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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.

    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

  7. 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.

  8. 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

  9. 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

  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. 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

  13. 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.

  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

    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

  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

    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

  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

    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.

  16. 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

  17. 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

  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. 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.

  10. 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.

  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. 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).

  11. 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

  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. 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.

  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. 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.

  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. 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.

  12. 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.

  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. 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.

  17. 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

  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. 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.

  20. 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

  1. 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.

  2. 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.

  3. 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.

  4. 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

  5. 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

  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. 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

  10. 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.

  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. 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.

  13. 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.

  14. 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.

  15. 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.

  16. 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

  17. 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.

  18. 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).

  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. 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

  3. 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.

  4. 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.

  5. 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

  6. 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).

  7. 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.

  8. 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

  9. 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.

  10. 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.

  11. 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.

  12. 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.

  13. 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

  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 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.

  3. 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.

  4. 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.

  5. 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

  6. 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.

  7. 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.

  8. 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.

  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. 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.

  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. 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.

  18. 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.

  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. 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

  2. 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.

  3. 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.

  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. 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

  11. 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.

  12. 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

  13. 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.

  14. 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.

  15. 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

  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. 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.

  19. 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

  20. 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.

  1. 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

  2. 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

  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. 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.

  12. 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.

  13. 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.

  14. 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.

  15. 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.

  16. 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.

  17. 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.

  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. 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.

  6. 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).

  7. 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

  8. 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.

  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.

    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

  12. 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.

  13. 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.

  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. 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

  18. 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

  19. 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.

  20. 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.

  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. 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

  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. 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.

  6. 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.

  7. 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.

  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.