bonding base was observed on optical excitation of the photoacid. The additional 55 +/- 10 fs solvation response was found to be about 35 % and 19% of the total C(t) of HPTA in dichloromethane (DCM) when it was hydrogen-bonded to dimethylsulfoxide (DMSO) and dioxane, respectively, and about 29% of the total C(t) of HPTA in dichloroethane (DCE) when it was hydrogen-bonded to DMSO. We have assigned this additional dynamic spectral shift to a transient change in the hydrogen bond (O-H...O) that links HPTA to the complexing base, after the electronic excitation of the photoacid. PMID:15499848

  1. Probing calculated O 2 + potential curves with an XUV-IR pump-probe experiment

    NASA Astrophysics Data System (ADS)

    Coerlin, Philipp; Fischer, Andreas; Schoenwald, Michael; Sperl, Alexander; Mizuno, Tomoya; Pfeifer, Thomas; Moshammer, Robert; Thumm, Uwe

    2015-05-01

    We study dissociative photo-ionization of O2 in a kinematically complete XUV-IR pump-probe experiment, preparing a vibrational wave packet in the potential of the binding O2+(a4Πu)state by ionization with a single XUV photon. After a variable time-delay the wave packet is promoted to the repulsive O2+(f4Πg)state by a weak IR probe pulse. Comparing the results of a coupled-channel simulation with the experimental kinetic-energy-release and quantum-beat spectra, we are able to discriminate between the adiabatic O2+potential-energy curves (PECs) calculated by. The overall agreement between simulated and experimental results is good; however, not all features of the experimental spectra could be reproduced using these PECs. Using a Morse potential adjusted to the experimental data instead, most features of the experimental spectra are well reproduced by our simulation. This optimized Morse potential is remarkably similar to the theoretically predicted PECs, demonstrating the sensitivity of our experimental method to small changes in the shape of the binding potential. Supported by the DoE, NSF, and Alexander von Humboldt foundation.

  2. In vivo pump-probe microscopy of melanoma and pigmented lesions

    NASA Astrophysics Data System (ADS)

    Wilson, Jesse W.; Degan, Simone; Mitropoulos, Tanya; Selim, M. Angelica; Zhang, Jennifer Y.; Warren, Warren S.

    2012-03-01

    A growing number of dermatologists and pathologists are concerned that the rapidly rising incidence of melanoma reflects not a true 'epidemic' but an increasing tendency to overdiagnose pigmented lesions. Addressing this problem requires both a better understanding of early-stage melanoma and new diagnostic criteria based on more than just cellular morphology and architecture. Here we present a method for in-vivo optical microscopy that utilizes pump-probe spectroscopy to image the distribution of the two forms of melanin in skin: eumelanin and pheomelanin. Images are acquired in a scanning microscope with a sensitive modulation transfer technique by analyzing back-scattered probe light with a lock-in amplifier. Early-stage melanoma is studied in a human skin xenografted mouse model. Individual melanocytes have been observed, in addition to pigmented keratinocytes. Combining the pump-probe images simultaneously with other noninvasive laser microscopy methods (confocal reflectance, multiphoton autofluorescence, and second harmonic generation) allows visualization of the skin architecture, framing the functional pump-probe image in the context of the surrounding tissue morphology. It is found that pump-probe images of melanin can be acquired with low peak intensities, enabling wide field-of-view pigmentation surveys. Finally, we investigate the diagnostic potential of the additional chemical information available from pump-probe microscopy.

  3. Magnetization precession of magnetic thin films studied by all optical pump-probe technique

    NASA Astrophysics Data System (ADS)

    Michalski, Steven A.

    The study of magnetization dynamics such as magnetization precession and precessional damping provides insights into the behavior of complex magnetic systems, and indeed may lead to a better understanding of the fundamental limits of magnetic reversal process. In this work, a time-resolved magneto-optic Kerr effect system (TRMOKE) was developed to study magnetization dynamics: Precession and damping. The system uses a femtosecond laser in a pump-probe experiment with direct optical excitation, very similar to the method introduced by Ganping Ju and coworkers. Also, a model based on the Landau-Lifshitz-Gilbert equation (LLG) was developed and used to interpret and analyze the experimental magnetization precession data of a single magnetic layer. The model can be used to predict the precession frequencies with and without damping, the eigenvectors of the magnetization and allows the Gilbert damping parameter (alpha) to be determined. The model is extended to a system of two magnetic layers coupled through a nonmagnetic spacer layer. The capabilities of the TRMOKE system and the LLG models, were demonstrated by studying the magnetization dynamics of Ni/Pt bilayers. Static and dynamic magnetic properties of exchange-coupled magnetic layers have been investigated by magneto-optical measurements. The samples are [Pt/Co] multilayers with perpendicular magnetic anisotropy (PMA) exchange-coupled to a Co layer with in-plane magnetic anisotropy. The exchange is indirect, realized and tuned by an intervening Pt layer of varying thickness. Both the strength and the angle of an external applied magnetic field were varied and for many samples, two modes with two distinct precession frequencies were observed in the precession measurements. The frequencies of both modes depend on the strength and the angle of the applied magnetic field. The LLG model predicts two precessional modes ("acoustic" and "optic") whose behaviors depend on the strength and sign of the exchange coupling

  4. A versatile and reconfigurable setup for all-terahertz time-resolved pump-probe spectroscopy

    NASA Astrophysics Data System (ADS)

    Elezzabi, A. Y.; Maraghechi, P.

    2012-05-01

    A versatile optical setup for all-terahertz (THz) time resolved pump-probe spectroscopy was designed and tested. By utilizing a dual THz pulse generator emitter module, independent and synchronized THz radiation pump and probe pulses were produced, thus eliminating the need for THz beam splitters and the limitations associated with their implementation. The current THz setup allows for precise control of the electric fields splitting ratio between the THz radiation pump and probe pulses, as well as in-phase, out-of-phase, and polarization dependent pump-probe spectroscopy. Since the present THz pump-probe setup does not require specialized THz radiation optical components, such as phase shifters, polarization rotators, or wide bandwidth beam splitters, it can be easily implemented with minimal alterations to a conventional THz time domain spectroscopy system. The present setup is valuable for studying the time dynamics of THz coherent phenomena in solid-state, chemical, and biological systems.

  5. Ultrafast pump-probe microscopy reveals the mechanism of selective fs laser structuring of transparent thin films for maskless micropatterning

    NASA Astrophysics Data System (ADS)

    Rapp, Stephan; Rosenberger, Janosch; Domke, Matthias; Heise, Gerhard; Huber, Heinz P.; Schmidt, Michael

    2014-01-01

    Maskless patterning of biocompatible Ta2O5/Pt/glass sensor chips can be realized by ultra-short laser pulse ablation. At a fluence of 0.2 J/cm2, the thin Ta2O5 film is selectively lifted-off by indirectly-induced ablation at laser wavelenghts where the Ta2O5 is transparent and the Pt absorbing. This enables precise and very fast structuring. Here, 660 fs laser pulses at a center wavelength of 1053 nm are applied. The driving physical effects of this ablation mechanism are revealed by pump-probe microscopy. This technique allows the observation of the whole ablation process ranging temporally from femtoseconds to microseconds. An ultrafast heat-expansion in the absorbing Pt, initiating a shock-wave to the Ta2O5 within the first 10 ps, bulges the Ta2O5 film after some nanoseconds. Bulging velocities of 750 m/s are determined corresponding to an extreme acceleration of about 1010 g. Exceeding the stress limit in the Ta2O5 causes film disintegration after 50 ns. A model, describing essential reaction steps, is developed. This model is also applicable to other industrial important layer systems, where thin transparent films have to be removed.

  6. A photoelectron-photoion coincidence imaging apparatus for femtosecond time-resolved molecular dynamics with electron time-of-flight resolution of {sigma}=18 ps and energy resolution {delta}E/E=3.5%

    SciTech Connect

    Vredenborg, Arno; Roeterdink, Wim G.; Janssen, Maurice H. M.

    2008-06-15

    We report on the construction and performance of a novel photoelectron-photoion coincidence machine in our laboratory in Amsterdam to measure the full three-dimensional momentum distribution of correlated electrons and ions in femtosecond time-resolved molecular beam experiments. We implemented sets of open electron and ion lenses to time stretch and velocity map the charged particles. Time switched voltages are operated on the particle lenses to enable optimal electric field strengths for velocity map focusing conditions of electrons and ions separately. The position and time sensitive detectors employ microchannel plates (MCPs) in front of delay line detectors. A special effort was made to obtain the time-of-flight (TOF) of the electrons at high temporal resolution using small pore (5 {mu}m) MCPs and implementing fast timing electronics. We measured the TOF distribution of the electrons under our typical coincidence field strengths with a temporal resolution down to {sigma}=18 ps. We observed that our electron coincidence detector has a timing resolution better than {sigma}=16 ps, which is mainly determined by the residual transit time spread of the MCPs. The typical electron energy resolution appears to be nearly laser bandwidth limited with a relative resolution of {delta}E{sub FWHM}/E=3.5% for electrons with kinetic energy near 2 eV. The mass resolution of the ion detector for ions measured in coincidence with electrons is about {delta}m{sub FWHM}/m=1/4150. The velocity map focusing of our extended source volume of particles, due to the overlap of the molecular beam with the laser beams, results in a parent ion spot on our detector focused down to {sigma}=115 {mu}m.

  7. Imaging pigment chemistry in melanocytic conjunctival lesions with pump-probe microscopy

    NASA Astrophysics Data System (ADS)

    Wilson, Jesse W.; Vajzovic, Lejla; Robles, Francisco E.; Cummings, Thomas J.; Mruthyunjaya, Prithvi; Warren, Warren S.

    2013-03-01

    We extend nonlinear pump-probe microscopy, recently demonstrated to image the microscopic distribution of eumelanin and pheomelanin in unstained skin biopsy sections, to the case of melanocytic conjunctival lesions. The microscopic distribution of pigmentation chemistry serves as a functional indicator of melanocyte activity. In these conjunctival specimens (benign nevi, primary acquired melanoses, and conjunctival melanoma), we have observed pump-probe spectroscopic signatures of eumelanin, pheomelanin, hemoglobin, and surgical ink, in addition to important structural features that differentiate benign from malignant lesions. We will also discuss prospects for an in vivo `optical biopsy' to provide additional information before having to perform invasive procedures.

  8. Gadolinium photoionization process

    DOEpatents

    Paisner, J.A.; Comaskey, B.J.; Haynam, C.A.; Eggert, J.H.

    1993-04-13

    A method is provided for selective photoionization of the odd-numbered atomic mass gadolinium isotopes 155 and 157. The selective photoionization is accomplished by circular or linear parallel polarized laser beam energy effecting a three-step photoionization pathway.

  9. Gadolinium photoionization process

    DOEpatents

    Paisner, Jeffrey A.; Comaskey, Brian J.; Haynam, Christopher A.; Eggert, Jon H.

    1993-01-01

    A method is provided for selective photoionization of the odd-numbered atomic mass gadolinium isotopes 155 and 157. The selective photoionization is accomplished by circular or linear parallel polarized laser beam energy effecting a three-step photoionization pathway.

  10. Optical pump-probe microscopy for biomedicine and art conservation

    NASA Astrophysics Data System (ADS)

    Fischer, Martin

    2013-03-01

    Nonlinear optical microscopy can provide contrast in highly heterogeneous media and a wide range of applications has emerged, primarily in biology, medicine, and materials science. Compared to linear microscopy methods, the localized nature of nonlinear interactions leads to high spatial resolution, optical sectioning, and larger possible imaging depth in scattering media. However, nonlinear contrast (other than fluorescence, harmonic generation or CARS) is generally difficult to measure because it is overwhelmed by the large background of detected illumination light. This background can be suppressed by using femtosecond pulse or pulse train shaping to encode nonlinear interactions in background-free regions of the frequency spectrum. We have developed this shaping technology to study novel intrinsic structural and molecular contrast in biological tissue, generally using less power than a laser pointer. For example we have recently been able to sensitively measure detailed transient absorption dynamics of melanin sub-types in a variety of skin lesions, showing clinically relevant differences of melanin type and distribution between cancerous and benign tissue.[1] Recently we have also applied this technology to paint samples and to historic artwork in order to provide detailed, depth-resolved pigment identification. Initial studies in different inorganic and organic pigments have shown a rich and pigment-specific nonlinear absorption signature.[2] Some pigments, for example lapis lazuli (natural ultramarine), even show marked differences in signal depending on its geographic origin and on age, demonstrating the potential of this technique to determine authenticity, provenance, technology of manufacture, or state of preservation of historic works of art.

  11. Frequency domain approach for time-resolved pump-probe microscopy using intensity modulated laser diodes

    NASA Astrophysics Data System (ADS)

    Miyazaki, J.; Kawasumi, K.; Kobayashi, T.

    2014-09-01

    We present a scheme for time-resolved pump-probe microscopy using intensity modulated laser diodes. The modulation frequencies of the pump and probe beams are varied up to 500 MHz with fixed frequency detuning typically set at 15 kHz. The frequency response of the pump-probe signal is detected using a lock-in amplifier referenced at the beat frequency. This frequency domain method is capable of characterizing the nanosecond to picosecond relaxation dynamics of sample species without the use of a high speed detector or a high frequency lock-in amplifier. Furthermore, as the pump-probe signal is based on the nonlinear interaction between the two laser beams and the sample, our scheme provides better spatial resolution than the conventional diffraction-limited optical microscopes. Time-resolved pump-probe imaging of fluorescence beads and aggregates of quantum dots demonstrates that this method is useful for the microscopic analysis of optoelectronic devices. The system is implemented using compact and low-cost laser diodes, and thus has a broad range of applications in the fields of photochemistry, optical physics, and biological imaging.

  12. Pump-probe surface photovoltage spectroscopy measurements on semiconductor epitaxial layers

    SciTech Connect

    Jana, Dipankar Porwal, S.; Sharma, T. K. Oak, S. M.; Kumar, Shailendra

    2014-04-15

    Pump-probe Surface Photovoltage Spectroscopy (SPS) measurements are performed on semiconductor epitaxial layers. Here, an additional sub-bandgap cw pump laser beam is used in a conventional chopped light geometry SPS setup under the pump-probe configuration. The main role of pump laser beam is to saturate the sub-bandgap localized states whose contribution otherwise swamp the information related to the bandgap of material. It also affects the magnitude of Dember voltage in case of semi-insulating (SI) semiconductor substrates. Pump-probe SPS technique enables an accurate determination of the bandgap of semiconductor epitaxial layers even under the strong influence of localized sub-bandgap states. The pump beam is found to be very effective in suppressing the effect of surface/interface and bulk trap states. The overall magnitude of SPV signal is decided by the dependence of charge separation mechanisms on the intensity of the pump beam. On the contrary, an above bandgap cw pump laser can be used to distinguish the signatures of sub-bandgap states by suppressing the band edge related feature. Usefulness of the pump-probe SPS technique is established by unambiguously determining the bandgap of p-GaAs epitaxial layers grown on SI-GaAs substrates, SI-InP wafers, and p-GaN epilayers grown on Sapphire substrates.

  13. Pump-probe surface photovoltage spectroscopy measurements on semiconductor epitaxial layers

    NASA Astrophysics Data System (ADS)

    Jana, Dipankar; Porwal, S.; Sharma, T. K.; Kumar, Shailendra; Oak, S. M.

    2014-04-01

    Pump-probe Surface Photovoltage Spectroscopy (SPS) measurements are performed on semiconductor epitaxial layers. Here, an additional sub-bandgap cw pump laser beam is used in a conventional chopped light geometry SPS setup under the pump-probe configuration. The main role of pump laser beam is to saturate the sub-bandgap localized states whose contribution otherwise swamp the information related to the bandgap of material. It also affects the magnitude of Dember voltage in case of semi-insulating (SI) semiconductor substrates. Pump-probe SPS technique enables an accurate determination of the bandgap of semiconductor epitaxial layers even under the strong influence of localized sub-bandgap states. The pump beam is found to be very effective in suppressing the effect of surface/interface and bulk trap states. The overall magnitude of SPV signal is decided by the dependence of charge separation mechanisms on the intensity of the pump beam. On the contrary, an above bandgap cw pump laser can be used to distinguish the signatures of sub-bandgap states by suppressing the band edge related feature. Usefulness of the pump-probe SPS technique is established by unambiguously determining the bandgap of p-GaAs epitaxial layers grown on SI-GaAs substrates, SI-InP wafers, and p-GaN epilayers grown on Sapphire substrates.

  14. Pump-probe surface photovoltage spectroscopy measurements on semiconductor epitaxial layers.

    PubMed

    Jana, Dipankar; Porwal, S; Sharma, T K; Kumar, Shailendra; Oak, S M

    2014-04-01

    Pump-probe Surface Photovoltage Spectroscopy (SPS) measurements are performed on semiconductor epitaxial layers. Here, an additional sub-bandgap cw pump laser beam is used in a conventional chopped light geometry SPS setup under the pump-probe configuration. The main role of pump laser beam is to saturate the sub-bandgap localized states whose contribution otherwise swamp the information related to the bandgap of material. It also affects the magnitude of Dember voltage in case of semi-insulating (SI) semiconductor substrates. Pump-probe SPS technique enables an accurate determination of the bandgap of semiconductor epitaxial layers even under the strong influence of localized sub-bandgap states. The pump beam is found to be very effective in suppressing the effect of surface/interface and bulk trap states. The overall magnitude of SPV signal is decided by the dependence of charge separation mechanisms on the intensity of the pump beam. On the contrary, an above bandgap cw pump laser can be used to distinguish the signatures of sub-bandgap states by suppressing the band edge related feature. Usefulness of the pump-probe SPS technique is established by unambiguously determining the bandgap of p-GaAs epitaxial layers grown on SI-GaAs substrates, SI-InP wafers, and p-GaN epilayers grown on Sapphire substrates. PMID:24784628

  15. Characterization of dilute optical lattices using pump-probe spectroscopy and photon correlation measurements

    NASA Astrophysics Data System (ADS)

    Clements, Ethan; Ross, Preston; Rapp, Anthony; Cai, Hong; Reigle, Alex; Schlonsky, Eli; Lee, Hoseong; Clemens, James; Bali, Samir

    2016-05-01

    We experimentally investigate optical lattices using three different methods: pump-probe spectroscopy of vibrational energy levels, photon correlation of light scattered by cold atoms, and fluorescence imaging. Photon correlations of the scattered light can be used to measure lattice dwell times and crossover times between lattice sites. From this information we can derive the diffusion constant which can then be compared to direct measurement via fluorescence imaging. Furthermore, by Fourier transforming the time delayed photon correlations we can obtain the intensity spectrum which can be compared directly to pump-probe spectroscopy of the vibrational energy levels. We plan to carefully study situations in which the atomic transport properties deviate from Boltzman Gibbs statistics.

  16. Individual loss distribution measurement in 32-branched PON using pulsed pump-probe Brillouin analysis.

    PubMed

    Takahashi, Hiroshi; Ito, Fumihiko; Kito, Chihiro; Toge, Kunihiro

    2013-03-25

    We describe loss distribution measurement in a passive optical network (PON) using pulsed pump-probe Brillouin analysis. A preliminary experiment is demonstrated using a 32-branched PON constructed in the laboratory. We analyze the signal to noise ratio of this measurement and show that the method can realize a 25 dB dynamic range in 90 seconds (10000 times averaging), with an event location resolution of 10 m, and a fiber length identification resolution of 2 m. PMID:23546056

  17. Pump-Probe Spectroscopy of Two-Body Correlations in Ultracold Gases

    SciTech Connect

    Koch, Christiane P.; Kosloff, Ronnie

    2009-12-31

    We suggest pump-probe spectroscopy to study pair correlations that determine the many-body dynamics in weakly interacting, dilute ultracold gases. A suitably chosen, short laser pulse depletes the pair density locally, creating a 'hole' in the electronic ground state. The dynamics of this nonstationary pair density is monitored by a time-delayed probe pulse. The resulting transient signal allows us to spectrally decompose the hole and to map out the pair correlation function.

  18. Pump-probe spectrometer for measuring x-ray induced strain.

    PubMed

    Loether, A; Adams, B W; DiCharia, A; Gao, Y; Henning, R; Walko, D A; DeCamp, M F

    2016-05-01

    A hard x-ray pump-probe spectrometer using a multi-crystal Bragg reflector is demonstrated at a third generation synchrotron source. This device derives both broadband pump and monochromatic probe pulses directly from a single intense, broadband x-ray pulse centered at 8.767 keV. We present a proof-of-concept experiment which directly measures x-ray induced crystalline lattice strain. PMID:27128053

  19. Polarized pump--probe spectroscopy of electronic excitation transport in photosynthetic antennas

    SciTech Connect

    Struve, W.S. )

    1990-08-01

    Polarized pump--probe spectroscopy was performed with 1.5--2 psec resolution on the bacteriochlorophyll a protein antenna complex from the green sulfur bacterium Prosthecochloris aestuarii and on native and enriched photosystem I particles from spinach. The resulting photobleaching profiles reflect the details of singlet electronic-excitation transport in these photosynthetic antennas, in which the pigments are complexed by proteins into clusters of five or more chromophores.

  20. Microwave pump-probe spectroscopy of the dipole-dipole interaction in a cold Rydberg gas

    NASA Astrophysics Data System (ADS)

    Park, Hyunwook; Gallagher, T. F.; Pillet, P.

    2016-05-01

    Microwave pump-probe experiments starting with a cold gas of Rb 34 s atoms confirm that cusped line shapes observed in dipole-dipole broadened microwave transitions are due to atoms which are widely separated and exhibit small dipole-dipole energy shifts. When the experiments are interpreted in terms of a nearest-neighbor model, they demonstrate that it is possible to select pairs of atoms based on their separation and orientation.

  1. Pump-probe quantum state tomography in a semiconductor optical amplifier.

    PubMed

    Grosse, N B; Owschimikow, N; Aust, R; Lingnau, B; Koltchanov, A; Kolarczik, M; Lüdge, K; Woggon, U

    2014-12-29

    Pump-probe quantum state tomography was applied to the transmission of a coherent state through an In(Ga)As based quantum dot optical amplifier during the interaction with an optical pump pulse. The Wigner function and the statistical moments of the field were extracted and used to determine the degree of population inversion and the signal-to-noise ratio in a sub-picosecond time window. PMID:25607214

  2. Comparing in vivo pump-probe and multiphoton fluorescence microscopy of melanoma and pigmented lesions.

    PubMed

    Wilson, Jesse W; Degan, Simone; Gainey, Christina S; Mitropoulos, Tanya; Simpson, Mary Jane; Zhang, Jennifer Y; Warren, Warren S

    2015-05-01

    We demonstrate a multimodal approach that combines a pump-probe with confocal reflectance and multiphoton autofluorescence microscopy. Pump-probe microscopy has been proven to be of great value in analyzing thin tissue sections of pigmented lesions, as it produces molecular contrast which is inaccessible by other means. However, the higher optical intensity required to overcome scattering in thick tissue leads to higher-order nonlinearities in the optical response of melanin (e.g., two-photon pump and one-photon probe) that present additional challenges for interpreting the data. We show that analysis of pigment composition in vivo must carefully account for signal terms that are nonlinear with respect to the pump and probe intensities. We find that pump-probe imaging gives useful contrast for pigmented structures over a large range of spatial scales (100 μm to 1 cm), making it a potentially useful tool for tracking the progression of pigmented lesions without the need to introduce exogenous contrast agents. PMID:25415567

  3. Comparing in vivo pump-probe and multiphoton fluorescence microscopy of melanoma and pigmented lesions

    NASA Astrophysics Data System (ADS)

    Wilson, Jesse W.; Degan, Simone; Gainey, Christina S.; Mitropoulos, Tanya; Simpson, Mary Jane; Zhang, Jennifer Y.; Warren, Warren S.

    2015-05-01

    We demonstrate a multimodal approach that combines a pump-probe with confocal reflectance and multiphoton autofluorescence microscopy. Pump-probe microscopy has been proven to be of great value in analyzing thin tissue sections of pigmented lesions, as it produces molecular contrast which is inaccessible by other means. However, the higher optical intensity required to overcome scattering in thick tissue leads to higher-order nonlinearities in the optical response of melanin (e.g., two-photon pump and one-photon probe) that present additional challenges for interpreting the data. We show that analysis of pigment composition in vivo must carefully account for signal terms that are nonlinear with respect to the pump and probe intensities. We find that pump-probe imaging gives useful contrast for pigmented structures over a large range of spatial scales (100 μm to 1 cm), making it a potentially useful tool for tracking the progression of pigmented lesions without the need to introduce exogenous contrast agents.

  4. Pump-probe imaging of pigmented cutaneous melanoma primary lesions gives insight into metastatic potential

    PubMed Central

    Robles, Francisco E.; Deb, Sanghamitra; Wilson, Jesse W.; Gainey, Christina S.; Selim, M. Angelica; Mosca, Paul J.; Tyler, Douglas S.; Fischer, Martin C.; Warren, Warren S.

    2015-01-01

    Metastatic melanoma is associated with a poor prognosis, but no method reliably predicts which melanomas of a given stage will ultimately metastasize and which will not. While sentinel lymph node biopsy (SLNB) has emerged as the most powerful predictor of metastatic disease, the majority of people dying from metastatic melanoma still have a negative SLNB. Here we analyze pump-probe microscopy images of thin biopsy slides of primary melanomas to assess their metastatic potential. Pump-probe microscopy reveals detailed chemical information of melanin with subcellular spatial resolution. Quantification of the molecular signatures without reference standards is achieved using a geometrical representation of principal component analysis. Melanin structure is analyzed in unison with the chemical information by applying principles of mathematical morphology. Results show that melanin in metastatic primary lesions has lower chemical diversity than non-metastatic primary lesions, and contains two distinct phenotypes that are indicative of aggressive disease. Further, the mathematical morphology analysis reveals melanin in metastatic primary lesions has a distinct “dusty” quality. Finally, a statistical analysis shows that the combination of the chemical information with spatial structures predicts metastatic potential with much better sensitivity than SLNB and high specificity, suggesting pump-probe microscopy can be an important tool to help predict the metastatic potential of melanomas. PMID:26417529

  5. Super Resolution Pump-Probe Microscopy with point spread function engineering

    NASA Astrophysics Data System (ADS)

    Mohajerani, Farzaneh

    Since the last decade, new techniques have made optical microscopy break the diffraction barrier of resolution where all of them are based on molecular fluorescence. Among them, stimulated emission depletion microscopy (STED) has reached less than 25 nm resolution by engineering the point spread function. However, the existing obstacles associated with fluorescence tagging makes it desirable to achieve label-free imaging. Recently the pump-probe method has made it possible to obtain image contrast from molecular absorption and vibration signatures that do not depend on fluorescence. We introduce Super Resolution Pump-Probe Microscopy (SRPPM), in which we combine both PSF engineering method and pump-probe method to achieve the goal of imaging non-fluorescent molecules with nanometer resolution. Our calculations for SRPPM show that we are able to reach less than 30nm resolution with the intensity of pump and probe beams that will not exceed 10 MW/cm2 . This intensity is much lower than the high intensities of the Doughnut beam in STED microscopy and it is compatible with bio-imaging goals of this microscope.

  6. Chasing charge localization and chemical reactivity following photoionization in liquid water.

    PubMed

    Marsalek, Ondrej; Elles, Christopher G; Pieniazek, Piotr A; Pluhařová, Eva; VandeVondele, Joost; Bradforth, Stephen E; Jungwirth, Pavel

    2011-12-14

    The ultrafast dynamics of the cationic hole formed in bulk liquid water following ionization is investigated by ab initio molecular dynamics simulations and an experimentally accessible signature is suggested that might be tracked by femtosecond pump-probe spectroscopy. This is one of the fastest fundamental processes occurring in radiation-induced chemistry in aqueous systems and biological tissue. However, unlike the excess electron formed in the same process, the nature and time evolution of the cationic hole has been hitherto little studied. Simulations show that an initially partially delocalized cationic hole localizes within ~30 fs after which proton transfer to a neighboring water molecule proceeds practically immediately, leading to the formation of the OH radical and the hydronium cation in a reaction which can be formally written as H(2)O(+) + H(2)O → OH + H(3)O(+). The exact amount of initial spin delocalization is, however, somewhat method dependent, being realistically described by approximate density functional theory methods corrected for the self-interaction error. Localization, and then the evolving separation of spin and charge, changes the electronic structure of the radical center. This is manifested in the spectrum of electronic excitations which is calculated for the ensemble of ab initio molecular dynamics trajectories using a quantum mechanics/molecular mechanics (QM∕MM) formalism applying the equation of motion coupled-clusters method to the radical core. A clear spectroscopic signature is predicted by the theoretical model: as the hole transforms into a hydroxyl radical, a transient electronic absorption in the visible shifts to the blue, growing toward the near ultraviolet. Experimental evidence for this primary radiation-induced process is sought using femtosecond photoionization of liquid water excited with two photons at 11 eV. Transient absorption measurements carried out with ~40 fs time resolution and broadband spectral probing

  7. Diagnosis and staging of female genital tract melanocytic lesions using pump-probe microscopy (Conference Presentation)

    NASA Astrophysics Data System (ADS)

    Robles, Francisco E.; Selim, Maria A.; Warren, Warren S.

    2016-02-01

    Melanoma of the vulva is the second most common type of malignancy afflicting that organ. This disease caries poor prognosis, and shows tendencies to recur locally and develop distant metastases through hematogenous dissemination. Further, there exists significant clinical overlap between early-stage melanomas and melanotic macules, benign lesions that are believed to develop in about 10% of the general female population. In this work we apply a novel nonlinear optical method, pump-probe microscopy, to quantitatively analyze female genitalia tract melanocytic lesions. Pump-probe microscopy provides chemical information of endogenous pigments by probing their electronic excited state dynamics, with subcellular resolution. Using unstained biopsy sections from 31 patients, we find significant differences between melanin type and structure in tissue regions with invasive melanoma, melanoma in-situ and non-malignant melanocytic proliferations (e.g., nevi, melanocytic macules). The molecular images of non-malignant lesion have a well-organized structure, with relatively homogenous pigment chemistry, most often consistent with that of eumelanin with large aggregate size or void of metals, such as iron. On the other hand, pigment type and structure observed in melanomas in-situ and invasive melanomas is typically much more heterogeneous, with larger contributions from pheomelanin, melanins with larger metal content, and/or melanins with smaller aggregate size. Of most significance, clear differences can be observed between melanocytic macules and vulvar melanoma in-situ, which, as discussed above, can be difficult to clinically distinguish. This initial study demonstrates pump-probe microscopy's potential as an adjuvant diagnostic tool by revealing systematic chemical and morphological differences in melanin pigmentation among invasive melanoma, melanoma in-situ and non-malignant melanocytic lesions.

  8. Femtosecond Synchronization of Laser Systems for the LCLS

    SciTech Connect

    Byrd, John; Doolittle, Lawrence; Huang, Gang; Staples, John; Wilcox, Russell; Arthur, John; Frisch, Josef; White, William; /SLAC

    2012-08-24

    The scientific potential of femtosecond x-ray pulses at linac-driven free-electron lasers such as the Linac Coherent Light Source is tremendous. Time-resolved pump-probe experiments require a measure of the relative arrival time of each x-ray pulse with respect to the experimental pump laser. An optical timing system based on stabilized fiber links has been developed for the LCLS to provide this synchronization. Preliminary results show synchronization of the installed stabilized links at the sub-20-femtosecond level. We present details of the implementation at LCLS and potential for future development.

  9. Pump-probe imaging of laser-induced periodic surface structures after ultrafast irradiation of Si

    SciTech Connect

    Murphy, Ryan D.; Torralva, Ben; Adams, David P.; Yalisove, Steven M.

    2013-09-30

    Ultrafast pump-probe microscopy has been used to investigate laser-induced periodic surface structure (LIPSS) formation on polished Si surfaces. A crater forms on the surface after irradiation by a 150 fs laser pulse, and a second, subsequent pulse forms LIPSS within the crater. Sequentially delayed images show that LIPSS with a periodicity slightly less than the fundamental laser wavelength of 780 nm appear on Si surfaces ∼50 ps after arrival of the second pump laser pulse, well after the onset of melting. LIPSS are observed on the same timescale as material removal, suggesting that their formation involves material ejection.

  10. Optical pump-probe measurements of local nuclear spin coherence in semiconductor quantum wells.

    PubMed

    Sanada, H; Kondo, Y; Matsuzaka, S; Morita, K; Hu, C Y; Ohno, Y; Ohno, H

    2006-02-17

    We demonstrate local manipulation and detection of nuclear spin coherence in semiconductor quantum wells by an optical pump-probe technique combined with pulse rf NMR. The Larmor precession of photoexcited electron spins is monitored by time-resolved Kerr rotation (TRKR) as a measure of nuclear magnetic field. Under the irradiation of resonant pulsed rf magnetic fields, Rabi oscillations of nuclear spins are traced by TRKR signals. The intrinsic coherence time evaluated by a spin-echo technique reveals the dependence on the orientation of the magnetic field with respect to the crystalline axis as expected by the nearest neighbor dipole-dipole interaction. PMID:16606048

  11. Ultra-broadband infrared pump-probe spectroscopy using synchrotron radiation and a tuneable pump

    SciTech Connect

    Carroll, Lee; Friedli, Peter; Stutz, Stefan; Sigg, Hans; Lerch, Philippe; Schneider, Joerg; Treyer, Daniel; Hunziker, Stephan

    2011-06-15

    Synchrotron infrared sources have become popular mainly because of their excellent broadband brilliance, which enables spectroscopically resolved spatial-mapping of stationary objects at the diffraction limit. In this article we focus on an often-neglected further advantage of such sources - their unique time-structure - to bring such broadband spectroscopy to the time domain, for studying dynamic phenomenon down to the 100 ps limit. We describe the ultra-broadband (12.5 to 1.1 {mu}m) Fourier transform pump-probe setup, for condensed matter transmission- and reflection-spectroscopy, installed at the X01DC infrared beam-line of the Swiss Light Source (SLS). The optical pump consists of a widely tuneable 100 ps 1 kHz laser system, covering 94% of the 16 to 1.1 {mu}m range. A thorough description of the system is given, including (i) the vector-modulator providing purely electronic tuning of the pump-probe overlap up to 1 ms with sub-ps time resolution, (ii) the 500 MHz data acquisition system interfaced with the experimental physics and industrial control system (EPICS) based SLS control system for consecutive pulse sampling, and (iii) the step-scan time-slice Fourier transform scheme for simultaneous recording of the dual-channel pumped, un-pumped, and difference spectra. The typical signal/noise ratio of a single interferogram in a 100 ps time slice is 300 (measured during one single 140 s TopUp period). This signal/noise ratio is comparable to that of existing gated Globar pump-probe Fourier transform spectroscopy, but brings up to four orders of magnitude better time resolution. To showcase the utility of broadband pump-probe spectroscopy, we investigate a Ge-on-Si material system similar to that in which optically pumped direct-gap lasing was recently reported. We show that the mid-infrared reflection-spectra can be used to determine the optically injected carrier density, while the mid- and near-infrared transmission-spectra can be used to separate the strong

  12. Towards pump probe experiments of defect dynamics with short ion beam pulses

    SciTech Connect

    Schenkel, T.; Lidia, S.; Weis, C. D.; Waldron, W. L.; Schwartz, J.; Minor, Andrew; Hosemann, P; Kwan, J. W.

    2013-01-01

    A novel, induction type linear accelerator, the Neutralized Drift Compression eXperiment (NDCX-II), is currently being commissioned at Berkeley Lab. This accelerator is designed to deliver intense (up to 3 1011 ions/pulse), 0.6 to 600 ns duration pulses of 0.05 1.2 MeV lithium ions at a rate of about 2 pulses per minute onto 1 10 mm scale target areas. When focused to mm-diameter spots, the beam is predicted to volumetrically heat micrometer thick foils to temperatures of 30,000 K. At lower beam power densities, the short excitation pulse with tunable intensity and time profile enables pump probe type studies of defect dynamics in a broad range of materials. We briefly describe the accelerator concept and design, present results from beam pulse shaping experiments and discuss examples of pump probe type studies of defect dynamics following irradiation of materials with intense, short ion beam pulses from NDCX-II.

  13. Towards pump-probe experiments of defect dynamics with short ion beam pulses

    NASA Astrophysics Data System (ADS)

    Schenkel, T.; Lidia, S. M.; Weis, C. D.; Waldron, W. L.; Schwartz, J.; Minor, A. M.; Hosemann, P.; Kwan, J. W.

    2013-11-01

    A novel, induction type linear accelerator, the Neutralized Drift Compression eXperiment (NDCX-II), is currently being commissioned at Berkeley Lab. This accelerator is designed to deliver intense (up to 3 × 1011 ions/pulse), 0.6 to ∼600 ns duration pulses of 0.05-1.2 MeV lithium ions at a rate of about 2 pulses per minute onto 1-10 mm scale target areas. When focused to mm-diameter spots, the beam is predicted to volumetrically heat micrometer thick foils to temperatures of ∼30,000 °K. At lower beam power densities, the short excitation pulse with tunable intensity and time profile enables pump-probe type studies of defect dynamics in a broad range of materials. We briefly describe the accelerator concept and design, present results from beam pulse shaping experiments and discuss examples of pump-probe type studies of defect dynamics following irradiation of materials with intense, short ion beam pulses from NDCX-II.

  14. Monitoring the Coherent Vibrational Control of Electronic Excitation Transfer Using Ultrafast Pump-Probe Polarization Spectroscopy

    NASA Astrophysics Data System (ADS)

    Biggs, Jason; Cina, Jeffrey

    2010-03-01

    The interplay between nuclear and electronic degrees of freedom in molecular energy-transfer complexes is a subject of current interest. We have proposed a method to use coherent nuclear motion to control the transfer of electronic excitation energy between donor and acceptor moieties in electronically coupled dimers. The underlying electronic and nuclear motion at the level of quantum mechanical amplitudes can be observed using nonlinear wave-packet interferometry(nl-WPI), a form of fluorescence-detected multidimensional electronic spectroscopy. In our control scheme, coherent nuclear motion is induced in the acceptor chromophore prior to direct electronic excitation of the donor. This nuclear motion affects the instantaneous resonance conditions between donor and acceptor moieties and thus affects subsequent energy transfer dynamics. We have developed the framework to simulate four-pulse nl-WPI experiments, and the pump-probe limit thereof, on energy-transfer systems after interaction with a control pulse that induces nuclear motion. We present simulations in the pump-probe limit from model energy-transfer systems subjected to prior impulsive vibrational excitation, and show how pulse polarization can be used to infer electronic dynamics from isotropically oriented dimers.

  15. Probing ultrafast spin dynamics with optical pump-probe scanning tunnelling microscopy.

    PubMed

    Yoshida, Shoji; Aizawa, Yuta; Wang, Zi-han; Oshima, Ryuji; Mera, Yutaka; Matsuyama, Eiji; Oigawa, Haruhiro; Takeuchi, Osamu; Shigekawa, Hidemi

    2014-08-01

    Studies of spin dynamics in low-dimensional systems are important from both fundamental and practical points of view. Spin-polarized scanning tunnelling microscopy allows localized spin dynamics to be characterized and plays important roles in nanoscale science and technology. However, nanoscale analysis of the ultrafast dynamics of itinerant magnetism, as well as its localized characteristics, should be pursued to advance further the investigation of quantum dynamics in functional structures of small systems. Here, we demonstrate the optical pump-probe scanning tunnelling microscopy technique, which enables the nanoscale probing of spin dynamics with the temporal resolution corresponding, in principle, to the optical pulse width. Spins are optically oriented using circularly polarized light, and their dynamics are probed by scanning tunnelling microscopy based on the optical pump-probe method. Spin relaxation in a single quantum well with a width of 6 nm was observed with a spatial resolution of ∼ 1 nm. In addition to spin relaxation dynamics, spin precession, which provides an estimation of the Landé g factor, was observed successfully. PMID:24974938

  16. Probing ultrafast spin dynamics with optical pump-probe scanning tunnelling microscopy

    NASA Astrophysics Data System (ADS)

    Yoshida, Shoji; Aizawa, Yuta; Wang, Zi-Han; Oshima, Ryuji; Mera, Yutaka; Matsuyama, Eiji; Oigawa, Haruhiro; Takeuchi, Osamu; Shigekawa, Hidemi

    2014-08-01

    Studies of spin dynamics in low-dimensional systems are important from both fundamental and practical points of view. Spin-polarized scanning tunnelling microscopy allows localized spin dynamics to be characterized and plays important roles in nanoscale science and technology. However, nanoscale analysis of the ultrafast dynamics of itinerant magnetism, as well as its localized characteristics, should be pursued to advance further the investigation of quantum dynamics in functional structures of small systems. Here, we demonstrate the optical pump-probe scanning tunnelling microscopy technique, which enables the nanoscale probing of spin dynamics with the temporal resolution corresponding, in principle, to the optical pulse width. Spins are optically oriented using circularly polarized light, and their dynamics are probed by scanning tunnelling microscopy based on the optical pump-probe method. Spin relaxation in a single quantum well with a width of 6 nm was observed with a spatial resolution of ~1 nm. In addition to spin relaxation dynamics, spin precession, which provides an estimation of the Landé g factor, was observed successfully.

  17. Pump-probe studies of fragmentation of a fast HD+ beam

    NASA Astrophysics Data System (ADS)

    Zohrabi, M.; Berry, Ben; Severt, T.; Jochim, Bethany; Feizollah, Peyman; Raju P., Kanaka; Rajput, Jyoti; Carnes, K. D.; Esry, B. D.; Ben-Itzhak, I.

    2016-05-01

    Studies of fast molecular ion beams in strong-field ultrafast lasers are of particular interest for benchmark molecules, like H2+,H3+and HeH+. However, the low target density of a typical ion beam puts severe limits on studies of the time evolution through the implementation of the pump-probe technique. We have recently conducted a first-of-its-kind NIR-pump - NIR-probe measurement on a few-keV HD+ beam target. Specifically, the first pulse initiates the dissociation of the HD+, while the second ionizes the molecule during its dissociation. We have observed enhancement in the ionization yield of the dissociating wave packet at about 24 and 200 fs, corresponding to internuclear distances estimated classically to be about 15 and 85 a.u., respectively. The unexpected enhancement at very large internuclear separation has not been previously observed in pump-probe studies of neutral hydrogen molecules. Supported by the Chemical Sciences, Geosciences, and Biosciences Division, Office of Basic Energy Sciences, Office of Science, U. S. Department of Energy. BJ was also supported in part by DOE-SCGF (DE-AC05-06OR23100).

  18. Quantum well intersubband lifetimes measured by mid-IR pump-probe experiments

    SciTech Connect

    Woods, G.L.; Sung, B.; Proctor, M.

    1995-12-31

    Semiconductor quantum wells exhibit quantum-confined electronic energy levels, or subbands, that are similar to one-dimensional {open_quotes}particle in a box{close_quotes} wavefunctions. The light effective mass of electrons allows large spatial extents of the wavefunctions and concomitantly large dipole overlaps between states. These large dipoles have been exploited in a variety of experiments including nonlinear frequency conversion, infrared photodetection, and lasing. A key parameter for many devices is the upper state lifetime. The decay of carriers in the upper state is believed to be dominated by optical phonon scattering and lifetimes on-the order of 1ps are expected. While Raman and saturation measurements have shown good agreement with theory, direct pump-probe measurements have reported longer lifetimes, partially due to carrier heating. In this paper, we discuss our mid-IR (5{mu}m) pump-probe measurements of intersubband lifetimes, performed at the Stanford Picosecond Free Electron Laser Center. At low excitation densities we observe lifetimes of about 1.5 ps, in good agreement with phonon theory. At high excitation densities the lifetime increases to 3.5 ps, demonstrating the transition from the low- to high-excitation agree.

  19. Vibrationally coherent photochemistry in the femtosecond primary event of vision.

    PubMed

    Wang, Q; Schoenlein, R W; Peteanu, L A; Mathies, R A; Shank, C V

    1994-10-21

    Femtosecond pump-probe experiments reveal the impulsive production of photoproduct in the primary event in vision. The retinal chromophore of rhodopsin was excited with a 35-femtosecond pulse at 500 nanometers, and transient changes in absorption were measured with 10-femtosecond probe pulses. At probe wavelengths within the photo-product absorption band, oscillatory features with a period of 550 femtoseconds (60 wavenumbers) were observed whose phase and amplitude demonstrate that they are the result of nonstationary vibrational motion in the ground state of the photoproduct. The observation of coherent vibrational motion of the photoproduct supports the idea that the primary step in vision is a vibrationally coherent process and that the high quantum yield of the cis-->trans isomerization in rhodopsin is a consequence of the extreme speed of the excited-state torsional motion. PMID:7939680

  20. Interpretation of negative birefringence observed in strong-field optical pump-probe experiments: High-order Kerr and plasma grating effects

    NASA Astrophysics Data System (ADS)

    Karras, G.; Béjot, P.; Houzet, J.; Hertz, E.; Billard, F.; Lavorel, B.; Faucher, O.

    2013-11-01

    The analysis of negative birefringence optically induced in major air components [Loriot , Opt. ExpressOPEXFF1094-408710.1364/OE.17.013429 17, 13429 (2009); Loriot , Opt. ExpressOPEXFF1094-408710.1364/OE.18.003011 18, 3011 (2010)] is revisited in light of the recently reported plasma grating-induced phase-shift effect predicted for strong-field pump-probe experiments [Wahlstrand and Milchberg, Opt. Lett.OPLEDP0146-959210.1364/OL.36.003822 36, 3822 (2011)]. The nonlinear birefringence induced by a short and intense laser pulse in argon is measured by femtosecond time-resolved polarimetry. The experiments are performed with degenerate colors, where the pump and probe beam share the same spectrum, or with two different colors and nonoverlapping spectra. The interpretation of the experimental results is substantiated using a numerical 3D+1 model accounting for nonlinear propagation effects, cross-beam geometry of the interacting laser pulses, and detection technique. The model also includes the ionization rate of argon and high-order Kerr indices introduced by Loriot , enabling one to assess the contribution of both terms to the observed effect. The results show that the ionization-induced phase shift has a minor contribution compared to the high-order Kerr effect formerly introduced, the latter allowing a reasonably good reproduction of the experimental data for the present conditions.

  1. Nondestructive Complete Mechanical Characterization of Zinc Blende and Wurtzite GaAs Nanowires Using Time-Resolved Pump-Probe Spectroscopy.

    PubMed

    Mante, Pierre-Adrien; Lehmann, Sebastian; Anttu, Nicklas; Dick, Kimberly A; Yartsev, Arkady

    2016-08-10

    We have developed and demonstrated an experimental method, based on the picosecond acoustics technique, to perform nondestructive complete mechanical characterization of nanowires, that is, the determination of the complete elasticity tensor. By means of femtosecond pump-probe spectroscopy, coherent acoustic phonons were generated in an ensemble of nanowires and their dynamics was resolved. Specific phonon modes were identified and the detection mechanism was addressed via wavelength dependent experiments. We calculated the exact phonon dispersion relation of the nanowires by fitting the experimentally observed frequencies, thus allowing the extraction of the complete elasticity tensor. The elasticity tensor and the nanowire diameter were determined for zinc blende GaAs nanowires and were found to be in a good agreement with literature data and independent measurements. Finally, we have applied this technique to characterize wurtzite GaAs nanowires, a metastable phase in bulk, for which no experimental values of elastic constants are currently available. Our results agree well with previous first principle calculations. The proposed approach to the complete and nondestructive mechanical characterization of nanowires will allow the efficient mechanical study of new crystal phases emerging in nanostructures, as well as size-dependent properties of nanostructured materials. PMID:27352041

  2. Deducing fast electron density changes in randomly orientated uncrystallized biomolecules in a pump-probe experiment.

    PubMed

    Pande, K; Schwander, P; Schmidt, M; Saldin, D K

    2014-07-17

    We propose a method for deducing time-resolved structural changes in uncrystallized biomolecules in solution. The method relies on measuring the angular correlations of the intensities, when averaged over a large number of diffraction patterns from randomly oriented biomolecules in solution in a liquid solvent. The experiment is somewhat like a pump-probe version of an experiment on small angle X-ray scattering, except that the data expected by the algorithm are not just the radial variation of the averaged intensities. The differences of these correlation functions as measured from a photoexcited and dark structure enable the direct calculation of the difference electron density with a knowledge of only the dark structure. We exploit a linear relation we derive between the difference in these correlation functions and the difference electron density, applicable for small structural changes. PMID:24914159

  3. Interface-Induced Magnetic Coupling in Multiferroic/Ferromagnetic Bilayer: An Ultrafast Pump-Probe Study

    NASA Astrophysics Data System (ADS)

    Chia, Elbert; La-O-Vorakiat, Chan; Tian, Y. F.; Wu, Tom; Panagopoulos, Christos; Zhu, Jian-Xin; Su, Haibin

    2014-03-01

    By use of optical pump-probe measurement, we study the relaxation dynamics of a muliferroic-ferromagnetic TbMnO3/La0.7Sr0.3MnO3 bilayer. The relaxation dynamics of both layers are well separated in time allowing us to investigate the magnetic coupling across the bilayer. We observe that the relaxation dynamics of the individual layers in the bilayer sample are the result of the interplay between the intrinsic magnetic order and the induced interfacial effect. Our data suggest the existence of induced ferromagnetic order in the TbMnO3 layer, and antiferromagnetic order in the La0.7Sr0.3MnO3 layer. Singapore NRF CRP (NRF-CRP4-2008-04) and MOE AcRF Tier 1 (RG 13/12).

  4. Picosecond pump-probe using an FEL and a synchrotron source

    SciTech Connect

    Denbeaux, G.; Straub, K.D.; Madey, J.M.J.

    1995-12-31

    Two color pump-probe experiments using both the Duke Storage Ring as a synchrotron light source for visible light the Mark III FEL as a tunable, high peak power IR source are possible. The visible synchrotron source can be used as a probe of vibrational excitation from the FEL in an experiment using vibrationally-assisted fluorescence as an indicator of overlap of the IR and the visible pulses. An optical delay line in the FEL beam will allow adjustment of the arrival time of the IR pulse relative to the visible probe. The storage ring RF booster and the Mark III FEL RF sources will be both driven by the same master oscillator with a timing jitter between sources of less than 20 psec. Exploration of coupling between electronic excitation and lifetimes of vibrational excitation of fluorescent compounds in solution can be carried out with this configuration.

  5. Fourier domain Pump-Probe Optical Coherence Tomography imaging of melanin.

    PubMed

    Jacob, Desmond; Shelton, Ryan L; Applegate, Brian E

    2010-06-01

    We report the development of a two-color Fourier domain Pump-Probe Optical Coherence Tomography (PPOCT) system. Tissue phantom experiments to characterize the system performance demonstrated imaging depths in excess of 725 microm, nearly comparable to the base Optical Coherence Tomography system. PPOCT A-line rates were also demonstrated in excess of 1 kHz. The physical origin of the PPOCT signal was investigated with a series of experiments which revealed that the signal is a mixture of short and long lifetime component signals. The short lifetime component was attributed to transient absorption while the long lifetime component may be due to a mixture of transient absorption and thermal effects. Ex vivo images of porcine iris demonstrated the potential for imaging melanin in the eye, where cancer of the melanocytes is the most common form of eye cancer in adults. PMID:20588366

  6. Pulsed laser noise analysis and pump-probe signal detection with a data acquisition card

    NASA Astrophysics Data System (ADS)

    Werley, Christopher A.; Teo, Stephanie M.; Nelson, Keith A.

    2011-12-01

    A photodiode and data acquisition card whose sampling clock is synchronized to the repetition rate of a laser are used to measure the energy of each laser pulse. Simple analysis of the data yields the noise spectrum from very low frequencies up to half the repetition rate and quantifies the pulse energy distribution. When two photodiodes for balanced detection are used in combination with an optical modulator, the technique is capable of detecting very weak pump-probe signals (ΔI/I0 ˜ 10-5 at 1 kHz), with a sensitivity that is competitive with a lock-in amplifier. Detection with the data acquisition card is versatile and offers many advantages including full quantification of noise during each stage of signal processing, arbitrary digital filtering in silico after data collection is complete, direct readout of percent signal modulation, and easy adaptation for fast scanning of delay between pump and probe.

  7. Resonant uv pump-probe spectroscopy of dipicolinic acid via impulsive excitation

    SciTech Connect

    Murawski, Robert K.; Rostovtsev, Yuri V.; Sariyanni, Zoe-Elizabeth; Sautenkov, Vladimir A.; Backus, Sterling; Raymondson, Daisy; Kapteyn, Henry C.; Murnane, Margaret M.; Scully, Marlan O.

    2008-02-15

    We present experimental evidence of coherent wave packet motion in dipicolinic acid (C{sub 7}H{sub 5}NO{sub 4}) which is an important marker molecule for bacterial spores. Resonant impulsive excitation is achieved by applying a uv pump pulse (267 nm, 16 fs) which has a duration that is shorter than the vibrational period of the molecules. The resulting dynamics is then probed with a weaker pulse of the same width and frequency. Evidence of the important 'fingerprint' region for this molecule (between 1000 cm{sup -1} and 1500 cm{sup -1}) is found in the transient absorption of the probe. We present simulations of the pump-probe experiment, based on the Liouville equation for the density matrix, and predict the optimal pulse width and detuning.

  8. In vivo pump-probe optical coherence tomography imaging in Xenopus laevis.

    PubMed

    Carrasco-Zevallos, Oscar; Shelton, Ryan L; Kim, Wihan; Pearson, Jeremy; Applegate, Brian E

    2015-01-01

    Currently, optical coherence tomography (OCT), is not capable of obtaining molecular information often crucial for identification of disease. To enable molecular imaging with OCT, we have further developed a technique that harnesses transient changes in light absorption in the sample to garner molecular information. A Fourier-domain Pump-Probe OCT (PPOCT) system utilizing a 532 nm pump and 830 nm probe has been developed for imaging hemoglobin. Methylene blue, a biological dye with well-know photophysics, was used to characterize the system before investigating the origin of the hemoglobin PPOCT signal. The first in vivo PPOCT images were recorded of the vasculature in Xenopus laevis. The technique was shown to work equally well in flowing and nonflowing vessels. Furthermore, PPOCT was compared with other OCT extensions which require flow, such as Doppler OCT and phase-variance OCT. PPOCT was shown to better delineate tortuous vessels, where nodes often restrict Doppler and phase-variance reconstruction. PMID:24282110

  9. Measuring excited state lifetime of Rb atoms with pump-probe technique

    SciTech Connect

    Zeng, X.; Boiko, D. L.

    2015-08-31

    A technique for measuring the excited state lifetime τ{sub ex} of optical transitions in alkali atoms is presented. It is a form of pump-probe technique based on time-resolved optical transmission through the atomic vapor cell. This technique can serve as an alternative to the traditionally used time-resolved photofluorescence methods when measuring alkali vapor cells with heavily quenched fluorescence, where the τ{sub ex} is expected to be on the order of a few nanoseconds, and the highly sensitive fluorescence detectors with sub-nanosecond temporal resolution that are required may not be available. We use this technique to measure the τ{sub ex} of Rb atoms in vapor cells with different buffer gas pressures.

  10. Numerical method to compute optical conductivity based on pump-probe simulations

    NASA Astrophysics Data System (ADS)

    Shao, Can; Tohyama, Takami; Luo, Hong-Gang; Lu, Hantao

    2016-05-01

    A numerical method to calculate optical conductivity based on a pump-probe setup is presented. Its validity and limits are tested and demonstrated via concrete numerical simulations on the half-filled one-dimensional extended Hubbard model both in and out of equilibrium. By employing either a steplike or a Gaussian-like probing vector potential, it is found that in nonequilibrium, the method in the narrow-probe-pulse limit can be identified with variant types of linear-response theory, which, in equilibrium, produce identical results. The observation reveals the underlying probe-pulse dependence of the optical conductivity calculations in nonequilibrium, which may have applications in the theoretical analysis of ultrafast spectroscopy measurements.

  11. Molecular imaging of hemoglobin using ground state recovery pump-probe optical coherence tomography

    NASA Astrophysics Data System (ADS)

    Applegate, Brian E.; Izatt, Joseph A.

    2007-02-01

    We have undertaken an effort to further develop ground state recovery Pump-Probe Optical Coherence Tomograpy (gsrPPOCT) to specifically target and measure 3-D images of hemoglobin concentration with the goals of mapping tissue vasculature, total hemoglobin, and hemoglobin oxygen saturation. As a first step toward those goals we have measured the gsrPPOCT signal from the hemoglobin in the filament arteries of a zebra danio fish. We have further processed the resulting signal to extract a qualitative map of the hemoglobin concentration. We have also demonstrated the potential to use ground state recovery times to differentiate between two chromophores which may prove to be an effective tool for differentiating between oxy and deoxy hemoglobin.

  12. Direct Detection of Pure ac Spin Current by X-Ray Pump-Probe Measurements.

    PubMed

    Li, J; Shelford, L R; Shafer, P; Tan, A; Deng, J X; Keatley, P S; Hwang, C; Arenholz, E; van der Laan, G; Hicken, R J; Qiu, Z Q

    2016-08-12

    Despite recent progress in spin-current research, the detection of spin current has mostly remained indirect. By synchronizing a microwave waveform with synchrotron x-ray pulses, we use the ferromagnetic resonance of the Py (Ni_{81}Fe_{19}) layer in a Py/Cu/Cu_{75}Mn_{25}/Cu/Co multilayer to pump a pure ac spin current into the Cu_{75}Mn_{25} and Co layers, and then directly probe the spin current within the Cu_{75}Mn_{25} layer and the spin dynamics of the Co layer by x-ray magnetic circular dichroism. This element-resolved pump-probe measurement unambiguously identifies the ac spin current in the Cu_{75}Mn_{25} layer. PMID:27563981

  13. Direct Detection of Pure ac Spin Current by X-Ray Pump-Probe Measurements

    NASA Astrophysics Data System (ADS)

    Li, J.; Shelford, L. R.; Shafer, P.; Tan, A.; Deng, J. X.; Keatley, P. S.; Hwang, C.; Arenholz, E.; van der Laan, G.; Hicken, R. J.; Qiu, Z. Q.

    2016-08-01

    Despite recent progress in spin-current research, the detection of spin current has mostly remained indirect. By synchronizing a microwave waveform with synchrotron x-ray pulses, we use the ferromagnetic resonance of the Py (Ni81Fe19 ) layer in a Py /Cu /Cu75Mn25/Cu /Co multilayer to pump a pure ac spin current into the Cu75Mn25 and Co layers, and then directly probe the spin current within the Cu75Mn25 layer and the spin dynamics of the Co layer by x-ray magnetic circular dichroism. This element-resolved pump-probe measurement unambiguously identifies the ac spin current in the Cu75Mn25 layer.

  14. Novel geminate recombination channel after indirect photoionization of water

    SciTech Connect

    Fischer, Martin K.; Rossmadl, Hubert; Iglev, Hristo

    2011-06-07

    We studied the photolysis of neat protonated and heavy water using pump-probe and pump-repump-probe spectroscopy. A novel recombination channel is reported leading to ultrafast quenching (0.7 {+-} 0.1 ps) of almost one third of the initial number of photo-generated electrons. The efficiency and the recombination rate of this channel are lower in heavy water, 27 {+-} 5% and (0.9 {+-} 0.1 ps){sup -1}, respectively. Comparison with similar data measured after photodetachment of aqueous hydroxide provides evidence for the formation of short-lived OH:e{sup -} (OD:e{sup -}) pairs after indirect photoionization of water at 9.2 eV.

  15. Tracking ultrafast relaxation dynamics of furan by femtosecond photoelectron imaging

    NASA Astrophysics Data System (ADS)

    Liu, Yuzhu; Knopp, Gregor; Qin, Chaochao; Gerber, Thomas

    2015-01-01

    Ultrafast internal conversion dynamics of furan has been studied by femtosecond photoelectron imaging (PEI) coupled with photofragmentation (PF) spectroscopy. Photoelectron imaging of single-color multi-photon ionization and two-color pump-probe ionization are obtained and analyzed. Photoelectron bands are assigned to the related states. The time evolution of the photoelectron signal by pump-probe ionization can be well described by a biexponential decay: two rapid relaxation pathways with time constants of ∼15 fs and 85 (±11) fs. The rapid relaxation is ascribed to the ultrafast internal conversion (IC) from the S2 state to the vibrationally hot S1 state. The second relaxation process is attributed to the redistributions and depopulation of secondarily populated high vibronic S1 state and the formation of α-carbene and β-carbene by H immigration. Additionally, the transient characteristics of the fragment ions are also measured and discussed as a complementary understanding.

  16. MBI facility at BESSY II for time-resolved pump-probe techniques with laser and undulator radiation

    NASA Astrophysics Data System (ADS)

    Gatzke, Johannes; Winter, Bernd J.; Quast, T.; Hertel, Ingolf V.

    1998-10-01

    The MBI develops a facility at BESSY II dedicated to pump- probe techniques combining synchrotron and laser radiation. The synchronization of laser and synchrotron pulses will allow time resolved experiments on the picosecond time scale at this. The features of the facility, the optical parameters of the synchrotron beamline, the synchronization technique and pulse stretching considerations will be outlined. Current developments will be reported.

  17. High efficiency photoionization detector

    DOEpatents

    Anderson, David F.

    1984-01-01

    A high efficiency photoionization detector using tetraaminoethylenes in a gaseous state having a low ionization potential and a relative photoionization cross section which closely matches the emission spectrum of xenon gas. Imaging proportional counters are also disclosed using the novel photoionization detector of the invention. The compound of greatest interest is TMAE which comprises tetrakis(dimethylamino)ethylene which has a measured ionization potential of 5.36.+-.0.02 eV, and a vapor pressure of 0.35 torr at 20.degree. C.

  18. High efficiency photoionization detector

    DOEpatents

    Anderson, D.F.

    1984-01-31

    A high efficiency photoionization detector is described using tetraaminoethylenes in a gaseous state having a low ionization potential and a relative photoionization cross section which closely matches the emission spectrum of xenon gas. Imaging proportional counters are also disclosed using the novel photoionization detector of the invention. The compound of greatest interest is TMAE which comprises tetrakis(dimethylamino)ethylene which has a measured ionization potential of 5.36 [+-] 0.02 eV, and a vapor pressure of 0.35 torr at 20 C. 6 figs.

  19. Control of wave packets in lithium dimers with a state-selected pump-probe scheme

    NASA Astrophysics Data System (ADS)

    Dai, Xingcan

    A state-selected pump-probe scheme is used to control wave packet dynamics in Li2. In this scheme, a cw laser selects one electronic transition from the thermally populated ground state to the launch state A1Sigmau+ of Li2, from which an ultrashort pump pulse creates a superstition state on the electronic states of Li2 followed by another ultrashort pulse to excite the wave packet to the ground state of Li2+. Usually, an unperturbed level at the A1Sigmau+ state of Li2 is selected by the cw laser pulses. However, if the level of A1Sigmau+ is perturbed by b3piu, and then the wave packets that consist of the triplet states as well as the singlet states of Li2 are detected from the mixed levels. Since one of the triplet states is predissociative, the fast decay of the amplitudes of the wave packets that have the components of this predissociative state is observed. In order to study coherent multiphoton processes, Raman wave packets are created and manipulated with a pulse shaping system. The phase difference between the amplitude coefficients induced by resonant and off-resonant Raman transitions is shown directly by comparing the phases of the Raman wave packets excited by the resonant and off-resonant Raman transitions. The ionization processes employed in the probe step of the state-selective pump-probe scheme is fully explored in the second pulse shaping system in the path of the probe beam. It shows that the direct transitions from the electronic states involved in the wave packets are unlikely; while the autoionization and collision induced ionization from highly-excited Rydberg states are the main sources of the final ion signals. Some degree of the control of the wave packet dynamics is realized by shaping the probe pulses. The decoherence rates of quantum beats at the shelf region of the E1Sigma g+ state are measured to test theoretical results about pure dephasing rate in Li2. Finally, some schemes and preliminary results on physical realization of quantum

  20. Femtosecond Raman induced polarization spectroscopy studies of coherent rotational dynamics in molecular fluids

    SciTech Connect

    Morgen, M M

    1997-05-01

    We develop a polarization-sensitive femtosecond pump probe technique, Raman induced polarization spectroscopy (RIPS), to study coherent rotation in molecular fluids. By observing the collisional dephasing of the coherently prepared rotational states, we are able to extract information concerning the effects of molecular interactions on the rotational motion. The technique is quite sensitive because of the zero background detection method, and is also versatile due to its nonresonant nature.

  1. Molecular photoionization dynamics

    SciTech Connect

    Dehmer, Joseph L.

    1982-05-01

    This program seeks to develop both physical insight and quantitative characterization of molecular photoionization processes. Progress is briefly described, and some publications resulting from the research are listed. (WHK)

  2. Ultrafast pump-probe ellipsometry setup for the measurement of transient optical properties during laser ablation.

    PubMed

    Rapp, Stephan; Kaiser, Michael; Schmidt, Michael; Huber, Heinz P

    2016-08-01

    Ultrashort pulsed lasers offer a high potential in precise and efficient material processing and deep understanding of the fundamental laser-material interaction aspects is of great importance. The transient pulse reflectivity in conjunction with the transient absorption influences decisively the laser-material interaction. Direct measurements of the absorption properties by ultrafast time-resolved ellipsometry are missing to date. In this work, a unique pump-probe ellipsometry microscope is presented allowing the determination of the transient complex refractive index with a sub-ps temporal resolution. Measurements on molybdenum show ultrafast optical penetration depth changes of -6% to + 77% already within the first 10 ps after the laser pulse impact. This indicates a significant absorption variation of the pump pulse or subsequent pulses irradiating the sample on this timescale and paves the road towards a better understanding of pulse duration dependent laser ablation efficiency, double or burst mode laser ablation and lattice modifications in the first ps after the laser pulse impact. PMID:27505728

  3. Probing ultrafast molecular dynamics in O2 using XUV/IR pump-probe studies

    NASA Astrophysics Data System (ADS)

    Ray, D.; Sturm, F. P.; Wright, T. W.; Ranitovic, P.; Shivaram, N. H.; Bocharova, I.; Belkacem, A.; Weber, Th.

    2015-05-01

    We investigate the molecular dynamics via different dissociative and autoionizing pathways in molecular oxygen using a pump-probe scheme with ultrashort extreme ultraviolet (XUV) laser pulses. Our primary focus is to study the molecular dynamics in the superexcited Rydberg states in a time-resolved manner. The O2 molecules are pumped by 20.2 eV and 23.1 eV XUV pulses (13th and 15th harmonics). Probing the relaxation dynamics with an infrared (IR) pulse at very long delays (100s of fs) enables us to measure the lifetimes of these Rydberg states. We also observe an enhancement and suppression of vibrational levels of the O2+ion due to the presence of IR. The high flux XUV pulses used for this experiment are generated in an Ar gas by IR pulses from our state-of-the-art 30 mJ, 50 Hz laser system. The pulses are overlapped with the supersonic jet in our Momentum Imaging for TimE Resolved Studies (MISTERS) setup. The cold target in our setup, combined with a very tight focussing geometry and a 3D momentum detection capability gives a high kinetic energy resolution. Molecular dynamics in other polyatomic molecules are also under investigation. Chemical Sciences Division, Lawrence Berkeley National Laboratory.

  4. Exciton and Trion Valley dynamics in WSe2 measured by two-color pump-probe

    NASA Astrophysics Data System (ADS)

    Singh, Akshay; Tran, Kha; Seifert, Joe; Wang, Yiping; Scott, Marie; Pleskot, Dennis; Gabor, Nathaniel; Yan, Jiaqiang; Mandrus, David; Xu, Xiaodong; Li, Xiaoqin

    Monolayer transition metal dichalcogenides are semiconducting materials demonstrating spin-valley coupling as well as quasiparticles with large binding energies. These quasiparticles, excitons and trions (charged excitons), have quite different spin polarization properties, with the trion having larger spin lifetimes than excitons. Photoluminescence and time resolved Kerr rotation techniques have been used earlier to measure spin lifetimes. However, most of these early optical measurements have relied on non-resonant excitation conditions which tend to mask the intrinsic valley (spin) scattering properties. Here, we use circularly polarized two-color pump probe spectroscopy to measure valley (spin) polarization in monolayer WSe2 at low temperatures. We utilize quasi-resonant excitation with pump 1 meV (0.5 nm) spectrally separated from the probe, thus resulting in very efficient valley initialization. We present polarization resolved measurements on resonantly excited excitons and trions, which suggest that trions have larger spin lifetimes. Further, we probe spin polarization of trions when pumping at exciton energies, and vice-versa. We discuss the relative importance of different scattering mechanism at play. We acknowledge support from ARO and AFOSR.

  5. Ultrafast dynamics in pentacene and tetracene probed using optical pump-probe spectroscopy

    NASA Astrophysics Data System (ADS)

    Thorsmølle, Verner; Averitt, Richard; Demsar, Jure; Chi, Xiaoliu; Tretiak, Sergie; Ramirez, Arthur; Taylor, Antoinette

    2004-03-01

    Here we present optical pump-probe measurements of photoinduced (PI) changes in the reflectivity and transmissivity of tetracene and pentacene single crystals. We studied the carrier relaxation dynamics as a function of probe photon energy aiming to elucidate the electronic structure and carrier dynamics in the singlet and triplet manifolds. We observe singlet exciton recombination, singlet fission, and triplet state absorption, which we can identify in the photoinduced (PI) absorption spectrum. In particular, both compounds display a broad long-lived (>>1ns) PI absorption. In tetracene this feature is centered at approximately 1.7 eV, while in pentacene it is centered around 1.4 eV and is very pronounced. The long relaxation time suggests that the state being probed is the triplet state T1 (i.e. T1->Tn). On the other hand, the width of the PI absorption band suggests that the final state is a band-like state at 1.7 eV (1.4 eV) above the triplet state in tetracene (pentacene). This observation supports the semiconductor band model.

  6. Indirect monitoring shot-to-shot shock waves strength reproducibility during pump-probe experiments

    NASA Astrophysics Data System (ADS)

    Pikuz, T. A.; Faenov, A. Ya.; Ozaki, N.; Hartley, N. J.; Albertazzi, B.; Matsuoka, T.; Takahashi, K.; Habara, H.; Tange, Y.; Matsuyama, S.; Yamauchi, K.; Ochante, R.; Sueda, K.; Sakata, O.; Sekine, T.; Sato, T.; Umeda, Y.; Inubushi, Y.; Yabuuchi, T.; Togashi, T.; Katayama, T.; Yabashi, M.; Harmand, M.; Morard, G.; Koenig, M.; Zhakhovsky, V.; Inogamov, N.; Safronova, A. S.; Stafford, A.; Skobelev, I. Yu.; Pikuz, S. A.; Okuchi, T.; Seto, Y.; Tanaka, K. A.; Ishikawa, T.; Kodama, R.

    2016-07-01

    We present an indirect method of estimating the strength of a shock wave, allowing on line monitoring of its reproducibility in each laser shot. This method is based on a shot-to-shot measurement of the X-ray emission from the ablated plasma by a high resolution, spatially resolved focusing spectrometer. An optical pump laser with energy of 1.0 J and pulse duration of ˜660 ps was used to irradiate solid targets or foils with various thicknesses containing Oxygen, Aluminum, Iron, and Tantalum. The high sensitivity and resolving power of the X-ray spectrometer allowed spectra to be obtained on each laser shot and to control fluctuations of the spectral intensity emitted by different plasmas with an accuracy of ˜2%, implying an accuracy in the derived electron plasma temperature of 5%-10% in pump-probe high energy density science experiments. At nano- and sub-nanosecond duration of laser pulse with relatively low laser intensities and ratio Z/A ˜ 0.5, the electron temperature follows Te ˜ Ilas2/3. Thus, measurements of the electron plasma temperature allow indirect estimation of the laser flux on the target and control its shot-to-shot fluctuation. Knowing the laser flux intensity and its fluctuation gives us the possibility of monitoring shot-to-shot reproducibility of shock wave strength generation with high accuracy.

  7. Ultrafast pump-probe spectroscopy of the photoreceptor stentorins from the ciliate stentor coeruleus

    SciTech Connect

    Savikhin, S.; Struve, W.S. ); Tao, N.; Song, P.S. )

    1993-11-25

    Polarized absorption difference profiles have been obtained with 3-6-ps resolution between 565 and 630 nm for the chromoproteins stentorin I and stentorin II, isolated from the protozoan ciliate Stentor coeruleus. Control experiments were performed on hypericin and on the stentorin chromophore in methanol. The isotropic decays of stentorin I and the stentorin chromophore are dominated by components with lifetimes conservatively longer than 1 ns. Stentorin I, the stentorin chromophore, and hypericin all develop, within <5 ps, an intense excited-state absorption band that is blue-shifted from and polarized essentially perpendicular to the main long-wavelength absorption band. The presence of this excited-state absorption band is signaled by the appearance of strongly wavelength-dependent initial anisotropies r(0), which assume large positive as well as negative values (>0.4 and <[minus]0.2). To our knowledge, such anisotropies have not been reported in polarized pump-probe studies of rotational diffusion in solution or of energy-transfer kinetics in photosynthetic antennae. Hypericin itself exhibits 0.4-6-ps excited-state absorption decay kinetics, which are likely associated with intramolecular excited-state proton transfer. 19 refs., 8 figs., 5 tabs.

  8. Nematicity in FeSe single crystals probed by pump-probe spectroscopy

    NASA Astrophysics Data System (ADS)

    Luo, C. W.; Cheng, P. C.; Wu, K. H.; Juang, J. Y.; Wang, S.-H.; Chiang, J.-C.; Lin, J.-Y.; Chareev, D. A.; Volkova, O. S.; Vasiliev, A. N.

    The anisotropic quasiparticle dynamics in FeSe single crystals have been studied by polarized pump-probe spectroscopy. Two distinguishable relaxation components were unambiguously observed in transient reflectivity changes (ΔR / R) . The orientation-dependent fast component with the timescale of 0.1-1.5 ps associated with the electronic structure clearly shows two-fold symmetry, which further reveals the gap opening along ky below the temperature of structure phase transition (Ts) and the electronic nematicity can persist up to 200 K. For the slow component with the timescale of 8-25 ps, it is assigned to the energy relaxation through spin sub-system and also shows a two-fold symmetry below Ts. However, this two-fold symmetry is dramatically weakened above Ts and surprisingly persists up to at least 200 K. Consequently, the high-temperature nematic fluctuations in FeSe may be driven by the order parameters which associated with both charge (orbital) and spin sub-systems. This project is financially sponsored by the MOST, Taiwan, (Grants No. 103-2923-M-009-001-MY3) and the MOE-ATU plan at NCTU.

  9. Pump-probe optical coherence tomography using microencapsulated methylene blue as a contrast agent (Conference Presentation)

    NASA Astrophysics Data System (ADS)

    Kim, Wihan; Zebrowski, Erin; Lopez, Hazel C.; Applegate, Brian E.; Charoenphol, Phapanin; Jo, Javier A.

    2016-03-01

    Molecular contrast imaging can target specific molecules or receptors to provide detailed information on the local biochemistry and yield enhanced visualization of pathological and physiological processes. When paired with Optical Coherence Tomography (OCT) it can simultaneously supply the morphological context for the molecular information. We recently demonstrated in vivo molecular contrast imaging of methylene blue (MB) using a 663 nm diode laser as a pump in a Pump-Probe OCT (PPOCT) system. The simple addition of a dichroic mirror in the sample arm enabled PPOCT imaging with a typical 830-nm band spectral-domain OCT system. Here we report on the development of a microencapsulated MB contrast agent. The poly lactic-co-glycolic acid (PLGA) microspheres loaded with MB offer several advantages over bare MB. The microsphere encapsulation improves the PPOCT signal both by enhancing the scattering and preventing the reduction of MB to leucomethylene blue. The surface of the microsphere can readily be functionalized to enable active targeting of the contrast agent without modifying the excited state dynamics of MB that enable PPOCT imaging. Both MB and PLGA are used clinically. PLGA is FDA approved and used in drug delivery and tissue engineering applications. 2.5 μm diameter microspheres were synthesized with an inner core containing 0.01% (w/v) aqueous MB. As an initial demonstration the MB microspheres were imaged in a 100 μm diameter capillary tube submerged in a 1% intralipid emulsion.

  10. Hyperfine Quantum Beat Spectroscopy of the Cs 8p level with Pulsed Pump-Probe Technique

    NASA Astrophysics Data System (ADS)

    Bayram, Burcin; Popov, Oleg; Kelly, Stephen; Boyle, Patrick; Salsman, Andrew

    2013-05-01

    Quantum beats arising from the hyperfine interaction were measured in a three-level excitation (lambda) scheme: pump for the 6s2S1 / 2 --> 8p2P3 / 2 and stimulated emission pump (probe) for the 8p2P3 / 2 --> 5d2D5 / 2 transitions of atomic cesium. In the technique, pump laser instantaneously excites the hot atomic vapor and creates anisotropy in the 8p2P3 / 2 level, and probe laser comes after some time delay. Delaying the probe time allows us to map out the motion of the polarized atoms like a stroboscope. According to the observed evolution of the hyperfine structure dependent parameters, e.g. alignment and atomic polarization, by delaying the arrival time of the stimulated emission pump laser (SEP), precise values of the magnetic dipole and electric quadrupole coefficients are obtained with an improved precision over previous results. The usefulness of the PUMP-SEP excitation scheme for the polarization hyperfine quantum beat measurements without complications from the Doppler effect will also be discussed. The financial support of the Research Corporation under the Grant number CC7133 and MiamiUniversity, College of the Arts and Sciences are acknowledged.

  11. Disentangling Multichannel Photodissociation Dynamics in Acetone by Time-Resolved Photoelectron-Photoion Coincidence Spectroscopy.

    PubMed

    Maierhofer, Paul; Bainschab, Markus; Thaler, Bernhard; Heim, Pascal; Ernst, Wolfgang E; Koch, Markus

    2016-08-18

    For the investigation of photoinduced dynamics in molecules with time-resolved pump-probe photoionization spectroscopy, it is essential to obtain unequivocal information about the fragmentation behavior induced by the laser pulses. We present time-resolved photoelectron-photoion coincidence (PEPICO) experiments to investigate the excited-state dynamics of isolated acetone molecules triggered by two-photon (269 nm) excitation. In the complex situation of different relaxation pathways, we unambiguously identify three distinct pump-probe ionization channels. The high selectivity of PEPICO detection allows us to observe the fragmentation behavior and to follow the time evolution of each channel separately. For channels leading to fragment ions, we quantitatively obtain the fragment-to-parent branching ratio and are able to determine experimentally whether dissociation occurs in the neutral molecule or in the parent ion. These results highlight the importance of coincidence detection for the interpretation of time-resolved photochemical relaxation and dissociation studies if multiple pathways are present. PMID:27459051

  12. Discriminating Bio-aerosols from Non-Bio-aerosols in Real-Time by Pump-Probe Spectroscopy.

    PubMed

    Sousa, Gustavo; Gaulier, Geoffrey; Bonacina, Luigi; Wolf, Jean-Pierre

    2016-01-01

    The optical identification of bioaerosols in the atmosphere and its discrimination against combustion related particles is a major issue for real-time, field compatible instruments. In the present paper, we show that by embedding advanced pump-probe depletion spectroscopy schemes in a portable instrument, it is possible to discriminate amino acid containing airborne particles (bacteria, humic particles, etc.) from poly-cyclic aromatic hydrocarbon containing combustion particles (Diesel droplets, soot, vehicle exhausts) with high selectivity. Our real-time, multi-modal device provides, in addition to the pump-probe depletion information, fluorescence spectra (over 32 channels), fluorescence lifetime and Mie scattering patterns of each individually flowing particle in the probed air. PMID:27619546

  13. In vivo pump-probe microscopy of melanoma: characterizing shifts in excited state photodynamics with respect to invasiveness

    NASA Astrophysics Data System (ADS)

    Wilson, Jesse W.; Degan, Simone; Gainey, Christina S.; Deb, Sanghamitra; Dall, Christopher P.; Tameze-Rivas, Yasmine; Zhang, Jennifer; Warren, Warren S.

    2015-03-01

    Pump-probe microscopy is a multiphoton technique that generates molecular contrast from absorptive pigments, such as melanin. It holds the potential to be used as a non-invasive screening tool to discern whether a given early-stage melanoma has acquired the capacity for metastasis. Here, we examined lesions in a Braf(V600E)-driven model of melanoma to assess whether loss of the tumor suppressor gene Pten in a is accompanied by a shift in pigment expression, as measured in vivo by pump-probe microscopy. The data were analyzed to determine differences in the excited-state lifetime of melanins expressed in Pten-competent and Pten-loss pigmented lesions. Loss of the tumor suppressor Pten was found to be accompanied by a statistically significant decrease in pixel-average excited state lifetime (p = 1.3e-4).

  14. Comparison of a near-field ferromagnetic resonance probe with pump-probe characterization of CoCrPt media

    NASA Astrophysics Data System (ADS)

    Clinton, T. W.; Benatmane, Nadjib; Hohlfeld, J.; Girt, Erol

    2008-04-01

    A near-field microwave technique is used to locally probe ferromagnetic resonance (FMR) in a series of CoCrPt alloys with varying perpendicular anisotropy (5kOepump-probe technique, where we observe relaxation times τ, considerably shorter than 500ps, using a damped sinusoid to model the magnetization dynamics. We find the local FMR measurements to yield time scales consistent with the pump-probe data, using the Fourier relationship, Δf =1/πτ. Thus, this near-field technique is capable of quantitative characterization of high-anisotropy and highly damped magnetic systems, something that has not been demonstrated before with a local FMR technique.

  15. Rate-equation model for quantitative concentration measurements in flames with picosecond pump-probe absorption spectroscopy.

    PubMed

    Fiechtner, G J; King, G B; Laurendeau, N M

    1995-02-20

    Measurement of radical concentrations is important in understanding the chemical kinetics involved in combustion. Application of optical techniques allows for the nonintrusive determination of specific radical concentrations. One of the most challenging problems for investigators is to obtain flame data that are independent of the collisional environment. We seek to obviate this difficulty by the use of picosecond pump-probe absorption spectroscopy. A picosecond pump-probe absorption model is developed by rate-equation analysis. Implications are discussed for a laser-pulse width that is much smaller than the excited-state lifetime of the absorbing atom or molecule. The possibility of quantitative, quenching-independent concentration measurements is discussed, and detection limits for atomic sodium and the hydroxyl radical are estimated. For a three-level absorber-emitter, the model leads to a novel pump-probe strategy, called dual-beam asynchronous optical sampling, that can be used to obtain both the electronic quenching-rate coefficient and the doublet mixing-rate coefficient during a single measurement. We discuss the successful demonstration of the technique in a companion paper [Appl. Opt. 34, XXX (1995)]. PMID:21037640

  16. Tracking speed bumps in organic field-effect transistors via pump-probe Kelvin-probe force microscopy

    NASA Astrophysics Data System (ADS)

    Murawski, J.; Mönch, T.; Milde, P.; Hein, M. P.; Nicht, S.; Zerweck-Trogisch, U.; Eng, L. M.

    2015-12-01

    One of the great challenges in designing modern organic field-effect transistors is lowering the injection barriers that arise at the interfaces between the metallic electrodes and the semiconducting transport channel. Currently, these barriers are quantified mostly by time-independent and external inspection, techniques lacking temporal insight into the most relevant switching dynamics. We address this problem here by pump-probe Kelvin-probe force microscopy, which combines the high spatial resolution of standard Kelvin-probe force microscopy with a pump-probe, enabling time resolution down to nanoseconds. When investigating a dynamically operated pentacene-based organic field-effect transistor, pump-probe Kelvin-probe force microscopy is capable of in-situ probing the temporal charge evolution at any sample spot within the device. Thus, Schottky-barriers arising at the boundaries between electrodes and transport channel are identified as speed bumps for high-speed organic field-effect transistor operation, manifested by residual charges that are retained within the organic film upon switching the device.

  17. Measurement of femtosecond atomic lifetimes using ion traps

    NASA Astrophysics Data System (ADS)

    Träbert, Elmar

    2014-01-01

    Two types of experiment are described that both employ an electron beam ion trap for the production of highly charged ion species with the aim of then measuring atomic level lifetimes in the femtosecond range. In one experiment (done by Beiersdorfer et al. some time ago), the lifetime measurement depends on the associated line broadening. In a recent string of experiments at Linac Coherent Light Source Stanford, the HI-LIGHT collaboration employed pump-probe excitation using the FEL as a short-pulse X-ray laser.

  18. Femtosecond Studies of Carrier Dynamics in GaN

    NASA Astrophysics Data System (ADS)

    Zhang, Zhuhong; Zeng, Wensheng; Xu, Su; Makinen, Antti J.; Wicks, Gary W.; Gao, Yongli

    1998-03-01

    Ultrafast carrier dynamics were measured in GaN by femtosecond two-color pump-probe technique with 150fs resolution. Undoped wurtzite GaN sample studied in this work was grown by moecular beam epitaxy on a (0001)-oriented sapphire substrate. Third harmonic wave from Ti:sapphire Regen was employed as pump and second harmonic as probe. Transient transmission measurement shows the electron-phonon scattering and longitutal optical phonons relaxation. A simply two temperature model is used to explain the results.

  19. Femtosecond time-resolved dynamical Franz-Keldysh effect

    NASA Astrophysics Data System (ADS)

    Otobe, T.; Shinohara, Y.; Sato, S. A.; Yabana, K.

    2016-01-01

    We theoretically investigate the dynamical Franz-Keldysh effect in femtosecond time resolution, that is, the time-dependent modulation of a dielectric function at around the band gap under an irradiation of an intense laser field. We develop a pump-probe formalism in two distinct approaches: first-principles simulation based on real-time time-dependent density functional theory and analytic consideration of a simple two-band model. We find that, while time-average modulation can be reasonably described by the static Franz-Keldysh theory, a remarkable phase shift is found to appear between the dielectric response and the applied electric field.

  20. Photoionization and Recombination

    NASA Technical Reports Server (NTRS)

    Nahar, Sultana N.

    2000-01-01

    Theoretically self-consistent calculations for photoionization and (e + ion) recombination are described. The same eigenfunction expansion for the ion is employed in coupled channel calculations for both processes, thus ensuring consistency between cross sections and rates. The theoretical treatment of (e + ion) recombination subsumes both the non-resonant recombination ("radiative recombination"), and the resonant recombination ("di-electronic recombination") processes in a unified scheme. In addition to the total, unified recombination rates, level-specific recombination rates and photoionization cross sections are obtained for a large number of atomic levels. Both relativistic Breit-Pauli, and non-relativistic LS coupling, calculations are carried out in the close coupling approximation using the R-matrix method. Although the calculations are computationally intensive, they yield nearly all photoionization and recombination parameters needed for astrophysical photoionization models with higher precision than hitherto possible, estimated at about 10-20% from comparison with experimentally available data (including experimentally derived DR rates). Results are electronically available for over 40 atoms and ions. Photoionization and recombination of He-, and Li-like C and Fe are described for X-ray modeling. The unified method yields total and complete (e+ion) recombination rate coefficients, that can not otherwise be obtained theoretically or experimentally.

  1. Ultrafast Multiphoton Pump-probe Photoemission Excitation Pathways in Rutile TiO2(110)

    SciTech Connect

    Argondizzo, Adam; Cui, Xuefeng; Wang, Cong; Sun, Huijuan; Shang, Honghui; Zhao, Jin; Petek, Hrvoje

    2015-04-27

    We investigate the spectroscopy and photoinduced electron dynamics within the conduction band of reduced rutile TiO2(110) surface by multiphoton photoemission (mPP) spectroscopy with wavelength tunable ultrafast (!20 fs) laser pulse excitation. Tuning the mPP photon excitation energy between 2.9 and 4.6 eV reveals a nearly degenerate pair of new unoccupied states located at 2.73 ± 0.05 and 2.85 ± 0.05 eV above the Fermi level, which can be analyzed through the polarization and sample azimuthal orientation dependence of the mPP spectra. Based on the calculated electronic structure and optical transition moments, as well as related spectroscopic evidence, we assign these resonances to transitions between Ti 3d bands of nominally t2g and eg symmetry, which are split by crystal field. The initial states for the optical transition are the reduced Ti3+ states of t2g symmetry populated by formation oxygen vacancy defects, which exist within the band gap of TiO2. Furthermore,we studied the electron dynamics within the conduction band of TiO2 by three-dimensional time-resolved pump-probe interferometric mPP measurements. The spectroscopic and time-resolved studies reveal competition between 2PP and 3PP processes where the t2g-eg transitions in the 2PP process saturate, and are overtaken by the 3PP process initiated by the band-gap excitation from the valence band of TiO2.

  2. Reduced-density-matrix description for pump-probe optical phenomena in moving atomic systems

    NASA Astrophysics Data System (ADS)

    Jacobs, V. L.

    2014-09-01

    Linear and nonlinear (especially coherent) electromagnetic interactions of moving many-electron atoms are investigated using a reduced-density-matrix description, which is applied to electromagnetically induced transparency and related resonant pump-probe optical phenomena. External magnetic fields are included on an equal footing with the electromagnetic fields and spin-Zeeman interactions are taken into account. Complimentary time-domain (equation-of-motion) and frequency-domain (resolvent-operator) formulations of the reduced-density-matrix description are self-consistently developed. The general nonperturbative and non-Markovian formulations provide a fundamental framework for systematic evaluations of corrections to the standard Born (lowest-order-perturbation) and Markov (short-memory-time) approximations. The macroscopic electromagnetic response is described semiclassically, employing a perturbation expansion of the reduced-density operator in powers of the classical electromagnetic field. Our primary results are compact Liouville-space operator expressions for the linear and general (nth-order) nonlinear macroscopic electromagnetic-response tensors, which can be evaluated for nonlocal and nonstationary optical media described by multilevel atomic-system representations. Interactions among atoms and with environmental photons are treated as line-broadening effects by means of a general Liouville-space self-energy operator, for which the tetradic-matrix elements are explicitly evaluated in the diagonal, lowest-order, and Markov approximations. The compact Liouville-space operator expressions that are derived for the macroscopic electromagnetic-response tensors are introduced into the dynamical description of the electromagnetic-field propagation. It is pointed out that a quantized-electromagnetic-field approach will be required for a fully self-consistent quantum-mechanical treatment of local-field effects and radiative corrections.

  3. A novel electro-optical pump-probe system for bioelectromagnetic investigations

    NASA Astrophysics Data System (ADS)

    De Angelis, Annalisa; Couderc, Vincent; Leproux, Philippe; Labruyère, Alexis; Tonello, Alessandro; El Amari, Saad; Arnaud-Cormos, Delia; Leveque, Philippe

    2012-10-01

    In the area of bioelectromagnetic studies there is a growing interest to understand the mechanisms leading to nanosecond electric fields induced electroporation. Real-time imaging techniques at molecular level could probably bring further advances on how electric fields interact with living cells. However the investigations are limited by the present-day lack of these kinds of advanced instrumentations. In this context, we present an innovative electro-optical pump-probe system. The aim of our project is to provide a performing and compact device for electrical stimulation and multiplex Coherent anti-Stokes Raman Scattering (M-CARS) imaging of biological cells at once. The system consists of a 1064 nm sub-nanosecond laser source providing both a monochromatic pump and a polychromatic Stokes optical beam used in a CARS process, as well as the trigger beam for the optoelectronic switching-based electrical pulse generator. The polychromatic Stokes beam (from 600 to 1700 nm) results from a supercontinuum generation in a photonic crystal fiber (PCF). A detailed spectro-temporal characterization of such a broadband spectrum shows the impact of the nonlinear propagation in the fiber on the Stokes wave. Despite the temporal distortions observable on Stokes pulse profiles, their spectral synchronization with the pump pulse remains possible and efficient in the interesting region between 1100 nm and 1700 nm. The electrical stimulation device consists of a customized generator combining microstrip-line technology and laser-triggered photoconductive semiconductor switches. Our experimental characterization highlights the capability for such a generator to control the main pulse parameters (profile, amplitude and duration) and to be easily synchronized with the imaging system. We finally test and calibrate the system by means of a KDP crystal. The preliminary results suggest that this electro-optical system provides a suitable tool for real-time investigation of

  4. Time-resolved shadowgraphs of transient plasma induced by spatiotemporally focused femtosecond laser pulses in fused silica glass.

    PubMed

    Wang, Zhaohui; Zeng, Bin; Li, Guihua; Xie, Hongqiang; Chu, Wei; He, Fei; Liao, Yang; Liu, Weiwei; Gao, Hui; Cheng, Ya

    2015-12-15

    We report on experimental observations of formation and evolution of transient plasma produced in fused silica glass with spatiotemporally focused (STF) femtosecond laser pulses using a pump-probe shadow imaging technique. Surprisingly, the observation shows that the track of the plasma is significantly curved, which is attributed to an asymmetric density distribution of the transient plasma produced in the focal volume caused by the pulse front tilt of the STF laser field. PMID:26670497

  5. Molecular photoionization studies

    SciTech Connect

    Dehmer, P.M.

    1983-01-01

    This program is concerned with the study of the electronic structure of small molecules and clusters of molecules. Of particular interest is the interaction of discrete electronic states with one another and with the various ionization and dissociation continua. Since the Second Annual Meeting of the DOE-OHER Program on The Physics and Chemistry of Energy-Related Atmospheric Pollutants in April 1981, significant progress has been made in the following areas: (1) the study of the electronic structure of dimers and small clusters of rare gas atoms using photoionization techniques; (2) similar studies on clusters of CO/sub 2/ molecules; (3) the study of electronic structure of rare gas dimers and trimers using photoelectron and photoelectron-photoion coincidence techniques; (4) the investigation of the relationship between Rydberg states in atoms, van der Waals molecules, and chemically-bonded molecules; (5) the extension of the study of photoabsorption, photoionization, and predissociation processes in H/sub 2/ to the unsymmetric isotope HD; (6) the study of photoelectron spectra of H/sub 2/ and C/sub 2/H/sub 2/; (7) a review of some of the aspects of dissociation processes in small molecules; and (8) the creation of a new program to study the spectra and dynamics of the photoionization processes in small molecules using the technique of multiphoton ionization followed by mass and electron energy analysis of the product ions and electrons. Some of the highlights of this work are reviewed.

  6. Photoionization-photoelectron research

    SciTech Connect

    Berkowitz, J.; Ruscic, B.

    1993-12-01

    The photoionization research program is aimed at understanding the basic processes of interaction of vacuum ultraviolet (VUV) light with atoms and molecules. This research provides valuable information on both thermochemistry and dynamics. Recent studies include atoms, clusters, hydrides, sulfides and an important fluoride.

  7. Femtosecond nonlinear optical properties of carbon nanoparticles

    NASA Astrophysics Data System (ADS)

    Li, Dan; Liu, Ye; Yang, Heqing; Qian, Shixiong

    2002-09-01

    The nonlinear optical properties and ultrafast electron-relaxation dynamics of carbon nanoparticles were investigated by using the femtosecond optical Kerr effect and pump-probe techniques. The blueshift of the absorption edge with the decrease of the size of the nanoparticles reveals the opening of the gap. The magnitude of chi(3) for carbon nanoparticles is calculated to be 8.3 x10-13 esu, which arises from the contribution of delocalized feature of the pi electrons. The decay of photobleaching includes a fast and a slow component, which are assigned to the relaxation of the free carriers and trapped carriers, respectively. It is found that the lifetimes of two components of bleaching decrease as temperature of heat treatment is increased.

  8. Theoretical Simulations and Ultrafast Pump-probe Spectroscopy Experiments in Pigment-protein Photosynthetic Complexes

    SciTech Connect

    Buck, D.R.

    2000-09-12

    Theoretical simulations and ultrafast pump-probe laser spectroscopy experiments were used to study photosynthetic pigment-protein complexes and antennae found in green sulfur bacteria such as Prosthecochloris aestuarii, Chloroflexus aurantiacus, and Chlorobium tepidum. The work focused on understanding structure-function relationships in energy transfer processes in these complexes through experiments and trying to model that data as we tested our theoretical assumptions with calculations. Theoretical exciton calculations on tubular pigment aggregates yield electronic absorption spectra that are superimpositions of linear J-aggregate spectra. The electronic spectroscopy of BChl c/d/e antennae in light harvesting chlorosomes from Chloroflexus aurantiacus differs considerably from J-aggregate spectra. Strong symmetry breaking is needed if we hope to simulate the absorption spectra of the BChl c antenna. The theory for simulating absorption difference spectra in strongly coupled photosynthetic antenna is described, first for a relatively simple heterodimer, then for the general N-pigment system. The theory is applied to the Fenna-Matthews-Olson (FMO) BChl a protein trimers from Prosthecochloris aestuarii and then compared with experimental low-temperature absorption difference spectra of FMO trimers from Chlorobium tepidum. Circular dichroism spectra of the FMO trimer are unusually sensitive to diagonal energy disorder. Substantial differences occur between CD spectra in exciton simulations performed with and without realistic inhomogeneous distribution functions for the input pigment diagonal energies. Anisotropic absorption difference spectroscopy measurements are less consistent with 21-pigment trimer simulations than 7-pigment monomer simulations which assume that the laser-prepared states are localized within a subunit of the trimer. Experimental anisotropies from real samples likely arise from statistical averaging over states with diagonal energies shifted by

  9. Femtosecond laser lithotripsy: feasibility and ablation mechanism

    NASA Astrophysics Data System (ADS)

    Qiu, Jinze; Teichman, Joel M. H.; Wang, Tianyi; Neev, Joseph; Glickman, Randolph D.; Chan, Kin Foong; Milner, Thomas E.

    2010-03-01

    Light emitted from a femtosecond laser is capable of plasma-induced ablation of various materials. We tested the feasibility of utilizing femtosecond-pulsed laser radiation (λ=800 nm, 140 fs, 0.9 mJ/pulse) for ablation of urinary calculi. Ablation craters were observed in human calculi of greater than 90% calcium oxalate monohydrate (COM), cystine (CYST), or magnesium ammonium phosphate hexahydrate (MAPH). Largest crater volumes were achieved on CYST stones, among the most difficult stones to fragment using Holmium:YAG (Ho:YAG) lithotripsy. Diameter of debris was characterized using optical microscopy and found to be less than 20 μm, substantially smaller than that produced by long-pulsed Ho:YAG ablation. Stone retropulsion, monitored by a high-speed camera system with a spatial resolution of 15 μm, was negligible for stones with mass as small as 0.06 g. Peak shock wave pressures were less than 2 bars, measured by a polyvinylidene fluoride (PVDF) needle hydrophone. Ablation dynamics were visualized and characterized with pump-probe imaging and fast flash photography and correlated to shock wave pressures. Because femtosecond-pulsed laser ablates urinary calculi of soft and hard compositions, with micron-sized debris, negligible stone retropulsion, and small shock wave pressures, we conclude that the approach is a promising candidate technique for lithotripsy.

  10. Bases for time-resolved probing of transient carrier dynamics by optical pump-probe scanning tunneling microscopy

    NASA Astrophysics Data System (ADS)

    Yokota, Munenori; Yoshida, Shoji; Mera, Yutaka; Takeuchi, Osamu; Oigawa, Haruhiro; Shigekawa, Hidemi

    2013-09-01

    The tangled mechanism that produces optical pump-probe scanning tunneling microscopy spectra from semiconductors was analyzed by comparing model simulation data with experimental data. The nonlinearities reflected in the spectra, namely, the excitations generated by paired laser pulses with a delay time, the logarithmic relationship between carrier density and surface photovoltage (SPV), and the effect of the change in tunneling barrier height depending on SPV, were examined along with the delay-time-dependent integration process used in measurement. The optimum conditions required to realize reliable measurement, as well as the validity of the microscopy technique, were demonstrated for the first time.

  11. Vibrational spectroscopy of water in hydrated lipid multi-bilayers. I. Infrared spectra and ultrafast pump-probe observables

    PubMed Central

    Gruenbaum, S. M.; Skinner, J. L.

    2011-01-01

    The vibrational spectroscopy of hydration water in dilauroylphosphatidylcholine lipid multi-bilayers is investigated using molecular dynamics simulations and a mixed quantum∕classical model for the OD stretch spectroscopy of dilute HDO in H2O. FTIR absorption spectra, and isotropic and anisotropic pump-probe decay curves have been measured experimentally as a function of the hydration level of the lipid multi-bilayer, and our goal is to make connection with these experiments. To this end, we use third-order response functions, which allow us to include non-Gaussian frequency fluctuations, non-Condon effects, molecular rotations, and a fluctuating vibrational lifetime, all of which we believe are important for this system. We calculate the response functions using existing transition frequency and dipole maps. From the experiments it appears that there are two distinct vibrational lifetimes corresponding to HDO molecules in different molecular environments. In order to obtain these lifetimes, we consider a simple two-population model for hydration water hydrogen bonds. Assuming a different lifetime for each population, we then calculate the isotropic pump-probe decay, fitting to experiment to obtain the two lifetimes for each hydration level. With these lifetimes in hand, we then calculate FTIR spectra and pump-probe anisotropy decay as a function of hydration. This approach, therefore, permits a consistent calculation of all observables within a unified computational scheme. Our theoretical results are all in qualitative agreement with experiment. The vibrational lifetime of lipid-associated OD groups is found to be systematically shorter than that of the water-associated population, and the lifetimes of each population increase with decreasing hydration, in agreement with previous analysis. Our theoretical FTIR absorption spectra successfully reproduce the experimentally observed red-shift with decreasing lipid hydration, and we confirm a previous interpretation

  12. Optical synchronization system for femtosecond X-ray sources

    DOEpatents

    Wilcox, Russell B.; Holzwarth, Ronald

    2011-12-13

    Femtosecond pump/probe experiments using short X-Ray and optical pulses require precise synchronization between 100 meter-10 km separated lasers in a various experiments. For stabilization in the hundred femtosecond range a CW laser is amplitude modulated at 1-10 GHz, the signal retroreflected from the far end, and the relative phase used to correct the transit time with various implementations. For the sub-10 fsec range the laser frequency itself is upshifted 55 MHz with an acousto-optical modulator, retroreflected, upshifted again and phase compared at the sending end to a 110 MHz reference. Initial experiments indicate less than 1 fsec timing jitter. To lock lasers in the sub-10 fs range two single-frequency lasers separated by several teraHertz will be lock to a master modelocked fiber laser, transmit the two frequencies over fiber, and lock two comb lines of a slave laser to these frequencies, thus synchronizing the two modelocked laser envelopes.

  13. Initial photochemistry of bilirubin probed by femtosecond spectroscopy.

    PubMed

    Zietz, Burkhard; Gillbro, Tomas

    2007-10-18

    Bilirubin is a breakdown product from heme catabolism, and reduced excretion of bilirubin can lead to jaundice. Phototherapy is the most common treatment for neonatal jaundice, a condition frequently encountered in newborn infants. Knowledge of the photochemistry of bilirubin, which is dominated by (ultra)fast components, is necessary for the profound understanding of the processes in phototherapy. Here, we report results from femtosecond fluorescence upconversion measurements on bilirubin and half-bilirubin model compounds, as well as pump-probe absorption measurements on bilirubin. A fast component of ca. 120 fs in the multiexponential fluorescence decay, being only visible in the bilirubin molecule, is interpreted as exciton localization within the molecular halves. The slower components of several hundreds of femtoseconds and a few picoseconds, occurring in bilirubin and the half-bilirubin model, are interpreted as relaxation to a (twisted) intermediate, which decays further with ca. 15 ps to the ground state. PMID:17927274

  14. Technical brief: Pump-probe paradigm in an integrating cavity to study photodecomposition processes

    PubMed Central

    Betts-Obregon, Brandi; Tsin, Andrew T.; DeSa, Richard J.

    2016-01-01

    dark” period allowed actinic flashes to be placed between scans. Exposure of the all-trans retinol to 366 nm flashes resulted in marked reduction in absorbance and a blue shift of the λmax. A white LED, despite its higher photon output, did not support all-trans retinol photolysis. Singular value decomposition (SVD) analysis revealed three spectral intermediates with mechanism, I -> II -> III. HPLC analysis of the reactants at the beginning and the conclusion of the light exposure confirmed the retinol photodecomposition. Conclusions The highly reflecting cavity acts as a multipass cuvette that markedly increased the light path length and, thus, sensitivity. Triggering the LED during a dark period within the scan time allowed the actinic flashes to be interleafed between scans in a pump-probe paradigm. Furthermore, the entire sample was exposed to scan beam and actinic flashes, which is not possible in traditional spectrophotometers. Finally, the integrating cavity cuvette allowed use of turbid samples. SVD was useful for resolving spectral intermediates. Although the identity of the intermediates was not determined here, the ability to define molecular intermediates during photodecomposition reactions will allow future studies to isolate and identify the degradation products and determine the mechanism of light-induced retinoid degradation and that of retinoid-binding protein-mediated photoprotection. PMID:27559291

  15. Photoionization of Li2

    NASA Astrophysics Data System (ADS)

    Li, Y.; Pindzola, M. S.; Ballance, C. P.; Colgan, J.

    2014-05-01

    Single and double photoionization cross sections for Li2 are calculated using a time-dependent close-coupling method. The correlation between the outer two electrons of Li2 is obtained by relaxation of the close-coupled equations in imaginary time. Propagation of the close-coupled equations in real time yields single and double photoionization cross sections for Li2. The two active electron cross sections are compared with one active electron distorted-wave and close-coupling results for both Li and Li2. 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.

  16. Photoionization of argon clusters

    SciTech Connect

    Dehmer, Patricia M.; Pratt, Stephen T.

    1982-01-01

    Argon clusters were produced in a free supersonic molecular beam expansion of pure argon at room temperature and the photoionization efficiency curves of the trimer through hexamer were measured in the wavelength regions from threshold to 700 Â. A study of the Ar⁺3 photoionization efficiency curve as a function of nozzle stagnation pressure shows that fragmentation of heavier clusters can dominate the spectrum, even near threshold, and even when the nozzle conditions are such that the Ar⁺4 intensity is only a small fraction of the Ar⁺3 intensity. The Ar⁺3 photoionization efficiency curve, obtained using nozzle stagnation conditions such that no heavier ions were detected, exhibits several broad peaks near threshold which show similarities to bands of the dimer. At high nozzle stagnation pressures, the photoionization efficiency curves for Ar⁺3 to Ar⁺6 are nearly identical due to the effects of fragmentation. These spectra exhibit two very broad features which are similar to features observed in the solid. The threshold regions for all the positive ions show extremely gradual onsets, making it difficult to determine the appearance potentials accurately. The appearance potentials for Ar⁺2 and Ar⁺3 are 855.0±1.5 and 865.0±1.5 Â, respectively, yielding a value of 0.18±0.05 eV for the dissociation energy of Ar⁺3. The appearance potentials for the heavier clusters Ar⁺4 through Ar⁺6 are all approximately 870±2 Â.

  17. Photocarrier dynamics in anatase TiO{sub 2} investigated by pump-probe absorption spectroscopy

    SciTech Connect

    Matsuzaki, H. E-mail: okamotoh@k.u-tokyo.ac.jp; Matsui, Y.; Uchida, R.; Yada, H.; Terashige, T.; Li, B.-S.; Sawa, A.; Kawasaki, M.; Tokura, Y.; Okamoto, H. E-mail: okamotoh@k.u-tokyo.ac.jp

    2014-02-07

    The dynamics of photogenerated electrons and holes in undoped anatase TiO{sub 2} were studied by femtosecond absorption spectroscopy from the visible to mid-infrared region (0.1–2.0 eV). The transient absorption spectra exhibited clear metallic responses, which were well reproduced by a simple Drude model. No mid-gap absorptions originating from photocarrier localization were observed. The reduced optical mass of the photocarriers obtained from the Drude-model analysis is comparable to theoretically expected one. These results demonstrate that both photogenerated holes and electrons act as mobile carriers in anatase TiO{sub 2}. We also discuss scattering and recombination dynamics of photogenerated electrons and holes on the basis of the time dependence of absorption changes.

  18. Following the dynamics of matter with femtosecond precision using the X-ray streaking method

    DOE PAGESBeta

    David, C.; Karvinen, P.; Sikorski, M.; Song, S.; Vartiainen, I.; Milne, C. J.; Mozzanica, A.; Kayser, Y.; Diaz, A.; Mohacsi, I.; et al

    2015-01-06

    X-ray Free Electron Lasers (FELs) can produce extremely intense and very short pulses, down to below 10 femtoseconds (fs). Among the key applications are ultrafast time-resolved studies of dynamics of matter by observing responses to fast excitation pulses in a pump-probe manner. Detectors with sufficient time resolution for observing these processes are not available. Therefore, such experiments typically measure a sample's full dynamics by repeating multiple pump-probe cycles at different delay times. This conventional method assumes that the sample returns to an identical or very similar state after each cycle. Here we describe a novel approach that can provide amore » time trace of responses following a single excitation pulse, jitter-free, with fs timing precision. We demonstrate, in an X-ray diffraction experiment, how it can be applied to the investigation of ultrafast irreversible processes.« less

  19. Following the dynamics of matter with femtosecond precision using the X-ray streaking method

    SciTech Connect

    David, C.; Karvinen, P.; Sikorski, M.; Song, S.; Vartiainen, I.; Milne, C. J.; Mozzanica, A.; Kayser, Y.; Diaz, A.; Mohacsi, I.; Carini, G. A.; Herrmann, S.; Färm, E.; Ritala, M.; Fritz, D. M.; Robert, A.

    2015-01-06

    X-ray Free Electron Lasers (FELs) can produce extremely intense and very short pulses, down to below 10 femtoseconds (fs). Among the key applications are ultrafast time-resolved studies of dynamics of matter by observing responses to fast excitation pulses in a pump-probe manner. Detectors with sufficient time resolution for observing these processes are not available. Therefore, such experiments typically measure a sample's full dynamics by repeating multiple pump-probe cycles at different delay times. This conventional method assumes that the sample returns to an identical or very similar state after each cycle. Here we describe a novel approach that can provide a time trace of responses following a single excitation pulse, jitter-free, with fs timing precision. We demonstrate, in an X-ray diffraction experiment, how it can be applied to the investigation of ultrafast irreversible processes.

  20. Following the dynamics of matter with femtosecond precision using the X-ray streaking method.

    PubMed

    David, C; Karvinen, P; Sikorski, M; Song, S; Vartiainen, I; Milne, C J; Mozzanica, A; Kayser, Y; Diaz, A; Mohacsi, I; Carini, G A; Herrmann, S; Färm, E; Ritala, M; Fritz, D M; Robert, A

    2015-01-01

    X-ray Free Electron Lasers (FELs) can produce extremely intense and very short pulses, down to below 10 femtoseconds (fs). Among the key applications are ultrafast time-resolved studies of dynamics of matter by observing responses to fast excitation pulses in a pump-probe manner. Detectors with sufficient time resolution for observing these processes are not available. Therefore, such experiments typically measure a sample's full dynamics by repeating multiple pump-probe cycles at different delay times. This conventional method assumes that the sample returns to an identical or very similar state after each cycle. Here we describe a novel approach that can provide a time trace of responses following a single excitation pulse, jitter-free, with fs timing precision. We demonstrate, in an X-ray diffraction experiment, how it can be applied to the investigation of ultrafast irreversible processes. PMID:25561027

  1. Following the dynamics of matter with femtosecond precision using the X-ray streaking method

    PubMed Central

    David, C.; Karvinen, P.; Sikorski, M.; Song, S.; Vartiainen, I.; Milne, C. J.; Mozzanica, A.; Kayser, Y.; Diaz, A.; Mohacsi, I.; Carini, G. A.; Herrmann, S.; Färm, E.; Ritala, M.; Fritz, D. M.; Robert, A.

    2015-01-01

    X-ray Free Electron Lasers (FELs) can produce extremely intense and very short pulses, down to below 10 femtoseconds (fs). Among the key applications are ultrafast time-resolved studies of dynamics of matter by observing responses to fast excitation pulses in a pump-probe manner. Detectors with sufficient time resolution for observing these processes are not available. Therefore, such experiments typically measure a sample's full dynamics by repeating multiple pump-probe cycles at different delay times. This conventional method assumes that the sample returns to an identical or very similar state after each cycle. Here we describe a novel approach that can provide a time trace of responses following a single excitation pulse, jitter-free, with fs timing precision. We demonstrate, in an X-ray diffraction experiment, how it can be applied to the investigation of ultrafast irreversible processes. PMID:25561027

  2. Photoionization of Li

    NASA Astrophysics Data System (ADS)

    Colgan, James

    2011-05-01

    The time-dependent close-coupling approach to multiple photoionization of lithium is presented. Double photoionization of lithium can be treated as a two-electron ejection process where the outgoing electrons move in the field of a ``frozen-core'' Li2+ 1 s state. Recent calculations of this process have resulted in total and triple differential cross sections that are in good agreement with other close-coupling approaches. The time-dependent approach can also be extended to treat the interaction of all three lithium electrons, as is required if triple photoionization is examined, that is, the simultaneous ejection of all three electrons from lithium. The most detailed information about this process is found in the fully angular and energy differential cross sections, which provide information as to how the ionized electrons leave the atom. We present our formulation of the fully differential cross section expression, and provide some convergence studies of the angular distributions. The Los Alamos National Laboratory is operated by Los Alamos National Security, LLC for the National Nuclear Security Administration of the U.S. Department of Energy under Contract No. DE-AC5206NA25396.

  3. Pump-probe studies of radiation induced defects and formation of warm dense matter with pulsed ion beams

    NASA Astrophysics Data System (ADS)

    Schenkel, T.; Persaud, A.; Gua, H.; Seidl, P. A.; Waldron, W. L.; Gilson, E. P.; Kaganovich, I. D.; Davidson, R. C.; Friedman, A.; Barnard, J. J.; Minior, A. M.

    2014-10-01

    We report results from the 2nd generation Neutralized Drift Compression Experiment at Berkeley Lab. NDCX-II is a pulsed, linear induction accelerator designed to drive thin foils to warm dense matter (WDM) states with peak temperatures of ~ 1 eV using intense, short pulses of 1.2 MeV lithium ions. Tunability of the ion beam enables pump-probe studies of radiation effects in solids as a function of excitation density, from isolated collision cascades to the onset of phase-transitions and WDM. Ion channeling is an in situ diagnostic of damage evolution during ion pulses with a sensitivity of <0.1% displacements per atom. We will report results from damage evolution studies in thin silicon crystals with Li + and K + beams. Detection of channeled ions tracks lattice disorder evolution with a resolution of ~ 1 ns using fast current measurements. We will discuss pump-probe experiments with pulsed ion beams and the development of diagnostics for WDM and multi-scale (ms to fs) access to the materials physics of collision cascades e.g. in fusion reactor materials. Work performed under auspices of the US DOE under Contract No. DE-AC02-05CH11231.

  4. Toward single atom qubits on a surface: Pump-probe spectroscopy and electrically-driven spin resonance

    NASA Astrophysics Data System (ADS)

    Paul, William

    We will discuss the characterization of spin dynamics by pump-probe spectroscopy and the use of gigahertz-frequency electric fields to drive spin resonance of a Fe atom on a MgO/Ag(001) surface. In the spirit of this session, the technical challenges in applying a precise voltage to the tip sample junction across a wide radio-frequency bandwidth will be described. The energy relaxation time, T1, of single spins on surfaces can be measured by spin-polarized pump-probe STM (scanning tunneling microscopy). To date, the relaxation times reported for Fe-Cu dimers on Cu2N insulating films have been of the order ~100 ns. A three-order-of-magnitude enhancement of lifetime, to ~200 μs, was recently demonstrated for Co on a single-monolayer of MgO. Here, we report on the tailoring of the T1 lifetime of single Fe atoms on single- and multi- layer MgO films grown on Ag(001). Next, we demonstrate electron spin resonance of an individual single Fe atom, driven by a gigahertz-frequency electric field applied across the tip-sample junction, and detected by a spin-polarized tunneling current. The principle parameters of the spin resonance experiment, namely the phase coherence time T2 and the Rabi rate, are characterized for Fe atoms adsorbed to the monolayer MgO film.

  5. Inner-shell photoionized x-ray lasers

    SciTech Connect

    Moon, S.J.

    1998-06-01

    } 0.1 {micro}J per pulse. The short duration of x-ray lasing (< 100 fs) combined with a 10-Hz repetition rate (P{sub avg} = 1{micro}W) makes this source of coherent x rays ideal for pump-probe experiments to study fast dynamical processes in chemistry and material science.

  6. State-To Spectroscopy and Dynamics of Ions and Neutrals by Photoionization and Photoelectron Methods

    NASA Astrophysics Data System (ADS)

    Ng, Cheuk-Yiu

    2014-06-01

    Recent advances in high-resolution photoionization, photoelectron, and photodissociation studies based on single-photon vacuum ultraviolet (VUV) and two-color infrared (IR)-VUV, visible (VIS)-ultraviolet (UV), and VUV-VUV laser excitations are illustrated with selected examples. We show that VUV laser photoionization coupled with velocity-map-imaging (VMI)-threshold photoelectron (VMI-TPE) detection can achieve comparable energy resolutions, but higher detection sensitivities than those observed in VUV laser pulsed field ionization-photoelectron (PFI-PE) measurements. For molecules with known intermediate states, IR-VUV and VIS-UV excitation schemes are highly sensitive for rovibronically selected and resolved PFI-PE studies. The successful applications of the VUV-PFI-PE, VUV-VMI-TPE and VIS-UV-PFI-PE methods to state-resolved and state-to-state photoelectron studies of transient radicals and transitional metal-containing molecules are highlighted. The most recently established VUV-VUV pump-probe time-slice VMI-photoion method is shown to be promising for state-to-state photodissociation studies of small molecules relevant to planetary atmospheres and for the fundamental understanding of photodissociation dynamics.

  7. State-to-State Spectroscopy and Dynamics of Ions and Neutrals by Photoionization and Photoelectron Methods

    NASA Astrophysics Data System (ADS)

    Ng, Cheuk-Yiu

    2014-04-01

    Recent advances in high-resolution photoionization, photoelectron, and photodissociation studies based on single-photon vacuum ultraviolet (VUV) and two-color infrared (IR)-VUV, visible (Vis)-ultraviolet (UV), and VUV-VUV laser excitations are illustrated with selected examples. VUV laser photoionization coupled with velocity-map-imaging threshold photoelectron (VMI-TPE) detection can achieve comparable energy resolution but has higher-detection sensitivities than those observed in VUV laser pulsed field ionization photoelectron (PFI-PE) measurements. For molecules with known intermediate states, IR-VUV and Vis-UV excitation schemes are highly sensitive for rovibronically selected and resolved PFI-PE studies. The successful applications of the VUV-PFI-PE, VUV-VMI-TPE, and Vis-UV-PFI-PE methods to state-resolved and state-to-state photoelectron studies of transient radicals and transitional metal-containing molecules are highlighted. The most recently established VUV-VUV pump-probe time-slice VMI photoion method is shown to be promising for state-to-state photodissociation studies of small molecules relevant to planetary atmospheres and for the fundamental understanding of photodissociation dynamics.

  8. Clean sub-8-fs pulses at 400 nm generated by a hollow fiber compressor for ultraviolet ultrafast pump-probe spectroscopy.

    PubMed

    Liu, Jun; Okamura, Kotaro; Kida, Yuichiro; Teramoto, Takahiro; Kobayashi, Takayoshi

    2010-09-27

    Clean 7.5 fs pulses at 400 nm with less than 3% energy in tiny satellite pulses were obtained by spectral broadening in a hollow fiber and dispersive compensating using a prism pair together with a deformable mirror system. As an example, this stable and clean pulse was used to study the ultrafast pump-probe spectroscopy of photoactive yellow protein. Moreover, the self-diffraction signal shows a smoothed and broadened laser spectrum and is expected to have a further clean laser pulse, which makes it more useful in the ultrafast pump-probe spectroscopy in the future. PMID:20940959

  9. Ultrafast dynamics of VO2 thin films measured in pump-probe configuration

    NASA Astrophysics Data System (ADS)

    Radue, Elizabeth; Kittiwatanakul, Salinporn; Lu, Jiwei; Wolf, S. A.; Fu, Zhengping; Yamaguchi, Masashi; Rossi, Enrico; Lukaszew, R. A.; Novikova, Irina

    The semiconductor-metal transition of VO2 continues to be a vigorously studied phenomenon due to complicated interplay between the structural change and the electronic bands. It is also potentially a very useful material, particularly because of its ultrafast transition to the metallic state excited with a femtosecond pulse. We have been exploring the effects of polarization of the pump in relation to the probe affects the sub-picosecond response of VO2 thin films, which will be important in designing ultrafast switches. We have also been looking at pumping our VO2 films with a THz source that directly pumps the lattice, and have found the film responds optically on a slower scale than when pumped with 800 nm, suggesting that there is an electronic response from disturbing the lattice. This project was sponsored by the NSF, DMR-1006013: Plasmon Resonances and Metal Insulator Transitions in Highly Correlated Thin Film Systems, and the NASA Virginia Space Grant Consortium. We also acknowledge support from the NRI/SRC sponsored ViNC center.

  10. Measuring the angle-dependent photoionization cross section of nitrogen using high-harmonic generation

    NASA Astrophysics Data System (ADS)

    Ren, Xiaoming; Makhija, Varun; Le, Anh-Thu; Troß, Jan; Mondal, Sudipta; Jin, Cheng; Kumarappan, Vinod; Trallero-Herrero, Carlos

    2013-10-01

    We exploit the relationship between high harmonic generation (HHG) and the molecular photorecombination dipole to extract the molecular-frame differential photoionization cross section (PICS) in the extreme ultraviolet (XUV) for molecular nitrogen. A shape resonance and a Cooper-type minimum are reflected in the pump-probe time delay measurements of different harmonic orders, where high-order rotational revivals are observed in N2. We observe the energy- and angle-dependent Cooper minimum and shape resonance directly in the laboratory-frame HHG yield by achieving a high degree of alignment, ≥0.8. The interplay between PICS and rotational revivals is confirmed by simulations using the quantitative rescattering theory. Our method of extracting molecular-frame structural information points the way to similar measurements in more complex molecules.

  11. Probing nonlinear magnetization dynamics in Fe/MgO(001) film by all optical pump-probe technique

    SciTech Connect

    He, Wei; Hu, Bo; Zhang, Xiang-Qun; Cheng, Zhao-Hua; Zhan, Qing-Feng

    2014-04-07

    An all-optical pump-probe technique has been employed to investigate the nonlinear magnetization dynamics of a 10 nm Fe/MgO(001) thin film in time domain. The magnetization precession was excited by pump-laser pulses and modulated by laser fluence variations. With increasing the laser fluence up to 7.1 mJ/cm{sup 2}, in addition to the uniform precession mode, a second harmonic signal was detected. The time evolution of the second harmonic signal was obtained in time-frequency domain. Based on the Landau-Lifshitz-Gilbert equation, the numerical simulation was performed to reproduce the observed the frequency doubling behaviors in Fe/MgO(001) film.

  12. Gauge invariance in the theoretical description of time-resolved angle-resolved pump/probe photoemission spectroscopy

    SciTech Connect

    Freericks, J. K.; Krishnamurthy, H. R.; Sentef, M. A.; Devereaux, T. P.

    2015-10-01

    Nonequilibrium calculations in the presence of an electric field are usually performed in a gauge, and need to be transformed to reveal the gauge-invariant observables. In this work, we discuss the issue of gauge invariance in the context of time-resolved angle-resolved pump/probe photoemission. If the probe is applied while the pump is still on, one must ensure that the calculations of the observed photocurrent are gauge invariant. We also discuss the requirement of the photoemission signal to be positive and the relationship of this constraint to gauge invariance. We end by discussing some technical details related to the perturbative derivation of the photoemission spectra, which involve processes where the pump pulse photoexcites electrons due to nonequilibrium effects.

  13. Ultrafast Pump-Probe Studies of the Light-Induced MIT and Recovery of Niobium Dioxide Thin Films

    NASA Astrophysics Data System (ADS)

    Beebe, Melissa; Klopf, J. Michael; Kittiwatanakul, Salinporn; Lu, Jiwei; Wolf, Stuart A.; Lukaszew, R. Alejandra

    Niobium dioxide (NbO2) is a highly correlated binary oxide that, like vanadium dioxide (VO2) , exhibits a first-order insulator-to-metal transition (IMT) at a material-dependent critical temperature, accompanied by a structural transformation from monoclinic to rutile. The nature of the IMT in VO2 has been discussed at length, while fewer studies have been carried out on NbO2. Previous studies show that the IMT can also be optically induced in VO2 on a sub-picosecond timescale; here, we present the first ultrafast pump-probe studies showing this optically-induced transition in NbO2 thin films and compare these results to similar ones carried out on VO2 thin films.

  14. Pump-probe studies of EUV and X-ray emission dynamics of laser-irradiated noble gas droplets

    NASA Astrophysics Data System (ADS)

    Parra, E.; McNaught, S. J.; Fan, J.; Milchberg, H. M.

    The interaction of high intensity 100-ps laser pulses with micron-sized noble gas (argon and krypton) droplets is experimentally investigated via a series of pump-probe experiments monitoring the delay-dependent X-ray and extreme ultraviolet (EUV) emission, and by imaging frequency-doubled probe light scattered from the interaction region. An understanding of the time scales for this interaction is important for optimization of EUV sources for next-generation lithography that utilizes laser-produced plasmas (LPP). Depending on the spectral region of interest, the type of emission, and the droplet characteristics, the effective emission lifetime was found to extend from a few hundred picoseconds to as long as several nanoseconds, in agreement with the expected plasma expansion, EUV excitation, and recombination emission time scales.

  15. Quantifying melanin distribution using pump-probe microscopy and a 2D morphological autocorrelation transformation for melanoma diagnosis

    NASA Astrophysics Data System (ADS)

    Robles, Francisco E.; Wilson, Jesse W.; Warren, Warren S.

    2014-03-01

    Pump-probe microscopy is a quantitative molecular imaging technique that yields diagnostically relevant information from endogenous pigments, like melanin, by probing their ultrafast photodynamic properties. Previously, the method was applied to image thin, pigmented, cutaneous samples at different stages of melanoma, and results have shown a correlation between melanin photodynamic behavior and malignancy. Here, we add to the diagnostic power of the method by applying principles of mathematical morphology to parameterize melanins' image structure. Along with bulk melanin chemical information, results show that this method can differentiate invasive melanomas from non-invasive and benign lesions with high sensitivity and specificity (92.3% and 97.5%, respectively, with N = 53). The mathematical method and the statistical analysis are described in detail and results from cutaneous and ocular conjuctival melanocytic lesions are presented.

  16. Time-integrated photoluminescence and pump-probe reflection spectroscopy of Si doped InN thin films

    SciTech Connect

    Mohanta, Antaryami; Jang, Der-Jun Wang, Ming-Sung; Tu, L. W.

    2014-01-28

    Temperature and excitation power dependent time-integrated photoluminescence of Si doped InN thin films are investigated. Photoluminescence (PL) spectra at low temperatures are described by single emission peak ensued due to “free-to-bound” recombination; whereas PL spectra at higher temperatures above 150 K are characterized by both “band-to-band” and “free-to-bound” transition. Carrier dynamics of Si doped InN thin films is studied using pump-probe reflection spectroscopy at room temperature. The hot electron cooling process is well described by electron-electron scattering. The dependence of the hot electron cooling rate on total electron density shows sublinear to linear behavior with increase of background electron density. The variation of the carrier recombination lifetime with total electron density implicates the dominance of the defect-related nonradiative recombination channel over other recombination processes.

  17. Nonlinear optical characterization of cluster dynamic in water in oil microemulsion by a pump probe laser beam technique

    NASA Astrophysics Data System (ADS)

    Vicari, L.

    2002-11-01

    We present a new pump probe laser beams configuration for the nonlinear optical characterization of microemulsions. We detect the variation of the on-axis optical intensity of the probe beam as generated by the concentration profile induced in an optically thin film of microemulsion by the pump beam. A mathematical model has been introduced to describe the phenomenon. The technique allows the determination of both Kerr-like optical nonlinearity and time constants and, therefore, it gives information both on cluster dimension and their shape. We discuss its application to WAD (water/AOT/decane, where AOT denotes sodium-bis-di-ethyl-sulfosuccinate) with the application of a strong electric field of optical source. Comparison between theoretical predictions and experimental results confirms the presence of giant optical nonlinearity in the absence of turbidity divergence. Chainlike shape of clusters, of the kind already reported with the application of strong electric field, could justify this result.

  18. Nonlinear optical characterization of cluster dynamic in water in oil microemulsion by a pump probe laser beam technique.

    PubMed

    Vicari, L

    2002-11-01

    We present a new pump probe laser beams configuration for the nonlinear optical characterization of microemulsions. We detect the variation of the on-axis optical intensity of the probe beam as generated by the concentration profile induced in an optically thin film of microemulsion by the pump beam. A mathematical model has been introduced to describe the phenomenon. The technique allows the determination of both Kerr-like optical nonlinearity and time constants and, therefore, it gives information both on cluster dimension and their shape. We discuss its application to WAD (water/AOT/decane, where AOT denotes sodium-bis-di-ethyl-sulfosuccinate) with the application of a strong electric field of optical source. Comparison between theoretical predictions and experimental results confirms the presence of giant optical nonlinearity in the absence of turbidity divergence. Chainlike shape of clusters, of the kind already reported with the application of strong electric field, could justify this result. PMID:15010903

  19. Pump-probe investigation of fs-LIOB in water by simultaneous spatial and temporal focusing

    NASA Astrophysics Data System (ADS)

    Kammel, Robert; Ackermann, Roland; Tünnermann, Andreas; Nolte, Stefan

    2013-03-01

    Femtosecond lasers are a versatile tool to process transparent materials like glasses, polymers or ophthalmic tissue. However, when focusing pulses of several μJ into the material, the high intensity near the laser focus leads to undesired nonlinear side effects like self-focusing and filamentation, resulting in an increased length of the induced plasma or the fragmentation of the breakdown volume. To overcome this limitation, we studied the influence of simultaneous spatial and temporal focusing (SSTF) on the laser induced optical breakdown (LIOB) in water. For this purpose, the incoming laser pulse is spectrally separated by a grating stretcher setup and recompressed by the focusing optics. Due to the increased pulse duration outside of the laser focus, the nonlinear laser-material interaction is confined to the focal region. We investigated the formation of the plasma and the resulting disruption in water by shadow imaging. With conventional focusing (τ = 70 fs, NA = 0.1) self-focusing, filamentation and breakup of the disruption volume was observed for pulse energies > 2 μJ, leading to a breakdown length of ~ 800 μm at a pulse energy of 8 μJ. With SSTF the axial length of the breakdown is significantly reduced by a factor of ~ 2. Plasma formation and the resulting disruption stay within the focal region. No self-focusing could be observed for pulse energies up to 8 μJ. Therefore, SSTF appears to be a promising tool to induce photodisruptions in transparent materials even with low numerical aperture, e.g. for precise fs-laser surgery within the posterior segment of the eye.

  20. Light Driven Energy Research at LCLS: Planned Pump-Probe X-ray Spectroscopy Studies on Photosynthetic Water Splitting

    NASA Astrophysics Data System (ADS)

    Bergmann, Uwe

    2010-02-01

    Arguably the most important chemical reaction on earth is the photosynthetic splitting of water to molecular oxygen by the Mn-containing oxygen-evolving complex (Mn-OEC) in the protein known as photosystem II (PSII). It is this reaction which has, over the course of some 3.8 billion years, gradually filled our atmosphere with O2 and consequently enabled and sustained the evolution of complex aerobic life. Coupled to the reduction of carbon dioxide, biological photosynthesis contributes foodstuffs for nutrition while recycling CO2 from the atmosphere and replacing it with O2. By utilizing sunlight to power these energy-requiring reactions, photosynthesis also serves as a model for addressing societal energy needs as we enter an era of diminishing fossil hydrocarbon resources. Understanding, at the molecular level, the dynamics and mechanism of how nature has solved this problem is of fundamental importance and could be critical to aid in the design of manufactured devices to accomplish the conversion of sunlight into useful electrochemical energy and transportable fuel in the foreseeable future. In order to understand the photosynthetic splitting of water by the Mn-OEC we need to be able to follow the reaction in real time at an atomic level. A powerful probe to study the electronic and molecular structure of the Mn-OEC is x-ray spectroscopy. Here, in particular x-ray emission spectroscopy (XES) has two crucial qualities for LCLS based time-dependent pump-probe studies of the Mn-OEC: a) it directly probes the Mn oxidation state and ligation, b) it can be performed with wavelength dispersive optics to avoid the necessity of scanning in pump probe experiments. Recent results and the planned time dependent experiments at LCLS will be discussed. )

  1. Production of high power femtosecond terahertz radiation

    SciTech Connect

    Neil, George R.; Carr, G.L.; Gubeli III, Joseph F.; Jordan, K.; Martin, Michael C.; McKinney, Wayne R.; Shinn, Michelle; Tani, Masahiko; Williams, G.P.; Zhang, X.-C.

    2003-07-11

    The terahertz (THz) region of the electromagnetic spectrum is attracting interest for a broad range of applications ranging from diagnosing electron beams to biological imaging. Most sources of short pulse THz radiation utilize excitation of biased semiconductors or electro-optic crystals by high peak power lasers. For example, this was done by using an un-doped InAs wafer irradiated by a femtosecond free-electron laser (FEL) at the Thomas Jefferson National Accelerator Facility. Microwatt levels of THz radiation were detected when excited with FEL pulses at 1.06 mm wavelength and 10W average power. Recently substantially higher powers of femtosecond THz pulses produced by synchrotron emission were extracted from the electron beamline. Calculations and measurements confirm the production of coherent broadband THz radiation from relativistic electrons with an average power of nearly 20W, a world record in this wavelength range by a factor of 10,000. We describe the source, presenting theoretical calculations and their experimental verification. Potential applications of this exciting new source include driving new non-linear phenomena, performing pump-probe studies of dynamical properties of novel materials, and studying molecular vibrations and rotations, low frequency protein motions, phonons, superconductor band gaps, electronic scattering, collective electronic excitations (e.g., charge density waves), and spintronics.

  2. Dual echelon femtosecond single-shot spectroscopy

    SciTech Connect

    Shin, Taeho; Wolfson, Johanna W.; Teitelbaum, Samuel W.; Kandyla, Maria; Nelson, Keith A.

    2014-08-15

    We have developed a femtosecond single-shot spectroscopic technique to measure irreversible changes in condensed phase materials in real time. Crossed echelons generate a two-dimensional array of time-delayed pulses with one femtosecond probe pulse. This yields 9 ps of time-resolved data from a single laser shot, filling a gap in currently employed measurement methods. We can now monitor ultrafast irreversible dynamics in solid-state materials or other samples that cannot be flowed or replenished between laser shots, circumventing limitations of conventional pump-probe methods due to sample damage or product buildup. Despite the absence of signal-averaging in the single-shot measurement, an acceptable signal-to-noise level has been achieved via background and reference calibration procedures. Pump-induced changes in relative reflectivity as small as 0.2%−0.5% are demonstrated in semimetals, with both electronic and coherent phonon dynamics revealed by the data. The optical arrangement and the space-to-time conversion and calibration procedures necessary to achieve this level of operation are described. Sources of noise and approaches for dealing with them are discussed.

  3. Production of high power femtosecond terahertz radiation

    NASA Astrophysics Data System (ADS)

    Neil, George R.; Carr, G. L.; Gubeli, Joseph F.; Jordan, K.; Martin, Michael C.; McKinney, Wayne R.; Shinn, Michelle; Tani, Masahiko; Williams, G. P.; Zhang, X.-C.

    2003-07-01

    The terahertz (THz) region of the electromagnetic spectrum is attracting interest for a broad range of applications ranging from diagnosing electron beams to biological imaging. Most sources of short pulse THz radiation utilize excitation of biased semiconductors or electro-optic crystals by high peak power lasers. For example, this was done by using an un-doped InAs wafer irradiated by a femtosecond free-electron laser (FEL) at the Thomas Jefferson National Accelerator Facility. Microwatt levels of THz radiation were detected when excited with FEL pulses at 1.06 μm wavelength and 10 W average power. Recently substantially higher powers of femtosecond THz pulses produced by synchrotron emission were extracted from the electron beamline. Calculations and measurements confirm the production of coherent broadband THz radiation from relativistic electrons with an average power of nearly 20 W, a world record in this wavelength range by a factor of 10,000. We describe the source, presenting theoretical calculations and their experimental verification. Potential applications of this exciting new source include driving new non-linear phenomena, performing pump-probe studies of dynamical properties of novel materials, and studying molecular vibrations and rotations, low frequency protein motions, phonons, superconductor bandgaps, electronic scattering, collective electronic excitations (e.g., charge density waves), and spintronics.

  4. Validity Using Pump-Probe Pulses to Determine the Optical Response of Niobate Crystals

    NASA Technical Reports Server (NTRS)

    Liu, Huimin; Jia, Weiyi

    1997-01-01

    A variety of niobate crystals have found their places in nonlinear optical applications as well as in laser devices. In recent years much attention has been paid to study the ultrafast optical response in a variety of photorefractive crystals such as KTa(1-x)Nb(x)O3 and KNbO3 crystals, glasses, semiconductors and polymers for applications in optical switching, information processing, optical computing, and all-optical device systems. Third-order optical nonlinearity is the most important property for realization of all-optical switching. Therefore experiments have been performed on the third order susceptibility using a variety of techniques such as the third-order harmonic generation, EFISH and degenerate four-wave mixing(DFWM). The latter has been conducted with a variety of pump wavelengths and with nanosecond, picosecond and femtosecond pulses. Niobate crystals, such as potassium niobate KNbO3, potassium tantalate niobate KTN family (KTa(1-x)Nb(x)O3), strontium barium niobate SBN (Sr(x)Ba(1-x)Nb2O6) and potassium-sodium niobate SBN (KNSBN) are attractive due to their photorefractive properties for application in optical storage and processing. The pulsed probe experiments performed on theses materials have suggested two types of time responses. These responses have been associated with an coherent response due to Chi(sup 3), and a long lived component due to excited state population. Recent study of DFWM on KNbO3 and KTN family reveals that the long lived component of those crystals depends on the crystal orientation. A slowly decaying signal is observable when the grating vector K(sub g) is not perpendicular to the C-axis of those photorefractive crystals', otherwise the optical response signal would be only a narrow coherent peak with FWHM equal to the cross-correlation width of the write beam pulses. Based on this understanding, we study the photodynamical process of a variety of niobate crystals using DFWM in a Kg perpindicular to C geometry with a ps

  5. Photoionization of Atomic Sc

    NASA Astrophysics Data System (ADS)

    Sossah, A. M.; Zhou, H.-L.; Manson, S. T.; Hibbert, A.

    2009-05-01

    Photoionization cross sections are calculated for the ground ([Mg] 3p^63d4s^2 ^2D^e) state of atomic Sc for photon energies from threshold to 40.0 eV. The discrete Sc^+ orbitals are generated using both the AUTOSTRUCTURE and CIV3 codes, and R-matrix is used to carry out the cross section calculations. The results are compared with each other, then with previous calculations and available experimental data for final-ionic states representing the 3d and 4s main lines and associated satellites (ionization with excitation) in the region of the 3p -> 3d giant resonances [1]. Reasonably good agreement between our non-relativistic results and experiment is obtained. This work is supported by US DOE and NSF [4pt] [1] S. B. Whitfield, K. Kehoe, R. Wehlitz, M. O. Krause, and C. D. Caldwell ->hys. Rev. A 64, 022701 (2001).

  6. Photoelectron photoion molecular beam spectroscopy

    SciTech Connect

    Trevor, D.J.

    1980-12-01

    The use of supersonic molecular beams in photoionization mass spectroscopy and photoelectron spectroscopy to assist in the understanding of photoexcitation in the vacuum ultraviolet is described. Rotational relaxation and condensation due to supersonic expansion were shown to offer new possibilities for molecular photoionization studies. Molecular beam photoionization mass spectroscopy has been extended above 21 eV photon energy by the use of Stanford Synchrotron Radiation Laboratory (SSRL) facilities. Design considerations are discussed that have advanced the state-of-the-art in high resolution vuv photoelectron spectroscopy. To extend gas-phase studies to 160 eV photon energy, a windowless vuv-xuv beam line design is proposed.

  7. Ultrafast spin-state photoswitching in a crystal and slower consecutive processes investigated by femtosecond optical spectroscopy and picosecond X-ray diffraction

    SciTech Connect

    Collet, Eric; Moisan, Nicolas; Baldé, Chérif; Bertoni, Roman; Trzop, Elzbieta; Laulhé, Claire; Lorenc, Maciej; Servol, Marina; Cailleau, Hervé; Tissot, Antoine; Boillot, Marie-Laure; Graber, Timothy; Henning, Robert; Coppens, Philip; Buron-Le Cointe, Marylise

    2013-02-20

    We report the spin state photo-switching dynamics in two polymorphs of a spin-crossover molecular complex triggered by a femtosecond laser flash, as determined by combining femtosecond optical pump-probe spectroscopy and picosecond X-ray diffraction techniques. The light-driven transformations in the two polymorphs are compared. Combining both techniques and tracking how the X-ray data correlate with optical signals allow understanding of how electronic and structural degrees of freedom couple and play their role when the switchable molecules interact in the active crystalline medium. The study sheds light on crossing the border between femtochemistry at the molecular scale and femtoswitching at the material scale.

  8. Photoionization-photoelectron research.

    SciTech Connect

    Ruscic, B.

    1998-03-06

    In the broad sense of a general definition, the fundamental goal of this research program is to explore, understand, and utilize the basic processes of interaction of vacuum UV light with atoms and molecules. In practical terms, this program uses photoionization mass spectrometry and other related techniques to study chemically relevant transient and metastable species that are intimately connected to energy-producing processes, such as combustion, or play-prominent roles in the associated environmental issues. Some recent examples of species that have been studied are: CH{sub 3}, CH{sub 2}, CH{sub 3}O, CH{sub 2}OH, CH{sub 3}S, CH{sub 2}SH, HCS, HNCO, NCO, HNCS, NCS, the isomers of C{sub 2}H{sub 5}O, HOBr, CF{sub 3} and CF{sub 3}OH. The ephemeral species of interest are produced in situ using various suitable techniques, such as sublimation, pyrolysis, microwave discharge, chemical abstraction reactions with H or F atoms, laser photodissociation, on-line synthesis, and others. The desired information is obtained by applying a variety of suitable photoionization methods, which use both conventional and coherent light sources in the vacuum W region. The spiritus movens of our studies is the need to provide the chemical community with essential information on the species of interest, such as accurate and reliable thermochemical, spectroscopic and structural data, and thus contribute to the global comprehension of the underlying chemical processes. The scientific motivation is also fueled by the necessity to unveil useful generalities, such as bonding patterns within a class of related compounds, or systematic behavior in the ubiquitous autoionization processes. In addition, the nature of the results obtained in this program is such that it generates a significant impetus for further theoretical work. The experimental work of this program is coordinated with other related experimental and theoretical efforts of the Chemical Dynamics Group to provide a broad perspective

  9. Backward nitrogen lasing actions induced by femtosecond laser filamentation: influence of duration of gain

    NASA Astrophysics Data System (ADS)

    Xie, Hongqiang; Li, Guihua; Chu, Wei; Zeng, Bin; Yao, Jinping; Jing, Chenrui; Li, Ziting; Cheng, Ya

    2015-07-01

    We experimentally investigate generation of backward 357 nm N2 laser in a gas mixture of N2/Ar using 800 nm femtosecond laser pulses, and examine the involved gain dynamics based on pump-probe measurements. Our findings show that a minimum duration of gain in the excited N2 molecules is required for generating intense backward nitrogen lasers, which is ∼0.8 ns under our experimental conditions. The results shed new light on the mechanism for generating intense backward lasers from nitrogen molecules, which are highly in demand for high sensitivity remote atmospheric sensing application.

  10. Control of femtosecond laser driven retro-Diels-Alder-like reaction of dicyclopentadiene

    PubMed Central

    Das, Dipak Kumar; Goswami, Tapas; Goswami, Debabrata

    2013-01-01

    Using femtosecond time resolved degenerate pump-probe mass spectrometry coupled with simple linearly chirped frequency modulated pulse, we elucidate that the dynamics of retro-Diels-Alder-like reaction of diclopentadiene (DCPD) to cyclopentadiene (CPD) in supersonic molecular beam occurs in ultrafast time scale. Negatively chirped pulse enhances the ion yield of CPD, as compared to positively chirped pulse. This indicates that by changing the frequency (chirp) of the laser pulse we can control the ion yield of a chemical reaction. PMID:23814449

  11. A flexible experimental setup for femtosecond time-resolved broad-band ellipsometry and magneto-optics

    SciTech Connect

    Boschini, F.; Hedayat, H.; Piovera, C.; Dallera, C.; Gupta, A.; Carpene, E.

    2015-01-15

    A versatile experimental setup for femtosecond time-resolved ellipsometry and magneto-optical Kerr effect measurements in the visible light range is described. The apparatus is based on the pump-probe technique and combines a broad-band probing beam with an intense near-infrared pump. According to Fresnel scattering matrix formalism, the analysis of the reflected beam at different polarization states of the incident probe light allows one to determine the diagonal and the off-diagonal elements of the dielectric tensor in the investigated sample. Moreover, the pump-probe method permits to study the dynamics of the dielectric response after a short and intense optical excitation. The performance of the experimental apparatus is tested on CrO{sub 2} single crystals as a benchmark.

  12. A flexible experimental setup for femtosecond time-resolved broad-band ellipsometry and magneto-optics.

    PubMed

    Boschini, F; Hedayat, H; Piovera, C; Dallera, C; Gupta, A; Carpene, E

    2015-01-01

    A versatile experimental setup for femtosecond time-resolved ellipsometry and magneto-optical Kerr effect measurements in the visible light range is described. The apparatus is based on the pump-probe technique and combines a broad-band probing beam with an intense near-infrared pump. According to Fresnel scattering matrix formalism, the analysis of the reflected beam at different polarization states of the incident probe light allows one to determine the diagonal and the off-diagonal elements of the dielectric tensor in the investigated sample. Moreover, the pump-probe method permits to study the dynamics of the dielectric response after a short and intense optical excitation. The performance of the experimental apparatus is tested on CrO2 single crystals as a benchmark. PMID:25638099

  13. A flexible experimental setup for femtosecond time-resolved broad-band ellipsometry and magneto-optics

    NASA Astrophysics Data System (ADS)

    Boschini, F.; Hedayat, H.; Piovera, C.; Dallera, C.; Gupta, A.; Carpene, E.

    2015-01-01

    A versatile experimental setup for femtosecond time-resolved ellipsometry and magneto-optical Kerr effect measurements in the visible light range is described. The apparatus is based on the pump-probe technique and combines a broad-band probing beam with an intense near-infrared pump. According to Fresnel scattering matrix formalism, the analysis of the reflected beam at different polarization states of the incident probe light allows one to determine the diagonal and the off-diagonal elements of the dielectric tensor in the investigated sample. Moreover, the pump-probe method permits to study the dynamics of the dielectric response after a short and intense optical excitation. The performance of the experimental apparatus is tested on CrO2 single crystals as a benchmark.

  14. Time-resolved investigations of the non-thermal ablation process of graphite induced by femtosecond laser pulses

    NASA Astrophysics Data System (ADS)

    Kalupka, C.; Finger, J.; Reininghaus, M.

    2016-04-01

    We report on the in-situ analysis of the ablation dynamics of the, so-called, laser induced non-thermal ablation process of graphite. A highly oriented pyrolytic graphite is excited by femtosecond laser pulses with fluences below the classic thermal ablation threshold. The ablation dynamics are investigated by axial pump-probe reflection measurements, transversal pump-probe shadowgraphy, and time-resolved transversal emission photography. The combination of the applied analysis methods allows for a continuous and detailed time-resolved observation of the non-thermal ablation dynamics from several picoseconds up to 180 ns. Formation of large, μm-sized particles takes place within the first 3.5 ns after irradiation. The following propagation of ablation products and the shock wave front are tracked by transversal shadowgraphy up to 16 ns. The comparison of ablation dynamics of different fluences by emission photography reveals thermal ablation products even for non-thermal fluences.

  15. Nodal Quasiparticle Meltdown in Ultra-High Resolution Pump-Probe Angle-Resolved Photoemission

    SciTech Connect

    Graf, Jeff; Jozwiak, Chris; Smallwood, Chris L.; Eisaki, H.; Kaindl, Robert A.; Lee, Dung-Hai; Lanzara, Alessandra

    2011-06-03

    , finding any strong dependencies of the nodal QPs will alter the conventional view and enrich our understanding of high temperature superconductivity. Time resolution through pump-and-probe techniques adds a new dimension to ARPES by directly measuring how the electronic structure of a material responds to perturbations on femtosecond time scales. Here we report a unique ultrafast time-resolved ARPES study of a high-T{sub c} cuprate superconductor. Compared to previous time-resolved studies, the primary advantage of this work is an unprecedented momentum (angular) resolution ({Delta} k~ 0.003 vs. 0.05 { Angstrom}{sup -1}), on par with that of state-of-the-art ARPES. This has allowed the time-resolved measurement of signi cantly sharper QP spectral peaks with strikingly larger peak-to-background ratios than previously reported.16 Additionally, a lower pump fluence is used (<40{micro} J/cm{sup 2} vs. 100 {micro}J/cm{sup 2}), which reduces pump-induced sample temperature increase and related thermal smearing of spectral features. This allows us to uncover a surprising meltdown of nodal QP spectral weight following pump laser excitation. This meltdown is only observed in the superconducting state and for QPs with binding energy less than the kink energy,19 revealing a link between nodal QPs and superconductivity.

  16. Atmospheric measurements of total OH reactivity: Intercomparison of the pump-probe technique and the comparative reactivity method

    NASA Astrophysics Data System (ADS)

    Dusanter, Sebastien; Hansen, Robert; Leonardis, Thierry; Schoemaecker, Coralie; Blocquet, Marion; Fittschen, Christa; Hanoune, Benjamin; Sinha, Vinayak; Stevens, Philip; Locoge, Nadine

    2013-04-01

    The hydroxyl radical (OH) drives the oxidation of organic trace gases that can lead to the production of ozone and secondary organic aerosols in the atmosphere. A complete understanding of the sources and sinks of OH is therefore important to address issues related to both air quality and climate change. However, recent measurements of total OH reactivity [1-2], which is the inverse of the OH lifetime, have pointed out that our understanding of OH sinks is still incomplete and important reactive trace gases have not yet been identified. These measurements of total OH reactivity are of particular interest since they provide a critical test of our understanding of the OH budget. Three techniques are available to measure the total OH reactivity, including the total OH loss rate method [3], the pump-probe method [4], and the comparative reactivity method (CRM) [5]. While the first two methods are based on direct measurements of OH decays using laser-induced fluorescence instruments, the CRM is based on a different approach in which a tracer molecule is detected instead of OH to determine the ambient OH loss rate. As these instruments were deployed in different field campaigns, intercomparison exercises would be useful to ensure the accuracy of the measurements. However, such intercomparisons have not yet been published. An informal intercomparison involving a CRM instrument from the Ecole des Mines de Douai (EMD) and a pump-probe instrument from the laboratory Physicochimie des Processus de Combustion et de l'Atmosphere (PC2A) took place in an urban environment at the university of Lille (France). The two OH reactivity instruments measured continuously side by side for a duration of two weeks. Collocated measurements of trace gases were also performed using O3, NOx and SO2 monitors, as well as two automated chromatographic instruments capable of measuring more than 50 volatile organic compounds (VOC). We will present cross calibrations of the two OH reactivity

  17. NDT of fiber-reinforced composites with a new fiber-optic pump-probe laser-ultrasound system.

    PubMed

    Pelivanov, Ivan; Buma, Takashi; Xia, Jinjun; Wei, Chen-Wei; O'Donnell, Matthew

    2014-06-01

    Laser-ultrasonics is an attractive and powerful tool for the non-destructive testing and evaluation (NDT&E) of composite materials. Current systems for non-contact detection of ultrasound have relatively low sensitivity compared to contact peizotransducers. They are also expensive, difficult to adjust, and strongly influenced by environmental noise. Moreover, laser-ultrasound (LU) systems typically launch only about 50 firings per second, much slower than the kHz level pulse repetition rate of conventional systems. As demonstrated here, most of these drawbacks can be eliminated by combining a new generation of compact, inexpensive, high repetition rate nanosecond fiber lasers with new developments in fiber telecommunication optics and an optimally designed balanced probe beam detector. In particular, a modified fiber-optic balanced Sagnac interferometer is presented as part of a LU pump-probe system for NDT&E of aircraft composites. The performance of the all-optical system is demonstrated for a number of composite samples with different types and locations of inclusions. PMID:25302156

  18. Dynamics of photon-induced processes in adsorbate-surface systems studied by laser-synchrotron pump-probe techniques

    NASA Astrophysics Data System (ADS)

    Winter, Bernd J.; Gatzke, Johannes; Quast, T.; Will, Ingo; Wick, Manfred T.; Liero, A.; Pop, D.; Hertel, Ingolf V.

    1998-12-01

    We report on the MBI User Facility at BESSY II, presently under construction, which is dedicated to study the dynamics of photo-induced processes by combining laser and synchrotron pulses. In this paper we focus on the synchronization of a modelocked ultrafast Ti:sapphire laser to the Berlin electron storage ring for synchrotron radiation (BESSY). Two different techniques have been applied -- one based on a digital phase comparator and the other based on analog high-harmonic mixing. Both schemes may be easily adjusted to either single, multi- or hybrid-bunch operation of the synchrotron. Moreover, the temporal accuracy of the synchronization unit suitably matches the widths of the synchrotron pulses (some ten picoseconds) to be expected at BESSY II. Therefore, the currently performed test experiments at BESSY I provide the basis for time- resolved photon-induced experiments which combine laser and SR-undulator pulses in a pump-probe scheme at BESSY II. This facility will be available within the first half of 1999.

  19. Laser-driven phase transitions in aqueous colloidal gold nanoparticles under high pressure: picosecond pump-probe study.

    PubMed

    Hashimoto, Shuichi; Katayama, Tetsuro; Setoura, Kenji; Strasser, Michael; Uwada, Takayuki; Miyasaka, Hiroshi

    2016-02-14

    Pump-probe transient extinction spectroscopy was used to analyze 355 nm picosecond laser heating-induced phenomena in 60 nm-diameter aqueous gold nanoparticles (AuNPs) under a high pressure of 60 MPa. Kinetic spectroscopy revealed that a supercritical layer surrounding the AuNP nucleated with a lifetime of approximately 1 ns during its dynamic expansion and decay for a fluence of 19.6 mJ cm(-2). Moreover, in the post-mortem transmission electron micrographs we observed a number of fragments, a small percentage of size-reduced cores, and erupted particles among the intact particles after 60 shots, suggesting that evaporation occurred under laser illumination. The particle temperature calculation indicated that evaporation begins with a liquid droplet AuNP surrounded by a supercritical layer at temperatures below the boiling point of gold. By applying high pressure, we obtained a clear picture of the evaporation event, which was not possible at ambient pressure because bubble formation caused particle temperatures to rise uncontrollably. In this study, we shed light on the critical role of the supercritical layer formed around the AuNP under high pressure during laser-induced evaporation. PMID:26812175

  20. Probing with randomly interleaved pulse train bridges the gap between ultrafast pump-probe and nanosecond flash photolysis.

    PubMed

    Nakagawa, Tatsuo; Okamoto, Kido; Hanada, Hiroaki; Katoh, Ryuzi

    2016-04-01

    Despite the long-standing importance of transient absorption (TA) spectroscopy, many researchers remain frustrated by the difficulty of measuring the nanosecond range in a wide spectral range. To address this shortcoming, we propose a TA spectrophotometer in which there is no synchronization between a pump pulse and a train of multiple probe pulses from a picosecond supercontinuum light source, termed the randomly-interleaved-pulse-train (RIPT) method. For each pump pulse, many monochromatized probe pulses impinge upon the sample, and the associated pump-probe time delays are determined passively shot by shot with subnanosecond accuracy. By repeatedly pumping with automatically varying time delays, a TA temporal profile that covers a wide dynamic range from subnanosecond to milliseconds is simultaneously obtained. By scanning wavelength, this single, simple apparatus acquires not only wide time range TA profiles, but also broadband TA spectra from the visible through the near-infrared regions. Furthermore, we present a typical result to demonstrate how the RIPT method may be used to correct for fluorescence, which often pollutes TA curves. PMID:27192271

  1. Picosecond-to-nanosecond dynamics of plasmonic nanobubbles from pump-probe spectral measurements of aqueous colloidal gold nanoparticles.

    PubMed

    Katayama, Tetsuro; Setoura, Kenji; Werner, Daniel; Miyasaka, Hiroshi; Hashimoto, Shuichi

    2014-08-12

    The photothermal generation of nanoscale vapor bubbles around noble metal nanoparticles is of significant interest, not only in understanding the underlying mechanisms responsible for photothermal effects, but also to optimize photothermal effects in applications such as photothermal cancer therapies. Here, we describe the dynamics in the 400-900 nm regime of the formation and evolution of nanobubbles around colloidal gold nanoparticles using picosecond pump-probe optical measurements. From excitations of 20-150 nm colloidal gold nanoparticles with a 355 nm, 15 ps laser, time-dependent optical extinction signals corresponding to nanobubble formation were recorded. The extinction spectra associated with nanobubbles of different diameters were simulated by considering a concentric spherical core-shell model within the Mie theory framework. In the simulations, we assumed an increase in particle temperature. From temporal changes in the experimental data of transient extinctions, we estimated the temporal evolution of the nanobubble diameter. Corrections to bubble-free temperature effects on the transient extinction decays were applied in these experiments by suppressing bubble formation using pressures as high as 60 MPa. The results of this study suggest that the nanobubbles generated around a 60 nm-diameter gold nanoparticle using a fluence of 5.2 mJ cm(-2) had a maximum diameter of 260 ± 40 nm, and a lifetime of approximately 10 ns. The combination of fast transient extinction spectral measurements and spectral simulations provides insights into plasmonic nanobubble dynamics. PMID:25083945

  2. Nonradiative Decay Dynamics of METHYL-4-HYDROXYCINNAMATE and its Monohydrated Complex Revealed by Picosecond Pump-Probe Spectroscopy

    NASA Astrophysics Data System (ADS)

    Ebata, T.; Shimada, D.; Kusaka, R.; Inokuchi, Y.; Ehara, M.

    2012-06-01

    The lifetimes of methyl 4-hydroxycinnamate (OMpCA) and its mono-hydrated complex (OMpCA-H_2O) in the S_1 state have been measured by picosecond pump-probe spectroscopy in a supersonic beam. For OMpCA, the lifetime of the S_1 - S_0 origin is 8 - 9 ps. On the other hand, the lifetime of OMpCA-H_2O complex at the origin is 930 ps, which is 100 times longer than that. Furthermore, in the complex the S_1 lifetime shows rapid decrease at an energy of 200 cm-1 above the origin and becomes as short as 9 ps at 500 cm-1. Theoretical calculations with symmetry-adapted cluster-configuration interaction (SAC-CI) method suggest that in OMpCA, the trans - cis isomerization occurs smoothly without a barrier on the S_1surface, while in OMpCA-H_2O complex, there exists a barrier along the isomerization coordinate. The calculated barrier height of OMpCA-H_2O is in good agreement with that estimated from the lifetime measurements.

  3. Carrier dynamics in femtosecond-laser-excited bismuth telluride

    NASA Astrophysics Data System (ADS)

    Wang, J. L.; Guo, L.; Ling, C.; Song, Y. M.; Xu, X. F.; Ni, Z. H.; Chen, Y. F.

    2016-04-01

    The carrier dynamics of B i2T e3 is studied using the femtosecond pump-probe technique. Three distinct processes, including free carrier absorption, band filling, and electron-hole recombination, are found to contribute to the reflectivity changes. The two-temperature model is used to describe the intraband energy relaxation process of carriers, and the Drude contribution well explains the intensity dependence of the peak values of the nonoscillatory component in the reflectivity signal. The combined effects of free carrier absorption and band filling result in a reflection minimum at about 2 ps after laser excitation. The nonzero background signal increases linearly with the pump fluence, which is attributed to the electron-hole recombination. Finally, our results provide an illustration of investigating the carrier dynamics in semiconductors from the ultrafast reflectivity spectra.

  4. Femtosecond Spectroscopy of Alkali Trimers on Helium Nanodroplets

    NASA Astrophysics Data System (ADS)

    Giese, C.; Grüner, B.; Fechner, L.; Mudrich, M.; Stienkemeier, F.; Hauser, A. W.; Ernst, W. E.

    2010-06-01

    Superfluid helium nanodroplets offer the opportunity to study dopant molecules in the sub-Kelvin range with only weak matrix perturbations. Femtosecond wave packet spectroscopy has been shown to be well suited to obtain high resolution vibrational spectra of cold alkali molecules in weakly bound high-spin states. In a pump-probe scheme a first laser pulse excites a vibrational wave packet that evolves on the molecular potential and is probed by a second ionizing pulse. We present spectroscopic data on Rb_3 and K_3 showing different vibronic progressions. These are assigned with the help of high level ab initio calculations of the electronic structure of the bare trimers. M. Mudrich, P. Heister, T. Hippler, C. Giese, O. Dulieu and F. Stienkemeier, Phys. Rev. A 80, 042512 (2009) J. Nagl, G. Auböck, A.W. Hauser, O. Allard, C. Callegari and W.E. Ernst, Phys. Rev. Lett. 100, 063001 (2008)

  5. Dissipative exciton motion in a chlorophyll a/b dimer of the light harvesting complex of photosystem II: Simulation of pump-probe spectra

    SciTech Connect

    Renger, T.; Voigt, J.; May, V.; Kuehn, O.

    1996-09-26

    The ultrafast dissipative exciton motion in a molecular dimer of the light harvesting complex II of higher plants is investigated theoretically. The density matrix formalism is applied to simulate the one- and two-color pump-probe spectra measured by Bittner et al. To incorporate coherent vibrational motion we use a representation in localized exciton vibrational states. The observed ultrafast transfer dynamics on the subpicosecond time scale can be well explained by means of a delocalization of the exciton wave function over both monomers. For the low-temperature one-color pump-probe measurement we predict quantum beats in the signal due to coherent nuclear wave packet motion. Furthermore, our calculations support the in-line geometry for the Chlorophyll a/b dimers in the pigment-protein complex. 32 refs., 9 figs., 2 tabs.

  6. Analysis of the contrast in normal-incidence surface plasmon photoemission microscopy in a pump-probe experiment with adjustable polarization

    NASA Astrophysics Data System (ADS)

    Podbiel, Daniel; Kahl, Philip; Meyer zu Heringdorf, Frank-J.

    2016-04-01

    We investigate the fringe contrast in surface plasmon polariton-based two-photon photoemission microscopy in a normal-incidence geometry. In a pump-probe experiment with freely adjustable polarization of the probe pulse, we find a maximum contrast whenever the probe pulse polarization is parallel (or anti-parallel) to the propagation direction of the surface plasmon polariton wave packet. The experimental observation is compared to a wave simulation based on the known TM solution for surface plasmon polaritons. We estimate that at the Au/vacuum interface the in-plane component of the electric field of the surface plasmon polariton inside the metal is about five times larger than its out-of-plane component. We conclude that the locations of maximum plasmon-related nonlinear photoemission yield in a pump-probe experiment are the ones where the in-plane component of the electric field of the surface plasmon polariton is maximal.

  7. Femtosecond Light Source for Phase-Controlled Multiphoton Ionization

    SciTech Connect

    Sokolov, A. V.; Walker, D. R.; Yavuz, D. D.; Yin, G. Y.; Harris, S. E.

    2001-07-16

    We describe a femtosecond Raman light source with more than an octave of optical bandwidth. We use this source to demonstrate phase control of multiphoton ionization under conditions where ionization requires eleven photons of the lowest frequency of the spectrum or five photons of the highest frequency. The nonlinearity of the photoionization process allows us to characterize the light source. Experiment-to-theory comparison implies generation of a near single-cycle waveform.

  8. New accelerators for femtosecond beam pump-and-probe analysis

    NASA Astrophysics Data System (ADS)

    Uesaka, Mitsuru; Sakumi, Akira; Hosokai, Tomonao; Kinoshita, Kenichi; Yamaoka, Nobuaki; Zhidkov, Alexei; Ohkubo, Takeru; Ueda, Toru; Muroya, Yusa; Katsumura, Yosuke; Iijima, Hokuto; Tomizawa, Hiromitsu; Kumagai, Noritaka

    2005-12-01

    Femtosecond electron beams are novel tool for pump-probe analysis of condensed matter. Progress in developing femtosecond electron beams with the use of both conventional accelerators and laser-plasma accelerators is discussed. In conventional accelerators, the critical issue is timing jitter and drift of the linac-laser synchronization system. Sophisticated electronic devices are developed to reduce the jitter to 330 fs (rms); the precise control of temperature at several parts of the accelerator lessens the drift to 1 ps (rms). We also report on a full-optical X-ray and e-beam system based on the laser-plasma cathode by using a 12 TW 50 fs laser, which enables 40 MeV (at maximum), 40 fs (cal.), 100 pC and quasi-monochromatic single electron bunches. Since the synchronization is done by a passive optical beam-splitter, this system intrinsically has no jitter and drift. It could achieve tens of femtoseconds time-resolved analysis in the near future.

  9. Photodissociation of Small Molecules and Photoionization of Free Radicals Using the VUV Velocity-Map Imaging Photoion and Photoelectron Method

    NASA Astrophysics Data System (ADS)

    Gao, Hong

    (2012). (Chapter 2) 2. Hong Gao, Yu Song, Lei Yang, Xiaoyu Shi, Qing-Zhu Yin, C. Y. Ng and William M. Jackson. "Branching ratio measurements of the predissociation of 12C16O by time-slice velocity-map ion imaging in the energy region from 108,000 to 110,500 cm-1", the Journal of Chemical Physics, 137, 034305 (2012). (Chapter 3) 3. Hong Gao, Yu Song, Yih-Chung Chang, Xiaoyu Shi, Qing-Zhu Yin, Roger C. Wiens, William M. Jackson, C. Y. Ng, "Branching Ratio Measurements for Vacuum Ultraviolet Photodissociation of 12C16O", the Journal of Physical Chemistry A. (article online ASAP). (Chapter 4) 4. Hong Gao, Yu Song, C. Y. Ng, William M. Jackson, " Communication: State-to-state photodissociation study by the two-color VUV-VUV laser pump-probe time-slice velocity-map-imaging-photoion method", the Journal of Chemical Physics, 138, 191102(2013). (Chapter 5) 5. Hong Gao, Zhou Lu, Lei Yang, Jingang Zhou, C. Y. Ng, "Communication: A vibrational study of propargyl cation using the vacuum ultraviolet laser velocity-map imaging photoelectron method", the Journal of Chemical Physics, 137, 161101(2012). (Chapter 6)

  10. Photoionization Dynamics of Small Molecules

    SciTech Connect

    Dehmer, Joseph L.; Dill, Dan; Parr, Albert C.

    1985-01-01

    The last decade has witnessed remarkable progress in characterizing dynamical aspects of the molecular photoionization process. The general challenge is to gain physical insight into those processes occuring during photo excitation and eventual escape of the photoelectron through the anisotropic molecular field, in terms of various observables such as photoionization cross-sections and branching ratios, photoelectron angular distributions and even newer probes mentioned below. Much of the progress in this field has mirrored earlier work in atomic photoionization dynamics where many key ideas were developed (e.g., channel interaction, quantum defect analysis, potential barrier phenomena and experimental techniques). However, additional concepts and techniques were required to deal with the strictly molecular aspects of the problem, particularly the anisotropy of the multicenter molecular field and the interaction among rovibronic modes.

  11. Macrospin dynamics in antiferromagnets triggered by sub-20 femtosecond injection of nanomagnons

    NASA Astrophysics Data System (ADS)

    Bossini, D.; Dal Conte, S.; Hashimoto, Y.; Secchi, A.; Pisarev, R. V.; Rasing, Th.; Cerullo, G.; Kimel, A. V.

    2016-02-01

    The understanding of how the sub-nanoscale exchange interaction evolves in macroscale correlations and ordered phases of matter, such as magnetism and superconductivity, requires to bridging the quantum and classical worlds. This monumental challenge has so far only been achieved for systems close to their thermodynamical equilibrium. Here we follow in real time the ultrafast dynamics of the macroscale magnetic order parameter in the Heisenberg antiferromagnet KNiF3 triggered by the impulsive optical generation of spin excitations with the shortest possible nanometre wavelength and femtosecond period. Our magneto-optical pump-probe experiments also demonstrate the coherent manipulation of the phase and amplitude of these femtosecond nanomagnons, whose frequencies are defined by the exchange energy. These findings open up opportunities for fundamental research on the role of short-wavelength spin excitations in magnetism and strongly correlated materials; they also suggest that nanospintronics and nanomagnonics can employ coherently controllable spin waves with frequencies in the 20 THz domain.

  12. Controlling the dynamics of a femtosecond laser-driven shock in hot dense plasma

    NASA Astrophysics Data System (ADS)

    Adak, Amitava; Singh, Prashant Kumar; Chatterjee, Gourab; Lad, Amit D.; Brijesh, P.; Kumar, G. Ravindra

    2015-11-01

    We present the dependence of the dynamics of a plasma super-critical layer on the laser intensity contrast in the regime of intense femtosecond laser-solid interaction. Time-resolved pump-probe diagnostics reveal the interplay of inward shock strength and laser contrast of a femtosecond laser at an intensity of 1018 W cm-2. The measurements show that the pulse with 2 orders of magnitude higher intensity contrast than that with a usual lower contrast one (~10-5) launches the shock-like disturbance (into the target) having 10 times more speed. This observation is further supplemented by employing an external prepulse (for manipulating the preplasma scale length) which helps to control the inward motion of the critical surface. This opens up the possibility of controlling the inward moving shock disturbance and leads to medical, science and engineering applications.

  13. Photoionized argon plasmas induced with intense soft x-ray and extreme ultraviolet pulses

    NASA Astrophysics Data System (ADS)

    Bartnik, A.; Wachulak, P.; Fok, T.; Węgrzyński, Ł.; Fiedorowicz, H.; Skrzeczanowski, W.; Pisarczyk, T.; Chodukowski, T.; Kalinowska, Z.; Dudzak, R.; Dostal, J.; Krousky, E.; Skala, J.; Ullschmied, J.; Hrebicek, J.; Medrik, T.

    2016-01-01

    In this work, photoionized plasmas were created by irradiation of gaseous argon with soft x-ray (SXR) and extreme ultraviolet (EUV) intense radiation pulses. Two different laser-produced plasma sources, employing a low energy Nd:YAG laser and a high energy iodine laser system (PALS), were used for creation of photoionized plasmas. In both cases the EUV or SXR beam irradiated the Ar stream, injected into a vacuum chamber synchronously with the radiation pulse. Emission spectra, measured for the Ar photoionized plasmas indicated strong differences in ionization degree for plasmas produced using low and high energy systems. In case of the the EUV driving pulses, emission lines corresponding to neutral atoms and singly charged ions were observed. In case of the SXR pulses utilized for the photoionized plasma creation, only Ar V–VIII emission lines were recorded. Additionally, electron density measurements were performed by laser interferometry employing a femtosecond laser system synchronized with the irradiating system. Maximum electron density for the Ar photoionized plasma, induced using the high energy system, reached 1.9 · 1018 cm‑3. Interferometric measurements performed for the moment of maximum intensity of the main laser pulse (t  =  0) revealed no fringe shift. Detection limit for the interferometric measurements was estimated. It allowed to estimate the upper limit for electron density at t  =  0 as 5 · 1016 cm‑3.

  14. Resonant soft x-ray scattering endstation for time-resolved pump-probe measurements at LCLS

    NASA Astrophysics Data System (ADS)

    Chuang, Yi-De; Doering, Dionisio; Cruz, Alejandro G.; Tahir, Nadeem; Andresen, Nord C.; Chow, Ken P.; Contarato, Devis; Cummings, Curtis L.; Domning, Edward E.; Joseph, John; Pepper, John S.; Smith, Brian V.; Zizka, G.; Ford, Christopher; Lee, Wei-Sheng; Weaver, Matt; Patthey, Luc; Weizeowick, John; Denes, Peter; Hussain, Zahid

    2012-10-01

    Localized charge, spin and orbital degrees of freedom can compete with electronic itinerancy and such competition lies at the heart of emergent material properties. To study these electronic orderings, resonant soft X-ray scattering (RSXS) spectroscopy has been demonstrated as one of the most powerful direct probes, and its time-resolved capability can be implemented through pump-probe technique. The ultrafast/ultra-intense X-ray pulses from LCLS can be used as the probe in the time-resolved RSXS experiments, but the inherent fluctuations in intensity and timing between pulses can degrade the superior temporal resolution. To overcome such fluctuations, a compact fast CCD (cFCCD) was developed to enable shot-by-shot data acquisitions and a dedicated RSXS endstation, constructed to house this cFCCD and other single-channel photon detectors, has been extensively used at both ALS and LCLS. Time-resolved RSXS experiments on La1.75Sr0.25 NiO4 nickelate have revealed an unexpected transient behavior of charge and spin ordering (CO/SO) states. After 800nm laser excitation, the CO can be fully suppressed at higher pump fluence while SO remains detectable, creating a transient state that is not accessible by tuning thermodynamic variables. Furthermore, two distinct time scales are identified in the recovery of CO and can be attributed to the amplitude (fast) and phase (slow) dynamics of order parameter. A new version of cFCCD, with eight times the detection area and the readout electronics moved into vacuum side to minimize the pickup noise, has been developed and will be incorporated into the RSXS endstation.

  15. Time delay in molecular photoionization

    NASA Astrophysics Data System (ADS)

    Hockett, P.; Frumker, E.; Villeneuve, D. M.; Corkum, P. B.

    2016-05-01

    Time-delays in the photoionization of molecules are investigated. As compared to atomic ionization, the time-delays expected from molecular ionization present a much richer phenomenon, with a strong spatial dependence due to the anisotropic nature of the molecular scattering potential. We investigate this from a scattering theory perspective, and make use of molecular photoionization calculations to examine this effect in representative homonuclear and hetronuclear diatomic molecules, nitrogen and carbon monoxide. We present energy and angle-resolved maps of the Wigner delay time for single-photon valence ionization, and discuss the possibilities for experimental measurements.

  16. Lifetime measurement of the cesium 6 P3 /2 level using ultrafast pump-probe laser pulses

    NASA Astrophysics Data System (ADS)

    Patterson, B. M.; Sell, J. F.; Ehrenreich, T.; Gearba, M. A.; Brooke, G. M.; Scoville, J.; Knize, R. J.

    2015-01-01

    Using the inherent timing stability of pulses from a mode-locked laser, we measure the cesium 6 P3 /2 excited-state lifetime. An initial pump pulse excites cesium atoms in two counterpropagating atomic beams to the 6 P3 /2 level. A subsequent synchronized probe pulse ionizes atoms that remain in the excited state and the photoions are collected and counted. By selecting pump pulses that vary in time with respect to the probe pulses, we obtain a sampling of the excited-state population in time, resulting in a lifetime value of 30.462(46) ns. The measurement uncertainty (0.15%) is slightly larger than our previous report of 0.12% [J. F. Sell et al., Phys. Rev. A 84, 010501(R) (2011), 10.1103/PhysRevA.84.010501] due to the inclusion of additional data and systematic errors. In this follow-up paper we present details of the primary systematic errors encountered in the measurement, which include atomic motion within the intensity profiles of the laser beams, quantum beating in the photoion signal, and radiation trapping. Improvements to further reduce the experimental uncertainty are also discussed.

  17. Mass-Selective Laser Photoionization.

    ERIC Educational Resources Information Center

    Smalley, R. E.

    1982-01-01

    Discusses the nature and applications of mass-selective laser photoionization. The ionization can be done with a single intense laser pulse lasting a few billionths of a second with no molecular fragmentation. Applications focus on: (1) benzene clusters, excimers, and exciplexes; (2) metal clusters; and (3) triplet formation and decay. (Author/JN)

  18. Photoionization in the Solar Wind

    NASA Astrophysics Data System (ADS)

    Landi, E.; Lepri, S. T.

    2015-10-01

    In this work we investigate the effects of photoionization on the charge state composition of the solar wind. Using measured solar EUV and X-ray irradiance, the Michigan Ionization Code and a model for the fast and slow solar wind, we calculate the evolution of the charge state distribution of He, C, N, O, Ne, Mg, Si, S, and Fe with and without including photoionization for both types of wind. We find that the solar radiation has significant effects on the charge state distribution of C, N, and O, causing the ionization levels of these elements to be higher than without photoionization; differences are largest for oxygen. The ions commonly observed for elements heavier than O are much less affected, except in ICMEs where Fe ions more ionized than 16+ can also be affected by the solar radiation. We also show that the commonly used O7+/O6+ density ratio is the most sensitive to photoionization; this sensitivity also causes the value of this ratio to depend on the phase of the solar cycle. We show that the O7+/O6+ ratio needs to be used with caution for solar wind classification and coronal temperature estimates, and recommend the C6+/C4+ ratio for these purposes.

  19. Femtosecond electronic dephasing and population relaxation of some novel semiconducting materials

    NASA Astrophysics Data System (ADS)

    Schneck, Jude Robert

    The dissipation of energy by excited carriers in semiconductors is crucial to device development. In particular, the carrier relaxation mechanisms are strongly modified by the degree of disorder introduced into the lattice via the growth process. The pump probe spectroscopic technique is ideally suited to monitor the energy dissipation process and elucidate the relaxation mechanisms contributing to the carrier decay. Additionally, phase breaking interactions of optical transitions, as measured via the photon echo spectroscopic technique, provides insight into the different homogeneous relaxation mechanisms contributing to the optical resonance. When compared to high quality semiconducting materials, the fundamental homogeneous relaxation mechanisms depend strongly on the disorder inherent in the material. The photon echo technique is ideal for quantifying the strength of these interactions. Femtosecond pump-probe responses of a GaN thin film excited above and below the UV band gap were measured to determine the kinetic relaxation pathways of carriers. A number of fluence dependent decay processes were identified, including carrier-carrier scattering, exciton decay, trapping to defect states, and hole state recovery. The characteristic timescales of these mechanisms ranged from <50 fs to >600 ps. In other measurements on GaN, two-pulse photon echoes due to the strongly dipole coupled excitons were observed as a function of temperature (10 -- 295K). A biexponential decay of the dephasing rate was found from these measurements and attributed to free and bound excitons. The dynamics of the E22 transition of (6,5) single walled carbon nanotubes was studied over a range of fluences via pump-probe spectroscopy. A fluence dependent dephasing rate was deduced from an analysis of the pump-probe signal intensity at a fixed short delay time allowing an effective cross section for exciton-exciton interactions to be determined. The relaxation kinetics of optically excited E22

  20. Flexible attosecond beamline for high harmonic spectroscopy and XUV/near-IR pump probe experiments requiring long acquisition times

    NASA Astrophysics Data System (ADS)

    Weber, S. J.; Manschwetus, B.; Billon, M.; Böttcher, M.; Bougeard, M.; Breger, P.; Géléoc, M.; Gruson, V.; Huetz, A.; Lin, N.; Picard, Y. J.; Ruchon, T.; Salières, P.; Carré, B.

    2015-03-01

    We describe the versatile features of the attosecond beamline recently installed at CEA-Saclay on the PLFA kHz laser. It combines a fine and very complete set of diagnostics enabling high harmonic spectroscopy (HHS) through the advanced characterization of the amplitude, phase, and polarization of the harmonic emission. It also allows a variety of photo-ionization experiments using magnetic bottle and COLTRIMS (COLd Target Recoil Ion Momentum Microscopy) electron spectrometers that may be used simultaneously, thanks to a two-foci configuration. Using both passive and active stabilization, special care was paid to the long term stability of the system to allow, using both experimental approaches, time resolved studies with attosecond precision, typically over several hours of acquisition times. As an illustration, applications to multi-orbital HHS and electron-ion coincidence time resolved spectroscopy are presented.

  1. Flexible attosecond beamline for high harmonic spectroscopy and XUV/near-IR pump probe experiments requiring long acquisition times

    SciTech Connect

    Weber, S. J. Manschwetus, B.; Billon, M.; Bougeard, M.; Breger, P.; Géléoc, M.; Gruson, V.; Lin, N.; Ruchon, T.; Salières, P.; Carré, B.

    2015-03-15

    We describe the versatile features of the attosecond beamline recently installed at CEA-Saclay on the PLFA kHz laser. It combines a fine and very complete set of diagnostics enabling high harmonic spectroscopy (HHS) through the advanced characterization of the amplitude, phase, and polarization of the harmonic emission. It also allows a variety of photo-ionization experiments using magnetic bottle and COLTRIMS (COLd Target Recoil Ion Momentum Microscopy) electron spectrometers that may be used simultaneously, thanks to a two-foci configuration. Using both passive and active stabilization, special care was paid to the long term stability of the system to allow, using both experimental approaches, time resolved studies with attosecond precision, typically over several hours of acquisition times. As an illustration, applications to multi-orbital HHS and electron-ion coincidence time resolved spectroscopy are presented.

  2. Flexible attosecond beamline for high harmonic spectroscopy and XUV/near-IR pump probe experiments requiring long acquisition times.

    PubMed

    Weber, S J; Manschwetus, B; Billon, M; Böttcher, M; Bougeard, M; Breger, P; Géléoc, M; Gruson, V; Huetz, A; Lin, N; Picard, Y J; Ruchon, T; Salières, P; Carré, B

    2015-03-01

    We describe the versatile features of the attosecond beamline recently installed at CEA-Saclay on the PLFA kHz laser. It combines a fine and very complete set of diagnostics enabling high harmonic spectroscopy (HHS) through the advanced characterization of the amplitude, phase, and polarization of the harmonic emission. It also allows a variety of photo-ionization experiments using magnetic bottle and COLTRIMS (COLd Target Recoil Ion Momentum Microscopy) electron spectrometers that may be used simultaneously, thanks to a two-foci configuration. Using both passive and active stabilization, special care was paid to the long term stability of the system to allow, using both experimental approaches, time resolved studies with attosecond precision, typically over several hours of acquisition times. As an illustration, applications to multi-orbital HHS and electron-ion coincidence time resolved spectroscopy are presented. PMID:25832212

  3. Polyatomic molecules under intense femtosecond laser irradiation.

    PubMed

    Konar, Arkaprabha; Shu, Yinan; Lozovoy, Vadim V; Jackson, James E; Levine, Benjamin G; Dantus, Marcos

    2014-12-11

    Interaction of intense laser pulses with atoms and molecules is at the forefront of atomic, molecular, and optical physics. It is the gateway to powerful new tools that include above threshold ionization, high harmonic generation, electron diffraction, molecular tomography, and attosecond pulse generation. Intense laser pulses are ideal for probing and manipulating chemical bonding. Though the behavior of atoms in strong fields has been well studied, molecules under intense fields are not as well understood and current models have failed in certain important aspects. Molecules, as opposed to atoms, present confounding possibilities of nuclear and electronic motion upon excitation. The dynamics and fragmentation patterns in response to the laser field are structure sensitive; therefore, a molecule cannot simply be treated as a "bag of atoms" during field induced ionization. In this article we present a set of experiments and theoretical calculations exploring the behavior of a large collection of aryl alkyl ketones when irradiated with intense femtosecond pulses. Specifically, we consider to what extent molecules retain their molecular identity and properties under strong laser fields. Using time-of-flight mass spectrometry in conjunction with pump-probe techniques we study the dynamical behavior of these molecules, monitoring ion yield modulation caused by intramolecular motions post ionization. The set of molecules studied is further divided into smaller sets, sorted by type and position of functional groups. The pump-probe time-delay scans show that among positional isomers the variations in relative energies, which amount to only a few hundred millielectronvolts, influence the dynamical behavior of the molecules despite their having experienced such high fields (V/Å). High level ab initio quantum chemical calculations were performed to predict molecular dynamics along with single and multiphoton resonances in the neutral and ionic states. We propose the

  4. Experimental Proof for the Role of Nonlinear Photoionization in Plasmonic Phototherapy.

    PubMed

    Minai, Limor; Zeidan, Adel; Yeheskely-Hayon, Daniella; Yudovich, Shimon; Kviatkovsky, Inna; Yelin, Dvir

    2016-07-13

    Targeting individual cells within a heterogeneous tissue is a key challenge in cancer therapy, encouraging new approaches for cancer treatment that complement the shortcomings of conventional therapies. The highly localized interactions triggered by focused laser beams promise great potential for targeting single cells or small cell clusters; however, most laser-tissue interactions often involve macroscopic processes that may harm healthy nearby tissue and reduce specificity. Specific targeting of living cells using femtosecond pulses and nanoparticles has been demonstrated promising for various potential therapeutic applications including drug delivery via optoporation, drug release, and selective cell death. Here, using an intense resonant femtosecond pulse and cell-specific gold nanorods, we show that at certain irradiation parameters cell death is triggered by nonlinear plasmonic photoionization and not by thermally driven processes. The experimental results are supported by a physical model for the pulse-particle-medium interactions. A good correlation is found between the calculated total number and energy of the generated free electrons and the observed cell death, suggesting that femtosecond photoionization plays the dominant role in cell death. PMID:27266996

  5. Attosecond Delays in Molecular Photoionization.

    PubMed

    Huppert, Martin; Jordan, Inga; Baykusheva, Denitsa; von Conta, Aaron; Wörner, Hans Jakob

    2016-08-26

    We report measurements of energy-dependent photoionization delays between the two outermost valence shells of N_{2}O and H_{2}O. The combination of single-shot signal referencing with the use of different metal foils to filter the attosecond pulse train enables us to extract delays from congested spectra. Remarkably large delays up to 160 as are observed in N_{2}O, whereas the delays in H_{2}O are all smaller than 50 as in the photon-energy range of 20-40 eV. These results are interpreted by developing a theory of molecular photoionization delays. The long delays measured in N_{2}O are shown to reflect the population of molecular shape resonances that trap the photoelectron for a duration of up to ∼110 as. The unstructured continua of H_{2}O result in much smaller delays at the same photon energies. Our experimental and theoretical methods make the study of molecular attosecond photoionization dynamics accessible. PMID:27610849

  6. Optical Synchronization Systems for Femtosecond X-raySources

    SciTech Connect

    Wilcox, Russell; Staples, John W.; Holzwarth, Ronald

    2004-05-09

    In femtosecond pump/probe experiments using short X-Ray and optical pulses, precise synchronization must be maintained between widely separated lasers in a synchrotron or FEL facility. We are developing synchronization systems using optical signals for applications requiring different ranges of timing error over 100 meter of glass fiber. For stabilization in the hundred femtosecond range a CW laser is amplitude modulated at 1 10 GHz, the signal retroreflected from the far end, and the relative phase used to correct the transit time with a piezoelectric phase modulator. For the sub-10 fsec range the laser frequency itself is upshifted 55 MHz with an acousto-optical modulator, retroreflected, upshifted again and phase compared at the sending end to a 110 MHz reference. Initial experiments indicate less than 1 fsec timing jitter. To lock lasers in the sub-10 fs range we will lock two single-frequency lasers separated by several tera Hertz to a master modelocked fiber laser, transmit the two frequencies over fiber, and lock two comb lines of a slave laser to these frequencies, thus synchronizing the two modelocked laser envelopes.

  7. A Bloch equation approach to intensity dependent optical spectra of light harvesting complex II: excitation dependence of light harvesting complex II pump-probe spectra.

    PubMed

    Richter, Marten; Renger, Thomas; Knorr, Andreas

    2008-01-01

    On the basis of the recent progress in the resolution of the structure of the antenna light harvesting complex II (LHC II) of the photosystem II, we propose a microscopically motivated theory to predict excitation intensity-dependent spectra. We show that optical Bloch equations provide the means to include all 2( N ) excited states of an oligomer complex of N coupled two-level systems and analyze the effects of Pauli Blocking and exciton-exciton annihilation on pump-probe spectra. We use LHC Bloch equations for 14 Coulomb coupled two-level systems, which describe the S (0) and S (1) level of every chlorophyll molecule. All parameter introduced into the Hamiltonian are based on microscopic structure and a quantum chemical model. The derived Bloch equations describe not only linear absorption but also the intensity dependence of optical spectra in a regime where the interplay of Pauli Blocking effects as well as exciton-exciton annihilation effects are important. As an example, pump-probe spectra are discussed. The observed saturation of the spectra for high intensities can be viewed as a relaxation channel blockade on short time scales due to Pauli blocking. The theoretical investigation is useful for the interpretation of the experimental data, if the experimental conditions exceed the low intensity pump limit and effects like strong Pauli Blocking and exciton-exciton annihilation need to be considered. These effects become important when multiple excitations are generated by the pump pulse in the complex. PMID:17924202

  8. Dynamics of femtosecond laser-induced periodic surface structures on silicon by high spatial and temporal resolution imaging

    SciTech Connect

    Jia, X.; Jia, T. Q. Peng, N. N.; Feng, D. H.; Zhang, S. A.; Sun, Z. R.

    2014-04-14

    The formation dynamics of periodic ripples induced by femtosecond laser pulses (pulse duration τ = 50 fs and central wavelength λ = 800 nm) are studied by a collinear pump-probe imaging technique with a temporal resolution of 1 ps and a spatial resolution of 440 nm. The ripples with periods close to the laser wavelength begin to appear upon irradiation of two pump pulses at surface defects produced by the prior one. The rudiments of periodic ripples emerge in the initial tens of picoseconds after fs laser irradiation, and the ripple positions keep unmoved until the formation processes complete mainly in a temporal span of 1500 ps. The results suggest that the periodic deposition of laser energy during the interaction between femtosecond laser pulses and sample surface plays a dominant role in the formation of periodic ripples.

  9. Measurement of non-instantaneous contribution to the χ(3) in different liquids using femtosecond chirped pulses

    NASA Astrophysics Data System (ADS)

    Langot, P.; Montant, S.; Freysz, E.

    2000-04-01

    In the Born-Oppenheimer approximation and considering a Debye nuclear motion, a theoretical computation of pump-probe two-beam coupling in liquids using femtosecond chirped pulses is proposed. This technique makes it possible to specifically evidence the non-instantaneous contribution to the third-order susceptibility χ(3). Our model, which is an extension at the femtosecond scale of the one proposed by Dogariu et al., describes the temporal evolution of the probe signal as a function of different parameters such as the linear laser chirp, the ratio between the pulse duration and the nuclear response time. Experimentally, this method is applied to characterize the non-instantaneous χ(3) contribution in transparent liquids such as CS 2, benzene and toluene. Time resolved pump-probe coupling data using parallel and perpendicular linear polarizations fit well with the model developed. The experimental ratio R between both fast and slow non-instantaneous χ(3)XXXX and χ(3)XYYX elements of the tensor is equal to 1.33±0.01 in all the liquids studied, and is in good agreement with the expected liquid nuclear symmetry.

  10. Cross-correlation measurement of femtosecond hard x-ray pulses from a laser plasma source: approaching 100 fs benchmark

    NASA Astrophysics Data System (ADS)

    Iqbal, Mazhar; Ijaz, M.; Stiel, H.; Noh, D. Y.; Janulewicz, K. A.

    2015-09-01

    Extremely fast processes happening on sub picosecond time scale can be captured by the well-known pump-probe scheme using ultrashort x-ray pulses as shutter. XFELs and femtosecond slicing beam lines on synchrotrons together-with ultra-short laser driven plasma x-ray sources (LPXs) as an attractive supplement offer exceptional parameters to unleash ultra-fast phenomenon. As pump-probe techniques based on the compact LPXs attract attention being jitter free, more precise knowledge of their emission duration, determining the measurement temporal resolution, became indispensable. We report here, for the first time, x-ray pulse duration from LPX using NIR pump x-ray probe cross-correlation method. The underlying mechanism is ultrafast relaxation of femtosecond laser-induced non-thermal electrons generated on the surface of transition metals. The emission duration of x-ray pulse is estimated by the evolution of transmission (110 +/-6 fs) and fluorescence signals (129 +/- 19 fs) and found in good agreement with the theoretical prediction of <=100 fs for LPXs.

  11. Direct mapping of recoil in the ion-pair dissociation of molecular oxygen by a femtosecond depletion method.

    PubMed

    Baklanov, Alexey V; Janssen, Liesbeth M C; Parker, David H; Poisson, Lionel; Soep, Benoit; Mestdagh, Jean-Michel; Gobert, Olivier

    2008-12-01

    Time-resolved dynamics of the photodissociation of molecular oxygen, O(2), via the (3)Sigma(u) (-) ion-pair state have been studied with femtosecond time resolution using a pump-probe scheme in combination with velocity map imaging of the resulting O(+) and O(-) ions. The fourth harmonic of a femtosecond titanium-sapphire (Ti:sapphire) laser (lambda approximately 205 nm) was found to cause three-photon pumping of O(2) to a level at 18.1 eV. The parallel character of the observed O(+) and O(-) images allowed us to conclude that dissociation takes place on the (3)Sigma(u) (-) ion-pair state. The 815 nm fundamental of the Ti:sapphire laser used as probe was found to cause two-photon electron photodetachment starting from the O(2) ion-pair state, giving rise to (O((3)P)+O(+)((4)S)) products. This was revealed by the observed depletion of the yield of the O(-) anion and the appearance of a new O(+) cation signal with a kinetic energy E(transl)(O(+)) dependent on the time delay between the pump and probe lasers. This time-delay dependence of the dissociation dynamics on the ion-pair state has also been simulated, and the experimental and simulated results coincide very well over the experimental delay-time interval from about 130 fs to 20 ps where two- or one-photon photodetachment takes place, corresponding to a change in the R(O(+),O(-)) interatomic distance from 12 to about 900 A. This is one of the first implementations of a depletion scheme in femtosecond pump-probe experiments which could prove to be quite versatile and applicable to many femtosecond time-scale experiments. PMID:19063560

  12. Biomedical applications of laser photoionization

    NASA Astrophysics Data System (ADS)

    Xiong, Xiaoxiong; Moore, Larry J.; Fassett, John R.; O'Haver, Thomas C.

    1991-07-01

    Trace elements are important for many essential metabolic functions. Zinc is a structural/functional component in more than 200 enzymes active in the biochemistry of cell division and tissue growth, neurology and endocrine control. Calcium is involved in intracellular control mechanisms and in skeletal bone building and resorption processes related to osteoporosis. Sensitive and selective laser photoionization is being developed to understand mechanisms in smaller samples and biological units approaching the cellular domain. Zinc has an ionization potential of 9.4 eV, or 75766.8 cm-1. Several processes are being explored, including two-photon resonant, three- photon ionization utilizing sequential UV transitions, e.g., 4s2 1S0 yields 4s4p 3P1 and 4s4p 3P1 yields 4s5d 3D1. Preliminary zinc stable isotope ratio data obtained by thermal atomization and laser photoionization agree with accepted values within 2 to 5%, except for anomalous 67Zn. Photoionization of calcium is being studied for isotope enrichment and ratio measurement using narrow and medium bandwidth lasers. Several ionization pathways, e.g., 4s2 1S0 - 2hv1 yields 4s10s - hv2 yields Ca+ (4s2S), are being investigated for isotopically selective ionization. Auto-ionization pathways are explored for greater efficiency in isotopic analysis. All studies have utilized a Nd:YAG- pumped laser system with one or two frequency-doubled tunable dye lasers coupled either to a magnetic sector or time-of-flight mass spectrometer.

  13. Photoionization of methanol and formaldehyde

    NASA Technical Reports Server (NTRS)

    Warneck, P.

    1971-01-01

    Photoions produced in methanol and formaldehyde by radiation in the spectral region 450-1150 A were analyzed mass spectrometrically, and their relative yields were determined as a function of wavelength. First ionization potentials were determined, and the ion yield curves were interpreted in terms of ionization processes in conjunction with other data. Fragment ions were detected on mass numbers of 31, 30, 29, 15, and 14 for methanol, and 29, 2, and 1 for formaldehyde. The associated appearance potentials were determined and were used to calculate heats of formation of the ions CH2OH(+) and HCO(+), and the radicals CH3, CH2, and HCO.

  14. Intercomparison of the comparative reactivity method (CRM) and pump-probe technique for measuring total OH reactivity in an urban environment

    NASA Astrophysics Data System (ADS)

    Hansen, R. F.; Blocquet, M.; Schoemaecker, C.; Léonardis, T.; Locoge, N.; Fittschen, C.; Hanoune, B.; Stevens, P. S.; Sinha, V.; Dusanter, S.

    2015-10-01

    The investigation of hydroxyl radical (OH) chemistry during intensive field campaigns has led to the development of several techniques dedicated to ambient measurements of total OH reactivity, which is the inverse of the OH lifetime. Three techniques are currently used during field campaigns, including the total OH loss rate method, the pump-probe method, and the comparative reactivity method. However, no formal intercomparison of these techniques has been published so far, and there is a need to ensure that measurements of total OH reactivity are consistent among the different techniques. An intercomparison of two OH reactivity instruments, one based on the comparative reactivity method (CRM) and the other based on the pump-probe method, was performed in October 2012 in a NOx-rich environment, which is known to be challenging for the CRM technique. This study presents an extensive description of the two instruments, the CRM instrument from Mines Douai (MD-CRM) and the pump-probe instrument from the University of Lille (UL-FAGE), and highlights instrumental issues associated with the two techniques. It was found that the CRM instrument used in this study underestimates ambient OH reactivity by approximately 20 % due to the photolysis of volatile organic compounds (VOCs) inside the sampling reactor; this value is dependent on the position of the lamp within the reactor. However, this issue can easily be fixed, and the photolysis of VOCs was successfully reduced to a negligible level after this intercomparison campaign. The UL-FAGE instrument may also underestimate ambient OH reactivity due to the difficulty to accurately measure the instrumental zero. It was found that the measurements are likely biased by approximately 2 s-1, due to impurities in humid zero air. Two weeks of ambient sampling indicate that the measurements performed by the two OH reactivity instruments are in agreement, within the measurement uncertainties for each instrument, for NOx mixing ratios

  15. Intercomparison of the comparative reactivity method (CRM) and pump-probe technique for measuring total OH reactivity in an urban environment

    NASA Astrophysics Data System (ADS)

    Hansen, R. F.; Blocquet, M.; Schoemaecker, C.; Léonardis, T.; Locoge, N.; Fittschen, C.; Hanoune, B.; Stevens, P. S.; Sinha, V.; Dusanter, S.

    2015-06-01

    The investigation of hydroxyl radical (OH) chemistry during intensive field campaigns has led to the development of several techniques dedicated to ambient measurements of total OH reactivity, which is the inverse of the OH lifetime. Three techniques are currently used during field campaigns, including the total OH loss rate method, the pump-probe method, and the comparative reactivity method. However, no formal intercomparison of these techniques has been published so far, and there is a need to ensure that measurements of total OH reactivity are consistent among the different techniques. An intercomparison of two OH reactivity instruments, one based on the Comparative Reactivity Method (CRM) and the other based on the pump-probe method, was performed in October 2012 in a NOx-rich environment, which is known to be challenging for the CRM technique. This study presents an extensive description of the two instruments, the CRM instrument from Mines Douai (MD-CRM) and the pump-probe instrument from the University of Lille (UL-FAGE), and highlights instrumental issues associated with the two techniques. It was found that the CRM instrument used in this study underestimates ambient OH reactivity by approximately 20 % due to the photolysis of Volatile Organic Compounds (VOCs) inside the sampling reactor; this value is dependent on the position of the lamp within the reactor. However, this issue can easily be fixed, and the photolysis of VOCs was successfully reduced to a negligible level after this intercomparison campaign. The UL-FAGE instrument may also underestimate ambient OH reactivity due to the difficulty to accurately measure the instrumental zero. It was found that the measurements are likely biased by approximately 2 s-1, due to impurities in humid zero air. Two weeks of ambient sampling indicate that the measurements performed by the two OH reactivity instruments are in agreement, within the measurement uncertainties for each instrument, for NOx mixing ratios

  16. Investigating vibrational relaxation in cyanide-bridged transition metal mixed-valence complexes using two-dimensional infrared and infrared pump-probe spectroscopies

    PubMed Central

    Slenkamp, Karla M.; Lynch, Michael S.; Brookes, Jennifer F.; Bannan, Caitlin C.; Daifuku, Stephanie L.; Khalil, Munira

    2016-01-01

    Using polarization-selective two-dimensional infrared (2D IR) and infrared pump-probe spectroscopies, we study vibrational relaxation of the four cyanide stretching (νCN) vibrations found in [(NH3)5RuIIINCFeII(CN)5]− (FeRu) dissolved in D2O or formamide and [(NC)5FeIICNPtIV(NH3)4NCFeII(CN)5]4− (FePtFe) dissolved in D2O. These cyanide-bridged transition metal complexes serve as models for understanding the role high frequency vibrational modes play in metal-to-metal charge transfers over a bridging ligand. However, there is currently little information about vibrational relaxation and dephasing dynamics of the anharmonically coupled νCN modes in the electronic ground state of these complexes. IR pump-probe experiments reveal that the vibrational lifetimes of the νCN modes are ∼2 times faster when FeRu is dissolved in D2O versus formamide. They also reveal that the vibrational lifetimes of the νCN modes of FePtFe in D2O are almost four times as long as for FeRu in D2O. Combined with mode-specific relaxation dynamics measured from the 2D IR experiments, the IR pump-probe experiments also reveal that intramolecular vibrational relaxation is occurring in all three systems on ∼1 ps timescale. Center line slope dynamics, which have been shown to be a measure of the frequency-frequency correlation function, reveal that the radial, axial, and trans νCN modes exhibit a ∼3 ps timescale for frequency fluctuations. This timescale is attributed to the forming and breaking of hydrogen bonds between each mode and the solvent. The results presented here along with our previous work on FeRu and FePtFe reveal a picture of coupled anharmonic νCN modes where the spectral diffusion and vibrational relaxation dynamics depend on the spatial localization of the mode on the molecular complex and its specific interaction with the solvent. PMID:27158634

  17. Photoabsorption and photoionization of HD

    SciTech Connect

    Dehmer, Patricia M.; Chupka, William A.

    1983-01-01

    Relative photoabsorption and photoionization cross sections have been measured for HD at a temperature of 78 K in the wavelength region from 735 to 805 Â. The present wavelength resolution of 0.016 Â represents an improvement of more than two orders of magnitude over that of previous photoionization studies of this molecule. Bands of the 3pπ D ¹Πu←X ¹Σg⁺ system are observed to v'=17, and ionization efficiencies are reported for a number of Rydberg states of low principal quantum number. As in the case of H2, the ionization efficiency is close to unity for Rydberg states that can autoionize with Δv= -1, but drops to zero for states that can autoionize only with a large change in vibrational quantum number and that are significantly predissociated (such as the 3pπ D ¹Πu state). The breakdown of (g,u) symmetry in HD and the resulting effects on the absorption spectrum and on the decay paths of the Rydberg states are discussed.

  18. Double photoionization of SO 2 and fragmentation spectroscopy of SO 2++ studied by a photoion-photoion coincidence method

    NASA Astrophysics Data System (ADS)

    Dujardin, Gérald; Leach, Sydney; Dutuit, Odile; Guyon, Paul-Marie; Richard-Viard, Martine

    1984-08-01

    Doubly charged sulphur dioxide cations (SO 2++) are produced by photoionization with synchrotron radiation from ACO in the excitation-energy range 34-54 eV. A new photoion-photoion coincidence (PIPICO) experiment is described in which coincidences between photoion fragments originating from the dissociation of the doubly charged parent cation are counted. This PIPICO method enables us to study the fragmentation of individual electronically excited states of SO 2++ and to determine the corresponding absolute double-photoionization partial cross sections as a function of the excitation energy. A tentative assignment of the three observed α, β and γ SO 2++ states is given. The dissociation processes of the α and β states into the products SO + + O + are found to be non-statistical in nature; the γ state dissociates completely into three atomic fragments S + + O + + O. Three main observed features of the double-photoionization cross-section curves are discussed in the text: appearance potentials, linear threshold laws, and constant double-photoionization cross sections relative to the total ionization cross section at high energies.

  19. Time-resolved pump-probe photoelectron spectroscopy of helium using a mode-locked laser synchronized with synchrotron radiation pulses

    NASA Astrophysics Data System (ADS)

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

    1994-12-01

    We report a new experimental setup consisting in the synchronization of 74.9094 MHz pulses from a mode-locked Ar + laser with 8.32 MHz pulses of vacuum ultraviolet (VUV) synchrotron radiation from the Super-ACO storage ring of the Laboratoire pour l'Utilisation du Rayonnement Electromagnétique (LURE). The capabilities of the setup are demonstrated in a time-resolved pump-probe (VUV + visible) experiment in which free helium atoms are resonantly ionized via the short-lived 1s3p ( 1P) state. This experiment allowed us to obtain the value of 1.12 ns for the temporal resolution (FWHM) of the experimental setup and to show the relevance of this technique for the investigation of nanosecond dynamics on gas phase species.

  20. Picosecond pump-probe measurement of bandgap changes in SiO2/TiO2 one-dimensional photonic bandgap structures

    NASA Astrophysics Data System (ADS)

    Hwang, Jisoo; Kim, Min Jung; Wu, J. W.; Mook Lee, Seung; Rhee, Bum Ku

    2006-02-01

    A picosecond pump-probe nonlinear optical measurement is performed in SiO2/TiO2 one-dimensional photonic bandgap structures fabricated by a solgel method. Both high and low band edges were examined by varying the probe wavelengths and angle tuning was also employed to further clarify the mechanism of a nonlinear optical response. The third-order nonlinear optical response in one-dimensional photonic bandgap structures that comprise TiO2 films is responsible for the nonlinear optical transmissions at both bandgap edges, with an 8% decrease at the low-energy edge and a 4.5% increase at the high-energy edge for a 355 nm pump intensity of 430 MW/cm2.

  1. Picosecond pump-probe measurement of bandgap changes in SiO2/TiO2 one-dimensional photonic bandgap structures.

    PubMed

    Hwang, Jisoo; Kim, Min Jung; Wu, J W; Lee, Seung Mook; Rhee, Bum Ku

    2006-02-01

    A picosecond pump-probe nonlinear optical measurement is performed in SiO2/TiO2 one-dimensional photonic bandgap structures fabricated by a solgel method. Both high and low band edges were examined by varying the probe wavelengths and angle tuning was also employed to further clarify the mechanism of a nonlinear optical response. The third-order nonlinear optical response in one-dimensional photonic bandgap structures that comprise TiO2 films is responsible for the nonlinear optical transmissions at both bandgap edges, with an 8% decrease at the low-energy edge and a 4.5% increase at the high-energy edge for a 355 nm pump intensity of 430 MW/cm2. PMID:16480214

  2. Measurement of the magneto-optical response of Fe and CrO2 epitaxial films by pump-probe spectroscopy: Evidence for spin-charge separation

    NASA Astrophysics Data System (ADS)

    Carpene, E.; Boschini, F.; Hedayat, H.; Piovera, C.; Dallera, C.; Puppin, E.; Mansurova, M.; Münzenberg, M.; Zhang, X.; Gupta, A.

    2013-05-01

    We have investigated the magneto-optical response of Fe and CrO2 epitaxial films by pump-probe polarimetry, showing that charge and spin dynamics can be unambiguously disentangled. The time-resolved Kerr ellipticity and rotation in the metallic sample are essentially identical after the initial transient (shorter than a picosecond), but they considerably differ in the oxide film, even tens of picoseconds past the optical excitation. These differences are determined by the combined effects of photoexcited charge carriers and spins on the Kerr signal, but a detailed polarimetric analysis can explicitly unravel these contributions. In addition, the diagonal and off-diagonal terms of the dielectric tensor can be retrieved, providing the complete dynamical characterization of magnetic and optical properties in a ferromagnet, which is of utmost importance to understand spin evolution in magnetically correlated complex oxide materials.

  3. Nuclear Fluxes in Diatomic Molecules Deduced from Pump-Probe Spectra with Spatiotemporal Resolutions down to 5 pm and 200 asec

    NASA Astrophysics Data System (ADS)

    Manz, Jörn; Pérez-Torres, Jhon Fredy; Yang, Yonggang

    2013-10-01

    When molecules move, their nuclei flow. The corresponding quantum observable, i.e., the nuclear flux density, was introduced by Schrödinger in 1926, but until now, it has not been measured. Here the first experimental results are deduced from high-resolution pump-probe measurements of the time-dependent nuclear densities in a vibrating diatomic molecule or molecular ion. The nuclear densities are converted to flux densities by means of the continuity equation. The flux densities are much more sensitive to time-dependent quantum effects than the densities. Applications to the sodium molecule and the deuterium molecular ion unravel four new effects; e.g., at the turns from bond stretch to compression, the flux of the nuclei exhibits multiple changes of directions, from small to large bond lengths, a phenomenon that we call the “quantum accordion.”

  4. Ultrafast pump-probe and 2DIR anisotropy and temperature-dependent dynamics of liquid water within the E3B model

    NASA Astrophysics Data System (ADS)

    Ni, Yicun; Skinner, J. L.

    2014-07-01

    Recently, Tainter et al. [J. Chem. Phys. 134, 184501 (2011)] reparameterized a new rigid water model (E3B) that explicitly includes three-body interactions in its Hamiltonian. Compared to commonly used water models such as SPC/E and TIP4P, the new model shows better agreement with experiment for many physical properties including liquid density, melting temperature, virial coefficients, etc. However, the dynamics of the E3B model, especially as a function of temperature, has not been systematically evaluated. Experimental nonlinear vibrational spectroscopy is an ideal tool to study the dynamics of matter in condensed phases. In the present study, we calculate linear and nonlinear vibrational spectroscopy observables for liquid water using the E3B model at five temperatures: 10, 30, 50, 70 and 90 °C. Specifically, we calculate absorption and Raman spectra and pump-probe anisotropy for HOD in H2O at all temperatures, frequency-resolved pump-probe anisotropy for HOD in both H2O and D2O at 30 °C, and 2DIR anisotropy for HOD in D2O at 30 °C. In all cases, we find reasonable agreement with experiment, and for the ultrafast spectroscopy our results are a significant improvement over those of the SPC/E model. A likely reason for this improvement is that the three-body interaction terms in the E3B model are able to model cooperative hydrogen bonding. We also calculate rotational and frequency relaxation times at all temperatures, and fit the results to the Arrhenius equation. We find that the activation energy for hydrogen-bond switching in liquid water is 3.8 kcal/mol, which agrees well with the experimental value of 3.7 kcal/mol obtained from anisotropy decay experiments.

  5. Dynamics of ultrafast internal conversion processes studied by femtosecond time-delayed photoelectron spectroscopy

    SciTech Connect

    Cyr, D.R.; Hayden, C.C.

    1995-08-01

    The authors have studied the dynamics of ultrafast internal conversion processes using femtosecond time-resolved photoionization and photoelectron spectroscopy. In hexatriene, following femtosecond pulse excitation at 250 nm, they use time-delayed photoionization to observe the formation and decay of an intermediate species on the subpicosecond time scale. With time-resolved photoelectron spectroscopy, the rapid evolution of vibrational excitation in this intermediate is observed, as electronic energy is converted to vibrational energy in the molecule. The photodynamics of cis and trans isomers of hexatriene are compared and found to be surprisingly different on the 2-3 psec time scale. These results are important for understanding the fundamental photochemical processes in linear polyenes, which have served as models for the active chromophores of many biological photosystems.

  6. Optical nonlinear dynamics in ZnS from femtosecond laser pulses

    SciTech Connect

    Wu, Yu-E; Ren, Mengxin Wang, Zhenhua; Li, Wenhua; Wu, Qiang; Zhang, Xinzheng Xu, Jingjun; Synergetic Innovation Center of Chemical Science and Engineering, Tianjin 300071 ; Yi, Sanming

    2014-05-15

    A wavelength swapping nondegenerate pump-probe technique to measure the magnitudes of the nonlinear optical dynamics as well as the relaxation time of electrons in high energy levels is presented using a ZnS single crystal wafer as an example. By pumping the sample with 800 nm femtosecond pulses and probing at 400 nm, nondegenerate two-photon absorption (N-2PA) happens exclusively, and the measured curves only show instantaneous features without relaxation tails. The N-2PA coefficient was derived explicitly as 7.52 cm/GW. Additionally, when the wavelengths of the pump and probe beams are swapped, extra information about the relaxation time of the hot electrons excited in the conduction band is obtained. The combined results above are helpful for evaluating the characteristics of an optical switches based on ZnS or other materials with respect to its nonlinear optical dynamic aspect.

  7. Gain dynamics of a free-space nitrogen laser pumped by circularly polarized femtosecond laser pulses

    NASA Astrophysics Data System (ADS)

    Yao, Jinping; Xie, Hongqiang; Zeng, Bin; Chu, Wei; Li, Guihua; Ni, Jielei; Zhang, Haisu; Jing, Chenrui; Zhang, Chaojin; Xu, Huailiang; Cheng, Ya; Xu, Zhizhan

    2014-08-01

    We experimentally demonstrate ultrafast dynamic of generation of a strong 337-nm nitrogen laser by injecting an external seed pulse into a femtosecond laser filament pumped by a circularly polarized laser pulse. In the pump-probe scheme, it is revealed that the population inversion between the excited and ground states of N2 for the free-space 337-nm laser is firstly built up on the timescale of several picoseconds, followed by a relatively slow decay on the timescale of tens of picoseconds, depending on the nitrogen gas pressure. By measuring the intensities of 337-nm signal from nitrogen gas mixed with different concentrations of oxygen gas, it is also found that oxygen molecules have a significant quenching effect on the nitrogen laser signal. Our experimental observations agree with the picture of electron-impact excitation.

  8. Gain dynamics of a free-space nitrogen laser pumped by circularly polarized femtosecond laser pulses.

    PubMed

    Yao, Jinping; Xie, Hongqiang; Zeng, Bin; Chu, Wei; Li, Guihua; Ni, Jielei; Zhang, Haisu; Jing, Chenrui; Zhang, Chaojin; Xu, Huailiang; Cheng, Ya; Xu, Zhizhan

    2014-08-11

    We experimentally demonstrate ultrafast dynamic of generation of the 337-nm nitrogen laser by injecting an external seed pulse into a femtosecond laser filament pumped by a circularly polarized laser pulse. In the pump-probe scheme, it is revealed that the population inversion between the C(3)Π(u) and B(3)Π(g) states of N(2) for the free-space 337-nm laser is firstly built up on the timescale of several picoseconds, followed by a relatively slow decay on the timescale of tens of picoseconds, depending on the nitrogen gas pressure. By measuring the intensities of 337-nm signal from nitrogen gas mixed with different concentrations of oxygen gas, it is also found that oxygen molecules have a significant quenching effect on the nitrogen laser signal. Our experimental observations agree with the picture of electron-impact excitation. PMID:25320986

  9. Femtosecond pump/supercontinuum-probe setup with 20 kHz repetition rate.

    PubMed

    Auböck, Gerald; Consani, Cristina; Monni, Roberto; Cannizzo, Andrea; van Mourik, Frank; Chergui, Majed

    2012-09-01

    We developed a fast multichannel detection system for pump-probe spectroscopy, capable of detecting single shot super-continuum spectra at the repetition rate (10-50 kHz) of an amplified femtosecond laser system. By tandem pumping the amplifier with three pump lasers we obtain very low noise operation, with less than 0.1% rms intensity fluctuations at the output of the amplifier. We also propose an alternative way of chopping the pump beam. With a synchronized scanning mirror two spots in the sample are illuminated by the train of pump pulses in an alternating fashion, such that when both spots are interrogated by the probe pulse, the duty cycle of the experiment is doubled. PMID:23020360

  10. Femtosecond wave-packet dynamics in cesium dimers studied through controlled stimulated emission

    SciTech Connect

    Yuan Luqi; Wang Xi; Patnaik, Anil K.; Sokolov, Alexei V.; Ariunbold, Gombojav O.; Murawski, Robert K.; Pestov, Dmitry; Sautenkov, Vladimir A.; Rostovtsev, Yuri V.; Scully, Marlan O.

    2010-05-15

    We study the dynamics of wave packets in cesium dimers using a femtosecond-controlled pump-probe technique. We implement configurations with one pulse (pump) or two pulses (pump and control) to produce vibrational wave packets on the electronic excited state. The transmission of an additional, variable-delay probe pulse is measured to monitor the time evolution of the wave packets. In the case of the pump-control-probe configuration, a superposition of two independent wave packets is observed. In order to elucidate the observed experimental data, we develop a theory based on the Liouville equation for the density matrix associated with the Franck-Condon factors. Both the numerical and analytical calculations are in good agreement with our experimental results.

  11. Femtosecond crystallography with ultrabright electrons and x-rays: capturing chemistry in action.

    PubMed

    Miller, R J Dwayne

    2014-03-01

    With the recent advances in ultrabright electron and x-ray sources, it is now possible to extend crystallography to the femtosecond time domain to literally light up atomic motions involved in the primary processes governing structural transitions. This review chronicles the development of brighter and brighter electron and x-ray sources that have enabled atomic resolution to structural dynamics for increasingly complex systems. The primary focus is on achieving sufficient brightness using pump-probe protocols to resolve the far-from-equilibrium motions directing chemical processes that in general lead to irreversible changes in samples. Given the central importance of structural transitions to conceptualizing chemistry, this emerging field has the potential to significantly improve our understanding of chemistry and its connection to driving biological processes. PMID:24604195

  12. Separating pairing from quantum phase coherence dynamics above the superconducting transition by femtosecond spectroscopy

    PubMed Central

    Madan, I.; Kurosawa, T.; Toda, Y.; Oda, M.; Mertelj, T.; Kusar, P.; Mihailovic, D.

    2014-01-01

    In classical superconductors an energy gap and phase coherence appear simultaneously with pairing at the transition to the superconducting state. In high-temperature superconductors, the possibility that pairing and phase coherence are distinct and independent processes has led to intense experimental search of their separate manifestations. Using femtosecond spectroscopy methods we now show that it is possible to clearly separate fluctuation dynamics of the superconducting pairing amplitude from the phase relaxation above the critical transition temperature. Empirically establishing a close correspondence between the superfluid density measured by THz spectroscopy and superconducting optical pump-probe response over a wide region of temperature, we find that in differently doped Bi2Sr2CaCu2O8+δ crystals the pairing gap amplitude monotonically extends well beyond Tc, while the phase coherence shows a pronounced power-law divergence as T → Tc, thus showing that phase coherence and gap formation are distinct processes which occur on different timescales. PMID:25014162

  13. Theoretical description of femtosecond fluorescence depletion spectrum of molecules in solution.

    PubMed

    Niu, Kai; Dong, Li-Qing; Cong, Shu-Lin

    2007-09-28

    A theoretical model used for calculating the fluorescence depletion spectrum (FDS) of molecules in liquids induced by femtosecond pump-probe laser pulses is proposed based on the reduced density matrix theory. The FDS intensity is obtained by calculating the stimulated emission of the excited electronic state. As an application of the theoretical model, the FDS of oxazine 750 (OX-750) molecule in acetone solution is calculated. The simulated FDS agrees with the experimental result of Liu et al. [J. Y. Liu et al., J. Phys. Chem. A 107, 10857 (2003)]. The calculated vibrational relaxation rate is 2.5 ps(-1) for the OX-750 molecule. Vibrational population dynamics and wave packet evolution in the excited state are described in detail. The effect of the probe pulse parameter on the FDS is also discussed. PMID:17902916

  14. Imaging molecular orbitals using photoionization

    NASA Astrophysics Data System (ADS)

    Santra, Robin

    2006-10-01

    The interpretation of a recent experiment using high-order harmonic generation [Itatani et al., Nature 432 (2004) 867] as a measurement of the highest occupied molecular orbital of a molecule is conceptually problematic, even if the independent-particle picture is taken seriously. Guided by the relationship between the amplitude for one-photon-induced electron emission and the electron-ion recombination amplitude in the three-step model of high-order harmonic generation, it is argued that synchrotron-based photoionization might be a superior approach to imaging molecular orbitals. Within the Hartree-Fock independent-particle picture, the molecular-frame photoelectron angular distributions, measured as a function of photon energy, could be used to reconstruct all orbitals occupied in the Hartree-Fock ground state of the molecule investigated. It is suggested that laser alignment techniques could be employed to facilitate the measurement of the molecular-frame photoelectron angular distributions.

  15. Cluster beam analysis via photoionization

    SciTech Connect

    Grover, J.R. ); Herron, W.J.; Coolbaugh, M.T.; Peifer, W.R.; Garvey, J.F. )

    1991-08-22

    A photoionization method for quantitatively analyzing the neutral products of free jet expansions is described. The basic principle is to measure the yield of an ion characterization of each component cluster at a photon energy just below that at which production of the same ion from larger clusters can be detected. Since there is then no problem with fragmentation, the beam density of each neutral cluster can be measured in the presence of larger clusters. Although these measurements must be done in the test ions' onset regions where their yields are often quite small, the technique is made highly practicable by the large intensities of widely tunable vacuum-ultraviolet synchrotron light now available at electron storage rings. As an example, the method is applied to the analysis of cluster beams collimated from the free jet expansion of a 200:1 ammonia-chlorobenzene mixture.

  16. Single and double photoionization of Li2

    NASA Astrophysics Data System (ADS)

    Pindzola, M. S.; Li, Ye; Colgan, J.

    2015-01-01

    Time-dependent close-coupling methods are used to study the single and double photoionization of Li2. Formulations for both one-active and two-active electron methods make use of Hartree with local exchange potentials for the core electrons. Both the single and double photoionization cross sections for Li2 are found to be larger for linear polarization than for circular polarization, in sharp contrast to that found before for H2. In particular the double photoionization cross sections for Li2 are found to be approximately five times larger than for H2 and thus more easily observed by future experiments.

  17. 2006 Photoions, Photoionization & Photodetachment held on January 29-February 3, 2006

    SciTech Connect

    Robert Continetti Nancy Ryan Gray

    2006-09-06

    The 4th Gordon Conference on Photoions, Photoionization and Photodetachment will be held January 29-February 3, 2006 at the Santa Ynez Valley Marriott in Buellton, California. This meeting will continue to cover fundamentals and applications of photoionization and photodetachment, including valence and core-level phenomena and applications to reaction dynamics, ultrashort laser pulses and the study of exotic molecules and anions. Further information will be available soon at the Gordon Conference Website, and will be announced.

  18. Compton Scattering and Its Applications: The PLEIADES Femtosecond X-ray Source at LLNL

    SciTech Connect

    Hartemann, F V; Brown, W J; Anderson, S G; Barty, C P J; Betts, S M; Booth, R; Crane, J K; Cross, R R; Fittinghoff, D N; Gibson, D J; Kuba, J; Rupp, B; Tremaine, A M; Springer, P T

    2003-05-01

    Remarkable developments in critical technologies including terawatt-class lasers using chirped-pulse amplification, high brightness photoinjectors, high-gradient accelerators, and superconducting linacs make it possible to design and operate compact, tunable, subpicosecond Compton scattering x-ray sources with a wide variety of applications. In such novel radiation sources, the collision between a femtosecond laser pulse and a low emittance relativistic electron bunch in a small ({micro}m{sup 3}) interaction volume produces Doppler-upshifted scattered photons with unique characteristics: the energy is tunable in the 5-500 keV range, the angular divergence of the beam is small (mrad), and the pulses are ultrashort (10 fs - 10 ps). Two main paths are currently being followed in laboratories worldwide: high peak brightness, using ultrahigh intensity femtosecond lasers at modest repetition rates, and high average brightness, using superconducting linac and high average power laser technology at MHz repetition rates. Targeted applications range from x-ray protein crystallography and high contrast medical imaging to femtosecond pump-probe and diffraction experiments. More exotic uses of such sources include the {gamma}-{gamma} collider, NIF backlighting, nonlinear Compton scattering, and high-field QED. Theoretical considerations and experimental results will be discussed within this context.

  19. Fine- and hyperfine-structure effects in molecular photoionization. I. General theory and direct photoionization.

    PubMed

    Germann, Matthias; Willitsch, Stefan

    2016-07-28

    We develop a model for predicting fine- and hyperfine intensities in the direct photoionization of molecules based on the separability of electron and nuclear spin states from vibrational-electronic states. Using spherical tensor algebra, we derive highly symmetrized forms of the squared photoionization dipole matrix elements from which we derive the salient selection and propensity rules for fine- and hyperfine resolved photoionizing transitions. Our theoretical results are validated by the analysis of the fine-structure resolved photoelectron spectrum of O2 reported by Palm and Merkt [Phys. Rev. Lett. 81, 1385 (1998)] and are used for predicting hyperfine populations of molecular ions produced by photoionization. PMID:27475368

  20. Ultrafast Space-time and Spectrum-time Resolved Diagnostics of Multicharged Femtosecond Laser Microplasma

    NASA Astrophysics Data System (ADS)

    Garnov, S. V.; Bukin, V. V.; Malyutin, A. A.; Strelkov, V. V.

    2009-07-01

    We present the review of the recent experimental studies of fundamental mechanisms of femtosecond laser plasma formation and evolution performed in A. M. Prokhorov General Physics Institute of Russian Academy of Sciences. The main object we dealt with was the micro-sized plasma produced in gases with high intensity (up to 5×1017 W/cm2), tightly focused (to a few microns in diameter) IR and UV femtosecond laser pulses. The main attention in the experiments was paid to the initial stage of microplasma formation and evolution characterized by strong laser-plasma coupling resulting in efficient ionization and heating of the medium, distortion of laser beam, and nonlinear spectral conversion of laser radiation to the continuum and laser harmonics. Using a precise pump-probe micro-interferometric technique the dynamics of plasma was studied with femtosecond time-resolution in a wide density range—from a minimal detectable electron concentration (1019 cm-3) to the almost total (down to nuclei) ionization of ions occurred under femtosecond excitation. The obtained time-dependences of plasma density were analyzed. It was observed, for the first time, that a characteristic time of femtosecond laser plasma formation in gases considerably (in times) exceeds the duration of the pump laser pulse. This postionization process is attributed to impact ionization of plasma by hot electrons. We compare the results of the experiments with what the developed theory predicts. Using an ultrafast streak-camera-based spectroscopy technique the temporal evolution of microplasma emission and the dynamics of spectral lines formation in UV-visible range were studied with picosecond time-resolution.

  1. Ultraviolet photoionization in CO2 TEA lasers

    NASA Astrophysics Data System (ADS)

    Scott, S. J.; Smith, A. L. S.

    1988-07-01

    The effects of gas composition and spark parameters on the UV emission in CO2 TEA laser gas mixtures were investigated together with the nature of photoionization process and the photoelectron-loss mechanism. A linear relationship was found between N2 concentration and photoionization (with no such dependence on C concentration, from CO and CO2), but the increases in photoionization that could be effected by optimizing the spark discharge circuit parameters were much higher than those produced by changes in gas composition. UV emission was directly proportional to the amount of stored electrical energy in the spark-discharge circuit and to the cube of the peak current produced in the spark by the discharge of this energy. Photoionization was also found to be proportional to the spark electrode gap. It was found that free-space sparks gave a considerably broader emission pattern than a surface-guided notched spark.

  2. Photoionized astrophysical plasmas in the laboratory

    SciTech Connect

    Hill, Edward; Rose, Steven

    2010-10-15

    The time-dependent collisional-radiative code ALICE [E. G. Hill and S. J. Rose, High Energy Density Phys. 5, 302 (2009)] is used to model the spectrum from a laboratory photoionized silicon plasma [S. Fujioka et al., Nat. Phys. 5, 821 (2009)]. The results show a good agreement with the laboratory spectrum and lend support to the accompanying analytical discussion of photoionized laboratory spectra, their parametrization, and relevance to astrophysics.

  3. Femtosecond beam science

    NASA Astrophysics Data System (ADS)

    Uesaka, Mitsuru

    1. Introduction -- 2. Femtosecond beam generation. 2.1. Theory and operation of femtosecond terawatt lasers. 2.2. Linear accelerator. 2.3. Synchrotron. 2.4. Laser plasma acceleration. 2.5. Inverse compton scattering x-ray generation. 2.6. Beam slicing by femtosecond laser. 2.7. Free electron lasers. 2.8. Energy recovery linac -- 3. Diagnosis and synchronization. 3.1. Pulse shape diagnostics. 3.2. Synchronization -- 4. Applications. 4.1. Radiation chemistry. 4.2. Time-resolved x-ray diffraction. 4.3. Protein dynamics. 4.4. Molecular dynamics simulation.

  4. Ultrafast imaging the light-speed propagation of a focused femtosecond laser pulse in air and its ionized electron dynamics and plasma-induced pulse reshaping

    NASA Astrophysics Data System (ADS)

    Yu, Yanwu; Jiang, Lan; Cao, Qiang; Shi, Xueshong; Wang, Qingsong; Wang, Guoyan; Lu, Yongfeng

    2016-03-01

    The light-speed propagation of a focused femtosecond (fs) laser pulse in air was recorded by a pump-probe shadowgraph imaging technique with femtosecond time resolution. The ultrafast dynamics of the laser-ionized electrons were studied, which revealed a strong reshaping of the laser field due to laser-air nonlinear interaction. The influence of laser fluence and focusing conditions on the pulse reshaping was studied, and it was found that: (1) double foci are formed due to the refocusing effect when the laser fluence is higher than 500 J/cm2 and the focusing numeric aperture (NA) is higher than 0.30; and (2) a higher NA focusing lens can better inhibit the prefocusing effect and nonlinear distortion in the Gaussian beam waist.

  5. Calculations of nonlinear wave-packet interferometry signals in the pump-probe limit as tests for vibrational control over electronic excitation transfer

    NASA Astrophysics Data System (ADS)

    Biggs, Jason D.; Cina, Jeffrey A.

    2009-12-01

    The preceding paper [J. D. Biggs and J. A. Cina, J. Chem. Phys. 131, 224101 (2009)] (referred to here as Paper 1), describes a strategy for externally influencing the course of short-time electronic excitation transfer (EET) in molecular dimers and observing the process by nonlinear wave-packet interferometry (nl-WPI). External influence can, for example, be exerted by inducing coherent intramolecular vibration in one of the chromophores prior to short-pulse electronic excitation of the other. Within a sample of isotropically oriented dimers having a specified internal geometry, a vibrational mode internal to the acceptor chromophore can be preferentially driven by electronically nonresonant impulsive stimulated Raman (or resonant infrared) excitation with a short polarized "control" pulse. A subsequent electronically resonant polarized pump then preferentially excites the donor, and EET ensues. Paper 1 investigates control-pulse-influenced nl-WPI as a tool for the spectroscopic evaluation of the effect of coherent molecular vibration on excitation transfer, presenting general expressions for the nl-WPI difference signal from a dimer following the action of a control pulse of arbitrary polarization and shape. Electronic excitation is to be effected and its interchromophore transfer monitored by resonant pump and probe "pulses," respectively, each consisting of an optical-phase-controlled ultrashort pulse-pair having arbitrary polarization, duration, center frequency, and other characteristics. Here we test both the control strategy and its spectroscopic investigation—with some sacrifice of amplitude-level detail—by calculating the pump-probe difference signal. That signal is the limiting case of the control-influenced nl-WPI signal in which the two pulses in the pump pulse-pair coincide, as do the two pulses in the probe pulse-pair. We present calculated pump-probe difference signals for (1) a model excitation-transfer complex in which two equal-energy monomers

  6. Complete photoionization experiments via ultrafast coherent control with polarization multiplexing.

    PubMed

    Hockett, P; Wollenhaupt, M; Lux, C; Baumert, T

    2014-06-01

    Photoelectron angular distributions (PADs) obtained from ionization of potassium atoms using moderately intense femtosecond IR fields (∼10^{12}  W cm^{-2}) of various polarization states are shown to provide a route to "complete" photoionization experiments. Ionization occurs by a net three-photon absorption process, driven via the 4s→4p resonance at the one-photon level. A theoretical treatment incorporating the intrapulse electronic dynamics allows for a full set of ionization matrix elements to be extracted from 2D imaging data. 3D PADs generated from the extracted matrix elements are also compared to experimental, tomographically reconstructed, 3D photoelectron distributions, providing a sensitive test of their validity. Finally, application of the determined matrix elements to ionization via more complex, polarization-shaped, pulses is demonstrated, illustrating the utility of this methodology towards detailed understanding of complex ionization control schemes and suggesting the utility of such "multiplexed" intrapulse processes as powerful tools for measurement. PMID:24949763

  7. 2001 Gordon Research Conference on Photoions, Photoionization and Photodetachment. Final progress report [agenda and attendees list

    SciTech Connect

    Johnson, Mark

    2001-07-13

    The Gordon Research Conference on Photoions, Photoionization and Photodetachment was held at Williams College, Williamstown, Massachusetts, July 8-13, 2001. The 72 conference attendees represented the spectrum of endeavor in this field, coming from academia, industry, and government laboratories, and including US and foreign scientists, senior researchers, young investigators, and students. Emphasis was placed on current unpublished research and discussion of the future target areas in this field. There was a conscious effort to stimulate discussion about the key issues in the field today. Time for formal presentations was limited. Sessions included the following topics: Vibrational structure, Time resolved studies: nuclear wavepackets, Valence photoionization, Clusters and networks, Resonance structures and decay mechanisms, Ultrafast photoionization, Threshold photoionization, Molecule fixed properties, and Collisional phenomena.

  8. Development of a pump-probe facility combining a far-infrared source with laser-like characteristics and a VUV free electron laser

    NASA Astrophysics Data System (ADS)

    Faatz, B.; Fateev, A. A.; Feldhaus, J.; Krzywinski, J.; Pflueger, J.; Rossbach, J.; Saldin, E. L.; Schneidmiller, E. A.; Yurkov, M. V.

    2001-12-01

    The TESLA Test Facility (TTF) at DESY is a facility producing sub-picosecond electron pulses for the generation of VUV or soft X-ray radiation in a free electron laser (FEL). The same electron pulses would also allow the direct production of high-power coherent radiation by passing the electron beam through an undulator. Intense, coherent far-infrared (FIR) undulator radiation can be produced from electron bunches at wavelengths longer than or equal to the bunch length. The source described in this paper provides, in the wavelength range 50- 300 μm, a train of about 1- 10 ps long radiation pulses, with about 1 mJ of optical energy per pulse radiated into the central cone. The average output power can exceed 50 W. In this conceptual design, we intend to use a conventional electromagnetic undulator with a 60 cm period length and a maximum field of 1.5 T. The FIR source will use the spent electron beam coming from the VUV FEL which allows one to significantly extend the scientific potential of the TTF without interfering with the main option of the TTF FEL operation. The pulses of the coherent FIR radiation are naturally synchronized with the VUV pulses from the main TTF FEL, enabling pump-probe techniques using either the FEL pulse as a pump or the FIR pulse as a probe, or vice versa.

  9. Optical pump-probe processes in Nd3+-doped KPb2Br5, RbPb2Br5, and KPb2Cl5

    NASA Astrophysics Data System (ADS)

    Rademaker, Katja; Payne, Stephen A.; Huber, Günter; Isaenko, Ludmila I.; Osiac, Eugen

    2005-12-01

    Recently, laser activity has been achieved in the low-phonon-energy, moisture-resistant bromide host crystals: neodymium-doped potassium lead bromide (Nd3+:KPb2Br5) and rubidium lead bromide (Nd3+:RbPb2Br5). Laser activity at 1.07 μm was observed for both crystalline materials. Laser operation at the new wavelengths of 1.18 and 0.97 μm resulting from the 4F5/2+2H9/2-->4IJ transitions (J=13/2 and 11/2) in Nd:RbPb2Br5 was achieved for the first time in a solid-state laser material. We present cw pump-probe spectra and discuss excited-state absorption and reabsorption processes due to the long-lived lower laser levels, as well as possible depopulation mechanisms feasible for more efficient laser operation in these crystals. The bromides are compared with potassium lead chloride (Nd3+:KPb2Cl5).

  10. Ultrafast pump-probe spectroscopy studies of CeO2 thin film deposited on Ni-W substrate by RF magnetron sputtering

    NASA Astrophysics Data System (ADS)

    Singh, Preetam; Srivatsa, K. M. K.; Jewariya, Mukesh

    2016-08-01

    This study presents the first investigation of rapid dynamical processes that occur in pure CeO2 thin film, using ultra fast pump-probe spectroscopy at room temperature. For this purpose we have used a single (200) oriented CeO2 film deposited on biaxially textured Ni-W substrate by RF magnetron sputtering technique. The ultrafast transient spectra show initial sharp rise transition followed by an exponential photon decay. This rise time is about 10 ps irrespective of the probe wavelengths range 500-800 nm. The initial decay constant (τ) at 500 nm probe wavelength is found to be 171 ps, while at 800 nm probe wavelength it is 107.5 ps. The ultrafast absorption spectra show two absorption peaks at 745 and 800 nm, and are attributed to the electronic transitions from 2F7/2-2F5/2 and 1S0-1F3 respectively. The relatively high intensity absorption peak at 745 nm indicates dominant f-f electronic transition. Further, the absorption peak at 745 nm splits into two distinct peaks with respect to delay time, and is attributed to the charge transfer in between Ce4+ and Ce3+ ions. These results indicate that CeO2 itself is a potential candidate and can be used for optical applications.

  11. Construction of a magnetic bottle spectrometer and its application to pulse duration measurement of X-ray laser using a pump-probe method

    NASA Astrophysics Data System (ADS)

    Namba, S.; Hasegawa, N.; Kishimoto, M.; Nishikino, M.; Ishino, M.; Kawachi, T.

    2015-11-01

    To characterize the temporal evolution of ultrashort X-ray pulses emitted by laser plasmas using a pump-probe method, a magnetic bottle time-of-flight electron spectrometer is constructed. The design is determined by numerical calculations of a mirror magnetic field and of the electron trajectory in a flight tube. The performance of the spectrometer is characterized by measuring the electron spectra of xenon atoms irradiated with a laser-driven plasma X-ray pulse. In addition, two-color above-threshold ionization (ATI) experiment is conducted for measurement of the X-ray laser pulse duration, in which xenon atoms are simultaneously irradiated with an X-ray laser pump and an IR laser probe. The correlation in the intensity of the sideband spectra of the 4d inner-shell photoelectrons and in the time delay of the two laser pulses yields an X-ray pulse width of 5.7 ps, in good agreement with the value obtained using an X-ray streak camera.

  12. Construction of a magnetic bottle spectrometer and its application to pulse duration measurement of X-ray laser using a pump-probe method

    SciTech Connect

    Namba, S.; Hasegawa, N.; Kishimoto, M.; Nishikino, M.; Ishino, M.; Kawachi, T.

    2015-11-15

    To characterize the temporal evolution of ultrashort X-ray pulses emitted by laser plasmas using a pump-probe method, a magnetic bottle time-of-flight electron spectrometer is constructed. The design is determined by numerical calculations of a mirror magnetic field and of the electron trajectory in a flight tube. The performance of the spectrometer is characterized by measuring the electron spectra of xenon atoms irradiated with a laser-driven plasma X-ray pulse. In addition, two-color above-threshold ionization (ATI) experiment is conducted for measurement of the X-ray laser pulse duration, in which xenon atoms are simultaneously irradiated with an X-ray laser pump and an IR laser probe. The correlation in the intensity of the sideband spectra of the 4d inner-shell photoelectrons and in the time delay of the two laser pulses yields an X-ray pulse width of 5.7 ps, in good agreement with the value obtained using an X-ray streak camera.

  13. A 1 kHz A-scan rate pump-probe laser-ultrasound system for robust inspection of composites.

    PubMed

    Pelivanov, Ivan; Shtokolov, Alex; Wei, Chen-Wei; O'Donnell, Matthew

    2015-09-01

    We recently built a fiber-optic laser-ultrasound (LU) scanner for nondestructive evaluation (NDE) of aircraft composites and demonstrated its greatly improved sensitivity and stability compared with current noncontact systems. It is also very attractive in terms of cost, stability to environmental noise and surface roughness, simplicity in adjustment, footprint, and flexibility. A new type of a balanced fiber-optic Sagnac interferometer is a key component of this all-optical LU pump-probe system. Very high A-scan rates can be achieved because no reference arm or stabilization feedback are needed. Here, we demonstrate LU system performance at 1000 A-scans/s combined with a fast 2-D translator operating at a scanning speed of 100 mm/s with a peak acceleration of 10 m/s(2) in both lateral directions to produce parallel B-scans at high rates. The fast scanning strategy is described in detail. The sensitivity of this system, in terms of noise equivalent pressure, was further improved to be only 8.3 dB above the Nyquist thermal noise limit. To our knowledge, this is the best reported sensitivity for a noncontact ultrasonic detector of this dimension used to inspect aircraft composites. PMID:26415130

  14. Discrimination of the effects of saturation and optical pumping in velocity-dependent pump-probe spectroscopy of rubidium: A simple analytical study

    SciTech Connect

    Noh, Heung-Ryoul; Moon, Geol; Jhe, Wonho

    2010-12-15

    This paper presents a simple analytical theory for the velocity-dependent pump-probe laser spectroscopy of {sup 87}Rb and {sup 85}Rb atoms where the pump and the probe beams are circularly or linearly polarized. The analytical solutions of the line shapes of the velocity-selective optical pumping spectroscopy [G. Moon and H. R. Noh, Phys. Rev. A 78, 032506 (2008)] and saturated absorption spectroscopy [G. Moon and H. R. Noh, J. Opt. Soc. Am. B 25, 701 (2008); 27, 1741 (2010)] obtained in the previous reports, expressed as a sum of several Lorentzian functions, could be approximated as one (or in some cases, two) Lorentzian function(s). In particular, the contributions of the saturation and optical pumping effects could be discriminated explicitly in these simple analytical solutions, which is not possible in existing theories such as Nakayama's model. The simple analytical results for the saturation spectroscopy were compared with experimental results, and good agreement between them was observed.

  15. Picosecond Time-Resolved Ir-Uv Pump-Probe Spectroscopic Study on Vibrational Energy Relaxation of Benzene Dimer and Trimer in the CH Stretching Region

    NASA Astrophysics Data System (ADS)

    Kusaka, Ryoji; Inokuchi, Yoshiya; Ebata, Takayuki

    2012-06-01

    Vibrational energy relaxation (VER) in the CH stretching region of benzene dimer (Bz_2) and trimer (Bz_3) has been studied by IR-UV pump-probe spectroscopy in supersonic beams. Firstly, we investigated isotope-substituted hd heterodimer, where h=C_6H_6 and d=_6D_6, because the Stem and Top sites in the hd dimer can be site-selectively excited, different from hh homodimer. The two h(stem)d(top) and h(top)d(stem) isomers show remarkable difference in the lifetimes of intracluster vibrational energy redistribution (IVR). In the transient UV spectra, we observed a broad electronic transition due to the bath modes. The time evolutions of the bath modes can be described by a three step VER model involving IVR and vibrational predissociation (VP). This model was also confirmed by the observed rise profile of the Bz fragment. Secondly, we investigated hh homodimer. The hh homodimer shows the stepwise VER process with time constants similar to those of the hd dimer, suggesting a very weak excitation-exchange coupling of the vibrations between the two sites of the hh dimer. Finally, we found that Bz_3 also exhibits the stepwise VER process, though each step is faster than Bz_2.

  16. Optical pump-probe processes in Nd 3+ doped KPb2Br5, RbPb2Br5, and KPb2CI5

    SciTech Connect

    Rademaker, K; Huber, G; Payne, S A; Osiac, E; Isaenko, L I

    2004-10-28

    Recently, laser activity has been achieved in the low phonon energy, moisture-resistant bromide host crystals, neodymium-doped potassium lead bromide (Nd{sup 3+}:KPb{sub 2}Br{sub 5}) and rubidium lead bromide (Nd{sup 3+}:RbPb{sub 2}Br{sub 5}). Laser activity at 1.07 {micro}m was observed for both crystalline materials. Laser operation at the new wavelengths 1.18 {micro}m and 0.97 {micro}m resulting from the {sup 4}F{sub 5/2}+{sup 2}H{sub 9/2} {yields} {sup 4}I{sub J} transitions (J=13/2 and 11/2) in Nd:RPB was achieved for the first time in a solid state laser material. In this paper we present cw pump-probe spectra in order to discuss excited state absorption, reabsorption processes due to the long lived lower laser levels as well as possible depopulation mechanisms feasible for more efficient laser operation in these crystals. The bromides will be compared with potassium lead chloride (Nd{sup 3+}:KPb{sub 2}Cl{sub 5}).

  17. Ultrafast dynamics of a near-solid-density layer in an intense femtosecond laser-excited plasma

    SciTech Connect

    Adak, Amitava; Chatterjee, Gourab; Kumar Singh, Prashant; Lad, Amit D.; Brijesh, P.; Kumar, G. Ravindra; Blackman, David R.; Robinson, A. P. L.; Pasley, John

    2014-06-15

    We report on the picosecond dynamics of a near-solid-density plasma generated by an intense, infrared (λ = 800 nm) femtosecond laser using time-resolved pump-probe Doppler spectrometry. An initial red-shift is observed in the reflected third harmonic (λ = 266 nm) probe pulse, which gets blue-shifted at longer probe-delays. A combination of particle-in-cell and radiation-hydrodynamics modelling is performed to model the pump laser interaction with the solid target. The results are post-processed to predict the Doppler shift. An excellent agreement is found between the results of such modelling and the experiment. The modelling suggests that the initial inward motion of the critical surface observed in the experiment is due to the passage of a shock-wave-like disturbance, launched by the pump interaction, propagating into the target. Furthermore, in order to achieve the best possible fit to the experimental data, it was necessary to incorporate the effects of bulk ion-acceleration resulting from the electrostatic field set up by the expulsion of electrons from the laser envelope. We also present results of time-resolved pump-probe reflectometry, which are corroborated with the spectrometry results using a 1-D reflectivity model.

  18. Photoionization cross section for He in the hyperspherical coordinate method

    SciTech Connect

    Miller, D.L.; Starace, A.F.

    1980-01-01

    In order to more fully explore the role of electron correlations in the photoionization process the hyperspherical coordinate method of Macek was employed in calculating photoionization cross sections of He. Results are presented and discussed. (WHK)

  19. Vacuum Ultraviolet Photoionization of Complex Chemical Systems

    NASA Astrophysics Data System (ADS)

    Kostko, Oleg; Bandyopadhyay, Biswajit; Ahmed, Musahid

    2016-05-01

    Tunable vacuum ultraviolet (VUV) radiation coupled to mass spectrometry is applied to the study of complex chemical systems. The identification of novel reactive intermediates and radicals is revealed in flame, pulsed photolysis, and pyrolysis reactors, leading to the elucidation of spectroscopy, reaction mechanisms, and kinetics. Mass-resolved threshold photoelectron photoion coincidence measurements provide unprecedented access to vibrationally resolved spectra of free radicals present in high-temperature reactors. Photoionization measurements in water clusters, nucleic acid base dimers, and their complexes with water provide signatures of proton transfer in hydrogen-bonded and π-stacked systems. Experimental and theoretical methods to track ion-molecule reactions and fragmentation pathways in intermolecular and intramolecular hydrogen-bonded systems in sugars and alcohols are described. Photoionization of laser-ablated molecules, clusters, and their reaction products inform thermodynamics and spectroscopy that are relevant to astrochemistry and catalysis. New directions in coupling VUV radiation to interrogate complex chemical systems are discussed.

  20. Vacuum Ultraviolet Photoionization of Complex Chemical Systems.

    PubMed

    Kostko, Oleg; Bandyopadhyay, Biswajit; Ahmed, Musahid

    2016-05-27

    Tunable vacuum ultraviolet (VUV) radiation coupled to mass spectrometry is applied to the study of complex chemical systems. The identification of novel reactive intermediates and radicals is revealed in flame, pulsed photolysis, and pyrolysis reactors, leading to the elucidation of spectroscopy, reaction mechanisms, and kinetics. Mass-resolved threshold photoelectron photoion coincidence measurements provide unprecedented access to vibrationally resolved spectra of free radicals present in high-temperature reactors. Photoionization measurements in water clusters, nucleic acid base dimers, and their complexes with water provide signatures of proton transfer in hydrogen-bonded and π-stacked systems. Experimental and theoretical methods to track ion-molecule reactions and fragmentation pathways in intermolecular and intramolecular hydrogen-bonded systems in sugars and alcohols are described. Photoionization of laser-ablated molecules, clusters, and their reaction products inform thermodynamics and spectroscopy that are relevant to astrochemistry and catalysis. New directions in coupling VUV radiation to interrogate complex chemical systems are discussed. PMID:26980311

  1. Time resolved digital-holographic analysis of femtosecond laser-induced photodisruption

    NASA Astrophysics Data System (ADS)

    Saerchen, Emanuel; Wenzel, Johannes; Antonopoulos, Georgios; Krueger, Alexander; Lubatschowski, Holger; Ripken, Tammo

    2016-03-01

    Femtosecond laser oscillator systems with low pulse energy (< 1 μJ) and high repetition rate (MHz) are increasingly used for precise, fast and safe eye surgery. Therefore, the laser tissue interaction process is of great interest to optimize and improve established and future surgical protocols. Besides, using faster laser systems leads to unintended self-induced interaction effects, where a femtosecond laser pulse modifies the vicinity in the material in such a way that the focus of following laser pulses is changed. We used a femtosecond oscillator laser system with high repetition rate and 66 nJ pulse energy to produce photodisruption in water. Water was used as phantom material for ocular tissue, because tissue mainly consists of water. A custom made digital-holographic system was used to measure the temporal material modification from picoseconds until seconds after occurrence of the photodisruption. For illumination of the sample we used either a continuously light source or the femtosecond laser pulse itself in a pump-probe configuration. The holographic system provides quantitative data of phase difference Δφ for the full field of view of several tenth of micrometers. Phase difference is equivalent to the laser induced change in the material's refractive index which can alter focusing conditions of following laser pulses and might impair surgical outcome. We obtained the largest change in Δφ during the first picoseconds, followed by a slow relaxation of Δφ within some milliseconds. The results of time resolved measurements of the laser induced material modification will help to optimize scanning schemes in ocular surgery.

  2. On the Resolution Limit of Femtosecond Stimulated Raman Spectroscopy: Modelling Fifth-Order Signals with Overlapping Pulses.

    PubMed

    Fumero, Giuseppe; Batignani, Giovanni; Dorfman, Konstantin E; Mukamel, Shaul; Scopigno, Tullio

    2015-11-16

    Femtosecond stimulated Raman scattering (FSRS) spectroscopy is a powerful pump-probe technique that can track electronic and vibrational dynamics with high spectral and temporal resolution. The investigation of extremely short-lived species, however, implies deciphering complex signals and is ultimately hampered by unwanted nonlinear effects once the time resolution limit is approached and the pulses overlap temporally. Using the loop diagrams formalism we calculate the fifth-order response of a model system and address the limiting case where the relevant dynamics timescale is comparable to the pump-pulse duration and, consequently, the pump and the probe overlap temporally. We find that in this regime, additional diagrams that do not contribute for temporally well separated pulses need to be taken into account, giving rise to new time-dependent features, even in the absence of photoinduced dynamics and for negative delays. PMID:26387662

  3. High power multi-color OPCPA source with simultaneous femtosecond deep-UV to mid-IR outputs.

    PubMed

    Baudisch, M; Wolter, B; Pullen, M; Hemmer, M; Biegert, J

    2016-08-01

    Many experimental investigations demand synchronized pulses at various wavelengths, ideally with very short pulse duration and high repetition rate. Here we describe a femtosecond multi-color optical parametric chirped pulse amplifier (OPCPA) with simultaneous outputs from the deep-UV to the mid-IR with optical synchronization. The high repetition rate of 160 kHz is well suited to compensate for low interaction probability or low cross section in strong-field interactions. Our source features high peak powers in the tens to hundreds of MW regime with pulse durations below 110 fs, which is ideal for pump-probe experiments of nonlinear and strong-field physics. We demonstrate its utility by strong-field ionization experiments of xenon in the near- to mid-IR. PMID:27472624

  4. Femtosecond time-resolved ionization spectroscopy of Na 3(B) and the question of the geometric phase

    NASA Astrophysics Data System (ADS)

    Schön, J.; Köppel, H.

    1994-12-01

    The femtosecond time-resolved ionization spectrum of the B-state of Na 3 has been studied theoretically, taking two nuclear degrees of freedom into account (bending mode and pseudorotation). Special emphasis is put on a comparison between different approaches to the pseudorotational dynamics of Na 3(B) proposed earlier in the literature: a Jahn-Teller treatment invoked in the original work versus a pseudo-Jahn-Teller treatment advanced in later studies. The time-dependent wave-packet dynamics is found to differ drastically in the two cases although it proceeds on (virtually) the same potential energy surface. This is interpreted as a consequence of the geometric phase which is nontrivial only in the Jahn-Teller case. A low-energy peak in the Fourier transform of the pump-probe spectrum of Baumert et al. (Chem. Phys. Letters 209 (1993) 29) is tentatively interpreted as evidence in favour of the pseudo-Jahn-Teller mechanism.

  5. New transient absorption observed in the spectrum of colloidal CdSe nanoparticles pumped with high-power femtosecond pulses

    SciTech Connect

    Burda, C.; Link, S.; Green, T.C.; El-Sayed, M.A.

    1999-12-09

    The power dependence of the transient absorption spectrum of CdSe nanoparticle colloids with size distribution of 4.0 {+-} 0.4 nm diameter is studied with femtosecond pump-probe techniques. At the lowest pump laser power, the absorption bleaching (negative spectrum) characteristic of the exciton spectrum is observed with maxima at 560 and 480 nm. As the pump laser power increases, two new transient absorptions at 510 and 590 nm with unresolved fast rise (<100 fs) and long decay times ({much{underscore}gt}150 ps) are observed. The energy of each of the positive absorption is red shifted from that of the bleach bands by {approximately}120 MeV. The origin of this shift is discussed in terms of the effect of the internal electric field of the many electron-hole pairs formed within the quantum dot at the high pump intensity, absorption from a metastable excited state or the formation of biexcitons.

  6. Ionic Liquid Dynamics Measured with 2D IR and IR Pump-Probe Experiments on a Linear Anion and the Influence of Potassium Cations.

    PubMed

    Tamimi, Amr; Fayer, Michael D

    2016-07-01

    The room-temperature ionic liquid EmimNTf2 (1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide) was studied with two-dimensional infrared (2D IR) spectroscopy and polarization selective pump-probe (PSPP) experiments using low-concentration selenocyanate (SeCN(-)) as the vibrational probe. SeCN(-) was added as EmimSeCN, which keeps the cation the same. KSeCN was also used, so K(+) was added. Two 2D IR polarization configurations were employed: ⟨XXXX⟩ (all pulses have the same polarization) and ⟨XXYY⟩ (the first two pulse polarizations are perpendicular to that of the third pulse and the echo). The spectral diffusion differs for the two configurations, demonstrating that reorientation-induced spectral diffusion, in addition to structural spectral diffusion (SSD), plays a role in the observed dynamics. The SSD was extracted from the 2D IR time-dependent data. The samples with EmimSeCN have dynamics on several fast time scales; however, when KSeCN is used, both the PPSP anisotropy decay and the 2D IR decays have low amplitude offsets (nondecaying values at long times). The size of the offsets increased with increased K(+) concentration. These results are explained in terms of a two-ensemble model. A small fraction of the SeCN(-) is located in the regions modified by the presence of K(+), causing a substantial slowing of the SeCN(-) orientational relaxation and spectral diffusion. Having a small ensemble of SeCN(-) that undergoes very slow dynamics is sufficient to explain the offsets. For the major ensemble, the dynamics with and without K(+) are the same. PMID:26872207

  7. Mixed Quantum-Classical Simulations of Transient Absorption Pump-Probe Signals for a Photo-Induced Electron Transfer Reaction Coupled to an Inner-Sphere Vibrational Mode.

    PubMed

    Martinez, Franz; Hanna, Gabriel

    2016-05-19

    In a previous study (Martinez, F.; Hanna, G. Chem. Phys. Lett. 2013, 573, 77-83), we demonstrated the ability of two approximate solutions of the quantum-classical Liouville equation (QCLE) for qualitatively capturing the electronic dynamics in the pump-probe transient absorption (TA) signal of a model of a condensed phase photoinduced electron transfer reaction whose ground and excited donor states have the same equilibrium geometry. However, the question remained as to the ability of these solutions to treat the more complex situation in which the electronic states are coupled to a low-frequency inner-sphere harmonic vibrational mode (representing an intramolecular mode of the donor-acceptor complex) that shifts their equilibrium geometries with respect to each other and thereby gives rise to signatures of vibrational dynamics in the TA signal. Thus, in this study, we investigated this situation by treating the vibrational mode both quantum mechanically and classically within the context of the approximate Poisson bracket mapping equation (PBME) and forward-backward trajectory solutions (FBTS) of the QCLE. Depending on the definition of the quantum subsystem, both PBME and FBTS are capable of qualitatively capturing several of the main features in the exact TA signal and quantitatively capturing the characteristic time scale of the vibrational dynamics, despite the moderately strong subsystem-bath coupling in this model. Particularly, we found that treating the vibrational mode quantum mechanically using either PBME or FBTS better captures the signatures of the vibrational dynamics, while treating it classically using FBTS better captures the decay in the signal. These findings underscore the utility of the PBME and FBTS approaches for efficiently modeling and interpreting TA signals. PMID:26766568

  8. Microscopic insight into the pump-probe relaxation dynamics of superconductors: Model study of MgB2relaxation within nonlinear response theory

    NASA Astrophysics Data System (ADS)

    Baňacký, Pavol; Szöcs, Vojtech

    2016-05-01

    Here we present a quantum-statistical formulation of third-order polarization P(3)(t), which is induced in a sample by a sequence of incident external fields, and serves as a source of an emitted radiation field detected as a signal in pump-probe (PP) experiments. Our treatment is based on the perturbation expansion of the non-equilibrium density matrix for calculation of multi-time correlation functions, and the corresponding response function, at finite temperature. As a model for our study, the high-temperature superconductor MgB2 has been selected. Knowledge of the electronic structure of the studied system, and of the corresponding Eliashberg function that represents pertinent electron-phonon (EP) interactions, enabled us to distinguish non-equilibrium processes running over different time-periods in a sequence of interactions with laser pulses on a microscopic level. We have also derived temperature-dependent relaxation dynamics as a function of delay time between the pump and probe pulses. For the studied model system of MgB2, we have shown that an abrupt increase of the relaxation time at Tc, as detected by experiments, is the direct consequence of sudden changes in the character of EP coupling in transition from an adiabatic to a stabilized superconducting anti-adiabatic state, as it predicts the anti-adiabatic theory of electron-vibration interactions. The BCS model, which preserves the adiabatic character of EP coupling also below the critical temperature of MgB2, is basically unable to reflect the enormous sudden increase of the relaxation time. Based on diagrammatic perturbation theory, differences in the optical pump-optical probe and the optical pump-terahertz probe settings of MgB2 PP relaxation dynamics are discussed.

  9. Correlation between photoeletron and photoion in ultrafast multichannel photoionization of Ar

    SciTech Connect

    Itakura, R.; Fushitani, M.; Hishikawa, A.; Sako, T.

    2015-12-31

    We theoretically investigate coherent dynamics of ions created through ultrafast multichannel photoionization from a viewpoint of photoelectron-photoion correlation. The model calculation on single-photon ionization of Ar reveals that the coherent hole dynamics in Ar{sup +} associated with a superposition of the spin-orbit states {sup 2}PJ (J = 3/2 and 1/2) can be identified by monitoring only the photoion created by a Fourier-transform limited extreme ultraviolet (EUV) pulse with the fs pulse duration, while the coherence is lost by a chirped EUV pulse. It is demonstrated that by coincidence detection of the photoelectron and photoion the coherent hole dynamics can be extracted even in the case of ionization by a chirped EUV pulse with the sufficiently wide bandwidth.

  10. Photoassociation and coherent transient dynamics in the interaction of ultracold rubidium atoms with shaped femtosecond pulses. I. Experiment

    SciTech Connect

    Mullins, Terry; Salzmann, Wenzel; Goetz, Simone; Albert, Magnus; Eng, Judith; Wester, Roland; Weidemueller, Matthias; Weise, Fabian; Merli, Andrea; Weber, Stefan M.; Sauer, Franziska; Woeste, Ludger; Lindinger, Albrecht

    2009-12-15

    We experimentally investigate various processes present in the photoassociative interaction of an ultracold atomic sample with shaped femtosecond laser pulses as an detailed extension of previous work [W. Salzmann et al., Phys. Rev. Lett. 100, 233003 (2008)]. We demonstrate the photoassociation of pairs of rubidium atoms into electronically excited, bound molecular states using spectrally cut femtosecond laser pulses tuned below the rubidium D{sub 1} or D{sub 2} asymptote. Time-resolved pump-probe spectra reveal oscillations of the molecular formation rate, which are due to coherent transient dynamics in the electronic excitation. The oscillation frequency corresponds to the detuning of the spectral cut position to the asymptotic transition frequency of the rubidium D{sub 1} or D{sub 2} lines, respectively. Measurements of the molecular photoassociation signal as a function of the pulse energy reveal a nonlinear dependence and indicate a nonperturbative excitation process. Chirping the association laser pulse allowed us to change the phase of the coherent transients. Furthermore, a signature for molecules in the electronic ground state is found, which is attributed to molecule formation by femtosecond photoassociation followed by spontaneous decay. In a subsequent article [A. Merli et al., Phys. Rev. A 80, 063417 (2009)] quantum mechanical calculations are presented, which compare well with the experimental data and reveal further details about the observed coherent transient dynamics.

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

    PubMed

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

    2012-02-23

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

  12. Goniometer-based femtosecond X-ray diffraction of mutant 30S ribosomal subunit crystals

    SciTech Connect

    Dao, E. Han; Sierra, Raymond G.; Laksmono, Hartawan; Lemke, Henrik T.; Alonso-Mori, Roberto; Coey, Aaron; Larsen, Kevin; Baxter, Elizabeth L.; Cohen, Aina E.; Soltis, S. Michael; DeMirci, Hasan

    2015-04-30

    In this work, we collected radiation-damage-free data from a set of cryo-cooled crystals for a novel 30S ribosomal subunit mutant using goniometer-based femtosecond crystallography. Crystal quality assessment for these samples was conducted at the X-ray Pump Probe end-station of the Linac Coherent Light Source (LCLS) using recently introduced goniometer-based instrumentation. These 30S subunit crystals were genetically engineered to omit a 26-residue protein, Thx, which is present in the wild-type Thermus thermophilus 30S ribosomal subunit. We are primarily interested in elucidating the contribution of this ribosomal protein to the overall 30S subunit structure. To assess the viability of this study, femtosecond X-ray diffraction patterns from these crystals were recorded at the LCLS during a protein crystal screening beam time. During our data collection, we successfully observed diffraction from these difficult-to-grow 30S ribosomal subunit crystals. Most of our crystals were found to diffract to low resolution, while one crystal diffracted to 3.2 Å resolution. These data suggest the feasibility of pursuing high-resolution data collection as well as the need to improve sample preparation and handling in order to collect a complete radiation-damage-free data set using an X-ray Free Electron Laser.

  13. Serial Femtosecond Crystallography and Ultrafast Absorption Spectroscopy of the Photoswitchable Fluorescent Protein IrisFP.

    PubMed

    Colletier, Jacques-Philippe; Sliwa, Michel; Gallat, François-Xavier; Sugahara, Michihiro; Guillon, Virginia; Schirò, Giorgio; Coquelle, Nicolas; Woodhouse, Joyce; Roux, Laure; Gotthard, Guillaume; Royant, Antoine; Uriarte, Lucas Martinez; Ruckebusch, Cyril; Joti, Yasumasa; Byrdin, Martin; Mizohata, Eiichi; Nango, Eriko; Tanaka, Tomoyuki; Tono, Kensuke; Yabashi, Makina; Adam, Virgile; Cammarata, Marco; Schlichting, Ilme; Bourgeois, Dominique; Weik, Martin

    2016-03-01

    Reversibly photoswitchable fluorescent proteins find growing applications in cell biology, yet mechanistic details, in particular on the ultrafast photochemical time scale, remain unknown. We employed time-resolved pump-probe absorption spectroscopy on the reversibly photoswitchable fluorescent protein IrisFP in solution to study photoswitching from the nonfluorescent (off) to the fluorescent (on) state. Evidence is provided for the existence of several intermediate states on the pico- and microsecond time scales that are attributed to chromophore isomerization and proton transfer, respectively. Kinetic modeling favors a sequential mechanism with the existence of two excited state intermediates with lifetimes of 2 and 15 ps, the second of which controls the photoswitching quantum yield. In order to support that IrisFP is suited for time-resolved experiments aiming at a structural characterization of these ps intermediates, we used serial femtosecond crystallography at an X-ray free electron laser and solved the structure of IrisFP in its on state. Sample consumption was minimized by embedding crystals in mineral grease, in which they remain photoswitchable. Our spectroscopic and structural results pave the way for time-resolved serial femtosecond crystallography aiming at characterizing the structure of ultrafast intermediates in reversibly photoswitchable fluorescent proteins. PMID:26866390

  14. A versatile femtosecond stimulated Raman spectroscopy setup with tunable pulses in the visible to near infrared

    SciTech Connect

    Zhu, Liangdong; Liu, Weimin; Fang, Chong

    2014-07-28

    We demonstrate a versatile and efficient setup to perform femtosecond stimulated Raman spectroscopy (FSRS). Technical innovations are implemented to achieve the wavelength tunability for both the picosecond narrowband Raman pump pulse and femtosecond broadband Raman probe pulse. Using a simplified one-grating scheme in a home-built second harmonic bandwidth compressor followed by a two-stage noncollinear optical parametric amplifier, we tune the Raman pump pulse from ca. 480 to 750 nm. To generate the suitable Raman probe pulse in tandem, we rely on our recently demonstrated broadband up-converted multicolor array technique that readily provides tunable broadband laser sidebands across the visible to near-infrared range. This unique setup has unparalleled flexibility for conducting FSRS. We measure the ground-state Raman spectra of a cyclohexane standard using tunable pump-probe pairs at various wavelengths across the visible region. The best spectral resolution is ∼12 cm{sup −1}. By tuning the pump wavelength closer to the electronic absorption band of a photoacid pyranine in water, we observe the pre-resonantly enhanced Raman signal. The stimulated Raman gain of the 1627 cm{sup −1} mode is increased by over 15 times.

  15. Goniometer-based femtosecond X-ray diffraction of mutant 30S ribosomal subunit crystals.

    PubMed

    Dao, E Han; Sierra, Raymond G; Laksmono, Hartawan; Lemke, Henrik T; Alonso-Mori, Roberto; Coey, Aaron; Larsen, Kevin; Baxter, Elizabeth L; Cohen, Aina E; Soltis, S Michael; DeMirci, Hasan

    2015-07-01

    In this work, we collected radiation-damage-free data from a set of cryo-cooled crystals for a novel 30S ribosomal subunit mutant using goniometer-based femtosecond crystallography. Crystal quality assessment for these samples was conducted at the X-ray Pump Probe end-station of the Linac Coherent Light Source (LCLS) using recently introduced goniometer-based instrumentation. These 30S subunit crystals were genetically engineered to omit a 26-residue protein, Thx, which is present in the wild-type Thermus thermophilus 30S ribosomal subunit. We are primarily interested in elucidating the contribution of this ribosomal protein to the overall 30S subunit structure. To assess the viability of this study, femtosecond X-ray diffraction patterns from these crystals were recorded at the LCLS during a protein crystal screening beam time. During our data collection, we successfully observed diffraction from these difficult-to-grow 30S ribosomal subunit crystals. Most of our crystals were found to diffract to low resolution, while one crystal diffracted to 3.2 Å resolution. These data suggest the feasibility of pursuing high-resolution data collection as well as the need to improve sample preparation and handling in order to collect a complete radiation-damage-free data set using an X-ray Free Electron Laser. PMID:26798805

  16. Macrospin dynamics in antiferromagnets triggered by sub-20 femtosecond injection of nanomagnons.

    PubMed

    Bossini, D; Dal Conte, S; Hashimoto, Y; Secchi, A; Pisarev, R V; Rasing, Th; Cerullo, G; Kimel, A V

    2016-01-01

    The understanding of how the sub-nanoscale exchange interaction evolves in macroscale correlations and ordered phases of matter, such as magnetism and superconductivity, requires to bridging the quantum and classical worlds. This monumental challenge has so far only been achieved for systems close to their thermodynamical equilibrium. Here we follow in real time the ultrafast dynamics of the macroscale magnetic order parameter in the Heisenberg antiferromagnet KNiF3 triggered by the impulsive optical generation of spin excitations with the shortest possible nanometre wavelength and femtosecond period. Our magneto-optical pump-probe experiments also demonstrate the coherent manipulation of the phase and amplitude of these femtosecond nanomagnons, whose frequencies are defined by the exchange energy. These findings open up opportunities for fundamental research on the role of short-wavelength spin excitations in magnetism and strongly correlated materials; they also suggest that nanospintronics and nanomagnonics can employ coherently controllable spin waves with frequencies in the 20 THz domain. PMID:26847766

  17. Room-Temperature Femtosecond Faraday Effect in CdMnTe Single Crystals

    NASA Astrophysics Data System (ADS)

    Wang, D.; Sobolewski, R.; Mikulics, M.; Mycielski, A.

    2006-03-01

    We report the subpicosecond Faraday effect, measured in high quality Cd1-xMnxTe (x = 0.12 and x = 0.09) single crystals at room temperature. Using a femtosecond pump-probe technique, we were able to generate sub-picosecond current pulses by illuminating a free-standing LT-GaAs photoswitch, couple those pulses to the CdMnTe probe crystal using a coplanar transmission line, and, finally, optically sample the temporal evolution of the resulting magnetic transients with subpicosecond resolution and the excellent signal-to-noise ratio. The ultrafast (below 600 fs) Faraday rotation, responsible for the observed magneto-optical effect, has been attributed to the ultrafast spin dynamics of holes in our p-type CdMnTe crystals. The observed femtosecond Faraday effect can be the basis for a development of a magneto-optical sampling system for ultrafast, time-resolved characterization of current transients in novel electronic and spintronic devices.

  18. Absolute partial photoionization cross sections of ozone.

    SciTech Connect

    Berkowitz, J.; Chemistry

    2008-04-01

    Despite the current concerns about ozone, absolute partial photoionization cross sections for this molecule in the vacuum ultraviolet (valence) region have been unavailable. By eclectic re-evaluation of old/new data and plausible assumptions, such cross sections have been assembled to fill this void.

  19. Femtosecond laser materials processing

    SciTech Connect

    Stuart, B.C.

    1997-02-01

    The use femtosecond pulses for materials processing results in very precise cutting and drilling with high efficiency. Energy deposited in the electrons is not coupled into the bulk during the pulse, resulting in negligible shock or thermal loading to adjacent areas.

  20. Intense-Field Photoionization of Molecules using Ultrashort Radiation Pulses: Carbon Disulfide and Carbon Dioxide

    NASA Astrophysics Data System (ADS)

    Beck, Joshua; Uiterwaal, Cornelis

    2016-05-01

    We experimentally investigate the photoionization and photofragmentation of molecules using intense fields from an 800 nm, femtosecond laser source and an experimental method that eliminates the focal volume effect without the need for data deconvolution. Targets include carbon disulfide and carbon dioxide. We show that ionization is insignificant for intensities that maximize alignment of carbon disulfide, which validates ultrafast electron diffraction experiments from aligned carbon disulfide. For comparison, we also investigate the analogous molecule carbon dioxide. In this molecule the molecular bonding orbitals include the n = 2 atomic orbitals of the oxygen atom, while in carbon disulfide the n = 3 orbitals of the sulfur atom contribute to the bonding. Recent work will be presented. This work supported by U.S. Dept. of Education GAANN Grants Nos. P200A090156 and P200A120188 and National Science Foundation EPSCoR RII Track-2 CA Award No. IIA-1430519 (Cooperative Nebraska-Kansas Grant).

  1. Adaptive Femtosecond Quantum Control

    NASA Astrophysics Data System (ADS)

    Gerber, Gustav

    2003-03-01

    Obtaining active control over the dynamics of quantum-mechanical systems is a fascinating perspective in modern physics. A promising tool for this purpose is available with femtosecond laser technologies. The intrinsically broad spectral distribution and the phase function of femtosecond laser pulses can be specifically manipulated by pulse shapers to drive molecular systems coherently into the desired reaction pathways [1]. The approach of adaptive femtosecond quantum control follows the suggestion of Judson and Rabitz [2], in which a computer-controlled pulse shaper is used in combination with a learning algorithm [3] and direct feedback from the experiment to achieve coherent control over quantum-mechanical processes in an automated fashion, without requiring any model for the system's response. This technique can be applied to the control of gas-phase photodissociation processes [4]. Different bond-cleaving reactions can be preferentially selected, resulting in chemically different products. Prior knowledge about molecular Hamiltonians or reaction mechanisms is not required in this automated control loop, and this scheme works for complex systems. Adaptive pulse-shaping techniques can be transferred to the control of photoprocesses in the liquid phase as well, motivated by the wish to achieve control at particle densities high enough for (bimolecular) synthetic-chemical applications. Chemically selective molecular excitation is achieved by many-parameter adaptive quantum control [5], despite the failure of typical single-parameter approaches (such as wavelength control, intensity control, or linear chirp control). This experiment demonstrates that photoprocesses in two different molecular species can be controlled simultaneously. Applications are envisioned in bimolecular reaction control where specific educt molecules could selectively be "activated" for purposes of chemical synthesis. A new technological development further increases the possibilities and

  2. Toward Femtosecond X-ray Spectroscopy at the Advanced Light Source

    SciTech Connect

    Chong, Henry Herng Wei

    2004-04-16

    The realization of tunable, ultrashort pulse x-ray sources promises to open new venues of science and to shed new light on long-standing problems in condensed matter physics and chemistry. Fundamentally new information can now be accessed. Used in a pump-probe spectroscopy, ultrashort x-ray pulses provide a means to monitor atomic rearrangement and changes in electronic structure in condensed-matter and chemical systems on the physically-limiting time-scales of atomic motion. This opens the way for the study of fast structural dynamics and the role they play in phase transitions, chemical reactions and the emergence of exotic properties in materials with strongly interacting degrees of freedom. The ultrashort pulse x-ray source developed at the Advanced Light Source at the Lawrence Berkeley Laboratory is based on electron slicing in storage rings, and generates {approx}100 femtosecond pulses of synchrotron radiation spanning wavelengths from the far-infrared to the hard x-ray region of the electromagnetic spectrum. The tunability of the source allows for the adaptation of a broad range of static x-ray spectroscopies to useful pump-probe measurements. Initial experiments are attempted on transition metal complexes that exhibit relatively large structural changes upon photo-excitation and which have excited-state evolution determined by strongly interacting structural, electronic and magnetic degrees of freedom. Specifically, iron(II) complexes undergo a spin-crossover transition upon optical irradiation. The dynamics of the transition involve a metal-to-ligand charge transfer, a {Delta}S=2 change in magnetic moment and 10% bond dilation in the first coordination shell of the iron. Studies of the electronic dynamics are studied with time-resolved optical absorption measurements. The current progress of time-resolved structural studies to complete the picture of the spin-crossover transition is presented.

  3. Full-band structure calculations of optical injection in semiconductors: Investigations of one-color, two-color, and pump-probe scenarios

    NASA Astrophysics Data System (ADS)

    Robinson, Michael

    Carrier, spin, charge current, and spin current injection by one- and two-color optical schemes are investigated within 30-band k ˙ p theory. Parameters of the band model are optimized to give full-Brillouin zone band structures for GaAs and Ge that give accurate Gamma-point effective masses and gyromagnetic factors and give access to the L valley, and to the E1 and E1 + Delta1 critical points in the linear optical absorption. Calculations of one- and two-photon carrier and spin injection and two-color current injection are performed for excitation energies in the range of 0--4 eV in GaAs and 0--3.5 eV in Ge. Significant spin and spin current injection occurs with 30% spin polarization in GaAs and Ge at photon energy matching the E1 critical point. Further, the anisotropy and disparity of the current injection between parallel and perpendicular linearly-polarized beam configurations are calculated. For light propagating along a <111> crystal axis, anisotropic contributions in coherent current control and two-photon spin injection give rise to normal current components and in-plane spin components. In Ge, contributions from the holes to spin, electrical current, and spin current injection are investigated. Optical orientation results in 83% spin-polarized holes at the band edge. The effects of carrier dynamics in Ge are treated within a rate-equation model. The detection of spin dynamics in a pump-probe setup is considered, and the Fermi-factor approach is justified for electrons but not for holes. Carrier and current injection are further investigated in single-layer and bilayer graphene within the tight-binding model. In single-layer graphene, the linear-circular dichroism in two-photon absorption yields an absorption coefficient that is twice as large for circularly polarized light compared to linearly polarized light. Coherent current injection is largest for co-circularly polarized beams and zero for cross-circularly polarized beams. For linearly polarized

  4. Direct deconvolution of two-state pump-probe x-ray absorption spectra and the structural changes in a 100 ps transient of Ni(II)-tetramesitylporphyrin.

    SciTech Connect

    Della-Longa, S.; Chen, L. X.; Frank, P.; Hayakawa, K.; Hatada, K.; Benfatto, M.; Chemical Sciences and Engineering Division; Univ. dell' Aquila; Lab. Nazionali di Frascati; Northwestern Univ.; Stanford Univ.; Museo storico della Fisica e Centro Studi e Ricerche

    2009-05-04

    Full multiple scattering (FMS) Minuit XANES (MXAN) has been combined with laser pump-probe K-edge X-ray absorption spectroscopy (XAS) to determine the structure of photoexcited Ni(II)tetramesitylporphyrin, Ni(II)TMP, in dilute toluene solution. It is shown that an excellent simulation of the XANES spectrum is obtained, excluding the lowest-energy bound-state transitions. In ground-state Ni(II)TMP, the first-shell and second-shell distances are, respectively, d(Ni-N) = (1.93 {+-} 0.02) {angstrom} and d(Ni-C) = (2.94 {+-} 0.03) {angstrom}, in agreement with a previous EXAFS result. The time-resolved XANES difference spectrum was obtained from the spectra of Ni(II)TMP in its photoexcited T{sub 1} state and its ground state, S{sub 0}. The XANES difference spectrum has been analyzed to obtain both the structure and the fraction of the T{sub 1} state. If the T{sub 1} fraction is kept fixed at the value (0.37 {+-} 0.10) determined by optical transient spectroscopy, a 0.07 {angstrom} elongation of the Ni-N and Ni-C distances [d(Ni-N) and d(Ni-C)] is found, in agreement with the EXAFS result. However, an evaluation of both the distance elongation and the T{sub 1} fraction can also be obtained using XANES data only. According to experimental evidence, and MXAN simulations, the T{sub 1} fraction is (0.60 {+-} 0.15) with d(Ni-N) = (1.98 {+-} 0.03) {angstrom} (0.05 {angstrom} elongation). The overall uncertainty of these results depends on the statistical correlation between the distances and T{sub 1} fraction, and the chemical shift of the ionization energy because of subtle changes of metal charge between the T{sub 1} and S{sub 0} states. The T{sub 1} excited-state structure results, independently obtained without the excited-state fraction from optical transient spectroscopy, are still in agreement with previous EXAFS investigations. Thus, full multiple scattering theory applied through the MXAN formalism can be used to provide structural information, not only on the ground

  5. Single and double photoionization of lithium

    NASA Astrophysics Data System (ADS)

    Huang, M.-T.; Wehlitz, R.; Azuma, Y.; Pibida, L.; Sellin, I. A.; Cooper, J. W.; Koide, M.; Ishijima, H.; Nagata, T.

    1999-05-01

    The photoion Li2+/Li+ production cross section ratio of ground-state atomic lithium has been measured for photon energies ranging from 80 to 424 eV. The absolute cross sections for the Li2+ and Li+ yield are also derived. In this energy region, the Li2+/Li+ ratio reaches a plateau of about 1.0% before reaching a maximum of about 4.5%, then decreases slowly. Good agreement is found between the measured total photoionization cross sections of lithium and theoretical calculations. The Li2+/Li+ ratio is also compared to the He2+/He+ ratio from excited He(1s2s) for photon energies up to 70 eV above threshold. The branching ratio of Li2+ to total Li ion production is also compared to the single-ionization cross section of electron impact on Li+ ions.

  6. Scheme for multistep resonance photoionization of atoms

    NASA Astrophysics Data System (ADS)

    Liu, Bo; Ning, Xi-Jing

    2001-07-01

    Traditional schemes for multistep resonance photoionization of atoms let every employed laser beam interact with the atoms simultaneously. In such a situation, analyses via time-dependent Schrödinger equation show that high ionization probability requires all the laser beams must be intense enough. In order to decrease laser intensity, we proposed a scheme that the laser beam used to pump the excited atoms (in a higher bound state) into an autoionization state does not interact with the atoms until all the population is transferred by the other lasers from a ground state to the bound state. As an interesting example, we examined three-step photoionization of 235U with our scheme, showing that the intensity of two laser beams can be lowered by two orders of magnitude without losing high ionization probability.

  7. Photoionization from excited states of helium

    NASA Technical Reports Server (NTRS)

    Jacobs, V. L.

    1973-01-01

    The cross sections for photoionization from the 2 1S, 2 3S, 2 1P and 2 3P excited states of helium are calculated for photoelectron energies below the n = 2 threshold of He(+) using Hylleraas bound state wave functions and 1s-2s-2p close coupling final state wave functions. The resonant structures associated with the lowest-lying 1S, 1P, 3P, and 1D autoionizing states of helium are found to be characterized by large values of the line profile parameter q. The cross sections and the photoelectron angular distribution asymmetry parameters for the P-states are calculated for various polarization states of the target atom and the incident photon. Experiments which would lead to the separate determinations of the S- and D- wave partial photoionization cross sections are discussed.

  8. Photoabsorbtion and Photoionization of Diatomic Molecules

    NASA Astrophysics Data System (ADS)

    Saenz, Alejandro; Dumitriu, Irina

    2008-05-01

    The photodissociation spectra of HeH^+ will be presented together with photoionization cross sections of the alkali dimer cations Li^+2, Na^+2, and LiNa^+. The latter have been calculated using two methods: a time-independent perturbative method and a time-dependent non-perturbative one. The photodissociation of HeH^+ which is of interest for astrophysics and the tritium neutrino-mass experiments currently draws special attention because of the newly developed FEL experimental set-up FLASH in Hamburg at which dissociation of HeH^+ by VUV radiation has been investigated [Phys. Rev. Lett. 98, 223202 (2007)]. The alkali dimer cations are presented as a first methodological step to the photoionization of the alkali dimers, but they are also interesting by themselves since no ab initio data were available for the continuum spectra.

  9. [Femtosecond lenticule extraction (FLEx)].

    PubMed

    Blum, M; Sekundo, W

    2010-10-01

    Starting in 2006 a new "all femto" method of refractive correction for myopia and myopic astigmatism was introduced. This new method was originally introduced as femtosecond lenticule extraction (FLEx) and further developed with a small incision into SMILE (small incision lenticule extraction). To simplify the terminology the manufacturer brought this onto the market in April 2010 as ReLEx (refractive lenticule extraction). In this procedure a lenticule of intrastromal corneal tissue and a flap-like access cut are subsequently cut utilizing the VisuMax® femtosecond system (Carl Zeiss Meditec, Jena, Germany). The lenticule is then manually removed and the flap repositioned (only by FLEx). In approximately 1,000 successful surgical operations only few side effects were found. The number of eyes treated is currently being expanded in order to further standardize this new clinical procedure. PMID:20694728

  10. Femtosecond Laser Materials Processing

    SciTech Connect

    Banks, P.S.; Stuart, B.C.; Komashko, A.M.; Feit, M.D.; Rubenchik, A.M.; Perry, M.D.

    2000-03-06

    The use of femtosecond lasers allows materials processing of practically any material with extremely high precision and minimal collateral damage. Advantages over conventional laser machining (using pulses longer than a few tens of picoseconds) are realized by depositing the laser energy into the electrons of the material on a time scale short compared to the transfer time of this energy to the bulk of the material, resulting in increased ablation efficiency and negligible shock or thermal stress. The improvement in the morphology by using femtosecond pulses rather than nanosecond pulses has been studied in numerous materials from biologic materials to dielectrics to metals. During the drilling process, we have observed the onset of small channels which drill faster than the surrounding material.

  11. Photoionization and photodissociation in diffuse interstellar clouds

    SciTech Connect

    Roberge, W.G.; Dalgarno, A.; Flannery, B.P.

    1981-02-01

    An accurate treatment of radiative transfer is used to explore the effects of grain scattering properties on the photoionization and photodissociation efficiencies of atomic and molecular constituents in diffuse clouds and to calculate the rates of heat deposition by photoelectric emission from grains. The observational data on ionization and dissociation are consistent with, but do not establish, a grain scattering model which is highly anisotropic at short wavelengths.

  12. Absolute photoionization cross sections of atomic oxygen

    NASA Technical Reports Server (NTRS)

    Samson, J. A. R.; Pareek, P. N.

    1985-01-01

    The absolute values of photoionization cross sections of atomic oxygen were measured from the ionization threshold to 120 A. An auto-ionizing resonance belonging to the 2S2P4(4P)3P(3Do, 3So) transition was observed at 479.43 A and another line at 389.97 A. The experimental data is in excellent agreement with rigorous close-coupling calculations that include electron correlations in both the initial and final states.

  13. Absolute photoionization cross sections of atomic oxygen

    NASA Technical Reports Server (NTRS)

    Samson, J. A. R.; Pareek, P. N.

    1982-01-01

    The absolute values of photoionization cross sections of atomic oxygen were measured from the ionization threshold to 120 A. An auto-ionizing resonance belonging to the 2S2P4(4P)3P(3Do, 3So) transition was observed at 479.43 A and another line at 389.97 A. The experimental data is in excellent agreement with rigorous close-coupling calculations that include electron correlations in both the initial and final states.

  14. Characterization of femtosecond electron bunches from a laser-wakefield accelerator using THz radiation

    NASA Astrophysics Data System (ADS)

    van Tilborg, Jeroen

    2005-10-01

    We report on the temporal characterization of laser-plasma-produced electron bunches, indicating ultra-short sub-50 fs charge structure. In the LOASIS laboratory at LBNL, the electron bunches are produced through the interaction of an intense (>10^19 Wcm-2) laser pulse with an underdense (˜10^19 cm-3) Helium plasma. The femtosecond multi-nanoCoulomb bunches have relativistic energies, with a 100% energy spread. As the bunch exits the plasma-vacuum interface, coherent transition radiation is emitted. Since the electron bunch is still dense and compact at the emission interface, the coherent spectrum of the intense radiation pulse covers the THz regime. Spectral and temporal measurements on the THz pulse are performed and correlated to the temporal properties of the electron bunch. Detection techniques such as Michelson interferometry, semiconductor switching, and electro-optic sampling are applied. The latter technique, where the THz electric field versus time is mapped out, provides detailed temporal structure of the radiation pulse, and by inference the electron bunch. The measurements indicate that THz radiation is emitted by a skewed bunch with a sub-50 fs rise time and a ˜600 fs tail (half-width-at-half-maximum), which is consistent with ballistic debunching of 100%-energy-spread beams during propagation. The electro-optic time resolution of the method was limited by the crystal properties. The Michelson interferometry and semiconductor switching experiments confirmed the femtosecond nature of the electron bunches. The electro-optic measurement also demonstrates shot-to-shot stability of the laser-wakefield accelerator (LWFA) as well as femtosecond synchronization between the electron bunch and the probe beam. This highlights the applicability of the LWFA in pump-probe experiments, where synchronized emission of x-rays, gamma rays, THz waves, NIR beams, and electron bunches is available. This work is supported by DoE under contract DE-AC02-05CH11231.

  15. Time-resolved study of femtosecond laser induced micro-modifications inside transparent brittle materials

    NASA Astrophysics Data System (ADS)

    Hendricks, F.; Matylitsky, V. V.; Domke, M.; Huber, Heinz P.

    2016-03-01

    Laser processing of optically transparent or semi-transparent, brittle materials is finding wide use in various manufacturing sectors. For example, in consumer electronic devices such as smartphones or tablets, cover glass needs to be cut precisely in various shapes. The unique advantage of material processing with femtosecond lasers is efficient, fast and localized energy deposition in nearly all types of solid materials. When an ultra-short laser pulse is focused inside glass, only the localized region in the neighborhood of the focal volume absorbs laser energy by nonlinear optical absorption. Therefore, the processing volume is strongly defined, while the rest of the target stays unaffected. Thus ultra-short pulse lasers allow cutting of the chemically strengthened glasses such as Corning Gorilla glass without cracking. Non-ablative cutting of transparent, brittle materials, using the newly developed femtosecond process ClearShapeTM from Spectra-Physics, is based on producing a micron-sized material modification track with well-defined geometry inside. The key point for development of the process is to understand the induced modification by a single femtosecond laser shot. In this paper, pump-probe microscopy techniques have been applied to study the defect formation inside of transparent materials, namely soda-lime glass samples, on a time scale between one nanosecond to several tens of microseconds. The observed effects include acoustic wave propagation as well as mechanical stress formation in the bulk of the glass. Besides better understanding of underlying physical mechanisms, our experimental observations have enabled us to find optimal process parameters for the glass cutting application and lead to better quality and speed for the ClearShapeTM process.

  16. Femtosecond laser materials processing

    SciTech Connect

    Stuart, B. C., LLNL

    1998-06-02

    Femtosecond lasers enable materials processing of most any material with extremely high precision and negligible shock or thermal loading to the surrounding area Applications ranging from drilling teeth to cutting explosives to making high-aspect ratio cuts in metals with no heat-affected zone are made possible by this technology For material removal at reasonable rates, we developed a fully computer-controlled 15-Watt average power, 100-fs laser machining system.

  17. Nondipole Photoionization Parameters of Atomic Mercury

    NASA Astrophysics Data System (ADS)

    Banerjee, T.; Manson, S. T.

    2005-05-01

    Over the past few years, photoionization parameters have been found to be affected by nondipole terms at much lower energies than was known earlier [1,2]. The primary motivation for the present investigation is to study the effect of interchannel coupling involving E1 and E2 photoionization channels from subshells with large orbital angular momentum (l>2). In an extension of earlier work [3], the nondipole photoelectron angular distribution asymmetry parameters γandδ from the 6s and 5d subshells of atomic mercury have been obtained in the energy range from the respective thresholds up to 45 au. Relativistic-Random-Phase Approximation (RRPA) theory at various levels of truncation of the RRPA was used which allowed us to pinpoint the effects of interchannel coupling. The role of interchannel coupling between the 6s and 5d photoionization channels and the 4f channels in both the dipole (E1) and the quadrupole (E2) manifolds has been detailed and has been found to be of considerable significance. This work was supported by DST and NSF. [1] A. Derevianko, W. R. Johnson and K. T. Cheng , At. Data Nucl. Data Tables 73, 153 (1999). [2] O. Hemmers, et al, Phys. Rev. Lett. 91, 053002 (2003); 93, 11301 (2004). [3] P. C. Deshmukh, Radiation Phys. and Chem. 70, 515 (2004) and references therein.

  18. Photoionization models of the CALIFA HII regions

    NASA Astrophysics Data System (ADS)

    Morisset, C.; Delgado-Inglada, G.; Sánchez, S. F.

    2016-06-01

    We present here a short summary of a forthcoming paper on photoionization models based on CALIFA observations of HII regions. For each of the ˜ 20,000 sources of the CALIFA H ii regions catalog, a grid of photoionization models is computed assuming the ionizing SED being described by the underlying stellar population obtained from spectral synthesis modeling. The nebular metallicity (associated to O/H) is defined using the classical strong line method O3N2. The remaining free parameters are the abundance ratio N/O and the ionization parameter U, which are determined by looking for the model fitting [N II]/Hα and [O III]/Hβ. The models are also selected to fit [O II]/Hβ. This process leads to a set of ˜ 3,200 models that reproduce simultaneously the three observations. We determine new relations between the nebular parameters, like the ionization parameter U and the [O II]/[O III] or [S II]/[S III] line ratios. A new relation between N/O and O/H is obtained, mostly compatible with previous empirical determinations (and not with previous results obtained using photoionization models). A new relation between U and O/H is also determined. All the models are publicly available on the Mexican Millions Models database 3MdB.

  19. Structured photoionization continuum of superheated cesium vapor

    NASA Astrophysics Data System (ADS)

    Pichler, G.; Makdisi, Y.; Kokaj, J.; Thomas, N.; Mathew, J.

    2015-08-01

    We studied the absorption spectrum of dense cesium vapor in an all-sapphire cell with a special emphasis on the highly structured photoionization continuum. This continuum appears to be composed of atomic and molecular contributions which can be separated by means of additional superheating of the cesium vapor in the sapphire cell. This was possible due to the small amount of cesium filling which completely evaporated at a temperature of around 450 °C. This enabled the overheating of cesium dimers which greatly reduced its concentration at a temperature of 900 °C, leaving almost pure atomic Cs vapor. The analysis of the thermal destruction indicated that the highly structured molecular component of the photoionization continuum can be entirely attributed to cesium dimers. We discuss the possible origin of the structured photoionization continuum as stemming from the absorption process from the ground state of the Cs2 molecule to the doubly excited Cs2** molecule located above Cs2+ molecular ionization limit. The corresponding potential curves are subjected to mutual interactions and autoionization.

  20. Structured photoionization continuum of cesium vapor

    NASA Astrophysics Data System (ADS)

    Pichler, Goran; Makdisi, Yacoub; Kokaj, Jahja; Thomas, Nicky; Mathew, Joseph; AMIP Team

    2015-05-01

    We studied absorption spectrum of dense cesium vapor in an all-sapphire cell with a special emphasis on the highly structured photoionization continuum. This continuum appears to be composed of atomic and molecular contributions which can be separated by means of additional superheating of the sapphire cell. This was possible due to the small amount of cesium filling which completely evaporated at temperature of about 450 °C. This enabled the overheating of cesium dimers which almost disappeared at a temperature of 900 °C leaving pure atomic Cs vapor. The analysis of the thermal destruction indicated that the highly structured molecular component of the photoionization continuum can be entirely attributed to cesium dimers. We discuss the possible origin of the structured photoionization continuum as stemming from the absorption process from the ground Cs2 molecule to the doubly excited Cs2** molecule located above the molecular ionization limit Cs2+.The corresponding potential curves are subjected to a mutual interactions and autoionization.

  1. Femtosecond probing around the K-edge of a laser heated plasma using X-rays from betatron oscillations in a laser wakefield accelerator

    NASA Astrophysics Data System (ADS)

    Behm, Keegan; Zhao, Tony; Maksimchuk, Anatoly; Yanovsky, Victor; Nees, John; Mangles, Stuart; Krushelnick, Karl; Thomas, Alexander; CenterUltrafast Optical Science Team; Plasmas Group Team

    2015-11-01

    Presented here are data from a two-beam pump-probe experiment. We used synchrotron-like X-rays created by betatron oscillations to probe a thin metal foil that is pumped by the secondary laser beam. The Hercules Ti:Sapph laser facility was operated with a pulse duration of 34 fs and a power of 65 TW split to drive a laser wakefield accelerator and heat the secondary target. We observed opacity changes around the K-edge of thin foils as they were heated by an ultrafast pump laser. To understand how the opacity is changing with heating and expansion of the plasma, the delay between the two laser paths was adjusted on a fs and ps time scale. Experimental data for polyvinylidene chloride (PVDC) and aluminum show variations in opacity around the Cl and Al K-edges with changes in the probe delay. The transmitted synchrotron-like spectrum was measured using single photon counting on an X-ray CCD camera and was available on a shot-by-shot basis. The success of this work demonstrates a practical application for X-rays produced from betatron oscillations in a wakefield accelerator. The compact size of these ``table-top'' accelerators and the ultrashort nature of the generated X-ray pulses allows pump-probe experiments that can probe events that occur on the femtosecond time scale.

  2. Analysis of Femtosecond Timing Noise and Stability in Microwave Components

    SciTech Connect

    Whalen, Michael R.; /Stevens Tech. /SLAC

    2011-06-22

    To probe chemical dynamics, X-ray pump-probe experiments trigger a change in a sample with an optical laser pulse, followed by an X-ray probe. At the Linac Coherent Light Source, LCLS, timing differences between the optical pulse and x-ray probe have been observed with an accuracy as low as 50 femtoseconds. This sets a lower bound on the number of frames one can arrange over a time scale to recreate a 'movie' of the chemical reaction. The timing system is based on phase measurements from signals corresponding to the two laser pulses; these measurements are done by using a double-balanced mixer for detection. To increase the accuracy of the system, this paper studies parameters affecting phase detection systems based on mixers, such as signal input power, noise levels, temperature drift, and the effect these parameters have on components such as the mixers, splitters, amplifiers, and phase shifters. Noise data taken with a spectrum analyzer show that splitters based on ferrite cores perform with less noise than strip-line splitters. The data also shows that noise in specific mixers does not correspond with the changes in sensitivity per input power level. Temperature drift is seen to exist on a scale between 1 and 27 fs/{sup o}C for all of the components tested. Results show that any components using more metallic conductor tend to exhibit more noise as well as more temperature drift. The scale of these effects is large enough that specific care should be given when choosing components and designing the housing of high precision microwave mixing systems for use in detection systems such as the LCLS. With these improvements, the timing accuracy can be improved to lower than currently possible.

  3. Photoionization of atoms and molecules. [of hydrogen, helium, and xenon

    NASA Technical Reports Server (NTRS)

    Samson, J. A. R.

    1976-01-01

    A literature review on the present state of knowledge in photoionization is presented. Various experimental techniques that have been developed to study photoionization, such as fluorescence and photoelectron spectroscopy, mass spectroscopy, are examined. Various atoms and molecules were chosen to illustrate these techniques, specifically helium and xenon atoms and hydrogen molecules. Specialized photoionization such as in positive and negative ions, excited states, and free radicals is also treated. Absorption cross sections and ionization potentials are also discussed.

  4. Double and triple photoionization of Li and Be

    SciTech Connect

    Colgan, J.; Pindzola, M.S.; Robicheaux, F.

    2005-08-15

    We present calculations for the double photoionization (with excitation) and the triple photoionization of Li and Be. We extend and more fully discuss the previous calculations made for Li by Colgan et al. [Phys. Rev. Lett. 93, 053201 (2004)] and present calculations for Be. The Be triple photoionization cross sections are compared with previous double shake-off model calculations of Kheifets and Bray [J. Phys. B 36, L211 (2003)], and our calculations are found to be significantly lower.

  5. Double and triple photoionization of Li and Be

    NASA Astrophysics Data System (ADS)

    Colgan, J.; Pindzola, M. S.; Robicheaux, F.

    2005-08-01

    We present calculations for the double photoionization (with excitation) and the triple photoionization of Li and Be. We extend and more fully discuss the previous calculations made for Li by Colgan et al. [Phys. Rev. Lett. 93, 053201 (2004)] and present calculations for Be. The Be triple photoionization cross sections are compared with previous double shake-off model calculations of Kheifets and Bray [J. Phys. B 36, L211 (2003)], and our calculations are found to be significantly lower.

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

    NASA Astrophysics Data System (ADS)

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

    2013-03-01

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

  7. Transformation of silver nanospheres embedded in glass to nanodisks using circularly polarized femtosecond pulses

    SciTech Connect

    Stalmashonak, A.; Graener, H.; Seifert, G.

    2009-05-11

    We prove by help of optical microspectroscopy that spherical Ag nanoparticles embedded in glass can be transformed to oblate (disklike) shapes by irradiation with circularly polarized femtosecond laser pulses. The symmetry axis (short axis) of the oblate spheroids produced by this method is oriented along the laser propagation direction. This observation also confirms the assumption that the mechanism of shape transformation starts with directed photoionization of nanoparticles induced by laser irradiation in combination with the electric field enhancement at the particle-glass interface.

  8. Advances in femtosecond laser technology

    PubMed Central

    Callou, Thais Pinheiro; Garcia, Renato; Mukai, Adriana; Giacomin, Natalia T; de Souza, Rodrigo Guimarães; Bechara, Samir J

    2016-01-01

    Femtosecond laser technology has become widely adopted by ophthalmic surgeons. The purpose of this study is to discuss applications and advantages of femtosecond lasers over traditional manual techniques, and related unique complications in cataract surgery and corneal refractive surgical procedures, including: LASIK flap creation, intracorneal ring segment implantation, presbyopic treatments, keratoplasty, astigmatic keratotomy, and intrastromal lenticule procedures. PMID:27143847

  9. Advances in femtosecond laser technology.

    PubMed

    Callou, Thais Pinheiro; Garcia, Renato; Mukai, Adriana; Giacomin, Natalia T; de Souza, Rodrigo Guimarães; Bechara, Samir J

    2016-01-01

    Femtosecond laser technology has become widely adopted by ophthalmic surgeons. The purpose of this study is to discuss applications and advantages of femtosecond lasers over traditional manual techniques, and related unique complications in cataract surgery and corneal refractive surgical procedures, including: LASIK flap creation, intracorneal ring segment implantation, presbyopic treatments, keratoplasty, astigmatic keratotomy, and intrastromal lenticule procedures. PMID:27143847

  10. Femtosecond real-time probing of transition state dynamics in a surface photoreaction: Methyl desorption from CH{sub 3}I on MgO(100)

    SciTech Connect

    Vaida, Mihai E.; Hindelang, Peter E.; Bernhardt, Thorsten M.

    2008-07-07

    A novel experimental approach to the investigation of surface adsorbate reaction dynamics is presented. The direct time-resolved monitoring of the surface reaction transition state and product formation dynamics were accomplished via pump-probe mass spectrometry. As an example, methyl iodide molecules adsorbed at submonolayer coverage on an ultrathin magnesia film on Mo(100) were photoexcited to the A-band by ultrafast laser pulse irradiation. Employing time-delayed multiphoton ionization the dynamics of the dissociative methyl iodide transition state and of the emerging methyl photoproduct could be detected with femtosecond resolution. The reaction times deduced from the temporal evolution of the methyl ion mass signal indicate a strong interaction of the methyl fragment with the substrate surface prior to desorption.

  11. On the absolute photoionization cross section and dissociative photoionization of cyclopropenylidene.

    PubMed

    Holzmeier, Fabian; Fischer, Ingo; Kiendl, Benjamin; Krueger, Anke; Bodi, Andras; Hemberger, Patrick

    2016-04-01

    We report the determination of the absolute photoionization cross section of cyclopropenylidene, c-C3H2, and the heat of formation of the C3H radical and ion derived by the dissociative ionization of the carbene. Vacuum ultraviolet (VUV) synchrotron radiation as provided by the Swiss Light Source and imaging photoelectron photoion coincidence (iPEPICO) were employed. Cyclopropenylidene was generated by pyrolysis of a quadricyclane precursor in a 1 : 1 ratio with benzene, which enabled us to derive the carbene's near threshold absolute photoionization cross section from the photoionization yield of the two pyrolysis products and the known cross section of benzene. The cross section at 9.5 eV, for example, was determined to be 4.5 ± 1.4 Mb. Upon dissociative ionization the carbene decomposes by hydrogen atom loss to the linear isomer of C3H(+). The appearance energy for this process was determined to be AE(0K)(c-C3H2; l-C3H(+)) = 13.67 ± 0.10 eV. The heat of formation of neutral and cationic C3H was derived from this value via a thermochemical cycle as Δ(f)H(0K)(C3H) = 725 ± 25 kJ mol(-1) and Δ(f)H(0K)(C3H(+)) = 1604 ± 19 kJ mol(-1), using a previously reported ionization energy of C3H. PMID:26975696

  12. 2008 Photoions, Photoionization & Photodetachment Gordon Research Conference January 27-February 1, 2008

    SciTech Connect

    Klaus Muller-Dethefs Nancy Ryan GRay

    2009-03-31

    This conference brings together scientists interested in a range of basic phenomena linked to the ejection and scattering of electrons from atoms, molecules, clusters, liquids and solids by absorption of light. Photoionization, a highly sensitive probe of both structure and dynamics, can range from perturbative single-photon processes to strong-field highly non-perturbative interactions. It is responsible for the formation and destruction of molecules in astrophysical and plasma environments and successfully used in advanced analytical techniques. Positive ions, which can be produced and studied most effectively using photoionization, are the major components of all plasmas, vital constituents of flames and important intermediates in many chemical reactions. Negative ions are significant as transient species and, when photodetached, the corresponding neutral species often undergoes remarkable, otherwise non-observable, dynamics. The scope of the meeting spans from novel observations in atomic and molecular physics, such as Coulomb Crystals, highly excited states and cold Rydberg plasmas, to novel energy resolved or ultrafast time-resolved experiments, photoionization in strong laser fields, theoretical method development for electron scattering, photoionization and photodetachment and more complex phenomena such as charge transfer and DNA and protein conductivity, important for biological and analytical applications.

  13. Femtosecond laser cataract surgery.

    PubMed

    Nagy, Zoltan Z; McAlinden, Colm

    2015-01-01

    Femtosecond laser (FSL) cataract surgery is in its infancy but is rapidly gaining popularity due to the improved consistency and predictability for corneal incisions and anterior capsulorhexis. It enables subsequently less phacoemulsification energy and time to be employed, which has gains in terms of reduced corneal oedema. In addition, the FSL allows better circularity of the anterior capsulotomy, capsule overlap, intraocular lens (IOL) placement and centration of the IOL. These advantages have resulted in improved visual and refractive outcomes in the short term. Complication rates are low which reduce with surgeon experience. This review article focuses on the Alcon LenSx system. PMID:26605364

  14. Femtosecond polarization pulse shaping.

    PubMed

    Brixner, T; Gerber, G

    2001-04-15

    We report computer-controlled femtosecond polarization pulse shaping where intensity, momentary frequency, and light polarization are varied as functions of time. For the first time to our knowledge, a pulse shaper is used to modulate the degree of ellipticity as well as the orientation of the elliptical principal axes within a single laser pulse by use of a 256-pixel two-layer liquid-crystal display inside a zero-dispersion compressor. Interferometric stability of the setup is not required. Complete pulse characterization is achieved by dual-channel spectral interferometry. This technology has a large range of applications, especially in the field of quantum control. PMID:18040384

  15. Spin effects in double photoionization of lithium

    SciTech Connect

    Kheifets, A. S.; Fursa, D. V.; Hines, C. W.; Bray, I.; Colgan, J.; Pindzola, M. S.

    2010-02-15

    We apply the nonperturbative convergent close-coupling (CCC) and time-dependent close coupling (TDCC) formalisms to calculate fully differential energy and angular resolved cross sections of double photoionization (DPI) of lithium. The equal energy sharing case is considered in which dynamics of the DPI process can be adequately described by two symmetrized singlet and triplet amplitudes. The angular width of these amplitudes serves as a measure of the strength of the angular correlation between the two ejected electrons. This width is interpreted in terms of the spin of the photoelectron pair.

  16. He photoionization dominated by doubly excited resonances

    SciTech Connect

    Chang, T.N.; Zhen, M.

    1993-05-01

    We present the theoretical He photoionization, cross sections from the ground and the {sup 1,3}S bound excited states using a B-spline based configuration-interaction procedure for continuum (CIC). The resonant structures associated with selected sp,2n{sup {plus_minus}} and 2pnd {sup 1,3}P autoionization series below the He{sup +} N=2 threshold will be expressed quantitatively in terms of their resonant energies, widths, and peak cross sections. Comparisons with earlier theoretical results and recent experimental measurement will be presented. The nonresonant spectra from the 1s2s {sup 1,3}S metastable states will also be reexamined.

  17. Double Photoionization of Aligned Molecular Hydrogen

    SciTech Connect

    Vanroose, Wim; Horner, Daniel A.; Martin, Fernando; Rescigno,Thomas N.; McCurdy, C. William

    2006-07-21

    We present converged, completely ab initio calculations ofthe triple differential cross sections for double photoionization ofaligned H2 molecules for a photon energy of 75.0 eV. The method ofexterior complex scaling, implemented with both the discrete variablerepresentation and B-splines, is used to solve the Schroedinger equationfor a correlated continuum wave function corresponding to a single photonhaving been absorbed by a correlated initial state. Results for a fixedinternuclear distance are compared with recent experiments and show thatintegration over experimental angular and energy resolutions is necessaryto produce good qualitative agreement, but does not eliminate somediscrepancies. Limitations of current experimental resolution are shownto sometimes obscure interesting details of the crosssection.

  18. Photoionization mass spectrometric study of HOCl: Photoionization efficiency spectrum and ionization energy

    SciTech Connect

    Thorn, R.P. Jr.; Stief, L.J.

    1999-02-18

    The photoionization efficiency (PIE) spectrum of HOCl was measured over the wavelength range {lambda} = 102--115 nm, using a discharge flow-photoionization mass spectrometer (DF-PIMS) apparatus coupled to a synchrotron radiation source. The PIE spectra displayed steplike behavior near threshold. This study represents the first determination of the HOCl photoionization efficiency spectrum and the photoionization threshold. A value of 11.12{sub 3} {+-} 0.01{sub 8} eV was obtained for the adiabatic ionization energy (IE) of HOCl from analysis of photoion thresholds, corresponding to the HOCl{sup +}(X{sup 2}A{double_prime}) {l_arrow} HOCl(X{sup 1}A{double_prime}) transition. The PIMS result is identical to the only previous experimental measurement and in good agreement with a recent ab initio calculation. From the result for IE(HOCl), a value of 999.4 {+-} 3.6 kJ mol{sup {minus}1} was calculated for {Delta}{sub f}H{degree}{sub 0}(HOCl{sup +}), and from the latter, the proton affinity of ClO at T = 0 K, PA{sub 0}(ClO), was determined to be 629.6 {+-} 3.6 kJ mol{sup {minus}1}. At 298 K, the computed values for {Delta}{sub f}H{degree}{sub 298}(HOCl{sup +}) and PA{sub 298}(ClO) are 996.5 {+-} 3.6 and 635.1 {+-} 3.6 kJ mol{sup {minus}1}, respectively.

  19. Spin-resolved photoelectron spectroscopy using femtosecond extreme ultraviolet light pulses from high-order harmonic generation.

    PubMed

    Plötzing, M; Adam, R; Weier, C; Plucinski, L; Eich, S; Emmerich, S; Rollinger, M; Aeschlimann, M; Mathias, S; Schneider, C M

    2016-04-01

    The fundamental mechanism responsible for optically induced magnetization dynamics in ferromagnetic thin films has been under intense debate since almost two decades. Currently, numerous competing theoretical models are in strong need for a decisive experimental confirmation such as monitoring the triggered changes in the spin-dependent band structure on ultrashort time scales. Our approach explores the possibility of observing femtosecond band structure dynamics by giving access to extended parts of the Brillouin zone in a simultaneously time-, energy- and spin-resolved photoemission experiment. For this purpose, our setup uses a state-of-the-art, highly efficient spin detector and ultrashort, extreme ultraviolet light pulses created by laser-based high-order harmonic generation. In this paper, we present the setup and first spin-resolved spectra obtained with our experiment within an acquisition time short enough to allow pump-probe studies. Further, we characterize the influence of the excitation with femtosecond extreme ultraviolet pulses by comparing the results with data acquired using a continuous wave light source with similar photon energy. In addition, changes in the spectra induced by vacuum space-charge effects due to both the extreme ultraviolet probe- and near-infrared pump-pulses are studied by analyzing the resulting spectral distortions. The combination of energy resolution and electron count rate achieved in our setup confirms its suitability for spin-resolved studies of the band structure on ultrashort time scales. PMID:27131684

  20. Spin-resolved photoelectron spectroscopy using femtosecond extreme ultraviolet light pulses from high-order harmonic generation

    NASA Astrophysics Data System (ADS)

    Plötzing, M.; Adam, R.; Weier, C.; Plucinski, L.; Eich, S.; Emmerich, S.; Rollinger, M.; Aeschlimann, M.; Mathias, S.; Schneider, C. M.

    2016-04-01

    The fundamental mechanism responsible for optically induced magnetization dynamics in ferromagnetic thin films has been under intense debate since almost two decades. Currently, numerous competing theoretical models are in strong need for a decisive experimental confirmation such as monitoring the triggered changes in the spin-dependent band structure on ultrashort time scales. Our approach explores the possibility of observing femtosecond band structure dynamics by giving access to extended parts of the Brillouin zone in a simultaneously time-, energy- and spin-resolved photoemission experiment. For this purpose, our setup uses a state-of-the-art, highly efficient spin detector and ultrashort, extreme ultraviolet light pulses created by laser-based high-order harmonic generation. In this paper, we present the setup and first spin-resolved spectra obtained with our experiment within an acquisition time short enough to allow pump-probe studies. Further, we characterize the influence of the excitation with femtosecond extreme ultraviolet pulses by comparing the results with data acquired using a continuous wave light source with similar photon energy. In addition, changes in the spectra induced by vacuum space-charge effects due to both the extreme ultraviolet probe- and near-infrared pump-pulses are studied by analyzing the resulting spectral distortions. The combination of energy resolution and electron count rate achieved in our setup confirms its suitability for spin-resolved studies of the band structure on ultrashort time scales.

  1. Double photoionization of helium with synchrotron x-rays: Proceedings

    SciTech Connect

    Not Available

    1994-01-01

    This report contains papers on the following topics: Overview and comparison of photoionization with charged particle impact; The ratio of double to single ionization of helium: the relationship of photon and bare charged particle impact ionization; Double photoionization of helium at high energies; Compton scattering of photons from electrons bound in light elements; Electron ionization and the Compton effect in double ionization of helium; Elimination of two atomic electrons by a single energy photon; Double photoionization of helium at intermediate energies; Double Photoionization: Gauge Dependence, Coulomb Explosion; Single and Double Ionization by high energy photon impact; The effect of Compton Scattering on the double to single ionization ratio in helium; and Double ionization of He by photoionization and Compton scattering. These papers have been cataloged separately for the database.

  2. Photoionization Dynamics in Pure Helium Droplets

    SciTech Connect

    Peterka, Darcy S.; Kim, Jeong Hyun; Wang, Chia C.; Poisson,Lionel; Neumark, Daniel M.

    2007-02-04

    The photoionization and photoelectron spectroscopy of pure He droplets are investigated at photon energies between 24.6 eV (the ionization energy of He) and 28 eV. Time-of-flight mass spectra and photoelectron images were obtained at a series of molecular beam source temperatures and pressures to assess the effect of droplet size on the photoionization dynamics. At source temperatures below 16 K, the photoelectron images are dominated by fast electrons produced via direct ionization of He atoms, with a small contribution from very slow electrons with kinetic energies below 1 meV arising from an indirect mechanism. The fast photoelectrons have as much as 0.5 eV more kinetic energy than those from atomic He at the same photon energy. This result is interpreted and simulated within the context of a 'dimer model', in which one assumes vertical ionization from two nearest neighbor He atoms to the attractive region of the He2+ potential energy curve. Possible mechanism for the slow electrons, which were also seen at energies below IE(He), are discussed, including vibrational autoionizaton of Rydberg states comprising an electron weakly bound to the surface of a large HeN+ core.

  3. Gas-Phase Photoionization Of A Protein

    NASA Astrophysics Data System (ADS)

    Milosavljevic, A. R.; Giuliani, A.; Nicolas, C.; Gil, J.-F.; Lemaire, J.; Refregiers, M.; Nahon, L.

    2010-07-01

    We present preliminary results on gas phase photoionization of electrosprayproduced multiply protonated cytochrome c protein (104 amino acids; ˜12.4 kDa), which has been achieved with a newly developed experimental system for spectroscopy of electrosprayed ions in a linear quadrupole ion trap using a monochromatized vacuum ultraviolet (VUV) synchrotron radiation and tandem mass spectrometry method. The investigation of proteins in the gas phase, where they are free of the influence of counterions and solvent molecules, offer a possibility to understand their intrinsic molecular properties. However, due to limited both ion densities and available number of photons, the use of synchrotron radiation for the trapped ions spectroscopy is a rather challenging task. The feasibility of coupling a Fourier transform ion cyclotron resonance ion trap with soft x-ray synchrotron beamline and the first successful use of synchrotron radiation for spectroscopy of electrosprayed negative ions stored in a three-dimensional quadrupole ion trap have been demonstrated only recently (R. Thissen et al., 2008, Phys. Rev. Lett., 100, 223001; A. Giulliani et al., Proc. 57th ASMS Conf., Philadelphia, 2009). The present results are the first reported on photoionization of kDa species in the gas phase and are valuable regarding both a fundamental interest of accessing physical properties of large biological ions isolated in vacuo and potential development of a new technique for proteomics.

  4. Femtosecond photoelectron point projection microscope

    SciTech Connect

    Quinonez, Erik; Handali, Jonathan; Barwick, Brett

    2013-10-15

    By utilizing a nanometer ultrafast electron source in a point projection microscope we demonstrate that images of nanoparticles with spatial resolutions of the order of 100 nanometers can be obtained. The duration of the emission process of the photoemitted electrons used to make images is shown to be of the order of 100 fs using an autocorrelation technique. The compact geometry of this photoelectron point projection microscope does not preclude its use as a simple ultrafast electron microscope, and we use simple analytic models to estimate temporal resolutions that can be expected when using it as a pump-probe ultrafast electron microscope. These models show a significant increase in temporal resolution when comparing to ultrafast electron microscopes based on conventional designs. We also model the microscopes spectroscopic abilities to capture ultrafast phenomena such as the photon induced near field effect.

  5. Femtosecond Stimulated Raman Spectroscopy.

    PubMed

    Dietze, Daniel R; Mathies, Richard A

    2016-05-01

    Femtosecond stimulated Raman spectroscopy (FSRS) is an ultrafast nonlinear optical technique that provides vibrational structural information with high temporal (sub-50 fs) precision and high spectral (10 cm(-1) ) resolution. Since the first full demonstration of its capabilities ≈15 years ago, FSRS has evolved into a mature technique, giving deep insights into chemical and biochemical reaction dynamics that would be inaccessible with any other technique. It is now being routinely applied to virtually all possible photochemical reactions and systems spanning from single molecules in solution to thin films, bulk crystals and macromolecular proteins. This review starts with an historic overview and discusses the theoretical and experimental concepts behind this technology. Emphasis is put on the current state-of-the-art experimental realization and several variations of FSRS that have been developed. The unique capabilities of FSRS are illustrated through a comprehensive presentation of experiments to date followed by prospects. PMID:26919612

  6. Photoionization research on atomic beams. 2: The photoionization cross section of atomic oxygen

    NASA Technical Reports Server (NTRS)

    Comes, F. J.; Speier, F.; Elzer, A.

    1982-01-01

    An experiment to determine the absolute value of the photo-ionization cross section of atomic oxygen is described. The atoms are produced in an electrical discharge in oxygen gas with 1% hydrogen added. In order to prevent recombination a crossed beam technique is employed. The ions formed are detected by a time-of-flight mass spectrometer. The concentration of oxygen atoms in the beam is 57%. The measured photoionization cross section of atomic oxygen is compared with theoretical data. The results show the participation of autoionization processes in ionization. The cross section at the autoionizing levels detected is considerably higher than the absorption due to the unperturbed continuum. Except for wavelengths where autoionization occurs, the measured ionization cross section is in fair agreement with theory. This holds up to 550 A whereas for shorter wavelengths the theoretical values are much higher.

  7. Femtosecond optical/hard X-ray timing diagnostics at an FEL: implementation and performance

    NASA Astrophysics Data System (ADS)

    Lemke, Henrik T.; Weaver, Matt; Chollet, Matthieu; Robinson, Joseph; Glownia, James M.; Zhu, Diling; Bionta, Mina R.; Cammarata, Marco; Harmand, Marion; Coffee, Ryan N.; Fritz, David M.

    2013-05-01

    The development of Free Electron Lasers has opened the possibility to investigate ultrafast processes using femtosecond hard x-ray pulses. In optical/x-ray light pump/probe experiments, however, the time resolution is mainly limited by the ability to synchronize both light sources over a long distance (<100 fs FWHM) rather than their pulse length (<10 fs FWHM). We have implemented a spectrally encoding x-ray to optical laser timing diagnostic into the XPP beamline at LCLS with a timing uncertainty down to 10 fs. An x-ray induced change of refractive index in a solid target is temporally probed for single pulses by a chirped white light pulse [4]. By resorting single shot data to the timestamps obtained by the diagnostics, the temporal data quality can be improved to basically pulse length limited time resolution. By interchangable targets and adjustable x-ray and laser foci, the method was successfully applied for very different x-ray parameters. These are different photon energies in the range of 6-20 keV, which at LCLS also includes application of 3rd Harmonic radiation, pulse energy, and bandwidth, when using a Si(111) monochromator.

  8. Femtosecond spectroscopy of multiferroic BiFeO3 thin films

    NASA Astrophysics Data System (ADS)

    Zhang, J.; Abreu, E.; Schneck, J. R.; Rana, D. S.; Kawayama, I.; Tonouchi, M.; Ziegler, L.; Averitt, R. D.

    2010-03-01

    BiFeO3 is a multiferroic material characterized by a room temperature antiferromagnetic and ferroelectric phase and a 2.6eV bandgap. Terahertz emission from BiFeO3 thin films following excitation above bandgap by UV femtosecond pulses has been observed [1]. The THz emission is related to ultrafast depolarization of the ferroelectric order in the film as observed from the hysteresis of the amplitude of the emitted THz signal as a function of a biasing electric field. Experiments probing the electronic and lattice dynamics with sub-picosecond resolution are an essential step towards identifying the intrinsic mechanism responsible for depolarization and THz emission in BiFeO3. In this study we investigate the carrier dynamics of epitaxial BiFeO3 thin films using degenerate pump-probe spectroscopy at 400 nm with sub-50 fs pulses. We have observed a 5 THz coherent optical phonon oscillation consistent with the A1 phonon mode as observed in Raman spectroscopy [2]. In this talk, the relation of the observed dynamics to the THz emission will be discussed. [1] D.S. Rana, et al., Advanced Materials 21, 2881 (2009). [2] S. Kamba, et al, Phys. Rev. B 75, 024403 (2007).

  9. Laser induced forward transfer of metals by temporally shaped femtosecond laser pulses.

    PubMed

    Klini, A; Loukakos, P A; Gray, D; Manousaki, A; Fotakis, C

    2008-07-21

    Temporally shaped, femtosecond laser pulses have been used for controlling the size and the morphology of micron-sized metallic structures obtained by using the Laser Induced Forward Transfer (LIFT) technique. We report the effect of pulse shaping on the size and morphology of the deposited structures of Au, Zn, Cr on a function of the pulse separation time ??t (from 0 to 10 ps) of double pulses of variable intensities generated by using a liquid crystal spatial light modulator (SLM). The observed differences in size and morphology are correlated with the outcome of pump-probe experiments for the study of electron-phonon scattering dynamics and subsequent energy transfer processes to the bulk in the different metals employed. We propose that in metals with weak electron-lattice coupling, the electron ballistic motion and the resulting fast electron scattering at the film surface, as well as the internal electron thermalization process are crucial to the morphology and size of the transferred material. Therefore, temporal shaping within the corresponding time scales of these processes may be used for tailoring the features of the metallic structures obtained by LIFT. PMID:18648449

  10. Ultrafast dynamics in helium nanodroplets probed by femtosecond time-resolved EUV photoelectron imaging

    SciTech Connect

    Kornilov, Oleg; Wang, Chia C.; Buenermann, Oliver; Healy, Andrew T.; Leonard, Mathew; Peng, Chunte; Leone, Stephen R.; Neumark, Daniel M.; Gessner, Oliver

    2010-07-09

    The dynamics of electronically excited helium nanodroplets are studied by femtosecond time-resolved photoelectron imaging. EUV excitation into a broad absorption band centered around 23.8 eV leads to an indirect photoemission process that generates ultraslow photoelectrons. A 1.58 eV probe pulse transiently depletes the indirect photoemission signal for pump-probe time delays <200 fs and enhances the signal beyond this delay. The depletion is due to suppression of the indirect ionization process by the probe photon, which generates a broad, isotropically emitted photoelectron band. Similar time scales in the decay of the high energy photoelectron signal and the enhancement of the indirect photoemission signal suggest an internal relaxation process that populates states in the range of a lower energy droplet absorption band located just below the droplet ionization potential (IP {approx} 23.0 eV). A nearly 70% enhancement of the ultraslow photoelectron signal indicates that interband relaxation plays a more dominant role for the droplet de-excitation mechanism than photoemission.

  11. Dynamics of femtosecond laser absorption of fused silica in the ablation regime

    SciTech Connect

    Lebugle, M. Sanner, N.; Varkentina, N.; Sentis, M.; Utéza, O.

    2014-08-14

    We investigate the ultrafast absorption dynamics of fused silica irradiated by a single 500 fs laser pulse in the context of micromachining applications. A 60-fs-resolution pump-probe experiment that measures the reflectivity and transmissivity of the target under excitation is developed to reveal the evolution of plasma absorption. Above the ablation threshold, an overcritical plasma with highly non-equilibrium conditions is evidenced in a thin layer at the surface. The maximum electron density is reached at a delay of 0.5 ps after the peak of the pump pulse, which is a strong indication of the occurrence of electronic avalanche. The results are further analyzed to determine the actual feedback of the evolution of the optical properties of the material on the pump pulse. We introduce an important new quantity, namely, the duration of absorption of the laser by the created plasma, corresponding to the actual timespan of laser absorption by inverse Bremsstrahlung. Our results indicate an increasing contribution of plasma absorption to the total material absorption upon raising the excitation fluence above the ablation threshold. The role of transient optical properties during the energy deposition stage is characterized and our results emphasize the necessity to take it into account for better understanding and control of femtosecond laser-dielectrics interaction.

  12. Goniometer-based femtosecond X-ray diffraction of mutant 30S ribosomal subunit crystals

    DOE PAGESBeta

    Dao, E. Han; Sierra, Raymond G.; Laksmono, Hartawan; Lemke, Henrik T.; Alonso-Mori, Roberto; Coey, Aaron; Larsen, Kevin; Baxter, Elizabeth L.; Cohen, Aina E.; Soltis, S. Michael; et al

    2015-04-30

    In this work, we collected radiation-damage-free data from a set of cryo-cooled crystals for a novel 30S ribosomal subunit mutant using goniometer-based femtosecond crystallography. Crystal quality assessment for these samples was conducted at the X-ray Pump Probe end-station of the Linac Coherent Light Source (LCLS) using recently introduced goniometer-based instrumentation. These 30S subunit crystals were genetically engineered to omit a 26-residue protein, Thx, which is present in the wild-type Thermus thermophilus 30S ribosomal subunit. We are primarily interested in elucidating the contribution of this ribosomal protein to the overall 30S subunit structure. To assess the viability of this study, femtosecondmore » X-ray diffraction patterns from these crystals were recorded at the LCLS during a protein crystal screening beam time. During our data collection, we successfully observed diffraction from these difficult-to-grow 30S ribosomal subunit crystals. Most of our crystals were found to diffract to low resolution, while one crystal diffracted to 3.2 Å resolution. These data suggest the feasibility of pursuing high-resolution data collection as well as the need to improve sample preparation and handling in order to collect a complete radiation-damage-free data set using an X-ray Free Electron Laser.« less

  13. Femtosecond OH bending dynamics of water nanopools confined in reverse micelles.

    PubMed

    Costard, Rene; Elsaesser, Thomas

    2013-12-12

    The relaxation of OH bend excitations of H2O confined in reverse micelles is studied by femtosecond broadband pump-probe spectroscopy for the two ionic systems dioctyl sodium sulfosuccinate (AOT) and dioleoylphosphatidylcholine (DOPC) and for the nonionic tetraethylene glycol dodecyl ether (Brij-30). In the ionic AOT/DOPC reverse micelles, the OH bending lifetime T1 decreases from T1 > 615 fs for a 3:1 ratio of water and AOT/DOPC molecules (w0 = 3) to T1 = 345 fs for a 16:1 ratio (w0 = 16). In contrast, H2O in Brij-30 reverse micelles shows a much shorter T1 = 400 fs at w0 = 2 which decreases to T1 = 250 fs at w0 = 8. OH bend relaxation proceeds mainly via librational overtones of the bend-excited water molecules with a rate correlating with the energy mismatch between the v = 1 OH bend state and the librational overtone. In the ionic systems, the lower librational frequencies at small w0 result in a larger mismatch and longer T1 times. In the nonionic case, the w0-independent librational frequencies with a small energy mismatch lead to shorter T1 times. For w0 ≥ 8, the energy flow into the first hydration shell of the bend-excited molecules makes an additional contribution to the relaxation rate in all systems. PMID:23721432

  14. Filamentation and damage in fused silica induced by tightly focused femtosecond laser pulses

    SciTech Connect

    Couairon, A.; Sudrie, L.; Franco, M.; Prade, B.; Mysyrowicz, A.

    2005-03-15

    We investigate experimentally and numerically the damage tracks induced by tightly focused (NA=0.5) infrared femtosecond laser pulses in the bulk of a fused silica sample. Two types of irreversible damage are observed. The first damage corresponds to a permanent change of refractive index without structural modifications (type I). It appears for input pulse energies beyond 0.1 {mu}J. It takes the form of a narrow track extending over more than 100 {mu}m at higher input powers. It is attributed to a change of the polarizability of the medium, following a filamentary propagation which generates an electron-hole plasma through optical field ionization. A second type of damage occurs for input pulse energies beyond 0.3 {mu}J (type II). It takes the form of a pear-shaped structural damage associated with an electron-ion plasma triggered by avalanche. The temporal evolution of plasma absorption is studied by pump-probe experiments. For type I damage, a fast electron-hole recombination is observed. Type II damage is linked with a longer absorption.

  15. Vacuum ultraviolet photoionization and photodissociation of polyatomic molecules and radicals

    SciTech Connect

    Ng, C.Y.

    1993-12-01

    In the past decade, tremendous progress has been made in understanding the photodissociation (PD) dynamics of triatomic molecules. However, the PD study of radicals, especially polyatomic radicals, has remained essentially an unexplored research area. Detailed state-to-state PD cross sections for radicals in the UV and VUV provide challenges not only for dynamical calculations, but also for ab initio quantum chemical studies. The authors have developed a laser based pump-probe apparatus for the measurement of absolute PD cross sections for CH{sub 3}S and HS is summarized.

  16. Adaptive control of lasers and their interactions with matter using femtosecond pulse shaping

    NASA Astrophysics Data System (ADS)

    Efimov, Anatoly

    Coherent control of chemical reactions, atomic and molecular systems, lattice dynamics, and electronic motion rely on femtosecond laser sources capable of producing programmable arbitrarily shaped waveforms. To enter the time scale of natural dynamic processes in many systems, femtosecond pulse shaping techniques must be extended to the ultrashort pulse domain (<50 fs). Concurrently, reliable high-fidelity amplification of shaped waveforms is required in many applications. We demonstrate ultrabroad bandwidth pulse shaping of 13 fs pulses with Fourier-domain phase-only filtering using a liquid crystal array. We further demonstrate the amplification of shaped pulses in a multipass chirped pulse amplifier (CPA) system to produce millijoule-level optical waveforms with 30 fs resolution. Recently, a new approach to coherent control of physical systems was introduced, which, instead of relying on formidable theoretical calculations of complex system dynamics, makes use of an appropriate experimental feedback from the system itself to control its evolution. We apply this adaptive feedback approach for enhancement of ionization rates in a femtosecond plasma with the goal of minimization of phase distortions in the amplifier system. With the help of a learning algorithm and survival principles of nature, we teach our laser to control its own phase by using spectral blueshifting in a rapidly created plasma as a feedback to the algorithm. Control of lattice vibrations has long been sought as a means of studying phonon-related processes in solids. In addition, generation and control of large-amplitude optical phonon modes may open a path to femtosecond time- resolved studies of structural phase transitions and production of ultrashort shaped X-ray pulses. We perform pump-probe phase-resolved measurements and control of optical A1g mode in sapphire through shaped-pulse impulsive stimulated Raman scattering (ISRS). We chose this material as a candidate for possible nonlinear

  17. Ultrafast supercontinuum fiber-laser based pump-probe scanning magneto-optical Kerr effect microscope for the investigation of electron spin dynamics in semiconductors at cryogenic temperatures with picosecond time and micrometer spatial resolution

    SciTech Connect

    Henn, T.; Kiessling, T. Ossau, W.; Molenkamp, L. W.; Biermann, K.; Santos, P. V.

    2013-12-15

    We describe a two-color pump-probe scanning magneto-optical Kerr effect microscope which we have developed to investigate electron spin phenomena in semiconductors at cryogenic temperatures with picosecond time and micrometer spatial resolution. The key innovation of our microscope is the usage of an ultrafast “white light” supercontinuum fiber-laser source which provides access to the whole visible and near-infrared spectral range. Our Kerr microscope allows for the independent selection of the excitation and detection energy while avoiding the necessity to synchronize the pulse trains of two separate picosecond laser systems. The ability to independently tune the pump and probe wavelength enables the investigation of the influence of excitation energy on the optically induced electron spin dynamics in semiconductors. We demonstrate picosecond real-space imaging of the diffusive expansion of optically excited electron spin packets in a (110) GaAs quantum well sample to illustrate the capabilities of the instrument.

  18. Transient electron density maps of ionic materials from femtosecond x-ray powder diffraction

    NASA Astrophysics Data System (ADS)

    Elsaesser, Thomas

    2014-05-01

    X-ray diffraction represents a key method for spatially resolving electron distributions in crystalline materials. So far, electron density maps have been derived from stationary diffraction patterns, providing detailed insight into the equilibrium charge distribution and crystal geometry. Functional processes in condensed matter are frequently connected with nonequilibrium excitations resulting in atomic motions and charge relocations on ultrashort time scales. Transient structures are resolved in space and time by novel x-ray diffraction methods with a femtosecond time resolution, giving access to the driving mechanisms and underlying interactions. In this talk, new results are presented on transient electron distributions of ionic materials mapped with the help of femtosecond x-ray powder diffraction. Experiments are based on a pump-probe approach in which an optical pulse initiates structural dynamics and a hard x-ray pulse from a synchronized laser-driven plasma source is diffracted from the excited powder sample. Such measurements reveal the interplay of lattice and charge motions in the photoexcited prototype material KDP (KH2PO4) which occur on distinctly different length scales. As a second topic, electron relocations induced by strong external optical fields will be discussed. This interaction mechanism allows for generating coherent superpositions of valence and conduction band quantum states and inducing fully reversible charge dynamics. While the materials LiBH4 and NaBH4 display electron relocations from the (BH4)- ions to the neighboring Li+ and Na+ ions, LiH exhibits an electron transfer from Li to H. The latter is a manifestation of electron correlations and in agreement with theoretical calculations.

  19. Near-UV supercontinua generated in photonic crystal fibers for femtosecond spectroscopy

    NASA Astrophysics Data System (ADS)

    Léonard, J.; Lecong, N.; Likforman, J.-P.; Crégut, O.; Leproux, P.; Couderc, V.; Haacke, S.

    2006-04-01

    We demonstrate the use of broad super-continua generated in photonic crystal fibers (PCFs) for a novel femtosecond absorption pump-probe experiment that records time- and wavelength resolved data. While such experiments relied up to now on amplified sources for the supercontinuum generation, the non-linearities in the microstructured fibers can be induced with a Ti:sapphire oscillator only. We test the performances of such a compact femtosecond spectrometer for the study of molecules in the liquid phase. The aim is to cover the 400-1100 nm spectral range with a single pulse shorter than 200 fs. A commercial Ti:Sapphire oscillator (KM Labs) cavity, delivering 40 fs pulses, has been extended so as to lower the repetition rate (27 MHz) and to increase the pulse energy. Up to 6 nJ are focussed into 8-mm long pieces of commercial (NL-710, Blazephotonics) and home-made PCFs using a microscope objective. The fiber output spectra are measured from 300-1100 nm with a Peltier-cooled CCD (Spec10, Roper Scientific). Most recently, using the fibers produced at XLIM, we have been able to generate a supercontinuum spectrum extending down to 380 nm. While a full characterization of the temporal properties of the home-built fibers is still in progress, we find a single pulse output for the commercial fibers, with negligible chirp for λ= 600-750 nm. Obviously in these short fiber lengths, soliton fission does not take place. With this system the photo-induced dynamics of malachite green have been studied with a noise-floor of 10 -4 relative absorption change.

  20. Photoionization in negative streamers: Fast computations and two propagation modes

    SciTech Connect

    Luque, Alejandro; Ebert, Ute; Montijn, Carolynne; Hundsdorfer, Willem

    2007-02-19

    Streamer discharges play a central role in electric breakdown of matter in pulsed electric fields, both in nature and in technology. Reliable and fast computations of the minimal model for negative streamers in simple gases such as nitrogen have recently been developed. However, photoionization was not included; it is important in air and poses a major numerical challenge. The authors here introduce a fast and reliable method to include photoionization into our numerical scheme with adaptive grids, and they discuss its importance for negative streamers. In particular, they identify different propagation regimes where photoionization does or does not play a role.0.

  1. Absorption spectroscopy of a laboratory photoionized plasma experiment at Z

    SciTech Connect

    Hall, I. M.; Durmaz, T.; Mancini, R. C.; Bailey, J. E.; Rochau, G. A.; Golovkin, I. E.; MacFarlane, J. J.

    2014-03-15

    The Z facility at the Sandia National Laboratories is the most energetic terrestrial source of X-rays and provides an opportunity to produce photoionized plasmas in a relatively well characterised radiation environment. We use detailed atomic-kinetic and spectral simulations to analyze the absorption spectra of a photoionized neon plasma driven by the x-ray flux from a z-pinch. The broadband x-ray flux both photoionizes and backlights the plasma. In particular, we focus on extracting the charge state distribution of the plasma and the characteristics of the radiation field driving the plasma in order to estimate the ionisation parameter.

  2. Terahertz radiation driven by two-color laser pulses at near-relativistic intensities: Competition between photoionization and wakefield effects

    NASA Astrophysics Data System (ADS)

    González de Alaiza Martínez, P.; Davoine, X.; Debayle, A.; Gremillet, L.; Bergé, L.

    2016-06-01

    We numerically investigate terahertz (THz) pulse generation by linearly-polarized, two-color femtosecond laser pulses in highly-ionized argon. Major processes consist of tunneling photoionization and ponderomotive forces associated with transverse and longitudinal field excitations. By means of two-dimensional particle-in-cell (PIC) simulations, we reveal the importance of photocurrent mechanisms besides transverse and longitudinal plasma waves for laser intensities >1015 W/cm2. We demonstrate the following. (i) With two-color pulses, photoionization prevails in the generation of GV/m THz fields up to 1017 W/cm2 laser intensities and suddenly loses efficiency near the relativistic threshold, as the outermost electron shell of ionized Ar atoms has been fully depleted. (ii) PIC results can be explained by a one-dimensional Maxwell-fluid model and its semi-analytical solutions, offering the first unified description of the main THz sources created in plasmas. (iii) The THz power emitted outside the plasma channel mostly originates from the transverse currents.

  3. Communication: Ultrafast time-resolved ion photofragmentation spectroscopy of photoionization-induced proton transfer in phenol-ammonia complex

    SciTech Connect

    Shen, Ching-Chi; Tsai, Tsung-Ting; Ho, Jr-Wei; Chen, Yi-Wei; Cheng, Po-Yuan

    2014-11-07

    Photoionization-induced proton transfer (PT) in phenol-ammonia (PhOH-NH{sub 3}) complex has been studied using ultrafast time-resolved ion photofragmentation spectroscopy. Neutral PhOH-NH{sub 3} complexes prepared in a free jet are photoionized by femtosecond [1+1] resonance-enhanced multiphoton ionization via the S{sub 1} state, and the subsequent dynamics occurring in the cations is probed by delayed pulses that result in ion fragmentation. The observed temporal evolutions of the photofragmentation spectra are consistent with an intracomplex PT reaction. The experiments revealed that PT in [PhOH-NH{sub 3}]{sup +} cation proceeds in two distinct steps: an initial impulsive wave-packet motion in ∼70 fs followed by a slower relaxation of about 1 ps that stabilizes the system into the final PT configuration. These results indicate that for a barrierless PT system, even though the initial PT motions are impulsive and ultrafast, the reaction may take a much longer time scale to complete.

  4. Terahertz radiation driven by two-color laser pulses at near-relativistic intensities: Competition between photoionization and wakefield effects

    PubMed Central

    González de Alaiza Martínez, P.; Davoine, X.; Debayle, A.; Gremillet, L.; Bergé, L.

    2016-01-01

    We numerically investigate terahertz (THz) pulse generation by linearly-polarized, two-color femtosecond laser pulses in highly-ionized argon. Major processes consist of tunneling photoionization and ponderomotive forces associated with transverse and longitudinal field excitations. By means of two-dimensional particle-in-cell (PIC) simulations, we reveal the importance of photocurrent mechanisms besides transverse and longitudinal plasma waves for laser intensities >1015 W/cm2. We demonstrate the following. (i) With two-color pulses, photoionization prevails in the generation of GV/m THz fields up to 1017 W/cm2 laser intensities and suddenly loses efficiency near the relativistic threshold, as the outermost electron shell of ionized Ar atoms has been fully depleted. (ii) PIC results can be explained by a one-dimensional Maxwell-fluid model and its semi-analytical solutions, offering the first unified description of the main THz sources created in plasmas. (iii) The THz power emitted outside the plasma channel mostly originates from the transverse currents. PMID:27255689

  5. Terahertz radiation driven by two-color laser pulses at near-relativistic intensities: Competition between photoionization and wakefield effects.

    PubMed

    González de Alaiza Martínez, P; Davoine, X; Debayle, A; Gremillet, L; Bergé, L

    2016-01-01

    We numerically investigate terahertz (THz) pulse generation by linearly-polarized, two-color femtosecond laser pulses in highly-ionized argon. Major processes consist of tunneling photoionization and ponderomotive forces associated with transverse and longitudinal field excitations. By means of two-dimensional particle-in-cell (PIC) simulations, we reveal the importance of photocurrent mechanisms besides transverse and longitudinal plasma waves for laser intensities >10(15) W/cm(2). We demonstrate the following. (i) With two-color pulses, photoionization prevails in the generation of GV/m THz fields up to 10(17) W/cm(2) laser intensities and suddenly loses efficiency near the relativistic threshold, as the outermost electron shell of ionized Ar atoms has been fully depleted. (ii) PIC results can be explained by a one-dimensional Maxwell-fluid model and its semi-analytical solutions, offering the first unified description of the main THz sources created in plasmas. (iii) The THz power emitted outside the plasma channel mostly originates from the transverse currents. PMID:27255689

  6. Nonlinear femtosecond near infrared laser structuring in oxide glasses

    NASA Astrophysics Data System (ADS)

    Royon, Arnaud

    nonlinear third-order susceptibility properties have been measured. Moreover, the structuring of fused silica at the subwavelength scale into "nanogratings" is observed and the form of birefringence induced by these structures is discussed. In addition to the fused silica samples, several oxide glasses presenting very distinct chemical compositions have been studied. A sodium-borophosphate glass containing niobium oxide exhibits micro-cracks and nano-crystallites following irradiation. A silicate glass with or without a silver component reveals fluorescent rings or "nanograting" structures. A zinc phosphate glass containing silver also presents fluorescent ring structures, with a size of the order of 80 nm, well below the diffraction limit. Pump-probe microscope techniques have been performed on this glass to investigate the laser-glass interaction. The absorption mechanism is determined to be four-photon absorption. The generated free electron density is ˜ 1017 cm-3, which suggests the conclusion that an electron gas rather than a plasma is formed during the laser irradiation.

  7. Ionization Correction Factors based on CALIFA photoionization models

    NASA Astrophysics Data System (ADS)

    Delgado-Inglada, G.; Morisset, C.; Sánchez, S.; Califa Collaboration

    2016-06-01

    We use a grid of photoionization models (especially constructed to reproduce the observations of ~5200 H II regions from the CALIFA survey) to explore the ionization correction factors usually adopted to calculate total element abundances.

  8. Photoionization of potassium atoms from the ground and excited states

    SciTech Connect

    Zatsarinny, O.; Tayal, S. S.

    2010-04-15

    The Dirac-based B-spline R-matrix method is used to investigate the photoionization of atomic potassium from the 4s ground and 4p, 5s-7s, 3d-5d excited states. The effect of the core polarization by the outer electron is included through the polarized pseudostates. Besides the dipole core polarization, we also found a noticeable influence of the quadrupole core polarization. We obtained excellent agreement with experiment for cross sections of the 4s photoionization, including accurate description of the near-threshold Cooper-Seaton minimum. We also obtained close agreement with experiment for the 4p photoionization, but there are unexpectedly large discrepancies with available experimental data for photoionization of the 5d and 7s excited states.

  9. Shape resonant features in the photoionization spectra of NO

    SciTech Connect

    Wallace, Scott; Dill, Dan; Dehmer, Joseph L.

    1982-01-01

    Calculations of core and valence level photoionization spectra of NO are presented and compared with available experimental data. A low-lying continuum shape resonance is identified in the sigma photoionization channel, which is the analog of similar states found in other first-row diatomic molecules. Both partial cross sections and photoelectron angular distributions are discussed, and the effect of nuclear motion on these observables is treated.

  10. Photoionization and photoelectron spectroscopy of doped helium nanodroplets

    NASA Astrophysics Data System (ADS)

    Neumark, Daniel

    2006-03-01

    Photoionization and photoelectron spectra for helium nanodroplets doped with rare gas atoms and SF6 will be reported. The experiments were conducted using tunable synchrotron radiation at the Advanced Light Source in the photon energy range of 14-26 eV. Time-of-flight mass spectra will be presented, along with photoion and photoelectron images. The results will be compared to previous electron impact ionization data.

  11. Photoionization of noble-gas atoms by ultrashort electromagnetic pulses

    SciTech Connect

    Astapenko, V. A. Svita, S. Yu.

    2014-11-15

    The photoionization of atoms of noble gases (Ar, Kr, and Xe) by ultrashort electromagnetic pulses of a corrected Gaussian shape is studied theoretically. Computations are performed in the context of perturbation theory using a simple expression for the total probability of photoionization of an atom by electromagnetic pulses. The features of this process are revealed and analyzed for various ranges of the parameters of the problem.

  12. Outer-shell double photoionization of CH2Cl2

    NASA Astrophysics Data System (ADS)

    Alcantara, K. F.; Gomes, A. H. A.; Wolff, W.; Sigaud, L.; Santos, A. C. F.

    2014-01-01

    In this work the roles of the shake-off and knockout processes in the double photoionization of the CH2Cl2 molecule have been studied. The probabilities for both mechanisms accompanying valence-shell photoionization have been estimated as a function of incident photon energy using Samson's (1990) [5] and Thomas's (1994) [3] models, respectively. The experimental results are in qualitative accord with the models.

  13. K-shell photoionization of Li-like Ti XX

    NASA Astrophysics Data System (ADS)

    Liang, Liang; Lu, Xu-yang; Zhou, Chao; Qing, Pang

    2015-04-01

    K-shell photoionization of Li-like Ti XX ions from ground state and first excited state has been studied using the R-matrix method. Through the combination of R-matrix and QB methods, we have not only studied the K-shell photoionization cross section between the first and ninth ionization threshold of Ti XX, but also identified the energy levels of K-shell excited state due to the twelve autoionization Rydberg series.

  14. CdS and Cd-Free Buffer Layers on Solution Phase Grown Cu2ZnSn(SxSe1- x)4 :Band Alignments and Electronic Structure Determined with Femtosecond Ultraviolet Photoemission Spectroscopy

    SciTech Connect

    Haight, Richard; Barkhouse, Aaron; Wang, Wei; Yu, Luo; Shao, Xiaoyan; Mitzi, David; Hiroi, Homare; Sugimoto, Hiroki

    2013-12-02

    The heterojunctions formed between solution phase grown Cu2ZnSn(SxSe1- x)4(CZTS,Se) and a number of important buffer materials including CdS, ZnS, ZnO, and In2S3, were studied using femtosecond ultraviolet photoemission spectroscopy (fs-UPS) and photovoltage spectroscopy. With this approach we extract the magnitude and direction of the CZTS,Se band bending, locate the Fermi level within the band gaps of absorber and buffer and measure the absorber/buffer band offsets under flatband conditions. We will also discuss two-color pump/probe experiments in which the band bending in the buffer layer can be independently determined. Finally, studies of the bare CZTS,Se surface will be discussed including our observation of mid-gap Fermi level pinning and its relation to Voc limitations and bulk defects.

  15. Model propagation of a femtosecond laser radiation in the vitreous of the human eye

    NASA Astrophysics Data System (ADS)

    Rogov, P. Y.; Bespalov, V. G.

    2016-04-01

    The paper presents a mathematical model of linear and nonlinear processes occurring due to propagation of femtosecond laser pulses in vitreous of the human eye. By methods of numerical simulation, we have solved a nonlinear spectral equation describing dynamics of two-dimensional TE-polarized radiation. The solution was performed in a homogeneous isotropic medium with instantaneous cubic nonlinearity without using slowly varying envelope approximation. For simulation we used medium with parameters close to the optical media of the eye. The model of femtosecond radiation takes into account the dynamics of the process of dispersion pulse broadening in time and occurrence of self-focusing of the retina when passing through vitreous body of the eye. The dependence between pulse duration on the retina and duration of the input pulse was found, as well as the values of power density at which self-focusing occurs. It was shown that the main mechanism of radiation damage caused while using Ti-sapphire laser is photoionization. The results coincide with the results obtained by other scientists. They can be used to create Russian laser safety standards for femtosecond laser systems.

  16. Dynamics of photoprocesses induced by femtosecond infrared radiation in free molecules and clusters of iron pentacarbonyl

    NASA Astrophysics Data System (ADS)

    Kompanets, V. O.; Lokhman, V. N.; Poydashev, D. G.; Chekalin, S. V.; Ryabov, E. A.

    2016-04-01

    The dynamics of photoprocesses induced by femtosecond infrared radiation in free Fe(CO)5 molecules and their clusters owing to the resonant excitation of vibrations of CO bonds in the 5-μm range has been studied. The technique of infrared excitation and photoionization probing (λ = 400 nm) by femtosecond pulses has been used in combination with time-of-flight mass spectrometry. It has been found that an infrared pulse selectively excites vibrations of CO bonds in free molecules, which results in a decrease in the yield of the Fe(CO)5 + molecular ion. Subsequent relaxation processes have been analyzed and the results have been interpreted. The time of the energy transfer from excited vibrations to other vibrations of the molecule owing to intramolecular relaxation has been measured. The dynamics of dissociation of [Fe(CO)5] n clusters irradiated by femtosecond infrared radiation has been studied. The time dependence of the yield of free molecules has been measured under different infrared laser excitation conditions. We have proposed a model that well describes the results of the experiment and makes it possible, in particular, to calculate the profile of variation of the temperature of clusters within the "evaporation ensemble" concept. The intramolecular and intracluster vibrational relaxation rates in [Fe(CO)5] n clusters have been estimated.

  17. Absolute photoionization cross-section of the methyl radical.

    SciTech Connect

    Taatjes, C. A.; Osborn, D. L.; Selby, T.; Meloni, G.; Fan, H.; Pratt, S. T.; Chemical Sciences and Engineering Division; SNL

    2008-01-01

    The absolute photoionization cross-section of the methyl radical has been measured using two completely independent methods. The CH{sub 3} photoionization cross-section was determined relative to that of acetone and methyl vinyl ketone at photon energies of 10.2 and 11.0 eV by using a pulsed laser-photolysis/time-resolved synchrotron photoionization mass spectrometry method. The time-resolved depletion of the acetone or methyl vinyl ketone precursor and the production of methyl radicals following 193 nm photolysis are monitored simultaneously by using time-resolved synchrotron photoionization mass spectrometry. Comparison of the initial methyl signal with the decrease in precursor signal, in combination with previously measured absolute photoionization cross-sections of the precursors, yields the absolute photoionization cross-section of the methyl radical; {sigma}{sub CH}(10.2 eV) = (5.7 {+-} 0.9) x 10{sup -18} cm{sup 2} and {sigma}{sub CH{sub 3}}(11.0 eV) = (6.0 {+-} 2.0) x 10{sup -18} cm{sup 2}. The photoionization cross-section for vinyl radical determined by photolysis of methyl vinyl ketone is in good agreement with previous measurements. The methyl radical photoionization cross-section was also independently measured relative to that of the iodine atom by comparison of ionization signals from CH{sub 3} and I fragments following 266 nm photolysis of methyl iodide in a molecular-beam ion-imaging apparatus. These measurements gave a cross-section of (5.4 {+-} 2.0) x 10{sup -18} cm{sup 2} at 10.460 eV, (5.5 {+-} 2.0) x 10{sup -18} cm{sup 2} at 10.466 eV, and (4.9 {+-} 2.0) x 10{sup -18} cm{sup 2} at 10.471 eV. The measurements allow relative photoionization efficiency spectra of methyl radical to be placed on an absolute scale and will facilitate quantitative measurements of methyl concentrations by photoionization mass spectrometry.

  18. Photoabsorption and photoionization of chlorine dioxide

    SciTech Connect

    Flesch, R.; Ruehl, E.; Hottmann, K.; Baumgaertel, H. )

    1993-01-28

    Photoprocesses of chlorine dioxide in the near-UV have become highly important for stratospheric photoprocesses at high latitudes, especially in Antarctica. Chlorine dioxide has been identified among other absorbers because of its specific absorption cross section in the near-UV. Possible contributions of chlorine dioxide photochemistry to polar ozone depletion have been discussed recently. The high-resolution He I photoelectron spectrum and the absolute (vacuum-UV) absorption cross section (6-25 eV) as well as the ionic fragmentation of chlorine dioxide (OCIO) are reported. The photoelectron spectrum is interpreted in terms of exchange splitting effects of the various singlet and triplet cation states as well as by comparison to chemically related molecules. The vacuum-UV absorption spectrum shows different Rydberg series converging to the cation states. These Rydberg series and their vibrational progressions are assigned by term value arguments, dipole selection rules, and comparison with the photoelectron spectrum. Photoionization mass spectrometry is used for measurements of the ionization and fragmentation threshold of OCIO. The major fragment is ClO[sup +] which occurs above 13.4 eV. Thermomechanical data such as heats of formation and bond dissociation energies are derived. No evidence for isomerization of OClO[sup +] is found, as observed for the electronically excited neutral molecule. 54 refs., 6 figs., 7 tabs.

  19. Vacuum ultraviolet photoionization of carbohydrates and nucleotides.

    PubMed

    Shin, Joong-Won; Bernstein, Elliot R

    2014-01-28

    Carbohydrates (2-deoxyribose, ribose, and xylose) and nucleotides (adenosine-, cytidine-, guanosine-, and uridine-5(')-monophosphate) are generated in the gas phase, and ionized with vacuum ultraviolet photons (VUV, 118.2 nm). The observed time of flight mass spectra of the carbohydrate fragmentation are similar to those observed [J.-W. Shin, F. Dong, M. Grisham, J. J. Rocca, and E. R. Bernstein, Chem. Phys. Lett. 506, 161 (2011)] for 46.9 nm photon ionization, but with more intensity in higher mass fragment ions. The tendency of carbohydrate ions to fragment extensively following ionization seemingly suggests that nucleic acids might undergo radiation damage as a result of carbohydrate, rather than nucleobase fragmentation. VUV photoionization of nucleotides (monophosphate-carbohydrate-nucleobase), however, shows that the carbohydrate-nucleobase bond is the primary fragmentation site for these species. Density functional theory (DFT) calculations indicate that the removed carbohydrate electrons by the 118.2 nm photons are associated with endocyclic C-C and C-O ring centered orbitals: loss of electron density in the ring bonds of the nascent ion can thus account for the observed fragmentation patterns following carbohydrate ionization. DFT calculations also indicate that electrons removed from nucleotides under these same conditions are associated with orbitals involved with the nucleobase-saccharide linkage electron density. The calculations give a general mechanism and explanation of the experimental results. PMID:25669546

  20. Coherent control of photoionization of atomic barium

    NASA Astrophysics Data System (ADS)

    Yamazaki, Rekishu

    We present the results of our study on coherent control of photoionization of atomic barium. Our study focused on the understanding of the controllability, especially due to the effect of the coherent interaction between the atomic system and the laser field. The first half of the study investigates the mechanisms of the control behind the previously observed laser phase-insensitive product state control. The controllability of this excitation scheme, two-color two-photon resonantly enhanced excitation, was analyzed from two aspects, the role of ac Stark shift introduced by the strong laser field and the multi-pathway quantum mechanical interferences. We have analyzed the excitation scheme from the analysis of the photoelectron angular distribution measured using the excitation scheme and the monitoring of the intermediate state population. Analysis of the data as well as the numerical simulation showed clear understanding of the role of two mechanisms in the product state control reported. We also investigated the control of the phase lag during the product state control. We conducted the control of the phase lag in the study of asymmetric photoelectron angular distribution, which arises from the concurrent even-odd parity outgoing electron wave excitation. The phase lag was controlled in full range, 2pi, and the results were analyzed in terms of the role of autoionizing resonance structures as well as the nature of outgoing electron waves at different locations of the autoionizing resonances.

  1. Vacuum ultraviolet photoionization of carbohydrates and nucleotides

    SciTech Connect

    Shin, Joong-Won; Bernstein, Elliot R.

    2014-01-28

    Carbohydrates (2-deoxyribose, ribose, and xylose) and nucleotides (adenosine-, cytidine-, guanosine-, and uridine-5{sup ′}-monophosphate) are generated in the gas phase, and ionized with vacuum ultraviolet photons (VUV, 118.2 nm). The observed time of flight mass spectra of the carbohydrate fragmentation are similar to those observed [J.-W. Shin, F. Dong, M. Grisham, J. J. Rocca, and E. R. Bernstein, Chem. Phys. Lett. 506, 161 (2011)] for 46.9 nm photon ionization, but with more intensity in higher mass fragment ions. The tendency of carbohydrate ions to fragment extensively following ionization seemingly suggests that nucleic acids might undergo radiation damage as a result of carbohydrate, rather than nucleobase fragmentation. VUV photoionization of nucleotides (monophosphate-carbohydrate-nucleobase), however, shows that the carbohydrate-nucleobase bond is the primary fragmentation site for these species. Density functional theory (DFT) calculations indicate that the removed carbohydrate electrons by the 118.2 nm photons are associated with endocyclic C–C and C–O ring centered orbitals: loss of electron density in the ring bonds of the nascent ion can thus account for the observed fragmentation patterns following carbohydrate ionization. DFT calculations also indicate that electrons removed from nucleotides under these same conditions are associated with orbitals involved with the nucleobase-saccharide linkage electron density. The calculations give a general mechanism and explanation of the experimental results.

  2. Femtosecond tunable light source

    NASA Astrophysics Data System (ADS)

    Miesak, Edward Jozef

    1999-09-01

    A practical source of continuously tunable coherent visible and infrared light would have an enormous impact on science, medicine and technology. While microwave and radio transmitters offer wide tunability at the ``turn of a knob,'' the best known source of coherent optical radiation, the laser, does not possess the same versatility. Dye lasers provide some degree of tunability, but many dyes are needed to cover even the visible region. Ti:sapphire lasers are tunable only over the red to near infra-red portion of the spectrum (about 65 0 nm to about 1.1μm). This presentation documents the development of a unique pulsed light source tunable across the visible and near infrared portion of the spectrum, a femtosecond optical parametric amplifier (OPA). Much work was expended in developing the system itself. But a great deal of work was also done in developing the support equipment (hardware and software) necessary to build as well as maintain and operate an OPA. Once completed, the system characteristics were measured and documented. Initially it possessed ``personality'' which had to be understood and removed as much as possible. In addition, the pump source for this OPA, a regenerative amplifier, is unique in that it uses Cr3+:LiSGaF as the gain medium. This regen was also characterized and compared to other more standard regenerative amplifiers. System verification was done by performing a standard experiment (Z-scan) on well known samples, several of which are well characterized at specific wavelengths (1.06 μm, 0.523 μm) in the nanosecond and picosecond regimes. The results were compared against previously published results. The OPA was also compared against another very similar system which became commercially available during the time of this research. The results were helpful in analyzing the light source(s) and data acquisition systems for areas that could be improved.

  3. Holographic vector-wave femtosecond laser processing

    NASA Astrophysics Data System (ADS)

    Hayasaki, Yoshio; Hasegawa, Satoshi

    2016-03-01

    Arbitrary and variable beam shaping of femtosecond pulses by a computer-generated hologram (CGH) displayed on a spatial light modulator (SLM) have been applied to femtosecond laser processing. The holographic femtosecond laser processing has been widely used in many applications such as two-photon polymerization, optical waveguide fabrication, fabrication of volume phase gratings in polymers, and surface nanostructuring. A vector wave that has a spatial distribution of polarization states control of femtosecond pulses gives good performances for the femtosecond laser processing. In this paper, an in- system optimization of a CGH for massively-parallel femtosecond laser processing, a dynamic control of spatial spectral dispersion to improve the focal spot shape, and the holographic vector-wave femtosecond laser processing are demonstrated.

  4. EMISSION SPECTRUM OF HELIUM-LIKE IONS IN PHOTOIONIZED PLASMAS

    SciTech Connect

    Wang, Feilu; Salzmann, David; Zhao, Gang; Takabe, Hideaki

    2012-10-01

    The aim of the present paper is to investigate the influence of inner-shell photoionization and photoexcitation on He{sub {alpha}} and its satellite's spectra in photoionized plasmas. An analysis is carried out on the relative importance of the various atomic processes in photoionized plasmas as a function of the electron temperature and irradiation conditions. In particular, we investigate the influence of K-shell photoionization of Li-like ions on the He{sub {alpha}} spectrum and of Be-like ions on the He{sub {alpha}} satellites. It is found that in photoionized plasmas these inner-shell processes contribute significantly under low radiation temperature and/or intensity, when Li- and Be-like ions are highly abundant but highly ionized H-like ions are rare. A short discussion is presented about the parameter space in which the excited 1s2p state has statistical or non-statistical distributions, and how such distributions affect the emission spectrum.

  5. Near-Threshold, Vibrationally-Resolved Photoionization of Molecular Nitrogen

    NASA Astrophysics Data System (ADS)

    Vangyseghem, Gaetan; Gorczyca, Thomas; Ballance, Connor

    2016-05-01

    Photoionization of molecular nitrogen N2 is investigated near the first ionization threshold using an R-matrix, multi-channel quantum defect theory (MQDT) approach. Building on an existing fixed-nuclei R-matrix photoionization model, which, in turn, is built on the UKRmol suite of codes, photoionization cross sections, as well as scattering and dipole matrices, are computed in the Born-Oppenheimer approximation. By varying the internuclear separation, potential energy curves have been constructed for the N2 and N 2 + states and compared to quantum chemistry calculations. Using these fixed-nuclei potential energy curves, and corresponding vibronic eigenenergies and eigenfunctions, a frame transformation is enacted on the fixed-nuclei scattering and dipole matrices, allowing for the calculation of vibrationally-resolved photoionization cross sections. The resultant photoionization cross sections are compared to high-resolution experimental data near threshold, a region complicated by multiple vibrationally-resolved, interacting Rydberg series.

  6. Photoionization of Ar2 at high resolution

    SciTech Connect

    Dehmer, Patricia M.

    1982-01-01

    The relative photoionization cross section of Ar2 was determined at a resolution of 0.07 Â in the wavelength region from 800 to 850 Â using a new photoionization mass spectrometer that combines a high intensity helium continuum lamp with a free supersonic molecular beam source. In the region studied, the photoionization cross section is dominated by autoionization of molecular Rydberg states, and the structure is diffuse owing to the combined effects of autoionization and predissociation. The molecular photoionization spectrum is extremely complex and shows little resemblence either to the corresponding atomic spectrum (indicating that the spectrum of the dimer is not simply a perturbed atomic spectrum) or to the molecular absorption spectrum at longer wavelengths. The regular vibrational progressions seen at longer wavelengths are absent above the first ionization potential. Detailed spectroscopic analysis is possible for only a small fraction of the observed features; however, vibrational intervals of 50--100 cm⁻¹ suggest that some of the Rydberg states have B ²Π3/2g ionic cores. A comparison of the absorption and photoionization spectra shows that, at wavelengths shorter than -835 Â, many of the excited states decay via mechanisms other than autoionization

  7. Photoionization of Highly Charged Argon Ions and Their Diagnostic Lines

    NASA Astrophysics Data System (ADS)

    Nahar, Sultana N.

    2012-06-01

    %TEXT OF YOUR ABSTRACT Lines of highly charged He-like and Li-like ions in the ultraviolet and X-ray regions provide useful diagnostics for the physical and chemical conditions of the astrophysical as well as fusion plasmas. For example, Ar XVII lines in a Syfert galaxy have been measured by the X-ray space observatory Chandra. Results on photoionization of Ar XVI and Ar XVII obtained from relativistic Breit-Pauli R-matrix method and close-coupling approximation will be presented. Important features for level-specific photoionization for the diagnostic w, x, y, z lines of He-like Ar XVII in the ultraviolet region will be illustrated. Although monotonous decay dominates the low energy photoionization for these ions, strong resonances appear in the high energy region indicating higher recombination, inverse process of photoionization, at high temperature. The spectra of the well known 22 diagnostics dielectronic satellite lines of Li-like Ar XVI will be shown produced from the the KLL resonances in photoionization. Acknowledgement: Partially supported by DOE, NSF; Computational work was carried out at the Ohio Supercomputer Center

  8. Development and demonstration of table-top synchronized fast-scan femtosecond time-resolved spectroscopy system by single-shot scan photo detector array

    NASA Astrophysics Data System (ADS)

    Yabushita, Atsushi; Kao, Chih-Hsien; Lee, Yu-Hsien; Kobayashi, Takayoshi

    2015-07-01

    Ultrafast dynamics is generally studied by pump-probe method with laser pulse, which scans optical delay by motorized stage step by step. Using ultrashort laser pulse shorter than typical molecular vibration periods, the pump-probe measurement can study both of electronic dynamics and vibration dynamics simultaneously. The probe wavelength dependence of the ultrafast electronic and vibration dynamics (UEVD) helps us to distinguish the signal contributions from the dynamics of the electronic ground state and that of the electronic excited states, which elucidates primary reaction mechanism after photoexcitation. Meanwhile, the measurement time of UEVD spectroscopy takes too long time to be used in realistic application. In our previous work, we have developed multi-channel lock-in amplifying (MLA) detectors to study UEVD at all probe wavelengths simultaneously, and synchronized it with laser and fast-scan delay stage to scan the data in five seconds. It enabled us to study UEVD spectroscopy even for photo-fragile materials. However, the home-made MLA detectors required for the measurement is expensive and massive in size and weight, thus not suitable for general researchers in the field of ultrafast time-resolved spectroscopy. In the present work, we have developed a table-top synchronized fast-scan femtosecond time-resolved spectroscopy system using single shot scan line CCD. This system measures time-resolved trace at all probe wavelengths simultaneously in five seconds. The CCD-based fast-scan time-resolved spectroscopy system enables us to study ultrafast dynamics of various materials even biomaterials, which have been thought to be hard or even impossible to be studied in previous methods.

  9. Rotational Doppler effect in x-ray photoionization

    SciTech Connect

    Sun Yuping; Wang Chuankui; Gel'mukhanov, Faris

    2010-11-15

    The energy of the photoelectron experiences a red or blue Doppler shift when the molecule recedes from the detector or approaches him. This results in a broadening of the photoelectron line due to the translational thermal motion. However, the molecules also have rotational degrees of freedom and we show that the translational Doppler effect has its rotational counterpart. This rotational Doppler effect leads to an additional broadening of the spectral line of the same magnitude as the Doppler broadening caused by translational thermal motion. The rotational Doppler broadening as well as the rotational recoil broadening is sensitive to the molecular orbital from which the photoelectron is ejected. This broadening should be taken into account in analysis of x-ray photoemission spectra of super-high resolution and it can be directly observed using x-ray pump-probe spectroscopy.

  10. Mid-infrared ultrafast laser pulses induced third harmonic generation in nitrogen molecules on an excited state

    PubMed Central

    Xie, Hongqiang; Li, Guihua; Yao, Jinping; Chu, Wei; Li, Ziting; Zeng, Bin; Wang, Zhanshan; Cheng, Ya

    2015-01-01

    We report on generation of third harmonic from nitrogen molecules on the excited state with a weak driver laser pulse at a mid-infrared wavelength. The excited nitrogen molecules are generated using a circularly polarized intense femtosecond pulse which produces energetic electrons by photoionization to realize collisional excitation of nitrogen molecules. Furthermore, since the third harmonic is generated using a pump-probe scheme, it enables investigation of the excited-state dynamics of nitrogen molecules produced under different conditions. We also perform a comparative investigation in excited argon atoms, revealing different decay dynamics of the molecules and atoms from the excited states in femtosecond laser induced filaments. PMID:26522886

  11. Development and Implementation of an Ultrafast Vacuum-UV (8eV) Light Source for use in UV-VUV Pump Probe Experiments of Neutral Excited State Dynamics

    NASA Astrophysics Data System (ADS)

    Liu, Yusong; Horton, Spencer; Matsika, Spiridoula; Weinacht, Thomas

    2016-05-01

    Probing neutral excited state dynamics in polyatomic molecules with ultrafast laser systems enables us to study phenomena such as internal conversion, isomerization, intersystem crossing, and dissociation. Using the third harmonic (260 nm) and the fifth harmonic (156 nm) of our laser system we have developed an apparatus to perform pump-probe experiments for the study neutral excited state dynamics in various polyatomic molecules. The fifth harmonic of our laser system is generated through the four-wave-mixing process of k5 ω = 2k3 ω -kω performed with a non-collinear geometry in an argon gas cell. In several polyatomic molecular systems of interest a photon with 8 eV of energy gives us the unique ability to ionize from essentially anywhere along the excited state potential, but does not produce any ionization yield from the ground state. This enables us to measure excited state lifetimes without the photon energy becoming too low to ionize while the nuclear wave-packet is traveling on the excited state potential. We also have the advantage of working in the perturbative weak-field ionization regime. These experiments can also be directly compare to strong-field ionization experiments conducted with a UV-pump and an IR-probe conducted on the same molecules.

  12. Deuteration Effect Study on the Vibrational Dynamics of Phenol and Phenol-Water Complex by Picosecond Time-Resolved Ir-Uv Pump-Probe Spectroscopy in a Supersonic Molecular Beam

    NASA Astrophysics Data System (ADS)

    Miyazaki, Yasunori; Inokuchi, Yoshiya; Ebata, Takayuki

    2012-06-01

    The vibrational energy relaxations of the OH and OD stretch of phenol-d_0 and phenol-d_0-(H_2O) complex and phenol-d_1 and phenol-d_1-(D_2O) complex, respectively, are investigated by picosecond IR-UV pump-probe spectroscopy. The key to understand their dynamic is well-suited to a two-step Tier model. For phenol-d_0, an energy flow is described by the intramolecularVR steps: "OH stretching level" → "doorway state" → "bath state". The intramolecularVR lifetime of phenol-d_0 is obtained to be 14 ps. On the other hand, the OD stretching vibration of phenol-d_1 exhibits quantum beats, followed by the intramolecularVR with a lifetime of 90 ps. In contrast, for the phenol-water complex, the intramolecularVR lifetime of OH(OD) stretch becomes 4.3 ps(12 ps) and an energy flow is described by the intramolecular and intermolecular processes, which lead to VP (vibratinal predisocciation). Although the energy difference is 1000 cm-1, no remarkable change of intermolecularVR and VP lifetimes is found in the hydrogen-bonded phenol-water complexes.

  13. Understanding photoexcitation dynamics in a three-step photoionization of atomic uranium and measurement of photoexcitation and photoionization cross sections

    NASA Astrophysics Data System (ADS)

    Mandal, P. K.; Sahoo, A. C.; Das, R. C.; Shah, M. L.; Pulhani, A. K.; Manohar, K. G.; Dev, Vas

    2015-09-01

    Photoexcitation dynamics in a three-step photoionization of atomic uranium has been investigated using time-resolved two-color three-photon and delayed three-color three-photon photoionization signals. Investigations are carried out in an atomic beam of uranium coupled to a high-resolution time-of-flight mass spectrometer using three tunable pulsed dye lasers. Dependence of both the signals on the second-step laser photon fluence is studied. Excited-level-to-excited-level photoexcitation cross section and photoionization cross section from the second excited level are simultaneously determined by analyzing the two-color three-photon and three-color three-photon photoionization signals using population rate equation model. Using this methodology, photoexcitation and photoionization cross sections at seven values of the second-step laser wavelength have been measured. From the measured values of the photoexcitation cross sections, we have obtained excited-level-to-excited-level transition probabilities and compared these with the values reported in the literature.

  14. Efficient photoionization loading of trapped ions with ultrafast pulses

    SciTech Connect

    Deslauriers, L.; Acton, M.; Blinov, B. B.; Brickman, K.-A.; Haljan, P. C.; Hensinger, W. K.; Hucul, D.; Katnik, S.; Kohn, R. N. Jr.; Lee, P. J.; Madsen, M. J.; Maunz, P.; Olmschenk, S.; Moehring, D. L.; Stick, D.; Sterk, J.; Yeo, M.; Younge, K. C.; Monroe, C.

    2006-12-15

    Atomic cadmium ions are loaded into radiofrequency ion traps by photoionization of atoms in a cadmium vapor with ultrafast laser pulses. The photoionization is driven through an intermediate atomic resonance with a frequency-quadrupled mode-locked Ti:sapphire laser that produces pulses of either 100-fs or 1-ps duration at a central wavelength of 229 nm. The large bandwidth of the pulses photoionizes all velocity classes of the Cd vapor, resulting in a high loading efficiency compared to previous ion trap loading techniques. Measured loading rates are compared with a simple theoretical model, and we conclude that this technique can potentially ionize every atom traversing the laser beam within the trapping volume. This may allow the operation of ion traps with lower levels of background pressures and less trap electrode surface contamination. The technique and laser system reported here should be applicable to loading most laser-cooled ion species.

  15. O1s photoionization dynamics in oriented NO2

    NASA Astrophysics Data System (ADS)

    Stener, Mauro; Decleva, Piero; Yamazaki, Masakazu; Adachi, Jun-ichi; Yagishita, Akira

    2011-05-01

    We have performed extensive density functional theory (DFT) calculations, partial cross sections, dipole prepared continuum orbitals, dipole amplitudes and phase shifts, asymmetry parameters β, and molecular frame photoelectron angular distributions, to elucidate the O1s photoionization dynamics of NO2 molecule with emphasis on the shape resonances in the O1s ionization continuum. In the shape resonance region, the β parameters and photoelectron angular distributions have been compared with our experimental results. Fairly good agreement between the theory and experiment has confirmed that the DFT level calculations can well describe the photoionization dynamics of the simple molecule such as NO2. Interference due to equivalent atom photoionization is theoretically considered, and the possibility of detection of the effect in the two degenerate channels with different combinations of light polarization and photoemission direction is discussed.

  16. Interchannel coupling effects in the valence photoionization of SF6

    NASA Astrophysics Data System (ADS)

    Jose, Jobin; Lucchese, Robert; Rescigno, Tom

    2014-05-01

    The complex Kohn and polyatomic Schwinger variational techniques have been employed to illustrate the interchannel coupling correlation effects in the valence photoionization dynamics of SF6. Partial photoionization cross sections and asymmetry parameters of six valence subshells (1t1 g, 5t1 u, 1t2 u, 3eg, 1t2 g, 4t1 u) are discussed in the framework of several theoretical and experimental studies. The complex Kohn results are in rather good agreement with experimental results, indicative of the fact that the interchannel coupling effects alter the photoionization dynamics significantly. We find that the dominant effect of interchannel coupling is to reduce the magnitude of shape resonant cross sections near threshold and to induce resonant features in other channels to which resonances are coupled.

  17. Triggering Excimer Lasers by Photoionization from Corona Discharges

    NASA Astrophysics Data System (ADS)

    Xiong, Zhongmin; Duffey, Thomas; Brown, Daniel; Kushner, Mark

    2009-10-01

    High repetition rate ArF (192 nm) excimer lasers are used for photolithography sources in microelectronics fabrication. In highly attaching gas mixtures, preionization is critical to obtaining stable, reproducible glow discharges. Photoionization from a separate corona discharge is one technique for preionization which triggers the subsequent electron avalanche between the main electrodes. Photoionization triggering of an ArF excimer laser sustained in multi-atmosphere Ne/Ar/F2/Xe gas mixtures has been investigated using a 2-dimensional plasma hydrodynamics model including radiation transport. Continuity equations for charged and neutral species, and Poisson's equation are solved coincident with the electron temperature with transport coefficients obtained from solutions of Boltzmann's equation. Photoionizing radiation is produced by a surface discharge which propagates along a corona-bar located adjacent to the discharge electrodes. The consequences of pulse power waveform, corona bar location, capacitance and gas mixture on uniformity, symmetry and gain of the avalanche discharge will be discussed.

  18. Efficient photoionization loading of trapped ions with ultrafast pulses

    NASA Astrophysics Data System (ADS)

    Deslauriers, L.; Acton, M.; Blinov, B. B.; Brickman, K.-A.; Haljan, P. C.; Hensinger, W. K.; Hucul, D.; Katnik, S.; Kohn, R. N., Jr.; Lee, P. J.; Madsen, M. J.; Maunz, P.; Olmschenk, S.; Moehring, D. L.; Stick, D.; Sterk, J.; Yeo, M.; Younge, K. C.; Monroe, C.

    2006-12-01

    Atomic cadmium ions are loaded into radiofrequency ion traps by photoionization of atoms in a cadmium vapor with ultrafast laser pulses. The photoionization is driven through an intermediate atomic resonance with a frequency-quadrupled mode-locked Ti:sapphire laser that produces pulses of either 100-fs or 1-ps duration at a central wavelength of 229nm . The large bandwidth of the pulses photoionizes all velocity classes of the Cd vapor, resulting in a high loading efficiency compared to previous ion trap loading techniques. Measured loading rates are compared with a simple theoretical model, and we conclude that this technique can potentially ionize every atom traversing the laser beam within the trapping volume. This may allow the operation of ion traps with lower levels of background pressures and less trap electrode surface contamination. The technique and laser system reported here should be applicable to loading most laser-cooled ion species.

  19. Femtosecond spectroscopy with vacuum ultraviolet pulse pairs

    SciTech Connect

    Allison, Tom; Wright, Travis; Stooke, Adam; Khurmi, Champak; van Tilborg, Jeroen; Liu, Yanwei; Falcone, Roger; Belkacem, Ali

    2011-06-17

    We combine different wavelengths from an intense high-order harmonics source with variable delay at the focus of a split-mirror interferometer to conduct pump-probe experiments on gas-phase molecules. We report measurements of the time resolution (< 44fs) and spatial profiles (4 {micro}m x 12 {micro}m) at the focus of the apparatus. We demonstrate the utility of this two-color, high-order-harmonic technique by time resolving molecular hydrogen elimination from C{sub 2} H{sub 4} excited into its absorption band at 161nm.

  20. Photoionization and electron-ion recombination of Ti I

    NASA Astrophysics Data System (ADS)

    Nahar, Sultana N.

    2016-07-01

    Study of the inverse processes of photoionization and electron-ion recombination of (Ti I + h ν ⇋ Ti II + e) using the unified method is reported. The method, based on close coupling (CC) approximation and R-matrix method, subsumes both the radiative recombination (RR) and dielectronic recombination (DR) in a unified manner and provides state-specific and total electron-ion recombination rate coefficients which are self-consistent with the state-specific photoionization cross sections. The present results include state-specific electron-ion recombination rates (αRC(i))and partial photoionization cross sections (σPI(i)) leaving the ion in the ground state of 813 bound states with n ≤ 10 and l ≤ 9 of Ti I. Various features of state-specific and total electron-ion recombination with temperature, and the corresponding photoionization cross sections with energies are discussed with illustrations. Due to closely lying excited states near the ground state of the core, photoionization cross sections show presence of narrow Rydberg resonances in low energy region near the ionization threshold. Many excited states also show broad and enhanced Seaton resonances due to PEC (photo-excitation-of-core) which contribute to the high temperature recombination. The total recombination rate coefficient is found to show a low hump around temperature 280 K and a high dielectronic recombination peak at temperature 25,000 K. Total spectrum of recombination cross sections and rates with photoelectron energy are also presented for experimental observation. Calculations were carried out using a CC wave function expansion of 36 states of the core ion Ti II. The large set of data for recombination rates and partial photoionization cross sections with resonances should provide a complete and accurate modelings of plasmas.

  1. Two-photon resonances in femtosecond time-resolved four-wave mixing spectroscopy: {beta}-carotene

    SciTech Connect

    Namboodiri, V.; Namboodiri, M.; Flachenecker, G.; Materny, A.

    2010-08-07

    Femtosecond time-resolved pump-degenerate four-wave mixing (pump-DFWM) spectroscopy has been used to study the ultrafast dynamics of {beta}-carotene involving several electronic and vibrational states. An initial pump pulse, resonant with the S{sub 0}-to-S{sub 2} transition, excites the molecular system and a DFWM process, resonant with the S{sub 1}-to-S{sub n} transition, is used to probe the relaxation pathways. The transient shows a peculiar decay behavior, which is due to the contributions of resonant DFWM signal of the excited S{sub 1} state, nonresonant DFWM signal of the ground S{sub 0} state and vibrational hot S{sub 0}{sup *} state, and the two-photon resonant DFWM signal of the ground S{sub 0} state. We have used a kinetic model including all the signal contributions to successfully fit the transient. The time constants extracted are in very good agreement with the known values for {beta}-carotene. For comparison, a two-pulse pump-probe experiment was performed measuring the transient absorption at the wavelength of the DFWM experiment.

  2. Growth and characterization of Cu(In,Ga)Se2 thin films by nanosecond and femtosecond pulsed laser deposition

    PubMed Central

    2014-01-01

    In this work, CuIn1 - x Ga x Se2 (CIGS) thin films were prepared by nanosecond (ns)- and femtosecond (fs)-pulsed laser deposition (PLD) processes. Different film growth mechanisms were discussed in perspective of the laser-produced plasmas and crystal structures. The fs-PLD has successfully improved the inherent flaws, Cu2 - x Se, and air voids ubiquitously observed in ns-PLD-derived CIGS thin films. Moreover, the prominent antireflection and excellent crystalline structures were obtained in the fs-PLD-derived CIGS thin films. The absorption spectra suggest the divergence in energy levels of radiative defects brought by the inhomogeneous distribution of elements in the fs-PLD CIGS, which has also been supported by comparing photoluminescence (PL) spectra of ns- and fs-PLD CIGS thin films at 15 K. Finally, the superior carrier transport properties in fs-PLD CIGS were confirmed by fs pump-probe spectroscopy and four-probe measurements. The present results indicate a promising way for preparing high-quality CIGS thin films via fs-PLD. PMID:24959108

  3. Femtosecond spectroscopy of a 13-demethylrhodopsin visual pigment analogue: The role of nonbonded interactions in the isomerization process

    SciTech Connect

    Wang, Q.; Shank, C.V.; Kochendoerfer, G.G.; Mathies, R.A.; Schoenlein, R.W.; Verdegem, P.J.E.; Lugtenburg, J.

    1996-10-24

    The photoisomerization reaction of the visual pigment analogue 11-cis-13-demethylrhodopsin is investigated using femtosecond pump-probe techniques. Following excitation with a 40-fs pump pulse at 500 nm, differential trasnsient absorption spectra are measured from 470 to 560 nm using a 10-fs probe pulse centered at 500 nm and from 560 to 650 nm using a 10-fs probe pulse centered at 620 nm. The persistence of the excited-state absorption, the recovery kinetics of the ground-state bleach, and the formation time of the photoproduct absorption all indicate that this photoisomerization reaction is complete on the 400-fs time scale. Comparison of the reaction dynamics of 11-cis-rhodopsin with 11-cis-13-demethylrhodopsin suggests that the removal of the nonbonded steric intersection between the C{sub 13}-methyl group and the C{sub 10}-hydrogen atom slows down the initial torsional dynamics and that this in turn results in a lower isomerization quantum yield and a slower overall reaction time. Our results support the hypothesis that the quantum yield and the speed of the isomerization reaction are coupled according to a dynamic potential-sulfate crossing mechanism. 27 refs., 5 figs.

  4. Manipulating femtosecond spin-orbit torques with laser pulse sequences to control magnetic memory states and ringing

    NASA Astrophysics Data System (ADS)

    Lingos, P. C.; Wang, J.; Perakis, I. E.

    2015-05-01

    Femtosecond (fs) coherent control of collective order parameters is important for nonequilibrium phase dynamics in correlated materials. Here, we propose such control of ferromagnetic order based on using nonadiabatic optical manipulation of electron-hole (e -h ) photoexcitations to create fs carrier-spin pulses with controllable direction and time profile. These spin pulses are generated due to the time-reversal symmetry breaking arising from nonperturbative spin-orbit and magnetic exchange couplings of coherent photocarriers. By tuning the nonthermal populations of exchange-split, spin-orbit-coupled semiconductor band states, we can excite fs spin-orbit torques that control complex magnetization pathways between multiple magnetic memory states. We calculate the laser-induced fs magnetic anisotropy in the time domain by using density matrix equations of motion rather than the quasiequilibrium free energy. By comparing to pump-probe experiments, we identify a "sudden" out-of-plane magnetization canting displaying fs magnetic hysteresis, which agrees with switchings measured by the static Hall magnetoresistivity. This fs transverse spin-canting switches direction with magnetic state and laser frequency, which distinguishes it from the longitudinal nonlinear optical and demagnetization effects. We propose that sequences of clockwise or counterclockwise fs spin-orbit torques, photoexcited by shaping two-color laser-pulse sequences analogous to multidimensional nuclear magnetic resonance (NMR) spectroscopy, can be used to timely suppress or enhance magnetic ringing and switching rotation in magnetic memories.

  5. Controlling the length of plasma waveguide up to 5 mm, produced by femtosecond laser pulses in atomic clustered gas.

    PubMed

    Mohamed, Walid Tawfik; Chen, Guanglong; Kim, Jaehoon; Tao, Geng Xiao; Ahn, Jungkwen; Kim, Dong Eon

    2011-08-15

    We report the observation of longitudinally uniform plasma waveguide with a controlled length of up to nearly 5 mm, in argon clustered gas jet. This self-channeling plasma is obtained using a 35 mJ, 30 fs FWHM pulse as a pump laser pulse to create the plasma channel. A 1 mJ pulse of the same laser is used for probing the plasma channels using interferometric diagnostics. The radial distribution of the electron density confirms the formation of a plasma waveguide. Clustered argon enhances the absorption efficiency of femtosecond pulses which enables the use of pump pulses of only 35 mJ, approximately 10 times less energy than required for heating conventional gas targets. The plasma channel length is controlled by the laser focus point (F), the laser intensity (I), the pump-probe delay time (t) and the laser height from a nozzle (z). The variation of the electron density for these parameters is also studied. We found that the highest density of 1.2 x 10(19) cm(-3) was obtained at I = 5.2 x 10(16) W/cm(2), z = 2 mm and t = 7.6 ns. It was demonstrated that by using a clustered jet, both the plasma waveguide length and the plasma density could be controlled. PMID:21934955

  6. Femtosecond pulse shaping using plasmonic snowflake nanoantennas

    SciTech Connect

    Tok, Ruestue Umut; Sendur, Kuersat

    2011-09-15

    We have theoretically demonstrated femtosecond pulse manipulation at the nanoscale using the plasmonic snowflake antenna's ability to localize light over a broad spectrum. To analyze the interaction of the incident femtosecond pulse with the plasmonic nanoantenna, we first decompose the diffraction limited incident femtosecond pulse into its spectral components. The interaction of each spectral component with the nanoantenna is analyzed using finite element technique. The time domain response of the plasmonic antenna is obtained using inverse Fourier transformation. It is shown that the rich spectral characteristics of the plasmonic snowflake nanoantenna allow manipulation of the femtosecond pulses over a wide spectrum. Light localization around the gap region of the nanoantenna is shown for femtosecond pulses. As the alignment of incident light polarization is varied, different antenna elements oscillate, which in turn creates a different spectrum and a distinct femtosecond response.

  7. Resonant double photoionization of lithium studied with medium energy resolution

    NASA Astrophysics Data System (ADS)

    Wehlitz, R.; Juranić, P. N.

    2006-10-01

    We have measured the relative photoionization cross section for the formation of Li2+ ions between 148 and 161eV photon energy with higher photon-energy resolution than in previous Li2+ studies. This energy region is characterized by double and triple excitations that lead to strong enhancements in the Li2+ cross section. As a result, the double-to-single photoionization ratio shows a dramatic resonance structure not seen before. We have determined the resonance positions and widths using Fano-profile fits to the Li2+ data and compare them to previously published values and a calculated Li2+ cross-section curve.

  8. Strong-Field Photoionization as Excited-State Tunneling.

    PubMed

    Serebryannikov, E E; Zheltikov, A M

    2016-03-25

    We show that, in an intense laser field, ultrafast photoionization can occur through quantum pathways that cannot be categorized as multiphoton ionization or ground-state tunneling. In this regime, the subcycle electron-wave-packet dynamics leading to photoionization occurs via electron excited states, from where the electrons tunnel to the continuum within a tiny fraction of the field cycle. For high field intensities, this ionization pathway is shown to drastically enhance the dynamic leakage of the electron wave packet into the continuum, opening an ionization channel that dominates over ground-state electron tunneling. PMID:27058079

  9. Two-electron photoionization of ground-state lithium

    SciTech Connect

    Kheifets, A. S.; Fursa, D. V.; Bray, I.

    2009-12-15

    We apply the convergent close-coupling (CCC) formalism to single-photon two-electron ionization of the lithium atom in its ground state. We treat this reaction as single-electron photon absorption followed by inelastic scattering of the photoelectron on a heliumlike Li{sup +} ion. The latter scattering process can be described accurately within the CCC formalism. We obtain integrated cross sections of single photoionization leading to the ground and various excited states of the Li{sup +} ion as well as double photoionization extending continuously from the threshold to the asymptotic limit of infinite photon energy. Comparison with available experimental and theoretical data validates the CCC model.

  10. Strong-Field Photoionization as Excited-State Tunneling

    NASA Astrophysics Data System (ADS)

    Serebryannikov, E. E.; Zheltikov, A. M.

    2016-03-01

    We show that, in an intense laser field, ultrafast photoionization can occur through quantum pathways that cannot be categorized as multiphoton ionization or ground-state tunneling. In this regime, the subcycle electron-wave-packet dynamics leading to photoionization occurs via electron excited states, from where the electrons tunnel to the continuum within a tiny fraction of the field cycle. For high field intensities, this ionization pathway is shown to drastically enhance the dynamic leakage of the electron wave packet into the continuum, opening an ionization channel that dominates over ground-state electron tunneling.

  11. Femtosecond lasers for machining of transparent, brittle materials: ablative vs. non-ablative femtosecond laser processing

    NASA Astrophysics Data System (ADS)

    Hendricks, F.; Matylitsky, V. V.

    2016-03-01

    This paper focuses on precision machining of transparent materials by means of ablative and non-ablative femtosecond laser processing. Ablation technology will be compared with a newly developed patent pending non-ablative femtosecond process, ClearShapeTM, using the Spectra-Physics Spirit industrial femtosecond laser.

  12. Photoelectron angular distributions in bichromatic atomic ionization induced by circularly polarized VUV femtosecond pulses

    NASA Astrophysics Data System (ADS)

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

    2016-03-01

    We investigate two-pathway interferences between nonresonant one-photon and resonant two-photon ionization of atomic hydrogen. In particular, we analyze in detail the photoionization mediated by the fundamental frequency and the second harmonic of a femtosecond VUV pulse when the fundamental is tuned near an intermediate atomic state. Following our recent study [Phys. Rev. A 91, 063418 (2015), 10.1103/PhysRevA.91.063418] of such effects with linearly polarized light, we analyze a similar situation with circularly polarized radiation. As a consequence of the richer structure in circularly polarized light, characterized by its right-handed or left-handed helicity, we present and discuss various important features associated with the photoelectron angular distribution.

  13. Nanoflow electrospinning serial femtosecond crystallography

    SciTech Connect

    Sierra, Raymond G.; Laksmono, Hartawan; Kern, Jan; Tran, Rosalie; Hattne, Johan; Alonso-Mori, Roberto; Lassalle-Kaiser, Benedikt; Glöckner, Carina; Hellmich, Julia; Schafer, Donald W.; Echols, Nathaniel; Gildea, Richard J.; Grosse-Kunstleve, Ralf W.; Sellberg, Jonas; McQueen, Trevor A.; Fry, Alan R.; Messerschmidt, Marc M.; Miahnahri, Alan; Seibert, M. Marvin; Hampton, Christina Y.; Starodub, Dmitri; Loh, N. Duane; Sokaras, Dimosthenis; Weng, Tsu-Chien; Zwart, Petrus H.; Glatzel, Pieter; Milathianaki, Despina; White, William E.; Adams, Paul D.; Williams, Garth J.; Boutet, Sébastien; Zouni, Athina; Messinger, Johannes; Sauter, Nicholas K.; Bergmann, Uwe; Yano, Junko; Yachandra, Vittal K.; Bogan, Michael J.

    2012-11-01

    A low flow rate liquid microjet method for delivery of hydrated protein crystals to X-ray lasers is presented. Linac Coherent Light Source data demonstrates serial femtosecond protein crystallography with micrograms, a reduction of sample consumption by orders of magnitude. An electrospun liquid microjet has been developed that delivers protein microcrystal suspensions at flow rates of 0.14–3.1 µl min{sup −1} to perform serial femtosecond crystallography (SFX) studies with X-ray lasers. Thermolysin microcrystals flowed at 0.17 µl min{sup −1} and diffracted to beyond 4 Å resolution, producing 14 000 indexable diffraction patterns, or four per second, from 140 µg of protein. Nanoflow electrospinning extends SFX to biological samples that necessitate minimal sample consumption.

  14. Femtosecond Photon-Counting Receiver

    NASA Technical Reports Server (NTRS)

    Krainak, Michael A.; Rambo, Timothy M.; Yang, Guangning; Lu, Wei; Numata, Kenji

    2016-01-01

    An optical correlation receiver is described that provides ultra-precise distance and/or time-pulse-width measurements even for weak (single photons) and short (femtosecond) optical signals. A new type of optical correlation receiver uses a fourth-order (intensity) interferometer to provide micron distance measurements even for weak (single photons) and short (femtosecond) optical signals. The optical correlator uses a low-noise-integrating detector that can resolve photon number. The correlation (range as a function of path delay) is calculated from the variance of the photon number of the difference of the optical signals on the two detectors. Our preliminary proof-of principle data (using a short-pulse diode laser transmitter) demonstrates tens of microns precision.

  15. Femtosecond Photon-Counting Receiver

    NASA Technical Reports Server (NTRS)

    Krainak, Michael A.; Rambo, Timothy M.; Yang, Guangning; Lu, Wei; Numata, Kenji

    2016-01-01

    An optical correlation receiver is described that provides ultra-precise distance and/or time/pulse-width measurements even for weak (single photons) and short (femtosecond) optical signals. A new type of optical correlation receiver uses a fourth-order (intensity) interferometer to provide micron distance measurements even for weak (single photons) and short (femtosecond) optical signals. The optical correlator uses a low-noise-integrating detector that can resolve photon number. The correlation (range as a function of path delay) is calculated from the variance of the photon number of the difference of the optical signals on the two detectors. Our preliminary proof-of principle data (using a short-pulse diode laser transmitter) demonstrates tens of microns precision.

  16. Nanoflow electrospinning serial femtosecond crystallography.

    PubMed

    Sierra, Raymond G; Laksmono, Hartawan; Kern, Jan; Tran, Rosalie; Hattne, Johan; Alonso-Mori, Roberto; Lassalle-Kaiser, Benedikt; Glöckner, Carina; Hellmich, Julia; Schafer, Donald W; Echols, Nathaniel; Gildea, Richard J; Grosse-Kunstleve, Ralf W; Sellberg, Jonas; McQueen, Trevor A; Fry, Alan R; Messerschmidt, Marc M; Miahnahri, Alan; Seibert, M Marvin; Hampton, Christina Y; Starodub, Dmitri; Loh, N Duane; Sokaras, Dimosthenis; Weng, Tsu-Chien; Zwart, Petrus H; Glatzel, Pieter; Milathianaki, Despina; White, William E; Adams, Paul D; Williams, Garth J; Boutet, Sébastien; Zouni, Athina; Messinger, Johannes; Sauter, Nicholas K; Bergmann, Uwe; Yano, Junko; Yachandra, Vittal K; Bogan, Michael J

    2012-11-01

    An electrospun liquid microjet has been developed that delivers protein microcrystal suspensions at flow rates of 0.14-3.1 µl min(-1) to perform serial femtosecond crystallography (SFX) studies with X-ray lasers. Thermolysin microcrystals flowed at 0.17 µl min(-1) and diffracted to beyond 4 Å resolution, producing 14,000 indexable diffraction patterns, or four per second, from 140 µg of protein. Nanoflow electrospinning extends SFX to biological samples that necessitate minimal sample consumption. PMID:23090408

  17. Photoionization of furan from the ground and excited electronic states

    NASA Astrophysics Data System (ADS)

    Ponzi, Aurora; Sapunar, Marin; Angeli, Celestino; Cimiraglia, Renzo; Došlić, Nada; Decleva, Piero

    2016-02-01

    Here we present a comparative computational study of the photoionization of furan from the ground and the two lowest-lying excited electronic states. The study aims to assess the quality of the computational methods currently employed for treating bound and continuum states in photoionization. For the ionization from the ground electronic state, we show that the Dyson orbital approach combined with an accurate solution of the continuum one particle wave functions in a multicenter B-spline basis, at the density functional theory (DFT) level, provides cross sections and asymmetry parameters in excellent agreement with experimental data. On the contrary, when the Dyson orbitals approach is combined with the Coulomb and orthogonalized Coulomb treatments of the continuum, the results are qualitatively different. In excited electronic states, three electronic structure methods, TDDFT, ADC(2), and CASSCF, have been used for the computation of the Dyson orbitals, while the continuum was treated at the B-spline/DFT level. We show that photoionization observables are sensitive probes of the nature of the excited states as well as of the quality of excited state wave functions. This paves the way for applications in more complex situations such as time resolved photoionization spectroscopy.

  18. Radiative recombination and excited-state photoionization of lithium

    SciTech Connect

    Lahiri, J. ); Manson, S.T. )

    1993-11-01

    The radiative-recombination rate coefficients for electrons impinging on Li[sup +], along with the associated excited-state photoionization cross sections for Li, are calculated in the low-energy region. In addition to the totals, the contribution of the recombination of individual excited states to the total is discussed.

  19. The operation of a pressurized ultraviolet photoionization threshold cherenkov counter

    NASA Astrophysics Data System (ADS)

    Harnew, N.; Meyer, D. I.

    We have successfully tested an ultraviolet photoionization Cherenkov counter in a 10 GeV/ c pion beam. The counter has been tested to 11 atm pressure for use as a π-K separator. The design and operation of the counter is described.

  20. Electron scattering from and photoionization of open- shell atoms

    NASA Astrophysics Data System (ADS)

    Lin, Dong

    1999-09-01

    The multiconfiguration Hartree-Fock (MCHF) approach, developed by Dr. H. P. Saha et al, has been proved to be extremely successful in the past few years in reproducing experimental results at a very high level of accuracy. The research projects we are interested consist of two areas. In the first area we performed ab initio calculations on elastic scattering of electrons from open-shell sulfur atoms. In the second area, in order to understand the electronic dynamics in photoionization of atoms, we carried out accurate calculations on valence and K-shell photoionization of three-electron systems from lithium through neon for photon energies from threshold to very high energies; to further identify the autoionization resonances which were observed near threshold and to understand the dynamics, we modifies the MCHF method to include relativistic effects and performed calculation on partial photoionization cross section, resonance structure and effect of spin-orbit interaction in photoionization of atomic bromine. The calculated results obtained in each of these investigations are compared with available experimental and theoretical data and are found to be in very good agreement. The research contribution made for the fulfillment of the degree, we understand, will be a valuable addition towards a better understanding of the open-shell systems.

  1. Radiative properties measurements of photoionized plasmas on Z

    NASA Astrophysics Data System (ADS)

    Loisel, Guillaume; Bailey, Jim; Nagayama, Taisuke; Hansen, Stephanie; Rochau, Greg; Liedahl, Duane; Fontes, Chris; Flaugh, Matt; Koepke, Mark; Lane, Ted; Mancini, Roberto

    2015-11-01

    Physical descriptions of accretion-powered objects such as black holes, x-ray binaries, or AGN are informed through the interpretation of emergent spectra from the photoionized plasmas that surround them. Line formation in photoionized plasmas is dependent on the details of the radiation transport treatment and the so-called Resonant Auger Destruction hypothesis typically required to interpret the relativistically broadened Fe K α emitted from near the black hole event horizon. The Z facility at Sandia National Laboratories can produced such photoionized plasmas producing 1.6MJ of x-rays from the z-pinch dynamic hohlraum. The extended suite of diagnostics allows for a detailed characterization of plasmas conditions through absorption spectroscopy. present accurate and high-resolution emergent intensity observed from a photoionized silicon plasma for a discrete set of column densities that will help us evaluate understanding for radiation transport in accretion powered objects. Sandia is a multi-program laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the United States Department of Energy under contract DE-AC04-94AL85000.

  2. Photoionization cross sections and oscillator strengths of neutral cesium

    NASA Astrophysics Data System (ADS)

    Haq, S. U.; Nadeem, Ali; Nawaz, M.

    2012-11-01

    The absolute photoionization cross sections from the 6p 2P1/2 excited state of cesium at threshold and above the threshold region have been measured using the saturation absorption technique. The photoionization cross section at the ionization threshold is determined as 22.6±3.6 Mb, whereas in the region above threshold its value ranges from 22 to 20 Mb for photoelectron energies up to 0.1 eV. A comparison of the photoionization cross sections with earlier reported theoretical and experimental data have been presented and are in good agreement within the uncertainty. In addition, the oscillator strengths of the 6p 2P1/2→n d 2D3/2 (21≤n≤60) Rydberg transitions of cesium have been calibrated using the threshold value of the photoionization cross section. A complete picture of the oscillator strengths from the present work and previously reported data from n=5-60 is presented.

  3. The dynamics of femtosecond pulsed laser removal of 20 nm Ni films from an interface

    NASA Astrophysics Data System (ADS)

    Schrider, Keegan J.; Torralva, Ben; Yalisove, Steven M.

    2015-09-01

    The dynamics of femtosecond laser removal of 20 nm Ni films on glass substrates was studied using time-resolved pump-probe microscopy. 20 nm thin films exhibit removal at two distinct threshold fluences, removal of the top 7 nm of Ni above 0.14 J/cm2, and removal of the entire 20 nm film above 0.36 J/cm2. Previous work shows the top 7 nm is removed through liquid spallation, after irradiation the Ni melts and rapidly expands leading to tensile stress and cavitation within the Ni film. This work shows that above 0.36 J/cm2 the 20 nm film is removed in two distinct layers, 7 nm and 13 nm thick. The top 7 nm layer reaches a speed 500% faster than the bottom 13 nm layer at the same absorbed fluence, 500-2000 m/s and 300-700 m/s in the fluence ranges studied. Significantly different velocities for the top 7 nm layer and bottom 13 nm layer indicate removal from an interface occurs by a different physical mechanism. The method of measuring film displacement from the development of Newton's rings was refined so it could be shown that the 13 nm layer separates from the substrate within 70 ps and accelerates to its final velocity within several hundred picoseconds. We propose that removal of the bottom 13 nm is consistent with heterogeneous nucleation and growth of vapor at the Ni-glass interface, but that the rapid separation and acceleration of the 13 nm layer from the Ni-glass interface requires consideration of exotic phases of Ni after excitation.

  4. Photodissociation and photoionization of organosulfur radicals

    SciTech Connect

    Hsu, Chia-Wei

    1994-05-27

    The dynamics of S({sup 3}P{sub 2,1,0}, {sup 1}D{sub 2}) production from the 193 nm photodissociation of CH{sub 3}SCH{sub 3}, H{sub 2}S and CH{sub 3}SH have been studied using 2 + 1 resonance-enhanced multiphoton ionization (REMPI) techniques. The 193 nm photodissociation cross sections for the formation of S from CH{sub 3}S and HS initially prepared in the photodissociation of CH{sub 3}SCH{sub 3} and H{sub 2}S are estimated to be 1 {times} 10{sup {minus}18} and 1.1 {times} 10{sup {minus}18} cm{sup 2}, respectively. The dominant product from CH{sub 3}S is S({sup 1}D), while that from SH is S({sup 3}P). Possible potential energy surfaces involved in the 193 nm photodissociation of CH{sub 3}S({tilde X}) and SH(X) have been also examined. Threshold photoelectron (PE) spectra for SH and CH{sub 3}S formed in the ultraviolet photodissociation of H{sub 2}S and CH{sub 3}SH, respectively, have been measured using the nonresonant two-photon pulsed field ionization (N2P-PFI) technique. The rotationally resolved N2P-PFI-PE spectrum obtained for SH indicates that photoionization dynamics favors the rotational angular momentum change {Delta}N < 0 with the {Delta}N value up to {minus}3, an observation similar to that found in the PFI-PE spectra of OH (OD) and NO. The ionization energies for SH(X{sup 2}{product}{sub 3,2}) and CH{sub 3}S({tilde X}{sup 2}E{sub 3/2}) are determined to be 84,057.5 {plus_minus} 3 cm{sup {minus}1} and 74,726 {plus_minus} 8 cm{sup {minus}1} respectively. The spin-orbit splittings for SH(X{sup 2}{product}{sub 3/2,1/2}) and CH{sub 3}S({tilde X}{sup 2}E{sub 3/2,1/2}) are found to be 377 {plus_minus} 2 and 257 {plus_minus} 5 cm{sup {minus}1}, respectively, in agreement with previous measurements. The C-S stretching frequency for CH{sub 3}S{sup +}({tilde X}{sup 3}A{sub 2}) is 733 {plus_minus} 5 cm{sup {minus}1}. This study illustrates that the PFI-PE detection method can be a sensitive probe for the nascent internal energy distribution of photoproducts.

  5. Photoionization of Fe7+ from the ground and metastable states

    NASA Astrophysics Data System (ADS)

    Tayal, S. S.; Zatsarinny, O.

    2015-01-01

    The B -spline Breit-Pauli R -matrix method is used to investigate the photoionization of Fe7 + from the ground and metastable states in the energy region from ionization thresholds to 172 eV. The present calculations were designed to resolve the large discrepancies between recent measurements and available theoretical results. The multiconfiguration Hartree-Fock method in connection with B -spline expansions is employed for an accurate representation of the initial- and final-state wave functions. The close-coupling expansion includes 99 fine-structure levels of the residual Fe8 + ion in the energy region up to 3 s23 p54 s states. It includes levels of the 3 s23 p6,3 s23 p53 d ,3 s23 p54 s , and 3 s 3 p63 d configurations and some levels of the 3 s23 p43 d2 configuration which lie in the energy region under investigation. The present photoionization cross sections in the length and velocity formulations exhibit excellent agreement. The present photoionization cross sections agree well with the Breit-Pauli R -matrix calculation by Sossah et al. and the TOPbase data in the magnitude of the background nonresonant cross sections but show somewhat richer resonance structures, which qualitatively agree with the measurements. The calculated cross sections, however, are several times lower than the measured cross sections, depending upon the photon energy. The cross sections for photoionization of metastable states were found to have approximately the same magnitude as the cross sections for photoionization of the ground state, thereby the presence of metastable states in the ion beam may not be the reason for the enhancement of the measured cross sections.

  6. Photoionized Plasma and Opacity Experiments on the Z Machine

    NASA Astrophysics Data System (ADS)

    Bailey, James

    2008-04-01

    Laboratory experiments at Z use high energy density to create plasma conditions similar to extreme astrophysical environments, including stellar interiors and accretion powered objects. The importance of radiation unifies these topics, even though the plasmas involved are very different. Understanding stellar interiors requires knowledge of radiation transport in dense, hot, collision-dominated plasma. A Z x-ray source was used to measure iron plasma transmission at 156 eV electron temperature, 2x higher than in prior work. The data provide the first experimental tests of absorption features critical for stellar interior opacity models and may provide insight into whether the present discrepancy between solar models and helioseismology originates in opacity model deficiencies or in some other aspect of the solar model. In contrast, accretion physics requires interpretation of x-ray spectra from lower density photoionization-dominated plasma. Exploiting astrophysical spectra requires a spectral model that connects the observations with a model that describes the overall picture of the astrophysical object. However, photoionized plasma spectral models are largely untested. Z-pinch radiation was used to create photoionized iron and neon plasmas with photoionization parameter 5-25 erg cm /s. Comparisons with the data improve x-ray photoionization models and promote more accurate interpretation of spectra acquired with astrophysical observatories. The prospects for new experiments at the higher radiation powers provided by the recently upgraded Z facility will be described.* In collaboration with scientists from CEA, LANL, LLNL, Oxford, Prism, Queens University, Swarthmore College, U. Nevada Reno, and Sandia ++Sandia is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the United States Department of Energy under contract DE-AC04-94AL85000.

  7. Extraction of Fixed-in-Space photoionization cross section and phase with high-order harmonic generation from aligned molecules

    NASA Astrophysics Data System (ADS)

    Le, Anh-Thu

    2010-03-01

    It has been known for over two decades that high-order harmonic generation (HHG) process occurs when an electron released earlier from an atom/molecule by an intense laser field returns to recombine with the parent ion. This relation between photo-recombination (or its time-reverse, photoionization process) and HHG has been firmly established on the quantitative level recently by the quantitative rescattering theory (QRS) [1]. According to the QRS, HHG signal can be expressed as a product of a returning electron wave packet and the laser-free photo-recombination differential cross section. The QRS has been carefully tested against available exact numerical solutions of the time-dependent Schroedinger equation. Here we report comparisons with recent experimental data for magnitude, phase, polarization state, and ellipticity of the emitted harmonics for aligned molecules, from which the molecular frame photoionization cross sections and phases can be probed in great details [2]. We also address the issue about the contribution from inner molecular orbitals [3,4]. Finally, we will discuss the possibility for future dynamic chemical imaging with femto-second temporal resolution on an example of probing molecular dynamics of vibrationally excited N2O4 [5]. In collaboration with C.D. Lin, R.R. Lucchese, T. Morishita, C. Jin.[4pt] [1] A.T. Le et al, Phys. Rev. A. 80, 013401 (2009).[0pt] [2] X. Zhou et al, Phys. Rev. Lett. 102, 073902 (2009).[0pt] [3] B.K. McFarland et al, Science 322, 1232 (2008).[0pt] [4] O. Smirnova et al, Nature 460, 972 (2009).[0pt] [5] W. Li et al, Science 322, 1207 (2008).

  8. Molecular fragmentation induced by a femtosecond laser

    NASA Astrophysics Data System (ADS)

    Kosmidis, Constantine E.; Ledingham, Kenneth W. D.; Kilic, H. S.; McCanny, T.; Singhal, Raghunandan P.; Smith, D.; Langley, Andrew J.

    1998-07-01

    The 90 femtosecond laser induced fragmentation at 375 nm for a number of different nitro-molecules is compared to that induced by a nanosecond laser at the same wavelength by means of time-of-flight mass spectrometry. The potential of femtosecond laser mass spectrometry for analytical purposes is discussed.

  9. VUV photoionization and dissociative photoionization of the prebiotic molecule acetyl cyanide: Theory and experiment

    NASA Astrophysics Data System (ADS)

    Bellili, A.; Schwell, M.; Bénilan, Y.; Fray, N.; Gazeau, M.-C.; Mogren Al-Mogren, M.; Guillemin, J.-C.; Poisson, L.; Hochlaf, M.

    2014-10-01

    The present combined theoretical and experimental investigation concerns the single photoionization of gas-phase acetyl cyanide and the fragmentation pathways of the resulting cation. Acetyl cyanide (AC) is inspired from both the chemistry of cyanoacetylene and the Strecker reaction which are thought to be at the origin of medium sized prebiotic molecules in the interstellar medium. AC can be formed by reaction from cyanoacetylene and water but also from acetaldehyde and HCN or the corresponding radicals. In view of the interpretation of vacuum ultraviolet (VUV) experimental data obtained using synchrotron radiation, we explored the ground potential energy surface (PES) of acetyl cyanide and of its cation using standard and recently implemented explicitly correlated methodologies. Our PES covers the regions of tautomerism (between keto and enol forms) and of the lowest fragmentation channels. This allowed us to deduce accurate thermochemical data for this astrobiologically relevant molecule. Unimolecular decomposition of the AC cation turns out to be very complex. The implications for the evolution of prebiotic molecules under VUV irradiation are discussed.

  10. VUV photoionization and dissociative photoionization of the prebiotic molecule acetyl cyanide: Theory and experiment

    SciTech Connect

    Bellili, A.; Hochlaf, M. E-mail: martin.schwell@lisa.u-pec.fr; Schwell, M. E-mail: martin.schwell@lisa.u-pec.fr; Bénilan, Y.; Fray, N.; Gazeau, M.-C.; Mogren Al-Mogren, M.; Guillemin, J.-C.; Poisson, L.

    2014-10-07

    The present combined theoretical and experimental investigation concerns the single photoionization of gas-phase acetyl cyanide and the fragmentation pathways of the resulting cation. Acetyl cyanide (AC) is inspired from both the chemistry of cyanoacetylene and the Strecker reaction which are thought to be at the origin of medium sized prebiotic molecules in the interstellar medium. AC can be formed by reaction from cyanoacetylene and water but also from acetaldehyde and HCN or the corresponding radicals. In view of the interpretation of vacuum ultraviolet (VUV) experimental data obtained using synchrotron radiation, we explored the ground potential energy surface (PES) of acetyl cyanide and of its cation using standard and recently implemented explicitly correlated methodologies. Our PES covers the regions of tautomerism (between keto and enol forms) and of the lowest fragmentation channels. This allowed us to deduce accurate thermochemical data for this astrobiologically relevant molecule. Unimolecular decomposition of the AC cation turns out to be very complex. The implications for the evolution of prebiotic molecules under VUV irradiation are discussed.

  11. Photoionized plasmas induced in neon with extreme ultraviolet and soft X-ray pulses produced using low and high energy laser systems

    SciTech Connect

    Bartnik, A.; Wachulak, P.; Fok, T.; Węgrzyński, Ł.; Fiedorowicz, H.; Pisarczyk, T.; Chodukowski, T.; Kalinowska, Z.; Dudzak, R.; Dostal, J.; Krousky, E.; Skala, J.; Ullschmied, J.; Hrebicek, J.; Medrik, T.

    2015-04-15

    A comparative study of photoionized plasmas created by two soft X-ray and extreme ultraviolet (SXR/EUV) laser plasma sources with different parameters is presented. The two sources are based on double-stream Xe/He gas-puff targets irradiated with high (500 J/0.3 ns) and low energy (10 J/1 ns) laser pulses. In both cases, the SXR/EUV beam irradiated the gas stream, injected into a vacuum chamber synchronously with the radiation pulse. Irradiation of gases resulted in formation of photoionized plasmas emitting radiation in the SXR/EUV range. The measured Ne plasma radiation spectra are dominated by emission lines corresponding to radiative transitions in singly charged ions. A significant difference concerns origin of the lines: K-shell or L-shell emissions occur in case of the high and low energy irradiating system, respectively. In high energy system, the electron density measurements were also performed by laser interferometry, employing a femtosecond laser system. A maximum electron density for Ne plasma reached the value of 2·10{sup 18 }cm{sup −3}. For the low energy system, a detection limit was too high for the interferometric measurements, thus only an upper estimation for electron density could be made.

  12. Nanoflow electrospinning serial femtosecond crystallography

    PubMed Central

    Sierra, Raymond G.; Laksmono, Hartawan; Kern, Jan; Tran, Rosalie; Hattne, Johan; Alonso-Mori, Roberto; Lassalle-Kaiser, Benedikt; Glöckner, Carina; Hellmich, Julia; Schafer, Donald W.; Echols, Nathaniel; Gildea, Richard J.; Grosse-Kunstleve, Ralf W.; Sellberg, Jonas; McQueen, Trevor A.; Fry, Alan R.; Messerschmidt, Marc M.; Miahnahri, Alan; Seibert, M. Marvin; Hampton, Christina Y.; Starodub, Dmitri; Loh, N. Duane; Sokaras, Dimosthenis; Weng, Tsu-Chien; Zwart, Petrus H.; Glatzel, Pieter; Milathianaki, Despina; White, William E.; Adams, Paul D.; Williams, Garth J.; Boutet, Sébastien; Zouni, Athina; Messinger, Johannes; Sauter, Nicholas K.; Bergmann, Uwe; Yano, Junko; Yachandra, Vittal K.; Bogan, Michael J.

    2012-01-01

    An electrospun liquid microjet has been developed that delivers protein microcrystal suspensions at flow rates of 0.14–3.1 µl min−1 to perform serial femtosecond crystallography (SFX) studies with X-ray lasers. Thermolysin microcrystals flowed at 0.17 µl min−1 and diffracted to beyond 4 Å resolution, producing 14 000 indexable diffraction patterns, or four per second, from 140 µg of protein. Nanoflow electrospinning extends SFX to biological samples that necessitate minimal sample consumption. PMID:23090408

  13. Attosecond Coherent Control of Single and Double Photoionization in Argon

    NASA Astrophysics Data System (ADS)

    Hogle, C. W.; Tong, X. M.; Martin, L.; Murnane, M. M.; Kapteyn, H. C.; Ranitovic, P.

    2015-10-01

    Ultrafast high harmonic beams provide new opportunities for coherently controlling excitation and ionization processes in atoms, molecules, and materials on attosecond time scales by employing multiphoton two-pathway electron-wave-packet quantum interferences. Here we use spectrally tailored and frequency tuned vacuum and extreme ultraviolet harmonic combs, together with two phase-locked infrared laser fields, to show how the total single and double photoionization yields of argon can be coherently modulated by controlling the relative phases of both optical and electronic-wave-packet quantum interferences. This Letter is the first to apply quantum control techniques to double photoionization, which is a fundamental process where a single, high-energy photon ionizes two electrons simultaneously from an atom.

  14. A non-invasive online photoionization spectrometer for FLASH2.

    PubMed

    Braune, Markus; Brenner, Günter; Dziarzhytski, Siarhei; Juranić, Pavle; Sorokin, Andrey; Tiedtke, Kai

    2016-01-01

    The stochastic nature of the self-amplified spontaneous emission (SASE) process of free-electron lasers (FELs) effects pulse-to-pulse fluctuations of the radiation properties, such as the photon energy, which are determinative for processes of photon-matter interactions. Hence, SASE FEL sources pose a great challenge for scientific investigations, since experimenters need to obtain precise real-time feedback of these properties for each individual photon bunch for interpretation of the experimental data. Furthermore, any device developed to deliver the according information should not significantly interfere with or degrade the FEL beam. Regarding the spectral properties, a device for online monitoring of FEL wavelengths has been developed for FLASH2, which is based on photoionization of gaseous targets and the measurements of the corresponding electron and ion time-of-flight spectra. This paper presents experimental studies and cross-calibration measurements demonstrating the viability of this online photoionization spectrometer. PMID:26698040

  15. Double Photoionization into Double Core-Hole States in Xe

    SciTech Connect

    Hikosaka, Y.; Kaneyasu, T.; Shigemasa, E.; Lablanquie, P.; Penent, F.; Eland, J. H. D.; Aoto, T.; Ito, K.

    2007-05-04

    Double photoionization (DPI) leading to double core-hole states of Xe{sup 2+} 4d{sup -2} has been studied using a magnetic bottle time-of-flight spectrometer. The assignments of the Xe{sup 2+} 4d{sup -2} states are confirmed by the Auger lines extracted from fourfold coincidences including two photoelectrons and two Auger electrons. It is estimated that the core-core DPI into Xe{sup 2+} 4d{sup -2} at a photon energy of 301.6 eV has a favored cross section of about 0.3 MB. The intense core-core DPI is due to mixing of the 4d{sup -2} continuum with the 4p single photoionization, which is manifested in the relative intensities of the Xe{sup 2+} 4d{sup -2} components.

  16. Double photoionization into double core-hole states in Xe.

    PubMed

    Hikosaka, Y; Lablanquie, P; Penent, F; Kaneyasu, T; Shigemasa, E; Eland, J H D; Aoto, T; Ito, K

    2007-05-01

    Double photoionization (DPI) leading to double core-hole states of Xe2+ 4d(-2) has been studied using a magnetic bottle time-of-flight spectrometer. The assignments of the Xe2+ 4d(-2) states are confirmed by the Auger lines extracted from fourfold coincidences including two photoelectrons and two Auger electrons. It is estimated that the core-core DPI into Xe2+ 4d(-2) at a photon energy of 301.6 eV has a favored cross section of about 0.3 MB. The intense core-core DPI is due to mixing of the 4d(-2) continuum with the 4p single photoionization, which is manifested in the relative intensities of the Xe2+ 4d(-2) components. PMID:17501570

  17. Communication: The influence of vibrational parity in chiral photoionization dynamics

    SciTech Connect

    Powis, Ivan

    2014-03-21

    A pronounced vibrational state dependence of photoelectron angular distributions observed in chiral photoionization experiments is explored using a simple, yet realistic, theoretical model based upon the transiently chiral molecule H{sub 2}O{sub 2}. The adiabatic approximation is used to separate vibrational and electronic wavefunctions. The full ionization matrix elements are obtained as an average of the electronic dipole matrix elements over the vibrational coordinate, weighted by the product of neutral and ion state vibrational wavefunctions. It is found that the parity of the vibrational Hermite polynomials influences not just the amplitude, but also the phase of the transition matrix elements, and the latter is sufficient, even in the absence of resonant enhancements, to account for enhanced vibrational dependencies in the chiral photoionization dynamics.

  18. Atomic Processes in X-ray Photoionized Gas

    NASA Technical Reports Server (NTRS)

    Kallman, Timothy

    2005-01-01

    It has long been known that photoionization and photoabsorption play a dominant role in determining the state of gas in nebulae surrounding hot stars and in active galaxies. Recent observations of X-ray spectra demonstrate that these processes are also dominant in highly ionized gas near compact objects, and also affect the transmission of X-rays from the majority of astronomical sources. This has led to new insights into the understanding of what is going on in these sources. It has also pointed out the need for a better atomic cross sections for photoionization and absorption, notably for processes involving inner shells. In this talk I will discuss these issues, what is known and where more work is needed.

  19. A non-invasive online photoionization spectrometer for FLASH2

    PubMed Central

    Braune, Markus; Brenner, Günter; Dziarzhytski, Siarhei; Juranić, Pavle; Sorokin, Andrey; Tiedtke, Kai

    2016-01-01

    The stochastic nature of the self-amplified spontaneous emission (SASE) process of free-electron lasers (FELs) effects pulse-to-pulse fluctuations of the radiation properties, such as the photon energy, which are determinative for processes of photon–matter interactions. Hence, SASE FEL sources pose a great challenge for scientific investigations, since experimenters need to obtain precise real-time feedback of these properties for each individual photon bunch for interpretation of the experimental data. Furthermore, any device developed to deliver the according information should not significantly interfere with or degrade the FEL beam. Regarding the spectral properties, a device for online monitoring of FEL wavelengths has been developed for FLASH2, which is based on photoionization of gaseous targets and the measurements of the corresponding electron and ion time-of-flight spectra. This paper presents experimental studies and cross-calibration measurements demonstrating the viability of this online photoionization spectrometer. PMID:26698040

  20. Attosecond Coherent Control of Single and Double Photoionization in Argon.

    PubMed

    Hogle, C W; Tong, X M; Martin, L; Murnane, M M; Kapteyn, H C; Ranitovic, P

    2015-10-23

    Ultrafast high harmonic beams provide new opportunities for coherently controlling excitation and ionization processes in atoms, molecules, and materials on attosecond time scales by employing multiphoton two-pathway electron-wave-packet quantum interferences. Here we use spectrally tailored and frequency tuned vacuum and extreme ultraviolet harmonic combs, together with two phase-locked infrared laser fields, to show how the total single and double photoionization yields of argon can be coherently modulated by controlling the relative phases of both optical and electronic-wave-packet quantum interferences. This Letter is the first to apply quantum control techniques to double photoionization, which is a fundamental process where a single, high-energy photon ionizes two electrons simultaneously from an atom. PMID:26551112

  1. Spatially resolved photoionization of ultracold atoms on an atom chip

    SciTech Connect

    Kraft, S.; Guenther, A.; Fortagh, J.; Zimmermann, C.

    2007-06-15

    We report on photoionization of ultracold magnetically trapped Rb atoms on an atom chip. The atoms are trapped at 5 {mu}K in a strongly anisotropic trap. Through a hole in the chip with a diameter of 150 {mu}m, two laser beams are focused onto a fraction of the atomic cloud. A first laser beam with a wavelength of 778 nm excites the atoms via a two-photon transition to the 5D level. With a fiber laser at 1080 nm the excited atoms are photoionized. Ionization leads to depletion of the atomic density distribution observed by absorption imaging. The resonant ionization spectrum is reported. The setup used in this experiment is suitable not only to investigate mixtures of Bose-Einstein condensates and ions but also for single-atom detection on an atom chip.

  2. Photoionization of Endohedral Atoms: Collective, Reflective and Collateral Emissions

    SciTech Connect

    Chakraborty, Himadri S.; McCune, Matthew A.; Hopper, Dale E.; Madjet, Mohamed E.; Manson, Steven T.

    2009-12-03

    The photoionization properties of a fullerene-confined atom differ dramatically from that of an isolated atom. In the low energy region, where the fullerene plasmons are active, the electrons of the confined atom emerge through a collective channel carrying a significant chunk of plasmon with it. The photoelectron angular distribution of the confined atom however shows far lesser impact of the effect. At higher energies, the interference between two single-electron ionization channels, one directly from the atom and another reflected off the fullerene cage, producuces oscillatory cross sections. But for the outermost atomic level, which transfers some electrons to the cage, oscillations are further modulated by the collateral emission from the part of the atomic charge density transferred to the cage. These various modes of emissions are studied for the photoionization of Ar endohedrally confined in C{sub 60}.

  3. Ultrafast spectroscopy of wavelength-dependent coherent photoionization cross sections of Li2 wave packets in the E1Σg+ state: The role of Rydberg states

    NASA Astrophysics Data System (ADS)

    Uberna, Radoslaw; Amitay, Zohar; Qian, Charles X. W.; Leone, Stephen R.

    2001-06-01

    The significance of Rydberg states in the probing (via ionization) of Li2 wave packets has been studied through quantitative measurements of the relative coherent ionization cross sections in a two-color pump-probe femtosecond experiment. Following the preparation of a single intermediate rovibronic state with a cw laser, a femtosecond pump pulse (around 800 nm) creates a single two-state rotational wave packet by coherent excitation of the E1Σg+ (ν=9; J=27 and 29) states. The wave packet is then probed through ionization using time-delayed, wavelength tunable pulses (in the region 508-690 nm) while the total energy of the system is kept below the dissociation limit of Li2+. The background-free coherent ionization yield (for each probe wavelength) is measured as the relative oscillation amplitude of the single quantum beat time-dependent signal. The experimental results closely follow a relatively simple theoretical model, which is based on the assumption that the coherent ionization predominantly takes place via the excitation of high-n bound singly excited Rydberg states in the ionization continuum converging to the X 2Σg+ ground electronic state of Li2+. The best interpretation is that the high-n Rydberg states (above n˜25) undergo collisional ionization or autoionization and contribute to the measured coherent ionization signal, while the low-n Rydberg states undergo predissociation and do not contribute to the measured signal. An implication of the results is that the final states of the Li2 system, accessed by the above probe pulses, can be better approximated by a corresponding set of isolated discrete levels rather than by a continuum. This conclusion is important to experimental, as well as theoretical, coherent control and wave packet dynamics studies, in particular, when phase- and amplitude-shaped pump and probe pulses are employed. This study is also the first to investigate ionization of lithium dimer slightly below the E 1Σg+ shelf region with

  4. Nonperturbative theory of double photoionization of the hydrogen molecule

    SciTech Connect

    Vanroose, W.; Martin, F.; Rescigno, T.N.; McCurdy, C.W.

    2004-10-01

    We present completely ab initio nonperturbative calculations of the integral and single differential cross sections for double photoionization of H2 for photon energies from 53.9 to 75.7 eV. The method of exterior complex scaling, implemented with B-splines, is used to solve the Schrodinger equation for a correlated continuum wave function corresponding to a single photon having been absorbed by a correlated initial state. The results are in good agreement with experimental integral cross sections.

  5. Differential cross sections of double photoionization of lithium

    SciTech Connect

    Kheifets, A. S.; Fursa, D. V.; Bray, I.; Colgan, J.; Pindzola, M. S.

    2010-08-15

    We extend our previous application of the convergent close-coupling (CCC) and time-dependent close-coupling (TDCC) methods [Phys. Rev. A 81, 023418 (2010)] to describe energy and angular resolved double photoionization (DPI) of lithium at arbitrary energy sharing. By doing so, we are able to evaluate the recoil ion momentum distribution of DPI of Li and make a comparison with recent measurements of Zhu et al. [Phys. Rev. Lett. 103, 103008 (2009)].

  6. Precision measurements on the photoionization of neutral atomic species

    NASA Astrophysics Data System (ADS)

    Stolte, Wayne

    2016-05-01

    In contrast to studies on rare gas atoms, experimental studies of open-shell atoms offers very challenging problems, such as creation of the atom, low signal, purity and stability. Because of this, studies of inner-shell excitations for open shell atoms are limited. In this talk I will discuss precision experimental measurements for photoionization of atomic oxygen, nitrogen, and chlorine over the last two decades on various beamlines at Lawrence Berkeley National Laboratories, Advanced Light Source.

  7. Capillary photoionization: a high sensitivity ionization method for mass spectrometry.

    PubMed

    Haapala, Markus; Suominen, Tina; Kostiainen, Risto

    2013-06-18

    We present a capillary photoionization (CPI) method for mass spectrometric (MS) analysis of liquid and gaseous samples. CPI utilizes a heated transfer capillary with a vacuum ultraviolet transparent MgF2 window, through which vacuum UV light (10 eV) from an external source enters the capillary. The liquid or gaseous sample, together with dopant, is introduced directly into the heated transfer capillary between the atmosphere and the vacuum of the MS. Since the sample is vaporized and photoionized inside the capillary, ion transmission is maximized, resulting in good overall sensitivity for nonpolar and polar compounds. As in atmospheric pressure photoionization, ionization in CPI occurs either by proton transfer or by charge exchange reactions. The feasibility of CPI was demonstrated with selected nonpolar and polar compounds. A particular advantage of CPI is that it enables the analysis of nonvolatile and nonpolar compounds in liquid samples with high ionization efficiency. This is not possible with existing capillary ionization methods. The performance of CPI as an interface between GC and MS and its applicability for the analysis of steroids in biological samples are also demonstrated. The GC-CPI-MS method shows good chromatographic resolution, linearity (R(2) > 0.993), limits of detection (LOD) in the range of 2-6 pg/mL and repeatability of injection with relative standard deviations of 4-15%. PMID:23713722

  8. Sum rules for the polarization correlations in photoionization and bremsstrahlung

    NASA Astrophysics Data System (ADS)

    Pratt, R. H.; Müller, R. A.; Surzhykov, A.

    2016-05-01

    The polarization correlations in doubly differential cross sections are investigated for photoionization and ordinary bremsstrahlung. These correlations describe the polarization transfer between incident light and ejected photoelectrons as well as between an incoming electron beam and bremsstrahlung light, respectively. They are characterized by a set of seven real parameters Ci j. We show that the squares of these parameters are connected by simple "sum rules." These sum rules can be applied for both one-electron systems and also for atoms, if the latter are described within the independent particle approximation. In particular, they are exact in their simplest form (i) for the photoionization of K -, LI ,I I-, and MI ,I I-atomic shells, as well as (ii) for bremsstrahlung in which the electron is scattered into s1 /2 or p1 /2 states, as in the tip (bremsstrahlung) region. Detailed calculations are performed to verify the derived identities and to discuss their possible applications for the analysis of modern photoionization and bremsstrahlung experiments. In particular, we argue that the sum rules may help to determine the entire set of (significant) polarization correlations in the case when not all Ci j are available for experimental observation.

  9. Theoretical photoionization processes for aluminum-like P2+

    NASA Astrophysics Data System (ADS)

    Wang, HongBin; Jiang, Gang; Duan, Jie

    2016-05-01

    The theoretical photoionization cross sections for the ground and metastable states of Al-like P2+ are first time investigated in the photon energy range of 30-43.5 eV by the Dirac R-matrix method, and a good agreement between the dipole length and velocity form is achieved. The effects of the partial photoionization on the total PI of ground and metastable states are discussed. Our theoretical results are consistent with the latest experimental measurement, only some discrepancies are found. The channel coupling effects play an important role in the photoionization of Al-like P2+. The resonance energies and quantum defects are obtained, where a comparison between the theoretical and experimental data is made. It is worth noting that the theoretical resonance is as large as 0.28 eV. Our results can serve as a reference to further study the PI of Al-like P2+ in theory and experiment and be regarded as a supplement for Opacity Project TOP base results.

  10. Electron-ion Recombination and Photoionization of P II

    NASA Astrophysics Data System (ADS)

    Nahar, Sultana

    2016-05-01

    Study of the inverse processes of photoionization and electron-ion recombination of P II will be reported. It is a highly reactive ion and has been difficult to detect without detailed information of its interactions. Although a low charged ion, present study shows features in photoionization resulting from relativistic fine structure couplings at low energy region near the ionization threshold of many levels. Unified method under the framework of close coupling approximation and R-matrix method and an extension of Bell and Seaton theory has been used to study the inverse processes. The method gives the level-specific as well as the total recombination rate coefficients which include both the radiative recombination (RR) and dielectronic recombination (DR) in a precise manner. The present results include level specific rates and photoionization cross sections of 475 fine structure levels with n <= 10. Preliminary results on the total recombination rates show considerable interference of RR and DR around 4000 K and a DR peak around 105 K. NSF,DOE,OSC.

  11. Solvent jet desorption capillary photoionization-mass spectrometry.

    PubMed

    Haapala, Markus; Teppo, Jaakko; Ollikainen, Elisa; Kiiski, Iiro; Vaikkinen, Anu; Kauppila, Tiina J; Kostiainen, Risto

    2015-03-17

    A new ambient mass spectrometry method, solvent jet desorption capillary photoionization (DCPI), is described. The method uses a solvent jet generated by a coaxial nebulizer operated at ambient conditions with nitrogen as nebulizer gas. The solvent jet is directed onto a sample surface, from which analytes are extracted into the solvent and ejected from the surface in secondary droplets formed in collisions between the jet and the sample surface. The secondary droplets are directed into the heated capillary photoionization (CPI) device, where the droplets are vaporized and the gaseous analytes are ionized by 10 eV photons generated by a vacuum ultraviolet (VUV) krypton discharge lamp. As the CPI device is directly connected to the extended capillary inlet of the MS, high ion transfer efficiency to the vacuum of MS is achieved. The solvent jet DCPI provides several advantages: high sensitivity for nonpolar and polar compounds with limit of detection down to low fmol levels, capability of analyzing small and large molecules, and good spatial resolution (250 μm). Two ionization mechanisms are involved in DCPI: atmospheric pressure photoionization, capable of ionizing polar and nonpolar compounds, and solvent assisted inlet ionization capable of ionizing larger molecules like peptides. The feasibility of DCPI was successfully tested in the analysis of polar and nonpolar compounds in sage leaves and chili pepper. PMID:25715054

  12. Interchannel coupling effects in the valence photoionization of SF6

    NASA Astrophysics Data System (ADS)

    Jose, J.; Lucchese, R. R.; Rescigno, T. N.

    2014-05-01

    The complex Kohn and polyatomic Schwinger variational techniques have been employed to illustrate the interchannel coupling correlation effects in the valence photoionization dynamics of SF6. Partial photoionization cross sections and asymmetry parameters of six valence subshells (1t1g, 5t1u, 1t2u, 3eg, 1t2g, 4t1u) are discussed in the framework of several theoretical and experimental studies. The complex Kohn results are in rather good agreement with experimental results, indicative of the fact that the interchannel coupling effects alter the photoionization dynamics significantly. We find that the dominant effect of interchannel coupling is to reduce the magnitude of shape resonant cross sections near the threshold and to induce resonant features in other channels to which resonances are coupled. The long-standing issue concerning ordering of the valence orbitals is addressed and confirmed 4t1u61t2g63eg4(5t1u6+1t2u6) 1t1g6 as the most likely ordering.

  13. Photoelectron wave function in photoionization: plane wave or Coulomb wave?

    PubMed

    Gozem, Samer; Gunina, Anastasia O; Ichino, Takatoshi; Osborn, David L; Stanton, John F; Krylov, Anna I

    2015-11-19

    The calculation of absolute total cross sections requires accurate wave functions of the photoelectron and of the initial and final states of the system. The essential information contained in the latter two can be condensed into a Dyson orbital. We employ correlated Dyson orbitals and test approximate treatments of the photoelectron wave function, that is, plane and Coulomb waves, by comparing computed and experimental photoionization and photodetachment spectra. We find that in anions, a plane wave treatment of the photoelectron provides a good description of photodetachment spectra. For photoionization of neutral atoms or molecules with one heavy atom, the photoelectron wave function must be treated as a Coulomb wave to account for the interaction of the photoelectron with the +1 charge of the ionized core. For larger molecules, the best agreement with experiment is often achieved by using a Coulomb wave with a partial (effective) charge smaller than unity. This likely derives from the fact that the effective charge at the centroid of the Dyson orbital, which serves as the origin of the spherical wave expansion, is smaller than the total charge of a polyatomic cation. The results suggest that accurate molecular photoionization cross sections can be computed with a modified central potential model that accounts for the nonspherical charge distribution of the core by adjusting the charge in the center of the expansion. PMID:26509428

  14. Photoionization Modeling and the K Lines of Iron

    NASA Technical Reports Server (NTRS)

    Kallman, T. R.; Palmeri, P.; Bautista, M. A.; Mendoza, C.; Krolik, J. H.

    2004-01-01

    We calculate the efficiency of iron K line emission and iron K absorption in photoionized models using a new set of atomic data. These data are more comprehensive than those previously applied to the modeling of iron K lines from photoionized gases, and allow us to systematically examine the behavior of the properties of line emission and absorption as a function of the ionization parameter, density and column density of model constant density clouds. We show that, for example, the net fluorescence yield for the highly charged ions is sensitive to the level population distribution produced by photoionization, and these yields are generally smaller than those predicted assuming the population is according to statistical weight. We demonstrate that the effects of the many strongly damped resonances below the K ionization thresholds conspire to smear the edge, thereby potentially affecting the astrophysical interpretation of absorption features in the 7-9 keV energy band. We show that the centroid of the ensemble of K(alpha) lines, the K(beta) energy, and the ratio of the K(alpha(sub 1)) to K(alpha(sub 2)) components are all diagnostics of the ionization parameter of our model slabs.

  15. Photoionized Mixing Layer Models of the Diffuse Ionized Gas

    NASA Astrophysics Data System (ADS)

    Binette, Luc; Flores-Fajardo, Nahiely; Raga, Alejandro C.; Drissen, Laurent; Morisset, Christophe

    2009-04-01

    It is generally believed that O stars, confined near the galactic midplane, are somehow able to photoionize a significant fraction of what is termed the "diffuse ionized gas" (DIG) of spiral galaxies, which can extend up to 1-2 kpc above the galactic midplane. The heating of the DIG remains poorly understood, however, as simple photoionization models do not reproduce the observed line ratio correlations well or the DIG temperature. We present turbulent mixing layer (TML) models in which warm photoionized condensations are immersed in a hot supersonic wind. Turbulent dissipation and mixing generate an intermediate region where the gas is accelerated, heated, and mixed. The emission spectrum of such layers is compared with observations of Rand of the DIG in the edge-on spiral NGC 891. We generate two sequence of models that fit the line ratio correlations between [S II]/Hα, [O I]/Hα, [N II]/[S II], and [O III]/Hβ reasonably well. In one sequence of models, the hot wind velocity increases, while in the other, the ionization parameter and layer opacity increase. Despite the success of the mixing layer models, the overall efficiency in reprocessing the stellar UV is much too low, much less than 1%, which compels us to reject the TML model in its present form.

  16. Absolute photoionization cross-section of the propargyl radical

    SciTech Connect

    Savee, John D.; Welz, Oliver; Taatjes, Craig A.; Osborn, David L.; Soorkia, Satchin; Selby, Talitha M.

    2012-04-07

    Using synchrotron-generated vacuum-ultraviolet radiation and multiplexed time-resolved photoionization mass spectrometry we have measured the absolute photoionization cross-section for the propargyl (C{sub 3}H{sub 3}) radical, {sigma}{sub propargyl}{sup ion}(E), relative to the known absolute cross-section of the methyl (CH{sub 3}) radical. We generated a stoichiometric 1:1 ratio of C{sub 3}H{sub 3} : CH{sub 3} from 193 nm photolysis of two different C{sub 4}H{sub 6} isomers (1-butyne and 1,3-butadiene). Photolysis of 1-butyne yielded values of {sigma}{sub propargyl}{sup ion}(10.213 eV)=(26.1{+-}4.2) Mb and {sigma}{sub propargyl}{sup ion}(10.413 eV)=(23.4{+-}3.2) Mb, whereas photolysis of 1,3-butadiene yielded values of {sigma}{sub propargyl}{sup ion}(10.213 eV)=(23.6{+-}3.6) Mb and {sigma}{sub propargyl}{sup ion}(10.413 eV)=(25.1{+-}3.5) Mb. These measurements place our relative photoionization cross-section spectrum for propargyl on an absolute scale between 8.6 and 10.5 eV. The cross-section derived from our results is approximately a factor of three larger than previous determinations.

  17. Neon Photoionization Experiments Driven By Z-Pinch Radiation

    NASA Astrophysics Data System (ADS)

    Bailey, J. E.; Cohen, D.; Chandler, G. A.; Cuneo, M. E.; Nash, T. J.; Stygar, W. A.; MacFarlane, J. J.; Jobe, D.; Lake, P.; Nielson, D.; Smelser, R.; Foord, M. E.; Heeter, R. F.; Liedahl, D. A.

    2000-10-01

    Present-day Z-pinch experiments generate 2 x 1021 erg/s, 5 nsec duration x-ray bursts that provide new possibilities to study radiation-heated matter. We are using this source to investigate plasmas in which photoionization dominates collisional ionization. Spectroscopic measurements of such plasmas can serve to benchmark photoionized-plasma atomic physics models that will be used to interpret data from the new generation of x-ray satellite spectrographs. This should be useful for understanding accretion-powered objects such as X-ray binaries and active galactic nuclei. These objects are frequently observed, but the interpretation of their spectra is difficult: state-of-the-art models for photoionized plasmas do not always agree on the expected ionization distribution. Our experiments use a 1-cm-scale gas cell to expose various gases to an x-ray flux of approximately 3 x 1019 erg/s/cm2. Thin mylar (1.5 micron) windows allow the radiation to flow into the cell. The ionization is monitored using emission and absorption spectroscopy. In initial experiments we acquired an absorption spectrum from Li- and He-like Ne. Analysis of the measurements and comparison with computer simulations are in progress. Sandia is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the United States Department of Energy under contract DE-AC04-94AL85000

  18. Photoionized Plasmas in the Z Facility and in Astrophysics

    NASA Astrophysics Data System (ADS)

    Mancini, Roberto

    2013-06-01

    Many astrophysical environments such as x-ray binaries, active galactic nuclei, and accretion disks of compact objects have photoionized plasmas. Detailed x-ray spectral observations performed with the Chandra and XMM-Newton orbiting telescopes provide critical information on the state of photoionized plasmas. However, the complexity of the astrophysical environment makes the spectral analysis challenging, and thus laboratory experiments are important for data interpretation and testing of modeling codes. The Z facility at Sandia National Laboratories is a powerful source of x-rays to produce and study in the laboratory photoionized plasmas relevant for astrophysics under well characterized conditions. We discuss an experimental and theory/modeling effort in which the intense x-ray flux emitted at the collapse of a z-pinch implosion conducted at the Z pulsed-power machine is employed to produce a neon photoionized plasma. The broadband x-ray radiation flux from the z-pinch is used to both create the photoionized plasma and provide a source of backlighting photons to study the atomic kinetics through K-shell line absorption spectroscopy. The plasma is contained in a cm-scale gas cell that can be located at different distances from the z-pinch, thus effectively controlling the x-ray flux producing the plasma. Time-integrated and gated transmission spectra are recorded with a spectrometer equipped with two elliptically-bent KAP crystals and a set of slits to record up to six spatially-resolved spectra per crystal in the same shot. The transmission data shows a rich line absorption spectrum that spans over several ionization stages of neon including Be-, Li-, He- and H-like ions. Modeling calculations are used to interpret the transmission spectra recorded in the Z experiments with the goal of extracting the charge- state distribution, electron temperature and the radiation flux driving the plasma, as well as to determine the ionization parameter of the plasma. This

  19. Fragmentation of doubly charged ammonia cations NH{3/++} studied by the photoion-photoion coincidence (PIPICO) method

    NASA Astrophysics Data System (ADS)

    Winkoun, D.; Dujardin, G.

    1986-03-01

    Doubly charged NH{3/++} cations were produced by double photoionization of neutral ammonia molecules by using the synchrotron radiation from ACO as a photon source of variable energy in the 35 49 eV energy range. The fragmentation of NH{3/++} was studied by the photoion-photoion coincidence (PIPICO) method. NH{3/++} cations were produced in thetilde X^1 A 1 andtilde B^1 electronic states of which the onset energies were measured at, respectively, 35.4±0.5 eV and 44.5±0.5 eV. It was shown that the NH{3/++} ions, initially produced in theirtilde X^1 A 1 state, rapidly dissociate (in less than 50 ns), into NH{2/+} + H+. Furthermore, the comparison with results obtained by other methods indicates that NH{3/++} ions can either be long-lived (τ>10 µs) or slowly dissociating (1 µs<τ<10 µs) or rapidly dissociating (τ<50 ns), depending on their geometry and/or internal energy in theirtilde X^1 E A 1 electronic state.

  20. Programmable femtosecond laser pulses in the ultraviolet

    SciTech Connect

    Hacker, M.; Feurer, T.; Sauerbrey, R.; Lucza, T.; Szabo, G.

    2001-06-01

    Using a combination of a zero-dispersion compressor and spectrally compensated sum-frequency generation, we have produced amplitude-modulated femtosecond pulses in the UV at 200 nm. {copyright} 2001 Optical Society of America

  1. 2 micron femtosecond fiber laser

    DOEpatents

    Liu, Jian; Wan, Peng; Yang, Lihmei

    2014-07-29

    Methods and systems for generating femtosecond fiber laser pulses are disclose, including generating a signal laser pulse from a seed laser oscillator; using a first amplifier stage comprising an input and an output, wherein the signal laser pulse is coupled into the input of the first stage amplifier and the output of the first amplifier stage emits an amplified and stretched signal laser pulse; using an amplifier chain comprising an input and an output, wherein the amplified and stretched signal laser pulse from the output of the first amplifier stage is coupled into the input of the amplifier chain and the output of the amplifier chain emits a further amplified, stretched signal laser pulse. Other embodiments are described and claimed.

  2. High energy femtosecond pulse compression

    NASA Astrophysics Data System (ADS)

    Lassonde, Philippe; Mironov, Sergey; Fourmaux, Sylvain; Payeur, Stéphane; Khazanov, Efim; Sergeev, Alexander; Kieffer, Jean-Claude; Mourou, Gerard

    2016-07-01

    An original method for retrieving the Kerr nonlinear index was proposed and implemented for TF12 heavy flint glass. Then, a defocusing lens made of this highly nonlinear glass was used to generate an almost constant spectral broadening across a Gaussian beam profile. The lens was designed with spherical curvatures chosen in order to match the laser beam profile, such that the product of the thickness with intensity is constant. This solid-state optics in combination with chirped mirrors was used to decrease the pulse duration at the output of a terawatt-class femtosecond laser. We demonstrated compression of a 33 fs pulse to 16 fs with 170 mJ energy.

  3. Photoemission using femtosecond laser pulses

    SciTech Connect

    Srinivasan-Rao, T.; Tsang, T.; Fischer, J.

    1991-10-01

    Successful operation of short wavelength FEL requires an electron bunch of current >100 A and normalized emittance < 1 mm-mrad. Recent experiments show that RF guns with photocathodes as the electron source may be the ideal candidate for achieving these parameters. To reduce the emittance growth due to space charge and RF dynamics effects, the gun may have to operate at high field gradient (hence at high RF frequency) and a spot size small compared to the aperture. This may necessitate the laser pulse duration to be in the subpicosecond regime to reduce the energy spread. We will present the behavior of metal photocathodes upon irradiation with femtosecond laser beams, comparison of linear and nonlinear photoemission, and scalability to high currents. Theoretical estimate of the intrinsic emittance at the photocathode in the presence of the anomalous heating of the electrons, and the tolerance on the surface roughness of the cathode material will be discussed.

  4. Femtosecond laser breakdown of gases and transparent solid states: ultrafast space-time and spectrum-time resolved diagnostics of multicharged microplasma

    NASA Astrophysics Data System (ADS)

    Garnov, Sergey V.; Bukin, Vladimir V.; Strelkov, Vasily V.; Malyutin, Alexander A.

    2008-10-01

    We present the results of experimental studies of formation and evolution of multiply ionized (multicharged) laser micro-size plasma produced in gases (air, nitrogen, argon and helium) and inside the transparent solids (fused silica) with high intensity (up to ~ 1017 W/cm2), ultrashort (τ ~100 fs), 800nm/400nm laser pulses tightly focused in a region of ~1.5 μm in diameter. The measuring techniques and experimental setups for generation and precise optical diagnostics of laser-induced plasma - pump-probe microinterferometry and ultrafast spectroscopy are described. The measured spatiotemporal distributions of plasma refractive index/electron density and plasma spectra are demonstrated. In the experiments, the main attention was paid to the most intriguing initial stage of ultrafast plasma formation and evolution characterized by strong laser-matter and laser-plasma coupling resulting in efficient photoionization of material and plasma heating. We found out that the almost complete ionization (down to nuclei) of the initial gas occurs even at the initial stage of plasma formation. Besides, it was observed, for the first time, that a characteristic time of laser plasma formation considerably (in times) exceeds the duration of the pump laser pulse. This postionization process is attributed to impact ionization of plasma by hot electrons heated due to inverse bremsstrahlung. A theoretical model describing the mechanism of plasma postionization by hot photoelectrons was proposed. We compare the results of the experiments with what the theory predicts - the results of electron density calculations are in good agreement with the experimental data. The dynamics of plasma emission (spectral continuum and spectral line formation) in UV-visible spectral range was investigated with a picosecond time resolution applying the developed ultrafast streak-camera-based spectrometer. The spatiotemporal distributions of refractive index of laser irradiated fused silica were recorded

  5. Observation and analysis of structural changes in fused silica by continuous irradiation with femtosecond laser light having an energy density below the laser-induced damage threshold.

    PubMed

    Nomura, Wataru; Kawazoe, Tadashi; Yatsui, Takashi; Naruse, Makoto; Ohtsu, Motoichi

    2014-01-01

    The laser-induced damage threshold (LIDT) is widely used as an index for evaluating an optical component's resistance to laser light. However, a degradation in the performance of an optical component is also caused by continuous irradiation with laser light having an energy density below the LIDT. Therefore, here we focused on the degradation in performance of an optical component caused by continuous irradiation with femtosecond laser light having a low energy density, i.e., laser-induced degradation. We performed an in situ observation and analysis of an increase in scattering light intensity in fused silica substrates. In experiments conducted using a pulsed laser with a wavelength of 800 nm, a pulse width of 160 fs and pulse repetition rate of 1 kHz, we found that the scattered light intensity increased starting from a specific accumulated fluence, namely, that the laser-induced degradation had a threshold. We evaluated the threshold fluence F t as 6.27 J/cm(2) and 9.21 J/cm(2) for the fused silica substrates with surface roughnesses of 0.20 nm and 0.13 nm in R a value, respectively, showing that the threshold decreased as the surface roughness increased. In addition, we found that the reflected light spectrum changed as degradation proceeded. We analyzed the details of the degradation by measuring instantaneous reflectance changes with a pump-probe method; we observed an increase in the generation probability of photogenerated carriers in a degraded silica substrate and a damaged silica substrate and observed a Raman signal originating from a specific molecular structure of silica. From these findings, we concluded that compositional changes in the molecular structure occurred during degradation due to femtosecond laser irradiation having an energy density below the LIDT. PMID:25247116

  6. Angular diagram of broadband emission of millimeter-sized water droplets exposed to gigawatt femtosecond laser pulses.

    PubMed

    Geints, Yurii E; Zemlyanov, Alexander A; Kabanov, Andrey M; Bykova, Elena E; Apeksimov, Dmitrii V; Bukin, Oleg A; Sokolova, Ekaterina B; Golik, Sergey S; Ilyin, Aleksey A

    2011-09-20

    We report on the experiments on the interaction of gigawatt femtosecond laser pulses with suspended millimeter-sized water droplets. The transparent droplets experienced laser-induced breakdown and explosive boiling up and emitted a broadband radiation. This radiation covers the spectral range from 450 to 1100 nm and consists of the spectrum of laser pulse scattered and transformed by the droplet due to self-phase modulation and plasma emission produced in water during photoionization. The droplet emission spectrum showed remarkable broadening at all viewing angles and is maximal in the direction of the laser exit from the droplet. The enlargement of the droplet results in additional spectral spreading of the emitted radiation. The depth and amount of laser pulse spectral self-transformations upon propagation through the water droplet are simulated by means of numerical calculations. PMID:21947048

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

    NASA Astrophysics Data System (ADS)

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

    2015-06-01

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

  8. The Photoionized Accretion Disk in Her X-1

    NASA Astrophysics Data System (ADS)

    Ji, L.; Schulz, N.; Nowak, M.; Marshall, H. L.; Kallman, T.

    2009-08-01

    We present an analysis of several high-resolution Chandra grating observations of the X-ray binary pulsar Her X-1. With a total exposure of 170 ks, the observations are separated by years and cover three combinations of orbital and superorbital phases. Our goal is to determine distinct properties of the photoionized emission and its dependence on phase-dependent variations of the continuum. We find that the continua can be described by a partial covering model which above 2 keV is consistent with recent results from Rossi X-Ray Timing Explorer studies and at low energies is consistent with recent XMM-Newton and BeppoSAX studies. Besides a power law with fixed index, an additional thermal blackbody of 114 eV is required to fit wavelengths above 12 Å (~1 keV). We find that likely all the variability is caused by highly variable absorption columns in the range (1-3) × 1023 cm-2. Strong Fe K line fluorescence in almost all observations reveals that dense, cool material is present not only in the outer regions of the disk but interspersed throughout the disk. Most spectra show strong line emission stemming from a photoionized accretion disk corona (ADC). We model the line emission with generic thermal plasma models as well as with the photoionization code XSTAR and investigate changes of the ionization balance with orbital and superorbital phases. Most accretion disk coronal properties such as disk radii, temperatures, and plasma densities are consistent with previous findings for the low state. We find that these properties change negligibly with respect to orbital and superorbital phases. A couple of the higher energy lines exhibit emissivities that are significantly in excess of expectations from a static ADC.

  9. Vacuum ultraviolet photoionization mass spectrometric study of cyclohexene.

    PubMed

    Chen, Jun; Cao, Maoqi; Wei, Bin; Ding, Mengmeng; Shan, Xiaobin; Liu, Fuyi; Sheng, Liusi

    2016-02-01

    In this work, photoionization and dissociation of cyclohexene have been studied by means of coupling a reflectron time-of-flight mass spectrometer with the tunable vacuum ultraviolet (VUV) synchrotron radiation. The adiabatic ionization energy of cyclohexene as well as the appearance energies of its fragment ions C6 H9 (+) , C6 H7 (+) , C5 H7 (+) , C5 H5 (+) , C4 H6 (+) , C4 H5 (+) , C3 H5 (+) and C3 H3 (+) were derived from the onset of the photoionization efficiency (PIE) curves. The optimized structures for the transition states and intermediates on the ground state potential energy surfaces related to photodissociation of cyclohexene were characterized at the ωB97X-D/6-31+g(d,p) level. The coupled cluster method, CCSD(T)/cc-pVTZ, was employed to calculate the corresponding energies with the zero-point energy corrections by the ωB97X-D/6-31+g(d,p) approach. Combining experimental and theoretical results, possible formation pathways of the fragment ions were proposed and discussed in detail. The retro-Cope rearrangement was found to play a crucial role in the formation of C4 H6 (+) , C4 H5 (+) and C3 H5 (+) . Intramolecular hydrogen migrations were observed as dominant processes in most of the fragmentation pathways of cyclohexene. The present research provides a clear picture of the photoionization and dissociation processes of cyclohexene in the 8- to 15.5-eV photon energy region. Copyright © 2016 John Wiley & Sons, Ltd. PMID:26889934

  10. Photoionization of the excited Na 4d state: Possible confirmation of a zero in the l. -->. l-1 channel

    SciTech Connect

    Msezane, A.Z.; Lahiri, J.; Manson, S.T.

    1986-06-01

    Hartree-Fock calculations of the photoionization cross section of the excited Na 4d state have been performed and compared with experiment. The results indicate an experimental confirmation of a zero in an l..-->..l-1 photoionizing transition.

  11. Ab initio calculations of the photoionization of diatomic molecules

    NASA Astrophysics Data System (ADS)

    Lefebvre-Brion, Helene; Raşeev, Georges

    2003-01-01

    A review is presented of the calculation of photoionization spectra, particularly in the spectral range where electron autoionization of diatomic molecules takes place. In addition to some interesting results obtained over years that compare favourably with experiment, the emphasis here is put on the relation between the methods developed for the calculation of observables associated with the continuum energy spectrum of the electrons and the Alchemy system of programs. This system of programs serves as a basis for initial and intermediate calculations. The examples presented show that diatomic molecules not only in gas phase but also oriented in space or physisorbed at surfaces may be studied readily.

  12. The photoionization spectrum of neutral aluminium, Al I

    NASA Technical Reports Server (NTRS)

    Roig, R. A.

    1975-01-01

    The absorption spectrum of Al I has been studied for the wavelength range 1160 to 2000 A by the flash pyrolysis technique. Wavelengths and derived energy levels are reported for 70 new lines converging on the 3s3p(3)P(0) limits of Al II. The autoionization parameters of the 3p(2)P(0)-3p(2)(2)S doublet have been measured. Good agreement is obtained with the experiment of Kohl and Parkinson and the recent calculation of Le Dourneuf et al. The relative photoionization cross section has been measured in the wavelength region 1200 A to 2000 A.

  13. Molecular photoionization studies of nucleobases and correlated systems

    SciTech Connect

    Poliakoff, Erwin D.

    2015-03-11

    We proposed molecular photoionization studies in order to probe correlated events in fundamental scattering phenomena. In particular, we suggested that joint theoretical-experimental studies would provide a window into the microscopic aspects that are of central importance in AMO and chemical physics generally, and would generate useful data for wide array of important DOE topics, such as ultrafast dynamics, high harmonic generation, and probes of nonadiabatic processes. The unifying theme is that correlations between electron scattering dynamics and molecular geometry highlight inherently molecular aspects of the photoelectron behavior.

  14. Short-time Chebyshev wave packet method for molecular photoionization

    NASA Astrophysics Data System (ADS)

    Sun, Zhaopeng; Zheng, Yujun

    2016-08-01

    In this letter we present the extended usage of short-time Chebyshev wave packet method in the laser induced molecular photoionization dynamics. In our extension, the polynomial expansion of the exponential in the time evolution operator, the Hamiltonian operator can act on the wave packet directly which neatly avoids the matrix diagonalization. This propagation scheme is of obvious advantages when the dynamical system has large Hamiltonian matrix. Computational simulations are performed for the calculation of photoelectronic distributions from intense short pulse ionization of K2 and NaI which represent the Born-Oppenheimer (BO) model and Non-BO one, respectively.

  15. Packet narrowing and quantum entanglement in photoionization and photodissociation

    SciTech Connect

    Fedorov, M.V.; Efremov, M.A.; Kazakov, A.E.; Chan, K.W.; Eberly, J.H.; Law, C.K.

    2004-05-01

    The narrowing of electron and ion wave packets in the process of photoionization is investigated, with the electron-ion recoil taken fully into account. Packet localization of this type is directly related to entanglement in the joint quantum state of the electron and ion, and to Einstein-Podolsky-Rosen localization. Experimental observation of such packet-narrowing effects is suggested via coincidence registration by two detectors, with a fixed position of one and varying position of the other. A similar effect, typically with an enhanced degree of entanglement, is shown to occur in the case of photodissociation of molecules.

  16. A simple photoionization scheme for characterizing electron and ion spectrometers

    NASA Astrophysics Data System (ADS)

    Wituschek, A.; von Vangerow, J.; Grzesiak, J.; Stienkemeier, F.; Mudrich, M.

    2016-08-01

    We present a simple diode laser-based photoionization scheme for generating electrons and ions with well-defined spatial and energetic (≲2 eV) structures. This scheme can easily be implemented in ion or electron imaging spectrometers for the purpose of off-line characterization and calibration. The low laser power ˜1 mW needed from a passively stabilized diode laser and the low flux of potassium atoms in an effusive beam make our scheme a versatile source of ions and electrons for applications in research and education.

  17. Double K-shell photoionization of atomic beryllium

    SciTech Connect

    Yip, F. L.; Martin, F.; McCurdy, C. W.; Rescigno, T. N.

    2011-11-15

    Double photoionization of the core 1s electrons in atomic beryllium is theoretically studied using a hybrid approach that combines orbital and grid-based representations of the Hamiltonian. The {sup 1} S ground state and {sup 1} P final state contain a double occupancy of the 2s valence shell in all configurations used to represent the correlated wave function. Triply differential cross sections are evaluated, with particular attention focused on a comparison of the effects of scattering the ejected electrons through the spherically symmetric valence shell with similar cross sections for helium, representing a purely two-electron target with an analogous initial-state configuration.

  18. K-shell photoionization of multielectron atomic systems

    NASA Technical Reports Server (NTRS)

    Gould, R. J.

    1980-01-01

    A simplified procedure is proposed for calculating the cross section for photoionization from the K-shell for a general atomic system that contains an arbitrary number of outer-shell electrons. The procedure retains the formalism of the one-electron atom case (pure Coulomb-field problem) by determining the effective nuclear charge reduced from Z by 'screening parameters' associated with the other K-shell electron and the outer-bound electrons. The parameters are determined essentially by fitting the atom's radial electric field to Coulomb form at the distance from the nucleus where the integrand of the dipole radial integral is peaked.

  19. Experimental observation of guanine tautomers with VUV photoionization

    SciTech Connect

    Zhou, Jia; Kostko, Oleg; Nicolas, Christophe; Tang, Xiaonan; Belau, Leonid; de Vries, Mattanjah S.; Ahmed, Musahid

    2008-12-01

    Two methods of preparing guanine in the gas phase, thermal vaporization and laser desorption, have been investigated. The guanine generated by each method is entrained in a molecular beam, single photon ionized with tunable VUV synchrotron radiation, and analyzed using reflectron mass spectrometry. The recorded photoionization efficiency (PIE) curves show a dramatic difference for experiments performed via thermal vaporization compared to laser desorption. The calculated vertical and adiabatic ionization energies for the eight lowest lying tautomers of guanine suggest the experimental observations arise from different tautomers being populated in the two different experimental methods.

  20. Photoionization and absorption spectrum of formaldehyde in the vacuum ultraviolet.

    NASA Technical Reports Server (NTRS)

    Mentall, J. E.; Gentieu, E. P.; Krauss, M.; Neumann, D.

    1971-01-01

    The measurements have been conducted in the spectral range from 600 to 2000 A. Integrated oscillator strengths were determined for a number of strong Rydberg transitions above 1200 A. From the photoionization curve the first adiabatic ionization potential was found to be 10.87 plus or minus 0.01 eV. As an aid in interpreting the absorption spectrum, theoretical calculations were made using a single-configuration self-consistent field procedure for the Rydberg states and a model which included mixing between the Rydberg and valence states.